F NTG

Research Society㻌➨ 㻠㻢 ᅇ㻌䝣䝷䞊䝺䞁䞉䝘䝜䝏䝳䞊䝤䞉䜾䝷䝣䜵䞁㻌⥲ྜ䝅䞁䝫䝆䜴䝮㻌㼀㼔㼑㻌㻠㻢㼠㼔㻌㻲㼡㼘㼘㼑㼞㼑㼚㼑㼟㻙㻺㼍㼚㼛㼠㼡㼎㼑㼟㻙㻳㼞㼍㼜㼔㼑㼚㼑㻌㻳㼑㼚㼑㼞㼍㼘㻌㻿㼥㼙㼜㼛㼟㼕㼡㼙㻌

 
 

ㅮ₇せ᪨㞟㻌
㻭㼎㼟㼠㼞㼍㼏㼠㼟㻌㻌㻌㻞㻜㻝㻠 ᖺ 㻟 ᭶ 㻟 ᪥䠄᭶䠅䡚㻌 㻡 ᪥䠄Ỉ䠅㻌ᮾி኱Ꮫ㻌 ఀ⸨ᅜ㝿Ꮫ⾡◊✲䝉䞁䝍䞊㻌 ఀ⸨ㅰᜠ䝩䞊䝹㻌㼀㼔㼑㻌㼁㼚㼕㼢㼑㼞㼟㼕㼠㼥㻌㼛㼒㻌㼀㼛㼗㼥㼛㻘㻌㻵㼠㼛㻌㻵㼚㼠㼑㼞㼚㼍㼠㼕㼛㼚㼍㼘㻌㻾㼑㼟㼑㼍㼞㼏㼔㻌㻯㼑㼚㼠㼑㼞㻌㻌୺ദ㻌 䝣䝷䞊䝺䞁䞉䝘䝜䝏䝳䞊䝤䞉䜾䝷䝣䜵䞁Ꮫ఍㻌㼀㼔㼑㻌㻲㼡㼘㼘㼑㼞㼑㼚㼑㼟㻘㻌㻺㼍㼚㼛㼠㼡㼎㼑㼟㻌㼍㼚㼐㻌㻳㼞㼍㼜㼔㼑㼚㼑㻌㻾㼑㼟㼑㼍㼞㼏㼔㻌㻿㼛㼏㼕㼑㼠㼥㻌㻌㻌ඹദ㻌 㻌 ᪥ᮏ໬Ꮫ఍㻌 㻌 㻌 㻌 㻌 㻌 㼀㼔㼑㻌㻯㼔㼑㼙㼕㼏㼍㼘㻌㻿㼛㼏㼕㼑㼠㼥㻌㼛㼒㻌㻶㼍㼜㼍㼚㻌㻶㻿㼀 ᡓ␎ⓗᅜ㝿ඹྠ◊✲䝥䝻䝆䜵䜽䝖 㻵㻾㻱㻺㻭㻌 㻌 㻌 㻵㻾㻱㻺㻭㻌㻼㼞㼛㼖㼑㼏㼠㻌㼎㼥㻌㻶㻿㼀㻙㻱㻯㻌㻰㻳㻌㻾㼀㻰㻘㻌 㻌㻿㼠㼞㼍㼠㼑㼓㼕㼏㻌㻵㼚㼠㼑㼞㼚㼍㼠㼕㼛㼚㼍㼘㻌㻯㼛㼘㼘㼍㼎㼛㼞㼍㼠㼕㼢㼑㻌㻾㼑㼟㼑㼍㼞㼏㼔㻌㻼㼞㼛㼓㼞㼍㼙㻘㻌㻿㻵㻯㻻㻾㻼㻌ᮾி኱Ꮫ 㻳㻹㻿㻵㻌 㻌 㻌 㼀㼔㼑㻌㼁㼚㼕㼢㼑㼞㼟㼕㼠㼥㻌㼛㼒㻌㼀㼛㼗㼥㼛㻌㻳㼞㼍㼐㼡㼍㼠㼑㻌㻼㼞㼛㼓㼞㼍㼙㻌㼒㼛㼞㻌㻹㼑㼏㼔㼍㼚㼕㼏㼍㼘㻌㻿㼥㼟㼠㼑㼙㼟㻌㻵㼚㼚㼛㼢㼍㼠㼕㼛㼚㻌㻌㻌༠㈶㻌 㻌 ᪥ᮏ≀⌮Ꮫ఍㻌 㻌 㻌 㻌 㼀㼔㼑㻌㻼㼔㼥㼟㼕㼏㼍㼘㻌㻿㼛㼏㼕㼑㼠㼥㻌㼛㼒㻌㻶㼍㼜㼍㼚㻌ᛂ⏝≀⌮Ꮫ఍㻌 㻌 㻌 㻌 㼀㼔㼑㻌㻶㼍㼜㼍㼚㻌㻿㼛㼏㼕㼑㼠㼥㻌㼛㼒㻌㻭㼜㼜㼘㼕㼑㼐㻌㻼㼔㼥㼟㼕㼏㼟㻌㧗ศᏊᏛ఍㻌 㻌 㻌 㻌 㻌 㻌 㼀㼔㼑㻌㻿㼛㼏㼕㼑㼠㼥㻌㼛㼒㻌㻼㼛㼘㼥㼙㼑㼞㻌㻿㼏㼕㼑㼚㼏㼑㻘㻌㻶㼍㼜㼍㼚㻌㟁Ẽ໬Ꮫ఍㻌 㻌 㻌 㻌 㻌 㻌 㼀㼔㼑㻌㻱㼘㼑㼏㼠㼞㼛㼏㼔㼑㼙㼕㼏㼍㼘㻌㻿㼛㼏㼕㼑㼠㼥㻌㼛㼒㻌㻶㼍㼜㼍㼚㻌インテル® シミュレーションを高速化

Parallel Studio XE 2013

高速化のための Fortran、C/C++ コンパイラー、性能解析ツール、パフォーマンス・ライブラリーなどが同梱された総合開発ツールです。 最新のプロセッサーや、インテル® Xeon Phi™ コプロ
セッサーに対応した高速なアプリケーションを開発することができます。

[ 主なバンドル製品 ]インテル® Composer XE 2013 マルチコア / メニーコア・プロセッサーの性能を最大限に引き出せるように、最適化されたバイナリーを生成する Fortran、C/C++ コンパイラー
 BLAS、LAPACK、高速フーリエ変換などを含む、最適化、並列化済みの数値
演算ライブラリー

インテル® VTune™ Amplifier XE 2013
数クリックのみでパフォーマンス問題の原因を特定できるマルチスレッド対応分析ツール

インテル® Inspector XE 2013
メモリーリーク、メモリー破壊、データ競合、デッドロックなどの問題を素早く検出する、
マルチスレッド・エラー / メモリーエラー検出ツール

インテル® Advisor XE 2013
マルチスレッド化の候補を見つけ出し、効果予測や問題の診断を行える並列化と高速化のアドバイスツール

性能に関するテストに使用されるソフトウェアとワークロードは、性能がインテル® マイクロプロセッサー用に最適化されていることがあります。SYSmark* や MobileMark* などの性能テストは、特定のコンピューター・システム、コンポーネント、ソフトウェア、操作、機能に基づいて行ったものです。結果はこれらの要因によって異なります。製品の購入を検討される場合は、他の製品と組み合わせた場合の本製品の性能など、ほかの情報や性能テストも参考にして、パフォーマンスを総合的に評価することをお勧めします。
Intel、インテル、Intel ロゴ、Cilk、Intel Core、VTune は、アメリカ合衆国および / またはその他の国における Intel Corporation の商標です。Windows、Visual Studio は、米国 Microsoft Corporation および / またはその関連会社の商標です。
* その他の社名、製品名などは、一般に各社の表示、商標または登録商標です。
最適化に関する注意事項 : インテル® コンパイラーは、互換マイクロプロセッサー向けには、インテル製マイクロプロセッサー向けと同等レベルの最適化が行われない可能性があります。 これには、インテル® ストリーミング SIMD 拡張命令 2 (インテル® SSE2)、インテル® ストリー
ミング SIMD 拡張命令 3 (インテル® SSE3)、ストリーミング SIMD 拡張命令 3 補足命令 (SSSE3) 命令セットに関連する最適化およびその他の最適化が含まれます。インテルでは、インテル製ではないマイクロプロセッサーに対して、最適化の提供、機能、効果を保証していません。
本製品のマイクロプロセッサー固有の最適化は、インテル製マイクロプロセッサーでの使用を目的としています。インテル® マイクロアーキテクチャーに非固有の特定の最適化は、インテル製マイクロプロセッサー向けに予約されています。この注意事項の適用対象である特定の命令セットの詳細は、該当する製品のユーザー・リファレンス・ガイドを参照してください。
改訂 #20110804

無料評価版はこちら

http://www.xlsoft.com/intel

製品の詳細に関するお問い合わせ先 :〒 108-0073 東京都港区三田 3-9-9 森伝ビル 6F
Tel: 03-5440-7875 Fax: 03-5440-7876 E-mail: intel@xlsoft.com
インテル® ソフトウェア製品のパフォーマンス / 最適化に関する詳細は、http://software.intel.com/en-us/articles/optimization-notice/#opt-jp を参照してください。
Intel、インテル、Intel ロゴ、Intel Xeon Phi、VTune は、アメリカ合衆国および / またはその他の国における Intel Corporation の商標です。* その他の社名、製品名などは、一般に各社の表示、商標または登録商標です。Ⓒ 2014 Intel Corporation. 無断での引用、転載を禁じます。
XLsoft のロゴ、XLsoft は XLsoft Corporation の商標です。Copyright Ⓒ 2014 XLsoft Corporation.

Contents
Time Table ࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭ i
Chairperson ࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭iii
Program   Japanese ࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭ iv
English ࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭ xix
Abstracts
Plenary Lecture, Special Lecture ࣭࣭࣭ 1
General Lecture ࣭࣭࣭࣭࣭࣭࣭࣭࣭ 9
Poster Preview ࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭43
Author Index ࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭193┠ḟ᪩ぢ⾲ ࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭ iᗙ㛗୍ぴ࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭iii
ࣉࣟࢢ࣒ࣛ ࿴ᩥ࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭ iv
ⱥᩥ࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭ xix
ㅮ₇ண✏  ᇶㄪㅮ₇࣭≉ูㅮ₇࣭࣭࣭࣭࣭࣭࣭࣭ 1୍⯡ㅮ₇࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭ 9
࣏ࢫࢱ࣮Ⓨ⾲࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭43Ⓨ⾲⣴ᘬ࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭࣭ 193

䚷䝥䝻䜾䝷䝮᪩ぢ⾲䠏᭶䠏᪥䚷䠄᭶䠅䠏᭶䠐᪥䚷䠄ⅆ䠅䠏᭶䠑᪥䚷䠄Ỉ䠅ཷ௜㛤ጞ䚷䠔䠖䠏䠌䡚ཷ௜㛤ጞ䚷䠔䠖䠏䠌䡚ㅮ₇㛤ጞ䚷䠕䠖䠌䠌䡚ཷ௜㛤ጞ䚷䠔䠖䠏䠌䡚ㅮ₇㛤ጞ䚷䠕䠖䠌䠌䡚ㅮ₇㛤ጞ䚷䠕䠖䠏䠌䡚㻥㻦㻟㻜 ᇶㄪㅮ₇䚷䠄బ䚻ᮌᖿኵ䠅㻌㻥㻦㻟㻜㻙㻝㻜㻦㻜㻜㻝㻜㻦㻜㻜୍⯡ㅮ₇䚷㻟௳㻔䝣䝷䞊䝺䞁䞉㔠ᒓෆໟ䝣䝷䞊䝺䞁䞉䝣䝷䞊䝺䞁䛾ᛂ⏝㻕㻌㻌㻝㻜㻦㻜㻜㻙㻝㻜㻦㻠㻡

㻝㻜㻦㻠㻡
㻝㻝㻦㻜㻜
㻝㻝㻦㻟㻜

ఇ᠁㻌㻌㻝㻜㻦㻠㻡㻙㻝㻝㻦㻜㻜≉ูㅮ₇䚷㻔㇏ᅧఙဢ㻕㻝㻝㻦㻜㻜㻙㻝㻝㻦㻟㻜୍⯡ㅮ₇䚷㻞௳㻥㻦㻜㻜㻥㻦㻟㻜㻔䝘䝜䝏䝳䞊䝤䛾⏕ᡂ䛸⢭〇䠅㻌

㻝㻟㻦㻝㻡
㻝㻟㻦㻠㻡

㻝㻠㻦㻠㻡

㻝㻡㻦㻠㻡

᫨㣗
䠄ᖿ஦఍䠅
㻝㻞㻦㻜㻜㻙㻝㻟㻦㻝㻡≉ูㅮ₇䚷㻔ୖ㔝ၨྖ㻕㻝㻟㻦㻝㻡㻙㻝㻟㻦㻠㻡୍⯡ㅮ₇䚷㻠௳㻔䜾䝷䝣䜵䞁䛾ᛂ⏝䞉䚷䚷䜾䝷䝣䜵䞁䛾≀ᛶ㻕㻌㻌㻝㻟㻦㻠㻡㻙㻝㻠㻦㻠㻡䝫䝇䝍䞊䝥䝺䝡䝳䞊䚷㻔㻌㻝㻼㻙㻝䚷䡚䚷㻝㻼㻙㻡㻜㻌㻕㻝㻠㻦㻠㻡㻙㻝㻡㻦㻠㻡

㻝㻜㻦㻟㻜
㻝㻜㻦㻠㻡
㻝㻝㻦㻝㻡

㻝㻞㻦㻝㻡

㻝㻤㻦㻜㻜

䝏䝳䞊䝖䝸䜰䝹
ㅮᖌ䠖㻌㻌኱㔝㞝㧗ྡྂᒇ኱Ꮫ㻌෸ᩍᤵ䠄ఀ⸨ㅰᜠ䝩䞊䝹䠅㻝㻤㻦㻜㻜㻙㻝㻥㻦㻟㻜

㻥㻦㻠㻡
㻝㻜㻦㻟㻜
㻝㻜㻦㻠㻡

ᤵ㈹ᘧ
㻝㻟㻦㻟㻜㻙㻝㻠㻦㻝㻡㻝㻠㻦㻝㻡䝫䝇䝍䞊䝥䝺䝡䝳䞊䚷㻔㻌㻞㻼㻙㻝䚷䡚䚷㻞㻼㻙㻡㻜㻌㻕㻝㻠㻦㻝㻡㻙㻝㻡㻦㻝㻡㻝㻡㻦㻝㻡䝫䝇䝍䞊䝉䝑䝅䝵䞁䠄ከ┠ⓗ䝇䝨䞊䝇䠅㻝㻡㻦㻝㻡㻙㻝㻣㻦㻜㻜

㻝㻝㻦㻠㻡

᫨㣗
㻝㻝㻦㻠㻡㻙㻝㻟㻦㻜㻜㻝㻟㻦㻜㻜䝫䝇䝍䞊䝥䝺䝡䝳䞊䚷㻔㻌㻟㻼㻙㻝䚷䡚䚷㻟㻼㻙㻡㻜㻌㻕㻝㻟㻦㻜㻜㻙㻝㻠㻦㻜㻜㻝㻠㻦㻜㻜䝫䝇䝍䞊䝉䝑䝅䝵䞁䠄ከ┠ⓗ䝇䝨䞊䝇䠅㻝㻠㻦㻜㻜㻙㻝㻡㻦㻠㻡㻝㻡㻦㻠㻡≉ูㅮ₇䚷䠄ᑠᯘಇஅ䠅㻝㻡㻦㻠㻡㻙㻝㻢㻦㻝㻡୍⯡ㅮ₇䚷㻡௳㻔䜾䝷䝣䜵䞁䛾≀ᛶ䞉䚷䚷䜾䝷䝣䜵䞁䛾ᛂ⏝䞉䜾䝷䝣䜵䞁⏕ᡂ㻕㻌㻌㻝㻢㻦㻝㻡㻙㻝㻣㻦㻟㻜

㻝㻢㻦㻝㻡

㻝㻣㻦㻟㻜

୍⯡ㅮ₇䚷㻟௳㻔䝘䝜䝏䝳䞊䝤䛾ᛂ⏝㻕㻌㻥㻦㻠㻡㻙㻝㻜㻦㻟㻜ఇ᠁㻌㻌㻝㻜㻦㻟㻜㻙㻝㻜㻦㻠㻡୍⯡ㅮ₇䚷㻠௳㻔䜾䝷䝣䜵䞁䛾ᛂ⏝㻕㻌㻝㻜㻦㻠㻡㻙㻝㻝㻦㻠㻡᫨㣗㻝㻞㻦㻝㻡㻙㻝㻟㻦㻟㻜㻝㻟㻦㻟㻜䝫䝇䝍䞊䝉䝑䝅䝵䞁䠄ከ┠ⓗ䝇䝨䞊䝇䠅㻝㻡㻦㻠㻡㻙㻝㻣㻦㻟㻜ఇ᠁㻌㻌㻝㻣㻦㻟㻜㻙㻝㻤㻦㻜㻜ఇ᠁㻌㻌㻝㻜㻦㻟㻜㻙㻝㻜㻦㻠㻡≉ูㅮ₇䚷㻔ᮏ㛫ⰾ࿴㻕㻝㻜㻦㻠㻡㻙㻝㻝㻦㻝㻡୍⯡ㅮ₇䚷㻠௳㻔䝘䝜䝏䝳䞊䝤䛾⏕ᡂ䛸⢭〇䞉䝘䝜䝏䝳䞊䝤䛾≀ᛶ䞉㻌䝘䝜䝏䝳䞊䝤䛾ᛂ⏝㻕㻌㻌㻝㻝㻦㻝㻡㻙㻝㻞㻦㻝㻡

㻝㻣㻦㻜㻜
㻝㻣㻦㻟㻜

㻥㻦㻜㻜 ᇶㄪㅮ₇㻌㻔㻱㼟㼗㼛㻌㻵㻚㻌㻷㼍㼡㼜㼜㼕㼚㼑㼚㻕㻥㻦㻜㻜㻙㻥㻦㻠㻡㻥㻦㻟㻜㻙㻝㻜㻦㻟㻜

䠄䢁䢅Ⅳ⣲⢏Ꮚ䞉䛭䛾௚䠅㻝㻝㻦㻟㻜㻙㻝㻞㻦㻜㻜㻝㻞㻦㻜㻜≉ูㅮ₇䚷䠄㼅㼍㼚㻌㻸㼕䠅㻥㻦㻜㻜㻙㻥㻦㻟㻜୍⯡ㅮ₇䚷㻠௳≉ูㅮ₇䚷䠄⏣ᓥྑ๪䠅㻝㻣㻦㻜㻜㻙㻝㻣㻦㻟㻜୍⯡ㅮ₇䚷㻠௳㻝㻣㻦㻟㻜㻔䝣䝷䞊䝺䞁䛾໬Ꮫ䞉䝣䝷䞊䝺䞁䛾ᛂ⏝䞉㔠ᒓෆໟ䝣䝷䞊䝺䞁㻕㻝㻤㻦㻟㻜㻝㻣㻦㻟㻜㻙㻝㻤㻦㻟㻜᠓ぶ఍䠄ከ┠ⓗ䝇䝨䞊䝇䠅㻝㻤㻦㻟㻜㻙㻞㻜㻦㻟㻜㻝㻥㻦㻟㻜䚷ᇶㄪㅮ₇䚷Ⓨ⾲䠐䠌ศ䞉㉁␲䠑ศ䚷≉ูㅮ₇䚷Ⓨ⾲䠎䠑ศ䞉㉁␲䠑ศ䚷୍⯡ㅮ₇䚷Ⓨ⾲䠍䠌ศ䞉㉁␲䠑ศ䢊䢛䡹䡼䡬䢈䢛䢖䢇䢚䡩䡬䚷Ⓨ⾲䠍ศ䞉㉁␲䛺䛧
㻞㻜㻦㻟㻜



㼀㼕㼙㼑㻌㼠㼍㼎㼘㼑㻹㼍㼞㼏㼔㻌㻟㻌㻔㻹㼛㼚㻚㻕㻾㼑㼓㼕㼟㼠㼞㼍㼠㼕㼛㼚㻌㼎㼑㼓㼕㼚㼟㻌㼍㼠㻌㻤㻦㻟㻜㻸㼑㼏㼠㼡㼞㼑㼟㻌㼎㼑㼓㼕㼚㻌㼍㼠㻌㻥㻦㻟㻜㻥㻦㻟㻜㻼㼘㼑㼚㼍㼞㼥㻌㻸㼑㼏㼠㼡㼞㼑㻌㻔㻹㼕㼗㼕㼛㻌㻿㼍㼟㼍㼗㼕㻕㻌㻌㻌㻥㻦㻟㻜㻙㻝㻜㻦㻜㻜㻝㻜㻦㻜㻜㻳㼑㼚㼑㼞㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㼟㻌㼇㻟㼉㻔㻲㼡㼘㼘㼑㼞㼑㼚㼑㼟䞉㻱㼚㼐㼛㼔㼑㼐㼞㼍㼘㻌㼙㼑㼠㼍㼘㼘㼛㼒㼡㼘㼘㼑㼞㼑㼚㼑㼟䞉䚷㻭㼜㼜㼘㼕㼏㼍㼠㼕㼛㼚㼟㻌㼛㼒㻌㼒㼡㼘㼘㼑㼞㼑㼚㼑㼟㻕㻌㻌㻝㻜㻦㻜㻜㻙㻝㻜㻦㻠㻡

㻝㻜㻦㻠㻡
㻝㻝㻦㻜㻜

㻯㼛㼒㼒㼑㼑㻌㻮㼞㼑㼍㼗㻌㻝㻜㻦㻠㻡㻙㻝㻝㻦㻜㻜㻿㼜㼑㼏㼕㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㻌㻔㻿㼔㼕㼚㼥㼍㻌㼀㼛㼥㼛㼗㼡㼚㼕㻕㻝㻝㻦㻜㻜㻙㻝㻝㻦㻟㻜㻝㻝㻦㻟㻜㻳㼑㼚㼑㼞㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㼟㻌㼇㻞㼉䠄㻯㼍㼞㼎㼛㼚㻌㼚㼍㼚㼛㼜㼍㼞㼠㼕㼏㼘㼑㼟䞉䚷䚷㻻㼠㼔㼑㼞㻌㼠㼛㼜㼕㼏㼟䠅㻝㻝㻦㻟㻜㻙㻝㻞㻦㻜㻜
㻝㻞㻦㻜㻜
㻸㼡㼚㼏㼔
㻔㻭㼐㼙㼕㼚㼕㼟㼠㼞㼍㼠㼕㼢㼑㻌㼙㼑㼑㼠㼕㼚㼓㻕㻝㻞㻦㻜㻜㻙㻝㻟㻦㻝㻡㻝㻟㻦㻝㻡 㻿㼜㼑㼏㼕㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㻌㻔㻷㼑㼕㼖㼕㻌㼁㼑㼚㼛㻕㻝㻟㻦㻝㻡㻙㻝㻟㻦㻠㻡㻝㻟㻦㻠㻡㻳㼑㼚㼑㼞㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㼟㻌㼇㻠㼉㻌㻌㻔㻭㼜㼜㼘㼕㼏㼍㼠㼕㼛㼚㼟㻌㼛㼒㻌㼓㼞㼍㼜㼔㼑㼚㼑䞉㻼㼞㼛㼜㼑㼞㼠㼕㼑㼟㻌㼛㼒㻌㼓㼞㼍㼜㼔㼑㼚㼑㻕㻌㻌㻝㻟㻦㻠㻡㻙㻝㻠㻦㻠㻡㻝㻠㻦㻠㻡㻼㼛㼟㼠㼑㼞㻌㻼㼞㼑㼢㼕㼑㼣䚷㻔㻌㻝㻼㻙㻝㻌㼠㼔㼞㼛㼡㼓㼔㻌㻝㻼㻙㻡㻜㻌㻕㻝㻠㻦㻠㻡㻙㻝㻡㻦㻠㻡㻝㻡㻦㻠㻡㻸㼑㼏㼠㼡㼞㼑㼟㻌㼎㼑㼓㼕㼚㻌㼍㼠㻌㻥㻦㻜㻜㻸㼑㼏㼠㼡㼞㼑㼟㻌㼎㼑㼓㼕㼚㻌㼍㼠㻌㻥㻦㻜㻜㻥㻦㻜㻜㻼㼘㼑㼚㼍㼞㼥㻌㻸㼑㼏㼠㼡㼞㼑㻌㻔㻱㼟㼗㼛㻌㻵㻚㻌㻷㼍㼡㼜㼜㼕㼚㼑㼚㻕㻥㻦㻜㻜㻙㻥㻦㻠㻡㻥㻦㻠㻡㻳㼑㼚㼑㼞㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㼟㻌㼇㻟㼉㻔㻭㼜㼜㼘㼕㼏㼍㼠㼕㼛㼚㼟㻌㼛㼒㻌㼚㼍㼚㼛㼠㼡㼎㼑㼟㻕㻌㻥㻦㻠㻡㻙㻝㻜㻦㻟㻜㻝㻜㻦㻟㻜 㻯㼛㼒㼒㼑㼑㻌㻮㼞㼑㼍㼗㻌㻝㻜㻦㻟㻜㻙㻝㻜㻦㻠㻡㻝㻜㻦㻠㻡㻳㼑㼚㼑㼞㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㼟㻌㼇㻠㼉㻔㻭㼜㼜㼘㼕㼏㼍㼠㼕㼛㼚㼟㻌㼛㼒㻌㼓㼞㼍㼜㼔㼑㼚㼑㻕㻌㻝㻜㻦㻠㻡㻙㻝㻝㻦㻠㻡㻔㻲㼛㼞㼙㼍㼠㼕㼛㼚㻌㼍㼚㼐㻌㼜㼡㼞㼕㼒㼕㼏㼍㼠㼕㼛㼚㻌㼛㼒㻌㻌㼚㼍㼚㼛㼠㼡㼎㼑㼟㻌䞉㻼㼞㼛㼜㼑㼞㼠㼕㼑㼟㻌㼛㼒㻌㼚㼍㼚㼛㼠㼡㼎㼑㼟䞉㻌㻭㼜㼜㼘㼕㼏㼍㼠㼕㼛㼚㼟㻌㼛㼒㻌㼚㼍㼚㼛㼠㼡㼎㼑㼟㻕㻝㻞㻦㻝㻡㻭㼣㼍㼞㼐㻌㻯㼑㼞㼑㼙㼛㼚㼥㻝㻟㻦㻟㻜㻙㻝㻠㻦㻝㻡㻝㻠㻦㻝㻡㻼㼛㼟㼠㼑㼞㻌㻼㼞㼑㼢㼕㼑㼣䚷㻔㻌㻞㻼㻙㻝㻌㼠㼔㼞㼛㼡㼓㼔㻌㻞㻼㻙㻡㻜㻌㻕㻝㻠㻦㻝㻡㻙㻝㻡㻦㻝㻡㻝㻡㻦㻝㻡㻼㼛㼟㼠㼑㼞㻌㻿㼑㼟㼟㼕㼛㼚㻔㻱㼢㼑㼚㼠㻌㻿㼜㼍㼏㼑㻕㻝㻡㻦㻝㻡㻙㻝㻣㻦㻜㻜

㻝㻣㻦㻟㻜

㻝㻝㻦㻠㻡

㻸㼡㼚㼏㼔
㻝㻝㻦㻠㻡㻙㻝㻟㻦㻜㻜㻝㻟㻦㻜㻜㻼㼛㼟㼠㼑㼞㻌㻼㼞㼑㼢㼕㼑㼣䚷㻔㻌㻟㻼㻙㻝㻌㼠㼔㼞㼛㼡㼓㼔㻌㻟㻼㻙㻡㻜㻌㻕㻝㻟㻦㻜㻜㻙㻝㻠㻦㻜㻜㻝㻠㻦㻜㻜㻼㼛㼟㼠㼑㼞㻌㻿㼑㼟㼟㼕㼛㼚㻔㻱㼢㼑㼚㼠㻌㻿㼜㼍㼏㼑㻕㻝㻠㻦㻜㻜㻙㻝㻡㻦㻠㻡㻌㻌㻝㻝㻦㻝㻡㻙㻝㻞㻦㻝㻡㻸㼡㼚㼏㼔㻝㻞㻦㻝㻡㻙㻝㻟㻦㻟㻜㻝㻟㻦㻟㻜㻼㼛㼟㼠㼑㼞㻌㻿㼑㼟㼟㼕㼛㼚㻔㻱㼢㼑㼚㼠㻌㻿㼜㼍㼏㼑㻕㻝㻡㻦㻠㻡㻙㻝㻣㻦㻟㻜㻯㼛㼒㼒㼑㼑㻌㻮㼞㼑㼍㼗㻌㻝㻣㻦㻟㻜㻙㻝㻤㻦㻜㻜㻹㼍㼞㼏㼔㻌㻡㻌㻔㼃㼑㼐㻚㻕㻾㼑㼓㼕㼟㼠㼞㼍㼠㼕㼛㼚㻌㼎㼑㼓㼕㼚㼟㻌㼍㼠㻌㻤㻦㻟㻜㻥㻦㻜㻜 㻿㼜㼑㼏㼕㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㻌䠄㼅㼍㼚㻌㻸㼕䠅㻌㻥㻦㻜㻜㻙㻥㻦㻟㻜㻥㻦㻟㻜㻳㼑㼚㼑㼞㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㼟㻌㼇㻠㼉㻔㻲㼛㼞㼙㼍㼠㼕㼛㼚㻌㼍㼚㼐㻌㼜㼡㼞㼕㼒㼕㼏㼍㼠㼕㼛㼚㻌㼛㼒㻌㼚㼍㼚㼛㼠㼡㼎㼑㼟䠅㻌㻥㻦㻟㻜㻙㻝㻜㻦㻟㻜㻝㻜㻦㻟㻜 㻯㼛㼒㼒㼑㼑㻌㻮㼞㼑㼍㼗㻌㻝㻜㻦㻟㻜㻙㻝㻜㻦㻠㻡㻝㻜㻦㻠㻡㻿㼜㼑㼏㼕㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㻔㼅㼛㼟㼔㼕㼗㼍㼦㼡㻌㻴㼛㼙㼙㼍㻕㻝㻜㻦㻠㻡㻙㻝㻝㻦㻝㻡㻝㻝㻦㻝㻡㻳㼑㼚㼑㼞㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㼟㻌㼇㻠㼉

㻝㻣㻦㻜㻜
㻝㻣㻦㻟㻜

㻹㼍㼞㼏㼔㻌㻠㻌㻔㼀㼡㼑㻚㻕㻾㼑㼓㼕㼟㼠㼞㼍㼠㼕㼛㼚㻌㼎㼑㼓㼕㼚㼟㻌㼍㼠㻌㻤㻦㻟㻜㻿㼜㼑㼏㼕㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑䠄㼅㼡㼟㼡㼗㼑㻌㼀㼍㼖㼕㼙㼍䠅㻝㻣㻦㻜㻜㻙㻝㻣㻦㻟㻜㻳㼑㼚㼑㼞㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㼟㻌㼇㻠㼉㻝㻡㻦㻠㻡㻿㼜㼑㼏㼕㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑䠄㼀㼛㼟㼔㼕㼥㼡㼗㼕㻌㻷㼛㼎㼍㼥㼍㼟㼔㼕䠅㻝㻡㻦㻠㻡㻙㻝㻢㻦㻝㻡㻝㻢㻦㻝㻡㻳㼑㼚㼑㼞㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㼟㻌㼇㻡㼉㻌㻌㻔㻼㼞㼛㼜㼑㼞㼠㼕㼑㼟㻌㼛㼒㻌㼓㼞㼍㼜㼔㼑㼚㼑䞉䚷㻭㼜㼜㼘㼕㼏㼍㼠㼕㼛㼚㼟㻌㼛㼒㻌㼓㼞㼍㼜㼔㼑㼚㼑䞉㻌㻳㼞㼍㼜㼔㼑㼚㼑㻌㼟㼥㼚㼠㼔㼑㼟㼕㼟㻕㻌㻌㻝㻢㻦㻝㻡㻙㻝㻣㻦㻟㻜㻝㻣㻦㻟㻜㻔㻯㼔㼑㼙㼕㼟㼠㼞㼥㻌㼛㼒㻌㼒㼡㼘㼘㼑㼞㼑㼚㼑㼟䞉㻌㻭㼜㼜㼘㼕㼏㼍㼠㼕㼛㼚㼟㻌㼛㼒㻌㻌㻌㻝㻤㻦㻜㻜㼀㼡㼠㼛㼞㼕㼍㼘
㻸㼑㼏㼠㼡㼞㼑㼞㻦㻌㻌㼅㼡㼠㼍㼗㼍㻌㻻㼔㼚㼛㻌㻺㼍㼓㼛㼥㼍㻌㼁㼚㼕㼢㼑㼞㼟㼕㼠㼥㻔㻵㼠㼛㻌㻴㼍㼘㼘㻕㻝㻤㻦㻜㻜㻙㻝㻥㻦㻟㻜㼒㼡㼘㼘㼑㼞㼑㼚㼑㼟䞉㻌㻱㼚㼐㼛㼔㼑㼐㼞㼍㼘㻌㼙㼑㼠㼍㼘㼘㼛㼒㼡㼘㼘㼑㼞㼑㼚㼑㼟㻕㻝㻤㻦㻟㻜㻝㻣㻦㻟㻜㻙㻝㻤㻦㻟㻜㻮㼍㼚㼝㼡㼑㼠㻌
㻔㻱㼢㼑㼚㼠㻌㻿㼜㼍㼏㼑㻕㻝㻤㻦㻟㻜㻙㻞㻜㻦㻟㻜㻝㻥㻦㻟㻜㻞㻜㻦㻟㻜 㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻼㼘㼑㼚㼍㼞㼥㻌㻸㼑㼏㼠㼡㼞㼑㻦㻌㻠㻜㼙㼕㼚㻌㻔㻼㼞㼑㼟㼑㼚㼠㼍㼠㼕㼛㼚㻕㻌㻗㻌㻡㼙㼕㼚㻌㻔㻰㼕㼟㼏㼡㼟㼟㼕㼛㼚㻕㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻿㼜㼑㼏㼕㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㻦㻌㻌㻞㻡㼙㼕㼚㻌㻔㻼㼞㼑㼟㼑㼚㼠㼍㼠㼕㼛㼚㻕㻌㻗㻌㻡㼙㼕㼚㻌㻔㻰㼕㼟㼏㼡㼟㼟㼕㼛㼚㻕㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻳㼑㼚㼑㼞㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㻦㻌㻝㻜㼙㼕㼚㻌㻔㻼㼞㼑㼟㼑㼚㼠㼍㼠㼕㼛㼚㻕㻌㻗㻌㻡㼙㼕㼚㻌㻔㻰㼕㼟㼏㼡㼟㼟㼕㼛㼚㻕㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻼㼛㼟㼠㼑㼞㻌㻼㼞㼑㼢㼕㼑㼣㻦㻌㻝㼙㼕㼚㻌㻔㻼㼞㼑㼟㼑㼚㼠㼍㼠㼕㼛㼚㻕

ii

ᗙ㛗୍ぴ
㻟᭶㻟᪥㻔᭶䠅

㻔ᩗ⛠␎䠅
᫬䚷䚷䚷㛫

ᗙ䚷䚷䚷㛗

ᇶㄪㅮ₇䠄బ䚻ᮌᖿኵ䠅㻌㻥䠖㻟㻜㻌䡚㻌㻝㻜䠖㻜㻜

⠛ཎ䚷ஂ඾

୍⯡ㅮ₇

㻝㻜䠖㻜㻜㻌䡚㻌㻝㻜䠖㻠㻡ᑠஂಖ䚷◊≉ูㅮ₇䠄㇏ᅧఙဢ䠅㻝㻝䠖㻜㻜䡚㻌㻝㻝䠖㻟㻜‫⏣‮‬ᆏ䚷㞞Ꮚ୍⯡ㅮ₇㻝㻝䠖㻟㻜㻌䡚㻌㻝㻞䠖㻜㻜‫⏣‮‬ᆏ䚷㞞Ꮚ≉ูㅮ₇䠄ୖ㔝ၨྖ䠅㻝㻟䠖㻝㻡㻌䡚㻌㻝㻟䠖㻠㻡㰻⸨䚷⌮୍㑻

୍⯡ㅮ₇㻝㻟䠖㻠㻡㻌䡚㻌㻝㻠䠖㻠㻡⏫⏣䚷཭ᶞ䝫䝇䝍䞊䝥䝺䝡䝳䞊㻝㻠䠖㻠㻡㻌䡚㻌㻝㻡䠖㻠㻡బ⸨䚷೺ኴ㑻
㔝ෆ䚷ு䝏䝳䞊䝖䝸䜰䝹䠄኱㔝㞝㧗䠅㻝㻤䠖㻜㻜㻌䡚㻌㻝㻥䠖㻟㻜

୸ᒣ䚷ⱱኵ

᫬䚷䚷䚷㛫

ᗙ䚷䚷䚷㛗

≉ูㅮ₇㻔㼅㼍㼚㻌㻸㼕䠅㻥䠖㻜㻜㻌䡚㻌㻥䠖㻟㻜

୸ᒣ䚷ⱱኵ

୍⯡ㅮ₇

㻌㻥䠖㻟㻜㻌䡚㻌㻝㻜䠖㻟㻜

༓㊊䚷᪼ᖹ≉ูㅮ₇㻔ᮏ㛫ⰾ࿴䠅㻝㻜䠖㻠㻡㻌䡚㻌㻝㻝䠖㻝㻡

ᒣᮏ䚷㈗༤

୍⯡ㅮ₇

㻝㻝䠖㻝㻡㻌䡚㻌㻝㻞䠖㻝㻡∦ᾆ䚷ᘯ㐨䝫䝇䝍䞊䝥䝺䝡䝳䞊㻝㻠䠖㻝㻡㻌䡚㻌㻝㻡䠖㻝㻡ᐑෆ䚷㞝ᖹ㻟᭶㻠᪥䠄ⅆ䠅ᖹ㔝䚷⠜≉ูㅮ₇㻔⏣ᓥྑ๪䠅㻝㻣䠖㻜㻜㻌䡚㻌㻝㻣䠖㻟㻜

ᯇᑿ䚷㇏

୍⯡ㅮ₇

㻝㻣䠖㻟㻜㻌䡚㻌㻝㻤䠖㻟㻜

ᯇᑿ䚷㇏

᫬䚷䚷䚷㛫

ᗙ䚷䚷䚷㛗

ᇶㄪㅮ₇㻔㻱㼟㼗㼛㻌㻵㻚㻌㻷㼍㼡㼜㼜㼕㼚㼑㼚䠅㻥䠖㻜㻜㻌䡚㻌㻥䠖㻠㻡

኱㔝䚷㞝㧗

୍⯡ㅮ₇

㻌㻥䠖㻠㻡㻌䡚㻌㻝㻜䠖㻟㻜࿃㒓䚷ᾈᶞ୍⯡ㅮ₇䚷䚷䚷䚷䚷䚷䚷䚷䚷㻝㻜䠖㻠㻡㻌䡚㻌㻝㻝䠖㻠㻡➉ᘏ䚷኱ᚿ䝫䝇䝍䞊䝥䝺䝡䝳䞊㻝㻟䠖㻜㻜㻌䡚㻌㻝㻠䠖㻜㻜ᐑ⏣䚷⪔඘㻟᭶㻡᪥䠄Ỉ䠅㛗㇂ᕝ䚷㤾≉ูㅮ₇㻔ᑠᯘಇஅ䠅㻝㻡䠖㻠㻡㻌䡚㻌㻝㻢䠖㻝㻡

㧗஭䚷࿴அ

୍⯡ㅮ₇

㻝㻢䠖㻝㻡㻌䡚㻌㻝㻣䠖㻟㻜

ᒸ⏣䚷᫴

iii

㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䠏᭶䠏᪥㻌䠄᭶䠅㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌ᇶㄪㅮ₇䚷䚷䚷Ⓨ⾲䠎䠑ศ䚷䞉䚷㉁␲ᛂ⟅䠑ศ㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌≉ูㅮ₇䚷䚷䚷Ⓨ⾲䠎䠑ศ䚷䞉䚷㉁␲ᛂ⟅䠑ศ㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌୍⯡ㅮ₇䚷䚷䚷Ⓨ⾲䠍䠌ศ䚷䞉䚷㉁␲ᛂ⟅䠑ศ㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䝫䝇䝍䞊䝥䝺䝡䝳䞊䚷䚷䚷Ⓨ⾲䠍ศ䚷䞉䚷㉁␲ᛂ⟅䛺䛧
ᇶㄪㅮ₇㻌㻌㻔㻥㻦㻟㻜㻙㻝㻜㻦㻜㻜㻕㻝㻿㻙㻝௻ᴗ䛾║䛛䜙ぢ䛯䝘䝜䜹䞊䝪䞁䛾⌧≧䛸ᑗ᮶ᒎᮃ㻝బ䚻ᮌ䚷ᖿኵ

୍⯡ㅮ₇㻌㻌㻔㻝㻜㻦㻜㻜㻙㻝㻜㻦㻠㻡㻕䝣䝷䞊䝺䞁䚷䞉䚷㔠ᒓෆໟ䝣䝷䞊䝺䞁䚷䞉䚷䝣䝷䞊䝺䞁䛾ᛂ⏝㻝㻙㻝㻲㻵㻮㻙㻿㻱㻹䛻䜘䜛㻯㻢㻜䝬䜲䜽䝻䝏䝳䞊䝤䛸㻭㻭㻻⭷᥋ྜ⏺㠃䛾ᵓ㐀ゎᯒ㻥㻌㻖㻌ᐑ⃝㻌⸅୍㻘㻌ୗᮧ㻌࿘୍㻘㻌ⱝཎ㻌Ꮥḟ㻘㻌ᶲ㻌຾

㻝㻙㻞

㻝㻜

༢ཎᏊෆໟ䝣䝷䠉䝺䞁䛾ග㟁Ꮚ䝇䝨䜽䝖䝹㻌㻖㻌ᐑᓮ㻌㝯ᩥ㻘㻌Ύ㔝㻌཭┿㻘㻌㔝⏣㻌⚈Ꮚ㻘㻌ඵᮌ㻌๰㻘㻌⠛ཎ㻌ஂ඾㻘㻌᪥㔝㻌↷⣧㻝㻙㻟䝏䜸䝣䜵䞁ྵ᭷䝣䝷䞊䝺䞁ㄏᑟయ䜢⏝䛔䛯᭷ᶵⷧ⭷ኴ㝧㟁ụ⣲Ꮚ≉ᛶ㻝㻝* ᯘ 㐩ஓ , Lee Heaseong, Im Inseob, Lee Seungjoo, Jang Jin, Pac Chyongjin, ᳃ᒣ ᗈᛮ㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䠚䠚䠚䠚䠚䠚䠚㻌ఇ᠁㻌㻌㻔㻝㻜㻦㻠㻡㻙㻝㻝㻦㻜㻜㻕㻌䠘䠘䠘䠘䠘䠘䠘≉ูㅮ₇㻌㻌㻔㻝㻝㻦㻜㻜㻙㻝㻝㻦㻟㻜㻕㻝㻿㻙㻞ከᒙ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䛻䛚䛔䛶୰⓶⭘Ⓨ䛜䜣䛻㛵䜟䜛㔜せᅉᏊ䛻䛴䛔䛶

㻞

㇏ᅧ䚷ఙဢ

୍⯡ㅮ₇㻌㻌㻔㻝㻝㻦㻟㻜㻙㻝㻞㻦㻜㻜㻕
䝘䝜Ⅳ⣲⢏Ꮚ䚷䞉䚷䛭䛾௚㻝㻙㻠㻝㻞⇿㎘ἲ䝘䝜䝎䜲䝲䝰䞁䝗䛾ศᩓ䠖᭱㏆䛾ᡂᯝ㻌㻖㻌బ䚻ᮌ㻌ಟ୍㻘㻌ᒣ㔝஭㻌ுᏊ㻘㻌኱⃝㻌ᫎ஧㻝㻙㻡」ᩘẁ䝖䝷䝑䝥Ẽ┦⛣ືᗘ㻝㻟ᐃ⿦⨨䛾㛤Ⓨ㻌㻖㻌Ⳣ஭㻌ಇᶞ㻘㻌ᘅⰪ㻌Ὀ♸㻘㻌ぢୖ㻌ோዉᏊ㻘㻌㝕ෆ㻌ᾴኴ㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䠚䠚䠚䠚䠚䠚䠚㻌᫨㣗㻌㻌㻔㻝㻞㻦㻜㻜㻙㻝㻟㻦㻝㻡㻕㻌䠘䠘䠘䠘䠘䠘䠘≉ูㅮ₇㻌㻌㻔㻝㻟㻦㻝㻡㻙㻝㻟㻦㻠㻡㻕㻝㻿㻙㻟䜹䝹䝁䝀䝘䜲䝗⣔ᒙ≧≀㉁䛾ཎᏊ⭷䜶䝺䜽䝖䝻䝙䜽䝇ᛂ⏝

㻟

ୖ㔝䚷ၨྖ

୍⯡ㅮ₇㻌㻌㻔㻝㻟㻦㻠㻡㻙㻝㻠㻦㻠㻡㻕䜾䝷䝣䜵䞁䛾ᛂ⏝䚷䞉䚷䜾䝷䝣䜵䞁䛾≀ᛶ㻝㻙㻢

Vertical transport in meal/2D crystal/graphene layered heterostructures* Yoshihisa Inoue, Takehiro Yamaguchi, Sei Morikawa, Satoru Masubuchi,
Kenji Watanabe, Takashi Taniguchi, Rai Moriya, Tomoki Machida

㻝㻠

㻝㻙㻣

Stabilities and Electronic Structures of Hexagonal Boron-Nitride Bilayers* Yoshitaka Fujimoto, Takashi Koretsune, Susumu Saito㻝㻡

iv㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䠏᭶䠏᪥㻌䠄᭶䠅
㻝㻙㻤

㻝㻙㻥

Effect of Band Nesting on Optical Properties in Two-dimensional Transition Metal
Dichalcogenides㻌㻖㻌ᑠ⃝㻌኱▱㻘㻌 Rajeev Sharma Kumar, Alexandra Carvalho, Amara Kiran Kumar,
Weijie Zhao, Minglin Toh, Ricardo Mendes Ribeiro, Antonio H. Castro Neto, 㻌ᯇ⏣㻌୍ᡂ㻘Ụ⏣㻌๛㍤䝀䞊䝖㟁ᅽ䛻䜘䜛䜾䝷䝣䜵䞁➃䛾ග໬Ꮫ䜶䝑䝏䞁䜾䛾ไᚚ㻝㻢㻝㻣㻌㻖㻌㔝ෆ㻌ு㻘㻌୕Ɫ㻌ఙᙪ㻘㻌ᯇᮏ㻌Ᏺᗈ䝫䝇䝍䞊䝥䝺䝡䝳䞊㻌㻌㻔㻝㻠㻦㻠㻡㻙㻝㻡㻦㻠㻡㻕䝫䝇䝍䞊䝉䝑䝅䝵䞁㻌㻌㻔㻝㻡㻦㻠㻡㻙㻝㻣㻦㻟㻜㻕䚷䚷䚷䚷䠄䖪䠅䚷ⱝᡭዡບ㈹ೃ⿵
䝣䝷䞊䝺䞁䛾໬Ꮫ㻝㻼㻙㻝◲㓟໬䝣䝷䞊䝺䞁䛾ศᏊ㌶㐨ィ⟬䛸⌮ㄽⓗホ౯㻠㻟㻌㻖㻌㔝ᆅ㻌┤ᶞ㻘㻌బ㔝㻌႐❶㻘㻌஭ୖ㻌࿴⨾㻘㻌∦ᒸ㻌ὒྑ㻘㻌⥴᪉㻌ၨ඾㻝㻼㻙㻞

Excited State Electronic Interactions in Push–Pull-Chromophore–[60]Fullerene Conjugates* Michio Yamada, Francesca Tancini, Michael Sekita, Dirk M. Guldi, Mariza N. Alberti,
W. Bernd Schweizer, François Diederich㻠㻠䝣䝷䞊䝺䞁䛾ᛂ⏝㻝㻼㻙㻟㻯㻢㻜㻙㻯㻣㻜䠎ᡂศ䝘䝜䜴䜱䝇䜹䞊䛾ྜᡂ㻠㻡㻌㻖㻌௒㔝㻌ಇ⏕㻘㻌ⱝཎ㻌Ꮥḟ㻘㻌ᐑ⃝㻌⸅୍㻝㻼㻙㻠Transport Characteristics of Fullerene Nano-Whisker Field Effect Transistor using Ionic
Liquid Gate
* Naoto Toriumi, Yoshiaki Ito, Daiki Momiyama, Wataru Akiyama, Naoto Nakamura,
Taishi Takenobu, Jonathan Bird, Yuichi Ochiai, Nobuyuki Aoki㻠㻢㔠ᒓෆໟ䝣䝷䞊䝺䞁䖪

Photoinduced Charge Separation in Supramolecules between Lithium-ion-encapsulated
PCBM Fullerene and Anionic Porphyrins
㻌㻖㻌ᕝᓥ㻌㞝ᶞ㻘㻌኱ஂಖ㻌ᩗ㻘㻌ᒸ⏣㻌ὒྐ㻘㻌ᯇᑿ㻌㇏㻘㻌⚟ఫ㻌ಇ୍㻝㻼㻙㻢✵䝣䝷䞊䝺䞁䛾ศᕸ䛛䜙䜏䛯㔠ᒓෆໟ䝣䝷䞊䝺䞁⏕ᡂ䝯䜹䝙䝈䝮䛾◊✲

㻝㻼㻙㻡

㻠㻣

㻠㻤

㻌㻖㻌ᑠᯘ㻌ᶞ᮶㻘㻌ඤ⋢㻌೺㻘㻌⸨⏣㻌΅㻘㻌⳥ᆅ㻌⪔୍㻘㻌㜿▱Ἴ㻌ὒḟ

䝣䝷䞊䝺䞁
㻝㻼㻙㻣

ỈศᏊ䜢ෆໟ䛧䛯㻯㻢㻜䝎䜲䝬䞊䛾䜶䝛䝹䜼䞊ㄽ㻠㻥㻌㻖㻌㔝ᮧ㻌࿴ဢ㻘㻌ᒸ⏣㻌᫴㻝㻼㻙㻤䖪High-Resolution Transmission Electron Microscopic Study of Electron-Beam-Irradiated C60
Single Crystal Films* Hideki Masuda, Hidehiro Yasuda, Jun Onoe㻡㻜䝘䝜䝏䝳䞊䝤䛾≀ᛶ㻝㻼㻙㻥༢ᒙ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤⭷䛾㟁Ẽఏᑟᛶ䛻䛚䛡䜛㼄⥺↷ᑕ䛾ᙳ㡪㻡㻝㻌㻖㻌Ⲩᮌ㻌ᣅ㤿㻘㻌ᮧୖ㻌ಇஓ㻘㻌ᮌ᭮⏣㻌㈼἞㻘㻌ఀᮾ㻌༓ᑜ

㻝㻼㻙㻝㻜
䖪

ෆ㒊⇕஺᥮ᘧ཯ᛂჾ䜢⏝䛔䛯䝃䝤䝭䝸䝯䞊䝍㛗䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䛾㻌ὶືᒙྜᡂ

㻝㻼㻙㻝㻝

Coherent G-band phonons in single wall carbon nanotubes
㻌㻖㻌䜰䝣䝬䝗㻌䝚䜾䝷䝝㻘㻌䜶䝑䝗䜴䜱㻌䝝䝇䝕䜸㻘㻌㰻⸨㻌⌮୍㑻㻡㻞㻌㻖㻌㝞㻌ᛅ᫂㻘㻌㛗㇂ᕝ㻌㻌㤾㻘㻌㔠㻌ᮾᴿ㻘㻌኱ἑ㻌㻌฼⏨㻘㻌㔝⏣㻌ඃ㻡㻟㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䠏᭶䠏᪥㻌䠄᭶䠅㻝㻼㻙㻝㻞䝥䝻䝢䝹䜰䝭䞁Ꮡᅾୗ䛻䛚䛡䜛㻿㼃㻺㼀㼟䛾ග໬Ꮫⓗᣲື㻡㻠㻌㻖㻌๓⏣䚷㻌ඃ㻘㻌ⶈụ㻌ᝆᖹ㻘㻌ᒣ⏣㻌㐨ኵ㻘㻌㛗㇂ᕝ㻌ṇ㻘㻌㉥㜰㻌೺

㻝㻼㻙㻝㻟
䖪

㓟⣲䝗䞊䝥༢ᒙ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䛻ᑐ䛩䜛䛭䛾ሙ䝣䜷䝖䝹䝭䝛䝑䝉䞁䝇ศග㟁Ẽ໬Ꮫ

㻡㻡

㻝㻼㻙㻝㻠

Far-Infrared and THz Spectroscopy of Multi-Walled Carbon Nanotubes* Keijiro Sakai, Takahiro Morimoto, Toshiya Okazaki

㻡㻢

㻝㻼㻙㻝㻡

Prediction of Redox Potentials of Semiconducting Single-Walled Carbon Nanotubes* Gergely Juhasz, Yasuhiko Hirana, Naotoshi Nakashima

㻡㻣

㻝㻼㻙㻝㻢
䖪

Photoluminescence Spectroelectrochemistry of a Single SWNT Molecule㻌㻖㻌ὥ㻌ὶ㻘㻌ẟ฼㻌┿୍㑻㻘㻌ᐑෆ㻌㞝ᖹ㻘㻌ᯇ⏣㻌୍ᡂ㻘㻌୰ᔱ㻌┤ᩄ

㻡㻤

㻝㻼㻙㻝㻣

Electric Characterization of Chirality Controlled Single-Walled Carbon Nanotubes㻌㻖㻌ὠ⏣㻌ᝆస㻘㻌┦Ⰻ㻌ᣅᐇ㻘㻌ྜྷ⏣㻌ᆂభ㻘㻌▼஭㻌ᏹ἞㻘㻌ᒣᕝ㻌೺୍㻘㻌▮ᓥ㻌༤ᩥ㻘㻌ᒾ⏣㻌ᒎᖾ㻘㻌ᒣᮏ㻌ᐶ㻡㻥㻌㻖㻌ⓑ▼㻌ᬛஓ㻘㻌⛅᭶㻌┤ே㻘㻌ᐑෆ㻌㞝ᖹ㻘㻌ᯇ⏣㻌୍ᡂ㻘㻌୰ᔱ㻌┤ᩄ䝘䝜䝏䝳䞊䝤䛾ᛂ⏝㻝㻼㻙㻝㻤䖪Hydrogen evolution from benzene with single-walled carbon nanotubes as a photocatalyst㻌㻖㻌㧗㔝㻌┤ᶞ㻘㻌኱ஂಖ㻌ᩗ㻘㻌⚟ఫ㻌ಇ୍㻝㻼㻙㻝㻥䝣䝺䜻䝋༳ๅ䝥䝻䝉䝇䛻䜘䜛䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤ⷧ⭷䝖䝷䞁䝆䝇䝍䛾㧗㏿〇㐀ᢏ⾡㻙ᚤ⣽䝖䝑䝥䝀䞊䝖⣲Ꮚ䛾స〇㻙

㻢㻜㻢㻝㻌㻖㻌๓⏣㻌㏔ᙪ㻘㻌ᵽཱྀ㻌೺ኴ㑻㻘㻌ᓊᮏ㻌ⱱ㻘㻌୰ᔱ㻌ຬኴ㻘㻌እᮧ㻌༟ஓ㻘㻌Ṋᒃ㻌ṇྐ㻘㻌⏿㻌ඞᙪ㻘㻌኱㔝㻌㞝㧗

㻝㻼㻙㻞㻜
䖪

㻯㻺㼀䝖䝷䞁䝆䝇䝍ື≉ᛶホ౯

㻢㻞

㻝㻼㻙㻞㻝

㐟ᫍ䝪䞊䝹䝭䝹䞉㻿㻼㻿䜢⏝䛔䛯㻭㼘㻙㻯㻺㼀」ྜయ䛾స〇ཬ䜃≉ᛶホ౯㻌㻖㻌Ẋෆ㻌つஅ㻘㻌㐲⸨㻌ᾈᖾ㻘㻌஧⎼㻌ྐ⾜㻘㻌἟⏣㻌⚽᫛㻘㻌ᶓ⏣㻌▱அ㻘㻌㛵㇂㻌Ẏ㻘㻌ᰁ㇂㻌㝯ኵ㻘㻌┾Ꮚ㻌㝯ᚿ㻢㻟㻌㻖㻌ᚋ⸨㻌໶㻘㻌ᑎᔱ㻌៞㉳㻘㻌㛵ᡞ㻌኱

㻝㻼㻙㻞㻞
䖪
㻝㻼㻙㻞㻟

Multi-walled carbon nanotubes and carbon black supported platinum nanoparticles forcatalyst of polymer electrolyte membrane fuel cells* Zehui Yang, Berber Mohamed, Tsuyohiko Fujigaya, Naotoshi Nakashima㟁⏺ቑᙉຠᯝ䛻䜘䜛㻯㻺㼀ⷧ⭷㟁ᴟ䛛䜙༙ᑟయⷧ⭷䜈䛾ప㟁ᅽ䜻䝱䝸䜰ὀධ㻢㻠㻢㻡㻌㻖㻌ᒣ⏣㻌❳ஓ㻘㻌ᓊᮏ㻌ⱱ㻘㻌኱㔝㻌㞝㧗㻝㻼㻙㻞㻠Highly durable membrane electrode assembly consists of poly(vinylphosphonic acid)polybenzimidazole electrolyte and carbon nanotubes based-electrocatalyst* Mohamed Berber, Tsuyohiko Fujigaya, Naotoshi Nakashima

㻝㻼㻙㻞㻡
䖪

༢ᒙ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䠋䜲䜸䞁ᾮయ䝫䝸䝬䞊䝘䝜䝁䞁䝫䝆䝑䝖䛾ቑᙉ䝊䞊䝧䝑䜽ຠᯝ㻝㻼㻙㻞㻢㼑㻰㻵㻼㻿䛾኱㔞༙㔠ศ㞳䛸㼀㻲㼀䜈䛾ᛂ⏝㻢㻢㻢㻣㻌㻖㻌୰㔝㻌ඖ༤㻘㻌㔝䚻ཱྀ㻌ᩫஅ㻘㻌୰ᔱ㻌⌶ஓ㻘㻌Ἑྜ㻌ኋ㻢㻤㻌⸨஭㻌ಇ἞㑻㻘㻌⏣୰㻌୔ኈ㻘㻌ᮡ⏣㻌▱Ꮚ㻘㻌ὸ㔝㻌ᩄ㻘㻌Ύᐑ㻌⥔᫓㻘㻌ᩪ⸨㻌Ẏ㻘㻌㻖㻌∦ᾆ㻌ᘯ㐨䝘䝜䝏䝳䞊䝤䛾⏕ᡂ䛸⢭〇㻝㻼㻙㻞㻣䠎ᾮ┦ศ㞳䛧䛯༢ᒙ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䛾䝷䝬䞁ศගἲ䛻䜘䜛㔠ᒓ㻛༙ᑟయẚホ౯㻢㻥㻌㔠⃝㻌ᑦᐅ㻘㻌㻖㻌㕥ᮌ㻌ಙ୕㻘㻌⏣୰㻌ඃ㻘㻌ᒣ㷂㻌᫡㻘㻌ᐑᓮ㻌኱㍤㻘㻌ᑠ㔝㻌ᬗ

㻝㻼㻙㻞㻤
䖪

㻣㻜

ᑠᚄ㻿㼃㻯㻺㼀䛾༢୍䜹䜲䝷䝸䝔䜱ศ㞳䛸ග≀ᛶ㻌㻖㻌㨯㻌ᑠᆒ㻘㻌ఀ⸨㻌㟹ᾈ㻘㻌ᖹᕝ㻌⌶ஓ㻘㻌ᖹ㔝㻌⠜㻘㻌⸨஭㻌ಇ἞㑻㻘㻌ᐑෆ㻌㞝ᖹ㻘㻌ᯇ⏣㻌୍ᡂ㻘㻌⏣୰㻌୔ኈ㻘
∦ᾆ㻌ᘯ㐨

vi

㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䠏᭶䠏᪥㻌䠄᭶䠅㻝㻼㻙㻞㻥▷ᑻ໬䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤స〇䛻ྥ䛡䛯㔠ᒓ䝘䝜䝻䝑䝗䛾స〇㻣㻝㻌㻖㻌బ⏣㻌㈗⏕㻘㻌⸨䞄㇂㻌๛ᙪ㻘㻌୰ᔱ㻌┤ᩄ

㻝㻼㻙㻟㻜

㻝㻼㻙㻟㻝
䖪
㻝㻼㻙㻟㻞

Growth of single-walled carbon nanotube from fullerene seeds by chemical vapor deposition
and in situ scanning electron microscopy observation㻌㻖㻌ứ㻌⳹㗓㻘㻌ᒣ⏣㻌༓ᝅ㻘㻌ຍ⸨㻌኱ᶞ㻘㻌ᮏ㛫㻌ⰾ࿴
Rapid separation of high-purity and micrometer-long semiconducting carbon nanotubes by
gel filtration* Boanerges Thendie, Yasumitsu Miyata, Haruka Omachi, Ryo Kitaura, Yuhei Miyauchi,
Kazunari Matsuda, Hisanori Shinohara㧗䝟䝹䝇䜰䞊䜽ᨺ㟁䛾ᅽຊไᚚ䛻䜘䜛஧ᒙ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䛾ຠ⋡ⓗ⏕ᡂ

㻣㻞

㻣㻟

㻣㻠

㻌㻖㻌⳥ᆅ㻌㞙ᩯ㻘㻌ᑎ⏣㻌຾ⱥ㻘㻌Ⳣ஭㻌ಇᶞ㻝㻼㻙㻟㻟㔠ᒓゐ፹㻺㼕㻙㼅䠉㻹㼛䜢⏝䛔䛯༢ᒙ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䠄㻿㼃㻺㼀㼟䠅䛾స〇䛸ホ౯㻣㻡㻌㻖㻌Ꮮ㻌༤㻘㻌஭ୖ㻌ᰤ㻘㻌㕥ᮌ㻌ᬛᏊ㻘㻌ᒣᮏ㻌㝯அ㻘㻌ᰗ㻌ᬛ኱㻘㻌Ᏻ⸨㻌⩏๎㻝㻼㻙㻟㻠㻲㼀㻙㻵㻯㻾㉁㔞ศᯒჾ䜢⏝䛔䛯Ỉ䛚䜘䜃㓟⣲䛸䝁䝞䝹䝖䜽䝷䝇䝍䞊䛾໬Ꮫ཯ᛂ䛾◊✲㻣㻢㻌㻖㻌ᡞᙇ㻌㞝ኴ㻘㻌ᑠ➟ཎ㻌୍ᶞ㻘㻌༓㊊㻌᪼ᖹ㻘㻌୸ᒣ㻌ⱱኵ㻘㻌Ⳣ஭㻌ಇᶞෆໟ䝘䝜䝏䝳䞊䝤
㻝㻼㻙㻟㻡㧗㓄ྥ䞉㧗ᐦᗘ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤⭷䜈䛾䜹䝹䝪䝷䞁ෆໟ㻣㻣㻌㻖㻌⸨⏣㻌㞙㻘㻌஌ᯇ㻌⯟㻘㻌ᴋ㻌⨾ᬛᏊ

㻝㻼㻙㻟㻢
䖪

ᅛᾮ⏺㠃᥋ゐ䜰䞊䜽ᨺ㟁ἲ䛻䜘䜛ᅛ┦ศ㞳䝇䝔䞁䝺䝇ྜ㔠ෆໟ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䛾⏕ᡂ㻝㻼㻙㻟㻣

㏱㐣㟁Ꮚ㢧ᚤ㙾ἲ䛾Ⅽ䛾㧗┿✵ୗ䛻䛚䛡䜛䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤ෆ㒊✵㛫䜈䛾䜺䝇ศᏊ䛾ᑒධἲ㻣㻤㻌㻖㻌┦Ⰻ㻌ᣅஓ㻘㻌⬌᱈㻌⪽㻘㻌ᯇ⏣㻌೺୍㻘㻌㕥ᮌ㻌⸅㻣㻥㻌㻖㻌ᑠᯘ㻌៞ኴ㻘㻌ᩪ⸨㻌Ẏ㻘㻌Ύᐑ㻌⥔᫓㻘㻌ಖ⏣㻌ⱥὒ䝘䝜䝩䞊䞁㻌
㻝㻼㻙㻟㻤

Light-assisted in-situ polymer formation on carbon nanohorns
Mei Yang, * Minfang Zhang, Masao Kunioka, Sumio Iijima, Masako Yudasaka

㻤㻜

㻝㻼㻙㻟㻥

䜹䞊䝪䞁䝘䝜䝩䞊䞁䛻ྵ䜎䜜䜛䜾䝷䝣䜯䜲䝖ᵝ䝅䞊䝖➃㒊䛾㑅ᢥⓗ䜹䝹䝪䜻䝅䝹໬㻤㻝㻌㻖㻌୰ᮧ㻌┿⣖㻘㻌ධỤ㻌㊰Ꮚ㻘㻌ᘪ๐㻌ுኴ㻘㻌ᕷᶫ㻌㗦ஓ㻘㻌㣤ᓥ㻌⃈⏨㻘㻌‫⏣‮‬ᆏ㻌㞞Ꮚ䜾䝷䝣䜵䞁⏕ᡂ㻝㻼㻙㻠㻜㻤㻞䜾䝷䝣䜵䞁䛾䝖䝫䝻䝆䞊ไᚚ䛥䜜䛯ྜᡂἲ㻌㻖㻌஭ୖ㻌㛗୕㻝㻼㻙㻠㻝䖪䜶䝑䝏䞁䜾ᯒฟἲ䛻䜘䜛䜾䝷䝣䜵䞁䛾ㄏ㟁యᇶᯈୖ┤᥋ྜᡂ㻝㻼㻙㻠㻞ᅛయཎᩱ䛸䛧䛶䝔䝖䝷䝣䜵䝙䝹䝫䝹䝣䜱䝸䞁䜢⏝䛔䛯❅⣲䝗䞊䝥䜾䝷䝣䜵䞁䛾㻯㼂㻰ᡂ㛗㻤㻟㻌㻖㻌ᑠᆏ㻌ᫀ㍤㻘㻌㛗㇂ᕝ㻌㤾㻘㻌㔝⏣㻌ඃ㻤㻠㻌㻖㻌ᮡᓮ㻌♸┿㻘㻌໭ᾆ㻌Ⰻ㻘㻌኱⏫㻌㑈㻘㻌⠛ཎ㻌ஂ඾㻝㻼㻙㻠㻟In situ doping of Electrochemical foliation- Mechanism* Shang-Lin Tsai, Mario Hofmann, Ya-Ping Hsieh

㻤㻡

㻝㻼㻙㻠㻠

䝦䝔䝻䜶䝢䝍䜻䝅䝱䝹㻯㼡ୖ䛷䛾㼙㼙䝃䜲䝈䛾䜾䝷䝣䜵䞁䜾䝺䜲䞁䛾㻯㼂㻰ᡂ㛗㻤㻢㻌Ἑཎ㻌᠇἞㻘㻌⚃㏕㻌భ㻘㻌㎷㻌ṇ἞㻘㻌㻖㻌࿃㒓㻌ᾈᶞ

vii㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䠏᭶䠏᪥㻌䠄᭶䠅䜾䝷䝣䜵䞁䛾≀ᛶ
㻝㻼㻙㻠㻡
䖪
㻝㻼㻙㻠㻢

Quantum interference in a ballistic graphene n-p-n junction: from Fabry-Perot to edge
channel interference㻌㻖㻌᳃ᕝ㻌⏕㻘㻌ቑῲ㻌ぬ㻘㻌Ᏺ㇂㻌㢗㻘㻌Ώ㑔㻌㈼ྖ㻘㻌㇂ཱྀ㻌ᑦ㻘㻌⏫⏣㻌཭ᶞ༢ᒙ㑄⛣㔠ᒓ䝎䜲䜹䝹䝁䝀䝘䜲䝗䛻䛚䛡䜛ບ㉳Ꮚᾘ⁛㻤㻣㻤㻤㻌㻖㻌ᑠ㘠㻌ဴ㻘㻌ᒸ⏣㻌᫴

㻝㻼㻙㻠㻣
䖪

༙ᑟయ䜾䝷䝣䜵䞁䝘䝜䝸䝪䞁䛾㟁Ꮚ㍺㏦䛻䛚䛡䜛䜶䝑䝆䝷䝣䝛䝇ຠᯝ㻤㻥㻌㻖㻌㧗ᓥ㻌೺ᝅ㻘㻌⸨஭㻌ᏹṊ㻘㻌ᒣᮏ㻌㈗༤

䛭䛾௚
㻝㻼㻙㻠㻤
䖪

༢ᒙ㼃㻿㼑㻞䛻䛚䛡䜛೫ග䝣䜷䝖䝹䝭䝛䝑䝉䞁䝇䛾

ᗘ౫Ꮡᛶ

㻝㻼㻙㻠㻥

༢ཎᏊᒙ㑄⛣㔠ᒓ䝎䜲䜹䝹䝁䝀䝘䜲䝗䛻䛚䛡䜛㠀⥺ᙧⓎග㻥㻜㻌㻖㻌࿘㻌฼୰㻘㻌ᐑෆ㻌㞝ᖹ㻘㻌ẟ฼㻌┿୍㑻㻘㻌䝖䞊㻌䝭䞁䝸䞁㻘㻌Ụ⏣㻌๛㍤㻘㻌ᯇ⏣㻌୍ᡂ㻥㻝㻌㻖㻌ẟ฼㻌┿୍㑻㻘㻌࿘㻌฼୰㻘㻌ኑ஭㻌భኟ㻘㻌ᐑෆ㻌㞝ᖹ㻘㻌䝖䞊㻌䝭䞁䝸䞁㻘㻌ᑠ㘠㻌ဴ㻘㻌Ụ⏣㻌๛㍤㻘㻌ᒸ⏣㻌᫴㻘
ᯇ⏣㻌୍ᡂ

㻝㻼㻙㻡㻜
䖪

㻯㼂㻰ἲ䜢⏝䛔䛶ྜᡂ䛧䛯༢ᒙ㻹㼛㻿㻞䛾Ⓨගᐃ㻌㻖㻌ኑ஭㻌భኟ㻘㻌ᑠ⃝㻌኱▱㻘㻌ᐑෆ㻌㞝ᖹ㻘㻌ẟ฼㻌┿୍㑻㻘㻌ᯇ⏣㻌୍ᡂ㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䠚䠚䠚䠚䠚䠚䠚㻌ఇ᠁㻌㻌㻔㻝㻣㻦㻟㻜㻙㻝㻤㻦㻜㻜㻕㻌䠘䠘䠘䠘䠘䠘䠘䝏䝳䞊䝖䝸䜰䝹㻌㻌㻔㻝㻤㻦㻜㻜㻙㻝㻥㻦㻟㻜㻕䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤ⷧ⭷䛾䜶䝺䜽䝖䝻䝙䜽䝇ᛂ⏝

኱㔝㻌㞝㧗

viii

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㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䠏᭶䠐᪥㻌䠄ⅆ䠅㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌≉ูㅮ₇䚷䚷䚷Ⓨ⾲䠎䠑ศ䚷䞉䚷㉁␲ᛂ⟅䠑ศ㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌୍⯡ㅮ₇䚷䚷䚷Ⓨ⾲䠍䠌ศ䚷䞉䚷㉁␲ᛂ⟅䠑ศ㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䝫䝇䝍䞊䝥䝺䝡䝳䞊䚷䚷䚷Ⓨ⾲䠍ศ䚷䞉䚷㉁␲ᛂ⟅䛺䛧≉ูㅮ₇㻌㻌㻔㻥㻦㻜㻜㻙㻥㻦㻟㻜㻕㻞㻿㻙㻠Structure and Property Controlled Growth of Single-Walled Carbon Nanotubes on Substrates* Yan Li, Feng Yang, Xiaojun Qin, Fei Peng, Juan Yang㻠୍⯡ㅮ₇㻌㻌㻔㻥㻦㻟㻜㻙㻝㻜㻦㻟㻜㻕䝘䝜䝏䝳䞊䝤䛾⏕ᡂ䛸⢭〇㻞㻙㻝༢ᒙ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤ᡂ㛗䛸ゐ፹཯ᛂ䛾ศᏊ䝅䝭䝳䝺䞊䝅䝵䞁㻝㻤㻌㻖㻌ஂ㛫㻌㤾㻘㻌ᕝ㕥ᮌ㻌ᬛဢ㻘㻌㔝ཱྀ㻌ᣅဢ㻘㻌༓㊊㻌᪼ᖹ㻘㻌ከ⏣㻌᭸ྐ㻘㻌୸ᒣ㻌ⱱኵ

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༙ᑟయ㻯㻺㼀䛾㑅ᢥⓗᡂ㛗䛸䝖䝷䞁䝆䝇䝍≉ᛶ㻌㻖㻌ᱜ஭㻌ಇ௓㻘㻌ᒣ⏣㻌┿ಖ㻘㻌୰ᮧ㻌⣫Ꮚ㻘㻌䝣䝍䝞㻌䝗䞁㻘㻌␊㻌㈼἞

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Low-temperature catalyst activator: Mechanism study of CNT forest densification by “STEP”
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growth method using synchrotron radiation
Akito Takashima, Yudai Izumi, Eiji Ikenaga, Takuo Ohkochi, Masato Kotsugi,
Tomohiro Matsushita, * Takayuki Muro, Akio Kawabata, Tomo Murakami, Mizuhisa Nihei,
Naoki Yokoyama㻔㻡㻘㻡㻕䛚䜘䜃㻔㻢㻘㻡㻕䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䛾ᡂ㛗ᶵᵓ㻞㻝㻌㻖㻌㜿▱Ἴ㻌ὒḟ㻘㻌ඤ⋢㻌೺㻘㻌ᶫᮏ㻌೺ᮁ㻘㻌ᇛ୸㻌᫓ኵ㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䠚䠚䠚䠚䠚䠚䠚㻌ఇ᠁㻌㻌㻔㻝㻜㻦㻟㻜㻙㻝㻜㻦㻠㻡㻕㻌䠘䠘䠘䠘䠘䠘䠘≉ูㅮ₇㻌㻌㻔㻝㻜㻦㻠㻡㻙㻝㻝㻦㻝㻡㻕㻞㻿㻙㻡㻡䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䛾Ỉ䛸䛾┦஫స⏝㻌㻖㻌ᮏ㛫㻌ⰾ࿴㻘㻌༓㊊㻌᪼ᖹ㻘䚷ᒣᮏ㻌㈗༤

୍⯡ㅮ₇㻌㻌㻔㻝㻝㻦㻝㻡㻙㻝㻞㻦㻝㻡㻕䝘䝜䝏䝳䞊䝤䛾⏕ᡂ䛸⢭〇䚷䞉㻌䝘䝜䝏䝳䞊䝤䛾≀ᛶ䚷䞉㻌䝘䝜䝏䝳䞊䝤䛾ᛂ⏝㻞㻙㻡⬺╔ྍ⬟䛺㉸ศᏊᆺྍ⁐໬๣䛻䜘䜛༙ᑟయᛶ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䛾㧗⣧ᗘ⢭〇㻞㻞㻌㻖㻌฼ග㻌ྐ⾜㻘㻌୰ᔱ㻌┤ᩄ㻞㻙㻢The effect of DNA adsorption on optical transitions in single-walled carbon nanotube㻌㻖㻌ఀ⸨㻌㞞ᾈ㻘㻌ఀ⸨㻌ᝆ௓㻘㻌஧஭㻌኱㍜㻘㻌ᱵᮧ㻌࿴ኵ㻘㻌ຍ⸨㻌኱ᶞ㻘㻌ᮏ㛫㻌ⰾ࿴

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䝀䝹䜢⏝䛔䛯༢ᒙ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䛾༙㔠ศ㞳䛾䝯䜹䝙䝈䝮㻞㻠㻌㻖㻌ᖹ㔝㻌⠜㻘㻌⏣୰㻌୔ኈ㻘㻌∦ᾆ㻌ᘯ㐨㻞㻙㻤༙ᑟయ༢ᒙ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䜰䝺䜲స〇䛻ྥ䛡䛯᭷ᶵⷧ⭷୰䛾඲㛗䝤䝺䜲䜽䝎䜴䞁㻌㻖㻌኱ሯ㻌៞࿃㻘㻌஭䝜ୖ㻌Ὀ㍤㻘㻌༓㊊㻌᪼ᖹ㻘㻌୸ᒣ㻌ⱱኵ㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䠚䠚䠚䠚䠚䠚䠚㻌᫨㣗㻌㻌㻔㻝㻞㻦㻝㻡㻙㻝㻟㻦㻟㻜㻕㻌䠘䠘䠘䠘䠘䠘䠘ix㻞㻡㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䠏᭶䠐᪥㻌䠄ⅆ䠅኱⃝㈹䞉㣤ᓥ㈹䞉ⱝᡭዡບ㈹䛾ᤵ㈹ᘧ㻌㻌㻔㻝㻟㻦㻟㻜㻙㻝㻠㻦㻝㻡㻕䝫䝇䝍䞊䝥䝺䝡䝳䞊㻌㻌㻔㻝㻠㻦㻝㻡㻙㻝㻡㻦㻝㻡㻕䝫䝇䝍䞊䝉䝑䝅䝵䞁㻌㻌㻔㻝㻡㻦㻝㻡㻙㻝㻣㻦㻜㻜㻕䚷䚷䚷䚷䠄䖪䠅䚷ⱝᡭዡບ㈹ೃ⿵
䝣䝷䞊䝺䞁䛾໬Ꮫ㻞㻼㻙㻝㼽㻴㻌㻺㻹㻾ศගἲ䛻䜘䜛Ỉ㓟໬䝣䝷䞊䝺䞁ᅛయ䛾ศᏊ䝎䜲䝘䝭䜽䝇䛾ホ౯㻥㻟㻌㻖㻌బ㔝㻌႐❶㻘㻌㤿ሙ㻌ၨ㍜㻘㻌⥴᪉㻌ၨ඾㻞㻼㻙㻞䖪䜿䝖䝷䜽䝍䝮ᵓ㐀䜢䜒䛴᪂䛧䛔㛤ཱྀ㻯㻢㻜ㄏᑟయ䛾ྜᡂ㻥㻠㻌㻖㻌ᶫᕝ㻌⚈ྐ㻘㻌ᮧ⏣㻌⌮ᑦ㻘㻌ⱝᐑ㻌῟ᚿ㻘㻌ᮧ⏣㻌㟹ḟ㑻䝣䝷䞊䝺䞁䛾ᛂ⏝㻞㻼㻙㻟

A Novel Ligand-free ZnO Particle for Fullerene:Polymer Inverted Organic Solar Cell
* IL Jeon, James Ryan, Kee Sheng Yeo, Tafu Nakazaki, Yuichi Negishi, Yutaka Matsuo

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᭷ᶵⷧ⭷ኴ㝧㟁ụ䜈䛾ᛂ⏝䛻ྥ䛡䛯䝁䝞䝹䝖䝆䝏䜸䝺䞁䝣䝷䞊䝺䞁㘒య䛾ྜᡂ㻥㻢㻌㻖㻌ᑠỮ㻌ె♸㻘㻌୰ᕝ㻌㈗ᩥ㻘㻌ᯇᑿ㻌㇏㻞㻼㻙㻡㻯㻢㻜ⷧ⭷䜈䛾ග↷ᑕ䛻䜘䜛ග㔜ྜయ䛾⾲㠃≉ᛶ㻥㻣㻌㻖㻌✝ᒣ㻌⯟㻘㻌⢄ᒣ㻌኱㍤㻘㻌㫽ᾏ㻌┤ே㻘㻌௰ᮧ㻌┤ே㻘㻌ᐑᮏ㻌ඞᙪ㻘㻌ᑿᯇ㻌Ꮥⱱ㻘㻌 Jonathan P Bird 㻘ⴠྜ㻌ຬ୍㻘㻌㟷ᮌ㻌ఙஅ㔠ᒓෆໟ䝣䝷䞊䝺䞁
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Extraction and Isolation of Missing Small-Bandgap Metallofullerenes through Exterior
Functionalization㻌㻖㻌⋤㻌ᚿỌ㻘㻌୰す㻌ຬ௓㻘㻌㔝⏣㻌⚈Ꮚ㻘㻌୹⩚㻌ᏹஅ㻘㻌 ⼇ 㻌 攍 ⱥ㻘㻌໭ᾆ㻌Ⰻ㻘㻌⠛ཎ㻌ஂ඾Supercapacitor using Lithium-Ion Endohedral Metallofullerene* Eunsang Kwon, Ken-ichirou Komatsu, Yoichi Yamada, Yuri Hasegawa, Sho Sato,
Seiji Sakai, Kazuhiko Kawachi, Kuniyoshi Yokoo, Shoichi Ono, Yasuhiko Kasama,
Shinobu Aoyagi, Tomoaki Endo, Tomoyuki Ogawa, Migaku Takahashi

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䝣䝷䞊䝺䞁
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㟁⏺䛻䜘䜛༑㔜௜ຍయ㻯㻢㻜䛾䝇䝢䞁ไᚚ㻝㻜㻜㻌㻖㻌ᡂ⏣㻌ᗣᖹ㻘㻌ᒸ⏣㻌᫴㻞㻼㻙㻥䖪㻯㻟㻞䝫䝸䝬䞊䛾Ᏻᐃᵓ㐀䛸㟁Ꮚ≧ែ㻝㻜㻝㻌㻖㻌୸ᒣ㻌ᐇ㑣㻘㻌ᒸ⏣㻌᫴䝘䝜䝏䝳䞊䝤䛾≀ᛶ㻞㻼㻙㻝㻜㼄⥺↷ᑕ䛻䜘䜛༢ᒙ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䛾㟁Ꮚᵓ㐀ኚ໬㻝㻜㻞㻌㻖㻌ᮧୖ㻌ಇஓ㻘㻌ᒣᮏ㻌ຬᶞ㻘㻌ᯇ⏣㻌඘᫭㻘㻌ᮌ᭮⏣㻌㈼἞㻘㻌すᇉ㻌ᏹ㻘㻌ⶈụ㻌⣖ᖾ㻘㻌᧛☻㻌ᘯ㻘㻌ఀᮾ㻌༓ᑜ㻞㻼㻙㻝㻝༢ᒙ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䛻䛚䛡䜛䝣䜷䝜䞁䛾㠀ㄪ࿴ຠᯝ㻝㻜㻟㻌㻖㻌Ỉ㔝㻌ᑗᚿ㻘㻌㰻⸨㻌⌮୍㑻

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㻿㼃㻺㼀⾲㠃ୖ䛷䛾䝁䞊䝹㓟䝘䝖䝸䜴䝮䛸㻰㻺㻭䛾⨨᥮཯ᛂ䛾ゎᯒ㻌㻖㻌⧰㻌᫂Ꮚ㻘㻌୰ᔱ㻌┤ᩄ㻝㻜㻠㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䠏᭶䠐᪥㻌䠄ⅆ䠅
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Chirality Dependence of Quantum Thermal Transport in Carbon Nanotubes at Low
Temperatures: A First-Principles Study㻌㻖㻌⏿㻌ᬛ⾜㻘㻌Ἑྜ㻌ᏹᶞ㻘㻌኱ᡞ㻌㐩ᙪ㻘㻌ᒣୗ㻌᫭୍༢ᒙ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䛻ෆໟ䛥䛫䛯䜰䞁䝖䝷䜻䝜䞁䛾䝸䝏䜴䝮䜲䜸䞁㟁ụ㟁ᴟ≉ᛶ

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㻌㻖㻌ᕝᓮ㻌᫴ྖ㻘㻌ᯇᾆ㻌ᬛᣅ㻘㻌⏣௦㻌ᗈ♸㻘㻌㻿㼛㼚㼓㻌㻴㼍㼥㼛㼚㼓

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Ỉ⵨Ẽ㞺ᅖẼୗ㻿㼃㻺㼀䛾㻾㻮㻹᣺ືᩘ䛾┤ᚄ౫Ꮡᛶ

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䠬䠨ศගἲ䜢⏝䛔䛯䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤ୖ䛻䛚䛡䜛DNAᵓ㐀ኚ໬䛾䝉䞁䝅䞁䜾㻌㻖㻌ఀ⸨㻌ᝆ௓㻘㻌ఀ⸨㻌㞞ᾈ㻘㻌஧஭㻌኱㍜㻘㻌ຍ⸨㻌኱ᶞ㻘㻌ᱵᮧ㻌࿴ኵ㻘㻌ᮏ㛫㻌ⰾ࿴

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Observation of a gate-induced photoluminescence peak in individual carbon nanotubes* Yuto Ueda, Masahiro Yoshida, Akihiro Ishii, Takushi Uda, Yuichiro K. Kato

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య✚⋡䜢ኚ䛘䛯ᆶ┤㓄ྥ㻿㼃㻺㼀⭷䛾ఏ⇕≉ᛶ㻝㻝㻜㻌㻖㻌ᮏ㛫㻌┤ᶞ㻘㻌༓㊊㻌᪼ᖹ㻘㻌ᮏ㛫㻌ⰾ࿴㻘㻌ᒣᮏ㻌㈗༤

㻌㻖㻌㌴㻌᣺㉪㻘㻌㛗㇂ᕝ㻌㤾㻘㻌༓㊊㻌᪼ᖹ㻘㻌୕ᾆ㻌㣕㫽㻘㻌䜲㻌䝆䝵䞁䝴䞁㻘㻌䝽䞊䝗䝹㻌䝤䝷䜲䜰䞁㻘㻌㔝⏣㻌ඃ㻘ሷぢ㻌῟୍㑻㻘㻌୸ᒣ㻌ⱱኵ䝘䝜䝏䝳䞊䝤䛾ᛂ⏝
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༙⤯⦕ᛶ䝅䝸䝁䞁䜹䞊䝞䜲䝗ୖ䛾㧗ᐦᗘ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䝣䜷䝺䝇䝖䛾㠃ෆ㟁ᑟ㻝㻝㻝㻌㻖㻌✄ⴥ㻌ඃᩥ㻘㻌ᮤ㻌ᬛᏱ㻘㻌㕥ᮌ㻌࿴┿㻘㻌῰㇂㻌ᜨ㻘㻌ᖹᒾ㻌⠜㻘㻌ቑ⏣㻌ె✑㻘㻌஌ᯇ㻌⯟㻘㻌ᴋ㻌⨾ᬛᏊ㻘ᕝཎ⏣㻌ὒ㼚ᆺ༢ᒙ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䛾స〇䛸⇕㟁Ⓨ㟁䝅䞊䝖䜈䛾ᒎ㛤㻝㻝㻞㻌㻖㻌㔝䚻ཱྀ㻌ᩫஅ㻘㻌኱ᶫ㻌㈼ḟ㻘㻌Ἑྜ㻌ኋ㻞㻼㻙㻞㻝䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤㻛䝅䝸䝁䞁䜹䞊䝞䜲䝗⏺㠃䛾᥋ゐ᢬ᢠཬ䜃㻿㼏㼔㼛㼠㼠㼗㼥㞀ቨ㧗䛥䛾ホ౯䖪㻌㻖㻌㕥ᮌ㻌࿴┿㻘㻌✄ⴥ㻌ඃᩥ㻘㻌῰㇂㻌ᜨ㻘㻌ᮤ㻌ᬛᏱ㻘㻌᫂㐨㻌୕✑㻘㻌ᖹᒾ㻌⠜㻘㻌ቑ⏣㻌ె✑㻘㻌஌ᯇ㻌⯟㻘ᴋ㻌⨾ᬛᏊ㻘㻌ᕝཎ⏣㻌ὒ㻞㻼㻙㻞㻞㧗⣧ᗘ༙ᑟయᆺ༢ᒙ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䝛䝑䝖䝽䞊䜽䜢⏝䛔䛯㉥እ⥺䝉䞁䝃䞊

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㻌㻖㻌ᕤ⸨㻌ග㻘㻌ຍ἞㻌⪷ஓ㻘㻌Ἑྜ㻌ⱥ㍤㻘㻌➉ᘏ㻌኱ᚿ㻘㻌ᰗ㻌࿴ᏹ㻞㻼㻙㻞㻟䝥䝷䝇䝏䝑䜽ᇶᯈୖ䛻స〇䛧䛯䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤㞟✚ᅇ㊰䛾ືస㏿ᗘྥୖ䖪㻌㻖㻌୕ၿ㻌฼ᛅ㻘㻌䜹䝇䜿䝷㻌䜰䞁䝔䜱㻘㻌䝷䜲䝩㻌䝟䝖䝸䝑䜽㻘㻌䝘䝅䝤䝸䞁㻌䜰䝹䝞䞊䝖㻘㻌ᓊᮏ㻌ⱱ㻘䜹䜴䝢䝛䞁㻌䜶䝇䝁㻘㻌኱㔝㻌㞝㧗㻞㻼㻙㻞㻠✵㛫㑅ᢥ㻯㼟ෆໟ㻿㼃㻺㼀㼟ⷧ⭷䛻䜘䜛㼜㼚䝩䝰᥋ྜ䛾ග㉳㟁ຊ≉ᛶ

㻝㻝㻡

㻝㻝㻢

㻌㻖㻌Ᏻᙪ㻌჆ᾈ㻘㻌ຍ⸨㻌ಇ㢧㻘㻌㉥㛫㻌ಇ⣖㻘㻌␊ᒣ㻌ຊ୕㻘㻌㔠Ꮚ㻌ಇ㑻

㻞㻼㻙㻞㻡
䖪
㻞㻼㻙㻞㻢

㻞㻼㻙㻞㻣

㔠ᒓᛶ䚸༙ᑟయᛶ༢ᒙ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䜈䛾ศᏊㄆ㆑㻝㻝㻣㻌㻖㻌㯤㻌ᩥ䝅䞁㻘㻌⸨䞄㇂㻌๛ᙪ㻘㻌୰ᔱ㻌┤ᩄ

High Photovoltaic Performance of MoO3-doped Single-walled Carbon Nanotube/Si Solar
Cells* Feijiu Wang, Daichi Kozawa, Yuhei Miyauchi, Shinichiro Mouri, Yutaka Ohno,
Kazunari Matsuda
Solubility control of SWCNTs by using photofunctional dispersants㻌㻖㻌ᯇ⃝㻌ὒᏊ㻘㻌㧗⏣㻌⿱Ꮚ㻘㻌ᮌཎ㻌⚽ඖ㻘㻌ྜྷ⏣㻌຾

xi

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㻝㻝㻥

㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䠏᭶䠐᪥㻌䠄ⅆ䠅䝘䝜䝏䝳䞊䝤䛾⏕ᡂ䛸⢭〇㻞㻼㻙㻞㻤ゐ፹ᢸᣢ᪉ἲ䛸䛧䛶䝕䜱䝑䝥䝁䞊䝖ἲ䜢⏝䛔䛯㻯㻺㼀䛾⏕ᡂ㻝㻞㻜㻌㻖㻌⸨஭㻌ᜨ௓㻘㻌Ᏻ⸨㻌⩏๎㻘㻌኱Ἑෆ㻌ṇே

㻞㻼㻙㻞㻥
䖪
㻞㻼㻙㻟㻜

䝣䝷䝡䞁ㄏᑟయ䛚䜘䜃䜲䝋䜰䝻䜻䝃䝆䞁ㄏᑟయ䛻䜘䜛༢ᒙ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䛾䜹䜲䝷䝸䝔䜱㑅ᢥⓗ
ྍ⁐໬

㻝㻞㻝

㻌㻖㻌⚟⃝㻌ᑗྐ㻘㻌฼ග㻌ྐ⾜㻘㻌ຍ⸨㻌㞝୍㻘㻌୰ᔱ㻌┤ᩄ⤖ᬗ㗪ᆺἲ䛻䜘䜛㔠ᒓᆺ㻛༙ᑟయᆺ㻿㼃㻯㻺㼀㼟㧗㓄ྥ㞟ྜయ䛾⮬ᕫ⤌⧊ᙧᡂ㻝㻞㻞㻌㻖㻌Ἑྜ㻌ⱥ㍤㻘㻌㛗㇂ᕝ㻌ถ㻘㻌ෆ⸨㻌Ὀஂ㻘㻌㧗ᮌ㻌ຬᶞ㻘㻌࿴⏣㻌⩏ྐ㻘㻌➉ᘏ㻌኱ᚿ㻘㻌ᰗ㻌࿴ᏹ

㻞㻼㻙㻟㻝
䖪
㻞㻼㻙㻟㻞

ΰྜ⏺㠃άᛶ๣䜢⏝䛔䛯䝀䝹䜹䝷䝮䜽䝻䝬䝖䜾䝷䝣䜱䞊䛻䛚䛡䜛༢ᒙ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䛾ᵓ㐀㑅
ᢥⓗ⬺╔

㻝㻞㻟

㻌㻖㻌ⶇ⏣㻌㝧ᖹ㻘㻌㒔⠏㻌┿⏤⨾㻘㻌ᖹ㔝㻌⠜㻘㻌⸨஭㻌ಇ἞㑻㻘㻌⏣୰㻌୔ኈ㻘㻌∦ᾆ㻌ᘯ㐨㻲㼀㻙㻵㻯㻾䛻䜘䜛㻯㼛䜽䝷䝇䝍䞊䜈䛾䜰䝉䝖䝙䝖䝸䝹྾╔཯ᛂศᯒ㻝㻞㻠㻌㻖㻌ᑠ➟ཎ㻌୍ᶞ㻘㻌ᡞᙇ㻌㞝ኴ㻘㻌༓㊊㻌᪼ᖹ㻘㻌Ⳣ஭㻌ಇᶞ㻘㻌୸ᒣ㻌ⱱኵෆໟ䝘䝜䝏䝳䞊䝤
㻞㻼㻙㻟㻟䖪Synthesis and TEM-based Structural Characterization of C 60-Flattened CNT Nanopeapods* Qing Wang, Ryo Kitaura, Yuta Yamamoto, Shigeo Arai, Hisanori Shinohara

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㻞㻼㻙㻟㻠

䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤ෆ㒊䛷䛾」ᩘ䝏䜸䝣䜵䞁䜸䝸䝂䝬䞊䛾㓄ྥ䛻㛵䛩䜛ᐦᗘỗ㛵ᩘἲィ⟬㻝㻞㻢㻌㻖㻌‫‮‬ᮧ㻌ᑦྐ㻘㻌ᒣୗ㻌⿱⏕

㻞㻼㻙㻟㻡
䖪

ከ⎔ⰾ㤶᪘Ⅳ໬Ỉ⣲ศᏊ䜢ෆໟ䛧䛯䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䛾䜶䝛䝹䜼䞊ㄽ䛸㟁Ꮚ≧ែ㻝㻞㻣㻌㻖㻌ᮌᬽ㻌⪷ኴ㻘㻌ᒸ⏣㻌᫴䝘䝜䝩䞊䞁㻌㻞㻼㻙㻟㻢ᶆⓗග⇕䛜䜣἞⒪䜢┠ᣦ䛧䛯䜹䞊䝪䞁䝘䝜䝩䞊䞁䛾ᶵ⬟໬㻝㻞㻤㻌㻖㻌ᙇ㻌Ẹⰾ㻘㻌᳿㻌ᱵ㻘㻌୎㻌ṊᏕ㻘㻌㣤ᓥ㻌⃈⏨㻘㻌‫⏣‮‬ᆏ㻌㞞Ꮚ㻞㻼㻙㻟㻣Ⅳ⣲⿕そ䛧䛯䜾䝷䝣䜯䜲䝖㻛Ẽ┦ᡂ㛗Ⅳ⣲⧄⥔㻛䜹䞊䝪䞁䝘䝜䝩䞊䞁」ྜయ䜢౑䛳䛯䝸䝏䜴䝮䜲䜸䞁㟁ụ䛾ᛴ㏿඘ᨺ㟁≉ᛶ㻝㻞㻥㻌㻖㻌ᘪ๐㻌ுኴ㻘㻌⏣ᮧ㻌ᐅஅ㻘㻌┾Ꮚ㻌㝯ᚿ㻘㻌୰㔝㻌჆୍㑻㻘㻌୰ཎ㻌ㅬኴ㑻䝘䝜䝽䜲䝲䞊
㻞㻼㻙㻟㻤䜹䞊䝪䞁䝘䝜䝇䝨䞊䝇䜢⏝䛔䛯䝶䜴໬㖟䝘䝜䝽䜲䝲䛾ྜᡂ䛸ᵓ㐀ゎᯒ㻝㻟㻜㻌㻖㻌ᡂ℩㻌䛧䜋䛾㻘㻌໭ᾆ㻌Ⰻ㻘㻌㔝⏣㻌ඃ㻘㻌⠛ཎ㻌ஂ඾䜾䝷䝣䜵䞁⏕ᡂ㻞㻼㻙㻟㻥High-yielding synthesis of graphene by supuercritical fluid㻌㻖㻌ᒸ㻌ఙே㻘㻌➚ᒃ㻌㧗᫂㻘㻌ᮏ㛫㻌᱁

㻝㻟㻝

㻞㻼㻙㻠㻜
䖪

Fabrication of wide terraces on SiC (0001) for pit-free graphene growth in Ar atmosphere* Wang Chenxing , Hitoshi Nakahara, Koji Asaka, Yahachi Saito

㻝㻟㻞

㻞㻼㻙㻠㻝

In situ observation of graphene formation on polycrystalline Cu* Huafeng Wang, Pei Zhao, Shohei Chiashi, Shigeo Maruyama, Yoshikazu Homma

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㻞㻼㻙㻠㻞
䖪

❅⣲㞺ᅖẼୗ䛷ᙧᡂ䛥䜜䜛䜾䝷䝣䜵䞁㻛㻿㼕㻯䛾⏺㠃ᵓ㐀㻝㻟㻠㻌㻖㻌ቑ⏣㻌ె✑㻘㻌஌ᯇ㻌⯟㻘㻌ᴋ㻌⨾ᬛᏊ

xii㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䠏᭶䠐᪥㻌䠄ⅆ䠅㻞㻼㻙㻠㻟䜰䞁䝆䝑䝥㻞ᒙ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䜢ᡂ㛗᰾䛸䛧䛯ከᒙ䜾䝷䝣䜵䞁䝘䝜䝸䝪䞁䛾ᙧᡂ㻝㻟㻡㻌㻖㻌໭ᕝ㻌἞ᶞ㻘㻌᰿ᓊ㻌Ⰻኴ㻘㻌⏣୰㻌ၨᩥ㻘㻌⚟᳃㻌⛱㻘㻌ᑠᕝ㻌⌶἞㻘㻌ᑠᯘ㻌៞⿱䜾䝷䝣䜵䞁䛾ᛂ⏝㻞㻼㻙㻠㻠䖪㼃㻿㼑㻞ⷧ⭷䜢⏝䛔䛯䝣䝺䜻䝅䝤䝹䝖䝷䞁䝆䝇䝍䛸䜲䞁䝞䞊䝍㻞㻼㻙㻠㻡㧗ᐦᗘ䞉㧗㓄ྥ䜾䝷䝣䜵䞁䝘䝜䝸䝪䞁䛾໬Ꮫಟ㣭䛻䜘䜛䝗䞊䝢䞁䜾ไᚚ㻝㻟㻢

* Kazuma Funahashi, Jiang Pu, Lain-Jong Li, Yoshihiro Iwasa, Taishi Takenobu
㻝㻟㻣㻌 * Solís-Fernández Pablo, Bissett Mark 㻘㻌㎷㻌ṇ἞㻘㻌࿃㒓㻌ᾈᶞ䜾䝷䝣䜵䞁䛾≀ᛶ
㻞㻼㻙㻠㻢

㻝㻟㻤

㓟໬䜾䝷䝣䜵䞁䛾Ⓨගᶵᵓ㻌㻖㻌ᶓ஭㻌⿱அ㻘㻌㇂ཱྀ㻌㈗❶㻘㻌㩾἟㻌㝣ኸ㻘㻌ᯇᮏ㻌Ὀ㐨

㻞㻼㻙㻠㻣
䖪

㓟໬䜾䝷䝣䜵䞁䛻䛚䛡䜛㏆㉥እⓎගᶵᵓ

㻝㻟㻥

㻞㻼㻙㻠㻤

㻞ᒙ䜾䝷䝣䜵䞁䛾ᒙ㛫䛾ỈศᏊ䛾ศᏊືຊᏛ䝅䝭䝳䝺䞊䝅䝵䞁㻌㻖㻌ᑠ⃝㻌኱▱㻘㻌ᐑෆ㻌㞝ᖹ㻘㻌ẟ฼㻌┿୍㑻㻘㻌ᕷ⏣㻌ṇኵ㻘㻌ᯇ⏣㻌୍ᡂ㻝㻠㻜㻌㻖㻌㰻⸨㻌⌮୍㑻㻘㻌Ỉ㔝㻌ᑗᚿ

䛭䛾௚
㻞㻼㻙㻠㻥

䜺䝇୰䜾䝷䝣䜯䜲䝖䝺䞊䝄䞊䜰䝤䝺䞊䝅䝵䞁䛻䜘䜛䝣䝷䞊䝺䞁䛸䝫䝸䜲䞁䛾⏕ᡂ㻝㻠㻝㻌㻖㻌㜿㒊㻌ⓒྜ㤶㻘㻌㐲⸨㻌▖㻘㻌㜿▱Ἴ㻌ὒḟ㻘㻌ᇛ୸㻌᫓ኵ㻞㻼㻙㻡㻜䝫䝸䜲䞁ศᏊ䛾⚗ไ㑄⛣䛻䛚䛡䜛᣺㟁┦஫స⏝䛾◊✲㻝㻠㻞㻌㻖㻌ⱝᯘ㻌▱ᡂ≉ูㅮ₇㻌㻌㻔㻝㻣㻦㻜㻜㻙㻝㻣㻦㻟㻜㻕㻞㻿㻙㻢䝣䝷䞊䝺䞁㓟໬≀䛾ྜᡂ䚸ᵓ㐀䛚䜘䜃ồ᰾⨨᥮཯ᛂ

㻢

⏣ᓥ㻌ྑ๪

୍⯡ㅮ₇㻌㻌㻔㻝㻣㻦㻟㻜㻙㻝㻤㻦㻟㻜㻕䝣䝷䞊䝺䞁䛾໬Ꮫ䚷䞉㻌㻌䝣䝷䞊䝺䞁䛾ᛂ⏝䚷䞉㻌㻌㔠ᒓෆໟ䝣䝷䞊䝺䞁㻞㻙㻥䝇䝢䝻䜰䝉䝍䞊䝹໬䝣䝷䞊䝺䞁䛾⎔❧య㓄ᗙ䛻䛚䛡䜛䜰䝜䝬䞊ຠᯝ㻞㻢㻌㻖㻌ᑠஂಖ㻌◊㻘㻌ᒣ㷂㻌ඃ㻘㻌ቑ⏣㻌ᐶஅ㻘㻌ఀ⇃㻌┤ᙪ㻞㻙㻝㻜䝞䝹䜽䝦䝔䝻䝆䝱䞁䜽䝅䝵䞁ᆺ᭷ᶵⷧ⭷ኴ㝧㟁ụ䛻䛚䛡䜛ඃ䜜䛯㻺ᆺ༙ᑟయᮦᩱ䜢ᚿྥ䛧䛯䝇䝢䝻䜰䝉䝍䞊䝹䛚䜘䜃䝏䜸䜰䝉䝍䞊䝹䝣䝷䞊䝺䞁䛾ኴ㝧㟁ụ≉ᛶホ౯㻞㻣㻌㻖㻌୕ᮌỤ㻌⩼㻘㻌బ఑㻌᫛⣖㻘㻌ቑ⏣㻌ᐶஅ㻘㻌ఀ⇃㻌┤ᙪ㻘㻌ᑠஂಖ㻌◊㻘㻌㛵㻌ಟᖹ㻞㻙㻝㻝㼇㻸㼕㻬㻯㻢㻜㼉㻔㻼㻲㻢㻕䛾ㄏ㟁ⓗ┦㌿⛣㻞㻤㻌㻖㻌㟷ᰗ㻌ᚸ㻘㻌ᮡᮏ㻌㑥ஂ㻘㻌ᒸ⏣㻌ὒྐ㻘㻌ᫍ㔝㻌ဴஂ㻘㻌ⰰᕝ㻌ᬛ⾜㻞㻙㻝㻞䝸䝏䜴䝮䜲䜸䞁ෆໟ䝣䝷䞊䝺䞁䛸䝫䝹䝣䜱䝸䝜䜲䝗䛾㉸ศᏊ㘒య䛾ග㟁Ꮚ⛣ື཯ᛂ䛸ග㟁ኚ᥮≉ᛶ㻌㻖㻌኱ஂಖ㻌ᩗ㻘㻌ᕝᓥ㻌㞝ᶞ㻘㻌㓇஭㻌㞙ே㻘㻌⩚᭯㒊㻌༟㻘㻌 Sastre-Santos Angela 㻘㻌⚟ఫ㻌ಇ୍

xiii

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㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䠏᭶䠑᪥㻌䠄Ỉ䠅㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌ᇶㄪㅮ₇䚷䚷䚷Ⓨ⾲䠐䠌ศ䚷䞉䚷㉁␲ᛂ⟅䠑ศ㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌≉ูㅮ₇䚷䚷䚷Ⓨ⾲䠎䠑ศ䚷䞉䚷㉁␲ᛂ⟅䠑ศ㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌୍⯡ㅮ₇䚷䚷䚷Ⓨ⾲䠍䠌ศ䚷䞉䚷㉁␲ᛂ⟅䠑ศ㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䝫䝇䝍䞊䝥䝺䝡䝳䞊䚷䚷䚷Ⓨ⾲䠍ศ䚷䞉䚷㉁␲ᛂ⟅䛺䛧
ᇶㄪㅮ₇㻌㻌㻔㻥㻦㻜㻜㻙㻥㻦㻠㻡㻕㻟㻿㻙㻣

Floating catalyst CVD synthesis of SWNTs for thin film electronics applications
Esko I. Kauppinen㻣୍⯡ㅮ₇㻌㻌㻔㻥㻦㻠㻡㻙㻝㻜㻦㻟㻜㻕䝘䝜䝏䝳䞊䝤䛾ᛂ⏝㻟㻙㻝‵ᘧ⣳⣒ἲ䛻䜘䜚స〇䛧䛯㧗䛔ᑟ㟁⋡䜢᭷䛩䜛䝫䝸䝬䞊䝣䝸䞊䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤⥺㻟㻜㻌㻖㻌ྥ㻌೺㻘㻌Ᏻ✚㻌Ḡᚿ㻘㻌ᮧୖ㻌ಇஓ㻘㻌ఀᮾ㻌༓ᑜ㻘㻌ᩪ⸨㻌Ẏ㻘㻌‫‮‬ᮧ㻌Ᏺ㞝㻟㻙㻞㍍㔞䞉㧗ᛶ⬟䞉ప䝁䝇䝖䛺㟁Ẽ໬Ꮫ䜻䝱䝟䝅䝍㟁ᴟ䜢┠ᣦ䛧䛯㻌䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤㻟ḟඖ㞟㟁య䛾㛤Ⓨ㻟㻝㻌㻖㻌䜻䞁䝔䞊䝻㻌䝸䜹䝹䝗㻘㻌㔠㻌ᮾᴿ㻘㻌㛗㇂ᕝ㻌㤾㻘㻌ᒣ⏣㻌⿱㈗㻘㻌ᒣ⏣㻌῟ኵ㻘㻌㔝⏣㻌ඃ㻟㻙㻟Green, scalable, binderless fabrication of a single-wall carbon nanotube nonwoven fabricbased on an ancient Japanese paper process㻌㻖㻌ᑠᶫ㻌࿴ᩥ㻘㻌ᖹᯘ㻌㐩ஓ㻘㻌㜿ከ㻌ㄔ௓㻘㻌ᒣ⏣㻌೺㑻㻘㻌䝣䝍䝞㻌䝗䞁㻘㻌␊㻌㈼἞

㻟㻞㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䠚䠚䠚䠚䠚䠚䠚㻌ఇ᠁㻌㻌㻔㻝㻜㻦㻟㻜㻙㻝㻜㻦㻠㻡㻕㻌䠘䠘䠘䠘䠘䠘䠘୍⯡ㅮ₇㻌㻌㻔㻝㻜㻦㻠㻡㻙㻝㻝㻦㻠㻡㻕䜾䝷䝣䜵䞁䛾ᛂ⏝㻟㻙㻠㻿㼕㻻㻞㻛㻿㼕ୖ䜾䝷䝣䜵䞁䝘䝜䝸䝪䞁䛾㟁Ꮚఏᑟ≉ᛶ䛻䛴䛔䛶䛾኱つᶍ➨୍ཎ⌮ィ⟬㻟㻟㻌㻖㻌ᐿᐆ㻌⚽ᖾ㻘㻌ᑿᓮ㻌Ὀຓ㻘㻌኱ῡ㻌┿⌮㻟㻙㻡䜲䞁䝍䞊䜹䝺䞊䝅䝵䞁䛧䛯㻯㼂㻰ྜᡂከᒙ䜾䝷䝣䜵䞁䛾ศᯒ㻟㻠㻌㻖㻌㏆⸨㻌኱㞝㻘㻌୰㔝㻌⨾ᑦ㻘㻌࿘㻌Ἴ㻘㻌஭㻌ளᕼᏊ㻘㻌ᯘ㻌㈼஧㑻㻘㻌ᒣཱྀ㻌῟୍㻘㻌㧗ᶫ㻌ៅ㻘㻌బ⸨㻌ಙኴ㑻㻘
ᶓᒣ㻌┤ᶞ

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Graphene as a Material for Next Generation Fuel Cells* Stephen Lyth, Jianfeng Liu, Thomas Bayer, Sean Bishop, Kazunari Sasaki

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Graphene enabled micromechanical switches* Shao-Wei Ma, Ya-Ping Hsieh㻟㻢㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䠚䠚䠚䠚䠚䠚䠚㻌᫨㣗㻌㻌㻔㻝㻝㻦㻠㻡㻙㻝㻟㻦㻜㻜㻕㻌䠘䠘䠘䠘䠘䠘䠘䝫䝇䝍䞊䝥䝺䝡䝳䞊㻌㻌㻔㻝㻟㻦㻜㻜㻙㻝㻠㻦㻜㻜㻕䝫䝇䝍䞊䝉䝑䝅䝵䞁㻌㻌㻔㻝㻠㻦㻜㻜㻙㻝㻡㻦㻠㻡㻕䚷䚷䚷䚷䠄䖪䠅䚷ⱝᡭዡບ㈹ೃ⿵
䝣䝷䞊䝺䞁䛾໬Ꮫ㻟㻼㻙㻝

Thermal Bis-silylation, Carbosilylation, and Bis-germylation of Fullerenes㻌㻖㻌✄ⴥ㻌኱ᶞ㻘㻌༡㻌࿴ஓ㻘㻌ᐑ㒊㻌ᜤ㍜㻘㻌㣤⏣㻌ு௓㻘㻌ຍᅛ㻌ᫀᐶ㻘㻌๓⏣㻌ඃ㻘㻌ᒣ⏣㻌㐨ኵ㻘㻌㛗㇂ᕝ㻌ṇ㻘
㉥㜰㻌೺

㻝㻠㻟

㻟㻼㻙㻞

᪂つ䝞䝹䜽䝦䝔䝻᥋ྜᆺ᭷ᶵⷧ⭷ኴ㝧㟁ụ䜈䛾ᛂ⏝䜢ど㔝䛻ධ䜜䛯䝣䝷䞊䝺䞁ㄏᑟయ䛾㛤Ⓨ㻝㻠㻠㻌㻖㻌ᚨ෠㻌ᑦᚿ㻘㻌㛵ᡞ㻌኱xiv㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䠏᭶䠑᪥㻌䠄Ỉ䠅㔠ᒓෆໟ䝣䝷䞊䝺䞁
㻟㻼㻙㻟
䖪
㻟㻼㻙㻠

㻝㻠㻡

㉸ཎᏊᆺ䝸䝏䜴䝮ෆໟ䝣䝷䞊䝺䞁䛾㟁ゎྜᡂ㻌㻖㻌ୖ㔝㻌⿱㻘㻌ఀ⇃㻌┤ᙪ㻘㻌኱ஂಖ㻌ᩗ㻘㻌᳃ᒣ㻌ᗈ㻘㻌⚟ఫ㻌ಇ୍㻘㻌ᑠஂಖ㻌◊཯ᛂ⣔୰䛷䛾䝖䝸䝣䝹䜸䝻䝯䝏䝹໬䛻䜘䜛ᑠ䛥䛺䝞䞁䝗䜼䝱䝑䝥䜢᭷䛩䜛㔠ᒓෆໟ䝣䝷䞊䝺䞁㻳㼐㻬㻯㻢㻜䛾㻝㻠㻢ศ㞳㻌㻖㻌୹⩚㻌ᏹஅ㻘㻌୰す㻌ຬ௓㻘㻌⋤㻌ᚿỌ㻘㻌໭ᾆ㻌Ⰻ㻘㻌኱⏫㻌㑈㻘㻌⠛ཎ㻌ஂ඾䝘䝜䝏䝳䞊䝤䛾≀ᛶ㻟㻼㻙㻡

Spontaneous exciton dissociation in carbon nanotubes
Yusuke Kumamoto, Masahiro Yoshida, Akihiro Ishii, Akio Yokoyama, * Takashi Shimada,Yuichiro K. Kato

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㻟㻼㻙㻢

Quantum interference effect in Raman spectra of metallic nanotubes and graphene㻌㻖㻌䝝䝇䝕䜸㻌䜶䝑䝗䜴䜲㻘㻌䝚䜾䝷䝝㻌䜰䝣䝬䝗㻘㻌㰻⸨㻌⌮୍㑻

㻝㻠㻤

㻟㻼㻙㻣
䖪

༢ᒙ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䛻䛚䛡䜛䜰䝑䝥䝁䞁䝞䞊䝆䝵䞁Ⓨග䛾ほ

㻝㻠㻥

㻟㻼㻙㻤

㟁Ⲵ⵳✚䛥䜜䛯Ḟ㝗䜢᭷䛩䜛㻯㻺㼀䛾㟁Ꮚ≧ែ㻌㻖㻌⛅᭶㻌┤ே㻘㻌ᐑෆ㻌㞝ᖹ㻘㻌ẟ฼㻌┿୍㑻㻘㻌ᯇ⏣㻌୍ᡂ㻝㻡㻜㻌㻖㻌▼ᒣ㻌భ㻘㻌ᒸ⏣㻌᫴㻟㻼㻙㻥༢ᒙ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䛾⺯ග䛚䜘䜃䝷䝬䞁䝇䝨䜽䝖䝹䛻䛚䛡䜛㔠ᒓ⵨╔ຠᯝ㻝㻡㻝㻌㻖㻌ᑠ➎㻌᫂ᙪ㻘㻌༓㊊㻌᪼ᖹ㻘㻌ᒣཱྀ㻌ඖኴ㻘㻌ᮏ㛫㻌ⰾ࿴

㻟㻼㻙㻝㻜
䖪
㻟㻼㻙㻝㻝

㻝㻟

㻯䜢⃰⦰䛧䛯༢ᒙ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䛻䛚䛡䜛㻺㻹㻾ᐃ㻝㻡㻞㻌㻖㻌ⱂ⏣㻌᪼㻘㻌୰஭㻌♸௓㻘㻌ᐑ⏣㻌⪔඘㻘㻌┿ᗞ㻌㇏㻘㻌ᩧ⸨㻌Ẏ

Numerical study of electronic states in double-walled carbon nanotubes ---Formation of
metallic bands by covalent bridge between tubes--* Yuhei Natsume

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㻟㻼㻙㻝㻞

Electronic Structure of Carbon and BN Nanotubes: A Comparative First Principles Study* Yuya Uchida, Takashi Koretsune, Susumu Saito

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㻟㻼㻙㻝㻟

Photoconductivity spectroscopy of individual suspended carbon nanotubes* Takushi Uda, Yusuke Kumamoto, Masahiro Yoshida, Akihiro Ishii, Yuichiro K. Kato㻝㻡㻡䝘䝜䝏䝳䞊䝤䛾ᛂ⏝
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⎔ቃ㈇Ⲵ䛾ᑠ䛥䛔Ỉ⁐ᛶ䝘䝜䝏䝳䞊䝤ྜᡂἲ㻌䝷䞊䝬䞁㻌䝰䝝䝬䝗㻌䝆䜵䝹䞊䝹㻘㻌㻖㻌୕㔜㔝㻌ဴ㻟㻼㻙㻝㻡㻭㻯㻯㼂㻰ἲ䜢⏝䛔䛯ከᏍ㉁䜺䝷䝇䠄㻼㻳㻕ᯈᮦ䜈䛾༢ᒙ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤సᡂ䛾ヨ䜏㻝㻡㻣㻌㛗ᑿ㻌ᮥᖹ㻘㻌㻖㻌㕥ᮌ㻌ಙ୕㻘㻌኱ୖ㻌┿ྖ㻘㻌ఀ⸨㻌ὒ௓㻘㻌㛗⃝㻌ᾈ㻘㻌㜿▱Ἴ㻌ὒḟ㻟㻼㻙㻝㻢༢ᒙ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䝞䞁䝗䝹䛾⁁䜢ㄆ㆑䛩䜛ศᏊ㻝㻡㻤㻌㻖㻌⸨䞄㇂㻌๛ᙪ㻘㻌䝴㻌䝆䝵䞁䝔㻘㻌୰ᔱ㻌┤ᩄ㻟㻼㻙㻝㻣໬Ꮫಟ㣭䛧䛯㻹㼃㻺㼀㻛㻼㻭㻢䝘䝜䝁䞁䝫䝆䝑䝖䛾㛤Ⓨ䛸≉ᛶホ౯㻝㻡㻥㻌㻖㻌ᮧᒸ㻌៞⨾㻘㻌బ⸨㻌ᏹ⣖㻘㻌㛵ᡞ㻌኱

㻟㻼㻙㻝㻤
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Printed SWCNT thin film CMOS inverters based on chemically doped ion gels㻌㻖㻌࿴⏣㻌⩏ྐ㻘㻌≸㣫㻌Ⰻኴ㻘㻌⸨ᮏ㻌ኴ㝧㻘㻌℈⏿㻌⿱⣖㻘㻌ᯇᓮ㻌᛭ᶞ㻘㻌ᰗ㻌࿴ᏹ㻘㻌➉ᘏ㻌኱ᚿ

xv

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㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䠏᭶䠑᪥㻌䠄Ỉ䠅㻟㻼㻙㻝㻥ග↷ᑕ䛻䜘䜚⏕䛨䜛䝧䞁䝆䝹䝷䝆䜹䝹ㄏᑟయ䛻䜘䜛ከᒙ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䛾⾲㠃ಟ㣭㻝㻢㻝㻌㻖㻌㧗⏣㻌▱ဢ㻘㻌䝞䝖䝤䝲䞁㻌䝮䞁䝣䜷䝗㻘㻌㜿㒊㻌⸅᫂”Laminated” ion-gel film as high capacitance insulator for carbon-nanotube transistor* Taiyo Fujimoto, Ryo Shimizu, Yuki Takagi, Yoshifumi Wada, Kazuhiro Yanagi,
Taishi Takenobu

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Polyglycerol-functionalized single-walled carbon nanotubes for drug loading and delivery* Qin Hongmei, Li Zhao, Keisuke Nakamura, Takahide Kimura, Naoki Komatsu

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䝣䝺䜻䝅䝤䝹䜶䝺䜽䝖䝻䝙䜽䝇䜢┠ᣦ䛧䛯䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䛾⡆᫆䛺䝻䝇䝣䝸䞊༳ๅᢏ⾡

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㻟㻼㻙㻞㻜
䖪

㻟㻼㻙㻞㻟

㻟㻼㻙㻞㻠

㻌㻖㻌ⓑỤ㻌ᏹஅ㻘㻌㔠㻌ᮾᴿ㻘㻌㛗㇂ᕝ㻌㤾㻘㻌㔝⏣㻌ඃChemical Vapor Deposition of MoS2 on Carbon Nanotube for Organic Thin Film Solar
Cells* IL JEON, Dai Kutsuzawa, Yu Hashimoto, Takashi Yanase, Taro Nagahama,Toshihiro Shimada, Yutaka Matsuo䝧䝹䝖ᆺඹᙺ㧗ศᏊ䛾㻿㼃㻯㻺㼀䛾䝷䝑䝢䞁䜾䛻䜘䜛㧗ᗘྍ⁐໬

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㻌㻖㻌బᕝ㻌ᘺ㻘㻌㧗ᶫ㻌ṇὒ㻘㻌ᓊᕝ㻌ᆂᕼ㻘㻌ᖾᮏ㻌㔜⏨䝘䝜䝏䝳䞊䝤䛾⏕ᡂ䛸⢭〇㻟㻼㻙㻞㻡ⷧ⭷䝖䝷䞁䝆䝇䝍ᛂ⏝䛻ྥ䛡䛯㻰㻺㻭ಟ㣭䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䛾䜹䜲䝷䝸䝔䜱ศ㞳㻝㻢㻣㻌㻖㻌᱓ཎ㻌᭷⣖㻘㻌஧⎼㻌ྐ⾜㻘㻌኱᳃㻌⁠࿴㻘㻌ᩪ⸨㻌Ẏ

㻟㻼㻙㻞㻢
䖪

䝟䝹䝇䝥䝷䝈䝬㻯㼂㻰䛻䜘䜛㧗⣧ᗘ䠄㻢㻘㻡䠅༢ᒙ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤ྜᡂ䛻䛚䛡䜛䝟䝹䝇ຠᯝ㻟㻼㻙㻞㻣䝰䝜䜰䝹䜻䝹㙐ྵ᭷䝫䝸䝣䝹䜸䝺䞁䛻䜘䜛ኴ䛔༙ᑟయᛶ༢ᒙ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䛾㑅ᢥⓗᢳฟ㻝㻢㻤㻌㻖㻌チ㻌ᩩ㻘㻌ຍ⸨㻌ಇ㢧㻘㻌ᮧ㉺㻌ᖾྐ㻘㻌㔠Ꮚ㻌ಇ㑻㻝㻢㻥㻌㻖㻌⚟୸㻌㈗ᘯ㻘㻌฼ග㻌ྐ⾜㻘㻌⸨䞄㇂㻌๛ᙪ㻘㻌୰ᔱ㻌┤ᩄ㻟㻼㻙㻞㻤䝏䝳䞊䝤➃䛛䜙䛾༢ᒙ㻯㻺㼀䛾䜽䝻䞊䝙䞁䜾ᡂ㛗㻝㻣㻜㻌㻖㻌ᾏ㔝㻌㈗ᚨ㻘㻌஭䝜ୖ㻌Ὀ㍤㻘㻌༓㊊㻌᪼ᖹ㻘㻌୸ᒣ㻌ⱱኵ

㻟㻼㻙㻞㻥
䖪
㻟㻼㻙㻟㻜

⇕ఏᑟᮦᩱᛂ⏝䛻ྥ䛡䛯㧗ᐦᗘ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤ᆶ┤㓄ྥ⭷䛾ྜᡂ㻝㻣㻝㻌㻖㻌⨶㻌䝚䝸㻘㻌㛗㇂ᕝ㻌㤾㻘㻌㔝⏣㻌ඃ

Selective Growth of Single-Walled Carbon Nanotubes with Specific Diameter and Chirality
by Irradiating Free Electron Laser during Growth㻌㻖㻌ྜྷ⏣㻌ᆂభ㻘㻌┦Ⰻ㻌ᣅᐇ㻘㻌ὠ⏣㻌ᝆస㻘㻌▼஭㻌ᏹ἞㻘㻌ᒣᕝ㻌೺୍㻘㻌▮ᓥ㻌༤ᩥ㻘㻌ᒾ⏣㻌ᒎᖾ㻘㻌ᒣᮏ㻌ᐶ㻝㻣㻞ෆໟ䝘䝜䝏䝳䞊䝤
㻟㻼㻙㻟㻝䖪༢ᒙ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䛻䛚䛡䜛≀㉁ෆໟ䛻䜘䜛䝊䞊䝧䝑䜽ಀᩘ䛾ไᚚ㻟㻼㻙㻟㻞ศᏊືຊᏛィ⟬䛻䜘䜛䝏䜸䝣䜵䞁䜸䝸䝂䝬䞊ෆໟ༢ᒙ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤䛾ศᏊ㓄ྥ㻝㻣㻟㻌㻖㻌ୖ⏣㻌ᬛ኱㻘㻌୰஭㻌♸௓㻘㻌ᐑ⏣㻌⪔඘㻘㻌┿ᗞ㻌㇏㻝㻣㻠㻌㻖㻌⏣⏿㻌⿱ክ㻘㻌㛵᰿㻌ு⣖㻘㻌஭ୖ㻌࿴⨾㻘㻌∦ᒸ㻌ὒభ㻘㻌⥴᪉㻌ၨ඾䜾䝷䝣䜵䞁⏕ᡂ㻟㻼㻙㻟㻟䖪䜾䝷䝣䜵䞁䛾໬Ꮫ཯ᛂᛶ䛻䛚䛡䜛ᡂ㛗ᇶᯈ䛾ᙳ㡪㻌㻖㻌஭ୖ㻌෽௓㻘㻌ᐑ⏣㻌⪔඘㻘㻌┿ᗞ㻌㇏

xvi

㻝㻣㻡

㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䠏᭶䠑᪥㻌䠄Ỉ䠅㻟㻼㻙㻟㻠Synthesis and Characterization of Metal Intercalated bilayers Graphene㻌㻖㻌௒஭㻌೺ኴ㑻㻘㻌ᯇᮌ㻌ᅜ἞㻘㻌బ⸨㻌⚈࿃㻘㻌ᒾ⏣㻌ᒎᖾ㻘㻌ᒣᮏ㻌ᐶ

㻝㻣㻢

㻟㻼㻙㻟㻡
䖪

㻯㼡㻔㻝㻜㻜㻕⾲㠃ୖ䛷䛾䜾䝷䝣䜵䞁䝘䝜䝸䝪䞁䛾㻯㼂㻰ᡂ㛗

㻝㻣㻣

㻟㻼㻙㻟㻢

䝖䝸䝣䜵䝙䝺䞁ㄏᑟయ䛻䜘䜛䜾䝷䝣䜯䜲䝖䛛䜙䜾䝷䝣䜵䞁䛾ᾮ┦๤㞳* Mohamad Yunus Rozan 㻘㻌ᐑୗ㻌㞞኱㻘㻌㎷㻌ṇ἞㻘㻌᪥ẚ㔝㻌ᾈᶞ㻘㻌࿃㒓㻌ᾈᶞ㻝㻣㻤㻌㻖㻌⯪ᶫ㻌❳௓㻘㻌๽㻌๛㻘㻌㟷἟㻌⚽ඣ㻘㻌ᮌᮧ㻌㝯ⱥ㻘㻌ᑠᯇ㻌┤ᶞ

㻟㻼㻙㻟㻣
䖪

ᛴ㏿ຍ⇕䝥䝷䝈䝬㻯㼂㻰䛻䜘䜛㻺㼕䝘䝜䝞䞊䛛䜙䛾䜾䝷䝣䜵䞁䝘䝜䝸䝪䞁ྜᡂ䛻䛚䛡䜛䝥䝷䝈䝬ຠᯝ㻟㻼㻙㻟㻤Influence of electrolyte concentration for electrochemical exfoliation of graphene㻌㻖㻌Ἀᮏ㻌἞ဢ㻘㻌㯮἟㻌ᐶ⣖㻘㻌బ㔝㻌ṇே㻝㻣㻥㻌㻖㻌㕥ᮌ㻌ᘯᮁ㻘㻌ຍ⸨㻌ಇ㢧㻘㻌㔠Ꮚ㻌ಇ㑻㻝㻤㻜䜾䝷䝣䜵䞁䛾ᛂ⏝㻟㻼㻙㻟㻥䖪㑄⛣㔠ᒓ䝎䜲䜹䝹䝁䝀䝘䜲䝗䜢⏝䛔䛯㧗䝀䜲䞁㻯㻹㻻㻿䜲䞁䝞䞊䝍㻟㻼㻙㻠㻜High efficiency graphene doping* Kai-Wen Cheng, Po-shin Lin, Ya-Ping Hsieh㻝㻤㻝㻌㻖㻌ⵦ㻌Ụ㻘㻌 Huang Jing-Kai, 㻌ᒾబ㻌⩏ᏹ㻘㻌 Li Lain-Jong 㻘㻌➉ᘏ㻌኱ᚿ㻝㻤㻞䜾䝷䝣䜵䞁䛾≀ᛶ㻟㻼㻙㻠㻝䝃䜲䝈ศ㞳䛥䜜䛯䜾䝷䝣䜵䞁㔞Ꮚ䝗䝑䝖䛻䛚䛡䜛๻ⓗ䛺Ⓨග≉ᛶ䛾ኚ໬㻝㻤㻟㻌㻖㻌෤㔝㻌┤ே㻘㻌ᑠ⃝㻌኱▱㻘㻌ᐑෆ㻌㞝ᖹ㻘㻌ẟ฼㻌┿୍㑻㻘㻌໭ᾆ㻌Ⰻ㻘㻌⠛ཎ㻌ஂ඾㻘㻌ಖ⏣㻌ᚨ㻘㻌ᑠᯇ㻌┤ᶞ㻘
ᯇ⏣㻌୍ᡂ

㻟㻼㻙㻠㻞
䖪

䜾䝷䝣䜵䞁➃䛾䜶䝛䝹䜼䞊ㄽ䛸㟁Ꮚ≧ែ㻟㻼㻙㻠㻟䜾䝷䝣䜯䜲䝖≧䜹䞊䝪䞁䛾㓟໬ᗘ䛾⢭ᐦไᚚ㻝㻤㻠㻌㻖㻌ᒣ୰㻌⥤㤶㻘㻌ᒸ⏣㻌᫴㻝㻤㻡㻌ோ⛉㻌ຬኴ㻘㻌㻖㻌᳃ᮏ㻌┤ᶞ䝘䝜Ⅳ⣲⢏Ꮚ
㻟㻼㻙㻠㻠

㻟㻼㻙㻠㻡

Structural and magnetic changes of nanodiamond-copper composites during HPHT Sintering㻝㻤㻢Process
Fedor Shakhov, Vladimir Osipov, Sergei Kidalov, * Kazuyuki Takai, Toshiaki Enoki,
Alexander Vul’䜹䞊䝪䞁䝘䝜䝬䝔䝸䜰䝹ୖ䛻ᢸᣢ䛥䜜䛯㻼㼠㻘㻌㻼㼠㻙㻾㼡⢏Ꮚ䛾ྜᡂ䛸≉ᛶホ౯㻝㻤㻣㻌㻖㻌᪩℩㻌຾ᖹ㻘㻌ྜྷ➉㻌ᬕᙪ㻘㻌⋤㻌ᚿ᭸㻘㻌⥴᪉㻌ၨ඾㻟㻼㻙㻠㻢Hydration of Nanodiamond Surface Revisited : Intercalation Hypothesis㻌㻖㻌ᒣ㔝஭㻌ுᏊ㻘㻌㻭㼙㼍㼚㼐㼍㻌㻮㼍㼞㼚㼍㼞㼐㻘㻌బ䚻ᮌ㻌ಟ୍㻘㻌኱⃝㻌ᫎ஧

㻝㻤㻤

䛭䛾௚
㻟㻼㻙㻠㻣

⮬ᕫ⤌⧊໬䛧䛯⏺㠃άᛶ๣⾲㠃䛷䛾㔠ᒓ◪㓟ሷỈ࿴≀䛾⦰ྜ䜢฼⏝䛧䛯㓟໬㕲䝘䝜䝏䝳䞊䝤䜈䛾
㻝㻤㻥
ள㖄䝗䞊䝥

㻌㻖㻌ᑠᮡ㻌ඃኴ㻘㻌ᆏᮾ㻌ಇ἞

㻟㻼㻙㻠㻤
䖪

㕲ᚤ⢊ᮎ䜢౑⏝䛧䛯䜹䞊䝪䞁䝘䝜䝁䜲䝹䛾䝅䞊䝖≧ྜᡂ≀⾲㠃䜈䛾㧗⣧ᗘྜᡂ䛚䜘䜃୙⣧≀䛾పῶ 㻝㻥㻜㻌㻖㻌ΎỈ㻌៞᫂㻘㻌୸ᒣ㻌ⓡྖ㻘㻌㣤⏣㻌ဴ⏕㻘㻌㡲⏣㻌ၿ⾜㻘㻌⏣ୖ㻌ⱥே㻘㻌⁪ᕝ㻌ᾈྐ㻘㻌᳜㻌ோᚿ㻘㻌ΎỈ㻌୍ᶞ㻘
ᱵ⏣㻌Ⰻே

xvii

㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䠏᭶䠑᪥㻌䠄Ỉ䠅㻟㻼㻙㻠㻥䖪㑄⛣㔠ᒓ䝎䜲䜹䝹䝁䝀䝘䜲䝗䛻䛚䛡䜛஧ḟඖ༙ᑟయ䝦䝔䝻᥋ྜ䛾ྜᡂ䛸ホ౯㻟㻼㻙㻡㻜㻹㼛㻿㻞䇷༢ᒙ䜹䞊䝪䞁䝘䝜䝏䝳䞊䝤」ྜⷧ⭷䛾㟁Ẽ໬Ꮫ≉ᛶ㻝㻥㻝㻌㻖㻌᳃㻌຾ᖹ㻘㻌ᐑ⏣㻌⪔඘㻘㻌┿ᗞ㻌㇏㻝㻥㻞㻌㐲⸨㻌⚽᫭㻘㻌㻖㻌Ἑྜ㻌ⱥ㍤㻘㻌㛗㇂ᕝ㻌ถ㻘㻌ຍ἞㻌⪷ஓ㻘㻌ᰗ㻌࿴ᏹ≉ูㅮ₇㻌㻌㻔㻝㻡㻦㻠㻡㻙㻝㻢㻦㻝㻡㻕㻟㻿㻙㻤䝋䝙䞊䛻䛚䛡䜛䜾䝷䝣䜵䞁◊✲㛤Ⓨ㻌㻌㻌䠉⁐ᾮ䝥䝻䝉䝇䛻䜘䜛㼀㻲㼀䛸㻯㼂㻰䛻䜘䜛㏱᫂ᑟ㟁⭷䠉

㻤

ᑠᯘ㻌ಇஅ

୍⯡ㅮ₇㻌㻌㻔㻝㻢㻦㻝㻡㻙㻝㻣㻦㻟㻜㻕䜾䝷䝣䜵䞁䛾≀ᛶ䚷䞉㻌㻌䜾䝷䝣䜵䞁䛾ᛂ⏝㻌䚷䞉㻌㻌䜾䝷䝣䜵䞁⏕ᡂ㻌㻟㻙㻤✚ᒙᵓ㐀䛜䛽䛨䜜䛯㻞ᒙ䜾䝷䝣䜵䞁䛻䛚䛡䜛㻳䝞䞁䝗ᙉᗘቑ኱䛾ゅᗘ౫Ꮡᛶ㻟㻣㻌㻖㻌బ⸨㻌೺ኴ㑻㻘㻌㰻⸨㻌⌮୍㑻

㻟㻙㻥

㻟㻤

ྵ❅⣲䜾䝷䝣䜵䞁䛾䠴⥺ග㟁Ꮚศගศᯒ

㻌㻖㻌ᒣ⏣㻌Ὀᘯ㻘㻌䜻䝮㻌䝆䝵䞁䝢䝹㻘㻌ᯇᑿ㻌᫴ኴ㑻㻘㻌బ⸨㻌ᬛྖ㻟㻙㻝㻜ᾮ┦ᡂ㛗ἲ䛻䜘䜚▼ⱥᇶᯈୖ䛾ᚤ⣽✰ෆ䛻ᙧᡂ䛥䜜䛯䜾䝷䝣䜵䞁⭷䛾ගᏛ䞉䝷䝬䞁ศග䛻䜘䜛ゎᯒ㻟㻥㻌㻖㻌᪥ᾆ㻌ⱥᩥ㻟㻙㻝㻝Novel transfer method for clean and high mobility CVD graphene
Ya-Ping Hsieh, Mario Hofmann, * Bo-Suei Chiang

㻠㻜

㻟㻙㻝㻞

Mechanism and impact of ad-layer formation on CPCVD graphene* Yi-Wen Wang, Ya-Ping Hsieh, Mario Hofmann

㻠㻝

xviii

㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻹㼍㼞㼏㼔㻌㻟㼞㼐㻘㻌㻹㼛㼚㻚㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻼㼘㼑㼚㼍㼞㼥㻌㻸㼑㼏㼠㼡㼞㼑㻦㻌㻞㻡㼙㼕㼚㻌㻔㻼㼞㼑㼟㼑㼚㼠㼍㼠㼕㼛㼚㻕㻌㻗㻌㻡㼙㼕㼚㻌㻔㻰㼕㼟㼏㼡㼟㼟㼕㼛㼚㻕㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻿㼜㼑㼏㼕㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㻦㻌㻞㻡㼙㼕㼚㻌㻔㻼㼞㼑㼟㼑㼚㼠㼍㼠㼕㼛㼚㻕㻌㻗㻌㻡㼙㼕㼚㻌㻔㻰㼕㼟㼏㼡㼟㼟㼕㼛㼚㻕㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻳㼑㼚㼑㼞㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㻦㻌㻝㻜㼙㼕㼚㻌㻔㻼㼞㼑㼟㼑㼚㼠㼍㼠㼕㼛㼚㻕㻌㻗㻌㻡㼙㼕㼚㻌㻔㻰㼕㼟㼏㼡㼟㼟㼕㼛㼚㻕㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻼㼛㼟㼠㼑㼞㻌㻼㼞㼑㼢㼕㼑㼣㻦㻌㻝㼙㼕㼚㻌㻔㻼㼞㼑㼟㼑㼚㼠㼍㼠㼕㼛㼚㻕㻼㼘㼑㼚㼍㼞㼥㻌㻸㼑㼏㼠㼡㼞㼑㻌㻌㻔㻥㻦㻟㻜㻙㻝㻜㻦㻜㻜㻕㻝㻿㻙㻝

Current Status and Vision of Fullerene Business in Mitsubishi Corporation
Mikio Sasaki㻝㻳㼑㼚㼑㼞㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㻌㻌㻔㻝㻜㻦㻜㻜㻙㻝㻜㻦㻠㻡㻕㻲㼡㼘㼘㼑㼞㼑㼚㼑㼟䚷䞉䚷㻱㼚㼐㼛㼔㼑㼐㼞㼍㼘㻌㼙㼑㼠㼍㼘㼘㼛㼒㼡㼘㼘㼑㼞㼑㼚㼑㼟䚷䞉䚷㻭㼜㼜㼘㼕㼏㼍㼠㼕㼛㼚㼟㻌㼛㼒㻌㼒㼡㼘㼘㼑㼞㼑㼚㼑㼟㻝㻙㻝Structural analysis of C60 microtube-AAO membrane joint interfaces by FIB-SEM* Kun'ichi Miyazawa, Shuichi Shimomura, Takatsugu Wakahara, Masaru Tachibana㻥㻝㻙㻞Photoelectron Spectra of Encapsulated Mono-metal fullerenes* Takafumi Miyazaki, Yuuma Seino, Shoko Noda, Hajime Yagi, Hisanori Shinohara,
Shojun Hino

㻝㻜

㻝㻙㻟

Organic Photovoltaic Device Characteristics using Fullerene Derivatives with a Thiophene
Moiety* Tatsuya Hayashi, Heaseong Lee, Inseob Im, Seungjoo Lee, Jin Jang, Chyongjin Pac,
Hiroshi Moriyama㻝㻝㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䠚䠚䠚䠚䠚䠚䠚㻌㻯㼛㼒㼒㼑㼑㻌㻮㼞㼑㼍㼗㻌㻌㻔㻝㻜㻦㻠㻡㻙㻝㻝㻦㻜㻜㻕㻌䠘䠘䠘䠘䠘䠘䠘㻿㼜㼑㼏㼕㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㻌㻌㻔㻝㻝㻦㻜㻜㻙㻝㻝㻦㻟㻜㻕㻝㻿㻙㻞

Critical factors in multi-walled carbon nanotubes in mesothelial carcinogenesis
Shinya Toyokuni㻞㻳㼑㼚㼑㼞㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㻌㻌㻔㻝㻝㻦㻟㻜㻙㻝㻞㻦㻜㻜㻕㻯㼍㼞㼎㼛㼚㻌㼚㼍㼚㼛㼜㼍㼞㼠㼕㼏㼘㼑㼟䚷䞉䚷㻻㼠㼔㼑㼞㻌㼠㼛㼜㼕㼏㼟㻝㻙㻠

Dispersion of detonation nanodiamond: A progress report* Shuichi Sasaki, Ryoko Yamanoi, Eiji Osawa

㻝㻞

㻝㻙㻡

Development of Ion Mobility System with Multi-stage Ion Trap
* Toshiki Sugai, Yasuhiro Hiroshiba, Ninako Mikami, Ryota Jinnouchi㻝㻟㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䠚䠚䠚䠚䠚䠚䠚㻌㻸㼡㼚㼏㼔㻌㼀㼕㼙㼑㻌㻌㻔㻝㻞㻦㻜㻜㻙㻝㻟㻦㻝㻡㻕㻌䠘䠘䠘䠘䠘䠘䠘㻿㼜㼑㼏㼕㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㻌㻌㻔㻝㻟㻦㻝㻡㻙㻝㻟㻦㻠㻡㻕㻝㻿㻙㻟

Application of layered chalcogenide materials to the aomic-layer electronics
Keiji Ueno㻟㻳㼑㼚㼑㼞㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㻌㻌㻔㻝㻟㻦㻠㻡㻙㻝㻠㻦㻠㻡㻕㻭㼜㼜㼘㼕㼏㼍㼠㼕㼛㼚㼟㻌㼛㼒㻌㼓㼞㼍㼜㼔㼑㼚㼑䚷䞉䚷㻼㼞㼛㼜㼑㼞㼠㼕㼑㼟㻌㼛㼒㻌㼓㼞㼍㼜㼔㼑㼚㼑㻌㻝㻙㻢

Vertical transport in meal/2D crystal/graphene layered heterostructures* Yoshihisa Inoue, Takehiro Yamaguchi, Sei Morikawa, Satoru Masubuchi, Kenji Watanabe,
Takashi Taniguchi, Rai Moriya, Tomoki Machida

xix

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㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻹㼍㼞㼏㼔㻌㻟㼞㼐㻘㻌㻹㼛㼚㻚
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Stabilities and Electronic Structures of Hexagonal Boron-Nitride Bilayers* Yoshitaka Fujimoto, Takashi Koretsune, Susumu Saito
Effect of Band Nesting on Optical Properties in Two-dimensional Transition Metal
Dichalcogenides* Daichi Kozawa, Rajeev Sharma Kumar, Alexandra Carvalho, Amara Kiran Kumar,
Weijie Zhao, Minglin Toh, Ricardo Mendes Ribeiro, Antonio H. Castro Neto,
Kazunari Matsuda, Goki Eda
Gate-controlled ultraviolet photo-etching of graphene edges* Ryo Nouchi, Nobuhiko Mitoma, Morihiro Matsumoto

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㻼㼛㼟㼠㼑㼞㻌㻼㼞㼑㼢㼕㼑㼣㻌㻌㻔㻝㻠㻦㻠㻡㻙㻝㻡㻦㻠㻡㻕㻼㼛㼟㼠㼑㼞㻌㻿㼑㼟㼟㼕㼛㼚㻌㻌㻔㻝㻡㻦㻠㻡㻙㻝㻣㻦㻟㻜㻕䚷䠄䖪䠅㻯㼍㼚㼐㼕㼐㼍㼠㼑㼟㻌㼒㼛㼞㻌㼠㼔㼑㻌㼅㼛㼡㼚㼓㻌㻿㼏㼕㼑㼚㼠㼕㼟㼠㻌㻼㼛㼟㼠㼑㼞㻌㻭㼣㼍㼞㼐㻯㼔㼑㼙㼕㼟㼠㼞㼥㻌㼛㼒㻌㼒㼡㼘㼘㼑㼞㼑㼚㼑㼟㻝㻼㻙㻝

Semiempirical molecular orbital estimation of the relative stability of sulfated fullerene* Naoki Noji, Yosiaki Sano, Kazumi Inoue, Yosuke Kataoka, Hironori Ogata

㻠㻟

㻝㻼㻙㻞

Excited State Electronic Interactions in Push–Pull-Chromophore–[60]Fullerene Conjugates* Michio Yamada, Francesca Tancini, Michael Sekita, Dirk M. Guldi, Mariza N. Alberti,
W. Bernd Schweizer, François Diederich㻠㻠㻭㼜㼜㼘㼕㼏㼍㼠㼕㼛㼚㼟㻌㼛㼒㻌㼒㼡㼘㼘㼑㼞㼑㼚㼑㼟
㻝㻼㻙㻟

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Synthesis of C60-C70 Two-Component Fullerene Nanowhiskers* Toshio Konno, Takatsugu Wakahara, Kun'ichi Miyazawa
Transport Characteristics of Fullerene Nano-Whisker Field Effect Transistor using Ionic
Liquid Gate
* Naoto Toriumi, Yoshiaki Ito, Daiki Momiyama, Wataru Akiyama, Naoto Nakamura,
Taishi Takenobu, Jonathan Bird, Yuichi Ochiai, Nobuyuki Aoki㻠㻡㻠㻢㻱㼚㼐㼛㼔㼑㼐㼞㼍㼘㻌㼙㼑㼠㼍㼘㼘㼛㼒㼡㼘㼘㼑㼞㼑㼚㼑㼟
㻝㻼㻙㻡
䖪
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Photoinduced Charge Separation in Supramolecules between Lithium-ion-encapsulated
PCBM Fullerene and Anionic Porphyrins* Yuki Kawashima, Kei Ohkubo, Hiroshi Okada, Yutaka Matsuo, Shunichi Fukuzumi
Formation mechanism of metallofullerenes suggested by the distribution of empty fullerenes* Tatsuki Kobayashi, Takeshi Kodama, Wataru Fujita, Koichi Kikuchi, Yohji Achiba㻠㻣㻠㻤㻲㼡㼘㼘㼑㼞㼑㼚㼑㼟
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㻝㻼㻙㻤
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Energetics of water molecules encapsulated into C 60 dimer* Kazuya Nomura, Susumu Okada
High-Resolution Transmission Electron Microscopic Study of Electron-Beam-Irradiated C60
Single Crystal Films* Hideki Masuda, Hidehiro Yasuda, Jun Onoe㻠㻥㻡㻜㻼㼞㼛㼜㼑㼞㼠㼕㼑㼟㻌㼛㼒㻌㼚㼍㼚㼛㼠㼡㼎㼑㼟㻝㻼㻙㻥

X-ray irradiation effect on the electric conductivity of single-walled carbon nanotube films* Takuma Araki, Toshiya Murakami, Kenji Kisoda, Chihiro Itohxx㻡㻝㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻹㼍㼞㼏㼔㻌㻟㼞㼐㻘㻌㻹㼛㼚㻚㻝㻼㻙㻝㻜䖪

Fluidized Bed CVD of Submillimeter-Long Carbon Nanotubes Using an Internal HeatExchange Reactor* Zhongming CHEN, Kei HASEGAWA, Dong Young KIM, Toshio OSAWA, Suguru NODA

㻡㻞

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Coherent G-band phonons in single wall carbon nanotubes* Ahmad Nugraha, Eddwi Hasdeo, Riichiro Saito

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Photochemical Behavior of Single-walled Carbon Nanotubes in the Presence of Propylamine* Yutaka Maeda, Yuhei Hasuike, Michio Yamada, Tadashi Hasegawa, Takeshi Akasaka

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In-situ Photoluminescence-spectroelectrochemistry of Oxygen-doped Single-walled Carbon
㻡㻡Nanotubes* Tomonari Shiraishi, Naoto Akizuki, Yuhei Miyauchi, Kazunari Matsuda, Naotoshi Nakashima㻝㻼㻙㻝㻠Far-Infrared and THz Spectroscopy of Multi-Walled Carbon Nanotubes* Keijiro Sakai, Takahiro Morimoto, Toshiya Okazaki

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Prediction of Redox Potentials of Semiconducting Single-Walled Carbon Nanotubes* Gergely Juhasz, Yasuhiko Hirana, Naotoshi Nakashima

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㻝㻼㻙㻝㻢
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Photoluminescence Spectroelectrochemistry of a Single SWNT Molecule* Liu Hong, Shinichiro Mouri, Yuhei Miyauchi, Kazunari Matsuda, Naotoshi Nakashima

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Electric Characterization of Chirality Controlled Single-Walled Carbon Nanotubes* Yusaku Tsuda, Takumi Sagara, Keisuke Yoshida, Koji Ishii, Kenichi Yamakawa,
Hirofumi Yajima, Nobuyuki Iwata, Hiroshi Yamamoto㻡㻥㻭㼜㼜㼘㼕㼏㼍㼠㼕㼛㼚㼟㻌㼛㼒㻌㼚㼍㼚㼛㼠㼡㼎㼑㼟
㻝㻼㻙㻝㻤
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㻝㻼㻙㻝㻥

㻝㻼㻙㻞㻜
䖪
㻝㻼㻙㻞㻝

㻝㻼㻙㻞㻞
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Hydrogen evolution from benzene with single-walled carbon nanotubes as a photocatalyst* Naoki Kohno, Kei Ohkubo, Shunichi Fukuzumi
High-throughput fabrication of carbon nanotube thin-film transistors with flexographic
printing process: Fabrication of short channel top-gate devices* Michihiko Maeda, Kentaro Higuchi, Shigeru Kishimoto, Yuta Nakajima, Takuya Tomura,
Masafumi Takesue, Katsuhiko Hata, Yutaka Ohno㻢㻜㻢㻝

Evaluation of Dynamic Performance of CNT Random Network Transistors* Noriyuki Tonouchi, Hiroyuki Endoh, Fumiyuki Nihey, Hideaki Numata, Tomoyuki Yokota,
Tsuyoshi Sekitani, Takao Someya, Manako Takashi㻢㻞Preparation of Al-CNT Nanocomposites using Mechanical Alloying* Takumi Goto, Yoshiki Terashima, Masaru Sekido

㻢㻟Multi-walled carbon nanotubes and carbon black supported platinum nanoparticles forcatalyst of polymer electrolyte membrane fuel cells* Zehui Yang, Berber Mohamed, Tsuyohiko Fujigaya, Naotoshi Nakashima
Low-voltage carrier injection into semiconductor thin film from CNT thin film utilizing fieldenhancement effect* Tatsuya Yamada, Shigeru Kishimoto, Yutaka Ohno
Highly durable membrane electrode assembly consists of poly(vinylphosphonic acid)polybenzimidazole electrolyte and carbon nanotubes based-electrocatalyst* Mohamed Berber, Tsuyohiko Fujigaya, Naotoshi Nakashima

xxi

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㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻹㼍㼞㼏㼔㻌㻟㼞㼐㻘㻌㻹㼛㼚㻚
㻝㻼㻙㻞㻡
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Single-Walled Carbon Nanotubes/Poly(Ionic Liquids) Nanocomposites for Extremely High
Thermovoltage* Motohiro Nakano, Yoshiyuki Nonoguchi, Takuya Nakashima, Tsuyoshi Kawai
Large-scale separation of eDIPS for application to TFTs
Shunjiro Fujii, Takeshi Tanaka, Tomoko Sugita, Satoshi Asano, Masaharu Kiyomiya,Takeshi Saito, * Hiromichi Kataura㻢㻣㻢㻤㻲㼛㼞㼙㼍㼠㼕㼛㼚㻌㼍㼚㼐㻌㼜㼡㼞㼕㼒㼕㼏㼍㼠㼕㼛㼚㻌㼛㼒㻌㼚㼍㼚㼛㼠㼡㼎㼑㼟
㻝㻼㻙㻞㻣

㻝㻼㻙㻞㻤
䖪
㻝㻼㻙㻞㻥

㻝㻼㻙㻟㻜

㻝㻼㻙㻟㻝
䖪
㻝㻼㻙㻟㻞

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Evaluation of the ratio of metal/semiconductive single-wall carbon nanotubes separated in
two immiscible aqueous solution phases by utilizing Raman spectroscopy technique
Naoki Kanazawa, * Shinzo Suzuki, Yu Tanaka, Akira Yamasaki, Daiki Miyazaki, Akira Ono
Single Chirality Separation and Optical Properties of Small-diameter Single-Wall Carbon
Nanotubes* Xiaojun Wei, Yasuhiro Ito, Takuya Hirakawa, Atsushi Hirano, Shunjiro Fujii,
Yuhei Miyauchi, Kazunari Matsuda, Takeshi Tanaka, Hiromichi Kataura
Fabrication of metal nanorods for the synthesis of short-carbon nanotubes* Takao Sada, Tsuyohiko Fujigaya, Naotoshi Nakashima
Growth of single-walled carbon nanotube from fullerene seeds by chemical vapor deposition
and in situ scanning electron microscopy observation* Huafeng Wang, Chisato Yamada, Hiroki Kato, Yoshikazu Homma
Rapid separation of high-purity and micrometer-long semiconducting carbon nanotubes by gel
filtration* Boanerges Thendie, Yasumitsu Miyata, Haruka Omachi, Ryo Kitaura, Yuhei Miyauchi,
Kazunari Matsuda, Hisanori Shinohara
Efficiency Synthesis of Double Wall Carbon Nanotubes by Pressure Control of Hightemperature Pulsed-arc Discharge* Hayato Kikuchi, Katsuhide Terada, Toshiki Sugai
Synthesis and Evaluation of Single-Walled Carbon Nanotubes Using Metal Catalyst Ni-Y-Mo* Bo Sun, Sakae Inoue, Tomoko Suzuki, Takayuki Yamamoto, Chihiro Yanagi, Yoshinori Ando
Studies on Chemical Reactions of Cobalt Clusters with Water and Oxygen by FT-ICR Mass
Spectrometer* Yuta Tobari, Kazuki Ogasawara, Shohei Chiashi, Shigeo Maruyama, Toshiki Sugai

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㻣㻝

㻣㻞

㻣㻟

㻣㻠

㻣㻡

㻣㻢

㻱㼚㼐㼛㼔㼑㼐㼞㼍㼘㻌㼚㼍㼚㼛㼠㼡㼎㼑㼟
㻝㻼㻙㻟㻡

㻝㻼㻙㻟㻢
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Encapsulating Carborane within Aligned and Dense Carbon Nanotubes on SiC Substrate* Hayato Fujita, Wataru Norimatsu, Michiko Kusunoki
Synthesis of a carbon nanotube filled with solid-phase separating stainless alloy by liquid andsolid interfacial arc discharge method* Takuya Sagara, Satoshi Kurumi, Ken-ichi Matsuda, Kaoru Suzuki
Containment method for transmission electron microscopy of gas molecules within the innerspace of carbon nanotubes under high vacuum* Keita Kobayashi, Takeshi Saito, Masaharu Kiyomiya, Hidehiro Yasuda

xxii

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㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻹㼍㼞㼏㼔㻌㻟㼞㼐㻘㻌㻹㼛㼚㻚㻺㼍㼚㼛㼔㼛㼞㼚㼟㻝㻼㻙㻟㻤Light-assisted in-situ polymer formation on carbon nanohorns
Mei Yang, * Minfang Zhang, Masao Kunioka, Sumio Iijima, Masako Yudasaka

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Selective carboxylation of graphite-like thin sheet edges in carbon nanohorn aggregates* Maki Nakamura, Michiko Irie, Ryota Yuge, Toshinari Ichihashi, Sumio Iijima,
Masako Yudasaka㻤㻝㻳㼞㼍㼜㼔㼑㼚㼑㻌㼟㼥㼚㼠㼔㼑㼟㼕㼟㻝㻼㻙㻠㻜

Topological Controlled Synthesis of Graphene Sheet* Chozo Inoue

㻤㻞

㻝㻼㻙㻠㻝
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Direct growth of graphene on dielectric substrates by etching-precipitation method* Masaki Kosaka, Kei Hasegawa, Suguru Noda

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CVD-growth of nitrogen-doped graphene using tetraphenyl porphyrin as a solid precursor* Yuma Sugisaki, Ryo Kitaura, Haruka Omachi, Hisanori Shinohara

㻤㻠

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In situ doping of Electrochemical foliation- Mechanism* Shang-Lin Tsai, Mario Hofmann, Ya-Ping Hsieh

㻤㻡

㻝㻼㻙㻠㻠

CVD Growth of Millimeter-Sized Graphene Grains on Heteroepitaxial Cu
Kenji Kawahara, T Iwaizako, Masaharu Tsuji, * Hiroki Ago㻤㻢㻼㼞㼛㼜㼑㼞㼠㼕㼑㼟㻌㼛㼒㻌㼓㼞㼍㼜㼔㼑㼚㼑㻝㻼㻙㻠㻡䖪

Quantum interference in a ballistic graphene n-p-n junction: from Fabry-Perot to edge
channel interference* Sei Morikawa, Satoru Masubuchi, Rai Moriya, Kenji Watanabe, Takashi Taniguchi,
Tomoki Machida

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Exciton-Exciton Annihilation in Monolayer Transition-Metal Dichalcogenides* Satoru Konabe, Susumu Okada

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㻝㻼㻙㻠㻣
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Edge-Roughness Effect on Electronic Transport in Semiconductor Graphene Nanoribbons* Kengo Takashima, Hiromu Fujii, Takahiro Yamamoto㻤㻥㻻㼠㼔㼑㼞㻌㼠㼛㼜㼕㼏㼟㻝㻼㻙㻠㻤䖪Temperature dependence of polarization-resolved photoluminescence in monolayer WSe2
㻥㻜
* Lizhong Zhou, Yuhei Miyauchi, Shinichiro Mouri, Minglin Toh, Goki Eda, Kazunari Matsuda

㻝㻼㻙㻠㻥Nonlinear Photoluminescence Properties in Monolayer Transition Metal Dichalcogenides* Shinichiro Mouri, Lizhong Zhou, Yuka Tsuboi, Yuhei Miyauchi, Minglin Toh,
Satoru Konabe, Goki Eda, Susumu Okada, Kazunari Matsuda

㻝㻼㻙㻡㻜
䖪

Photoluminescence Imaging of Monolayer MoS2 Synthesized by Chemical Vapor Deposition
Method* Yuka Tsuboi, Daichi Kozawa, Yuhei Miyauchi, Shinichiro Mouri, Kazunari Matsuda㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䠚䠚䠚䠚䠚䠚䠚㻌㻯㼛㼒㼒㼑㼑㻌㻮㼞㼑㼍㼗㻌㻌㻔㻝㻣㻦㻟㻜㻙㻝㻤㻦㻜㻜㻕㻌䠘䠘䠘䠘䠘䠘䠘㼀㼡㼠㼛㼞㼕㼍㼘㻌㻌㻔㻝㻤㻦㻜㻜㻙㻝㻥㻦㻟㻜㻕
Electronics applications of carbon nanotube thin films
Yutaka Ohno

xxiii

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㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻹㼍㼞㼏㼔㻌㻠㼠㼔㻘㻌㼀㼡㼑㻚㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻿㼜㼑㼏㼕㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㻦㻌㻞㻡㼙㼕㼚㻌㻔㻼㼞㼑㼟㼑㼚㼠㼍㼠㼕㼛㼚㻕㻌㻗㻌㻡㼙㼕㼚㻌㻔㻰㼕㼟㼏㼡㼟㼟㼕㼛㼚㻕㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻳㼑㼚㼑㼞㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㻦㻌㻝㻜㼙㼕㼚㻌㻔㻼㼞㼑㼟㼑㼚㼠㼍㼠㼕㼛㼚㻕㻌㻗㻌㻡㼙㼕㼚㻌㻔㻰㼕㼟㼏㼡㼟㼟㼕㼛㼚㻕㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻼㼛㼟㼠㼑㼞㻌㻼㼞㼑㼢㼕㼑㼣㻦㻌㻝㼙㼕㼚㻌㻔㻼㼞㼑㼟㼑㼚㼠㼍㼠㼕㼛㼚㻕㻿㼜㼑㼏㼕㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㻌㻌㻔㻥㻦㻜㻜㻙㻥㻦㻟㻜㻕㻞㻿㻙㻠Structure and Property Controlled Growth of Single-Walled Carbon Nanotubes on Substrates* Yan Li, Feng Yang, Xiaojun Qin, Fei Peng, Juan Yang㻠㻳㼑㼚㼑㼞㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㻌㻌㻔㻥㻦㻟㻜㻙㻝㻜㻦㻟㻜㻕㻲㼛㼞㼙㼍㼠㼕㼛㼚㻌㼍㼚㼐㻌㼜㼡㼞㼕㼒㼕㼏㼍㼠㼕㼛㼚㻌㼛㼒㻌㼚㼍㼚㼛㼠㼡㼎㼑㼟
㻞㻙㻝

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Molecular Simulations of Single-Walled Carbon Nanotube Growth and Chemical Reaction of
Catalyst Cluster* Kaoru Hisama, Tomoya Kawasuzuki, Takuya Noguchi, Shohei Chiashi, Tomofumi Tada,
Shigeo Maruyama
Synthesis and transfer properties of single-walled carbon nanotubes array withsemiconductor-type selectivity* Shunsuke Sakurai, Maho Yamada, Hiroko Nakamura, Don Futaba, Kenji Hata
Low-temperature catalyst activator: Mechanism study of CNT forest densification by “STEP”
growth method using synchrotron radiation
Akito Takashima, Yudai Izumi, Eiji Ikenaga, Takuo Ohkochi, Masato Kotsugi,
Tomohiro Matsushita, * Takayuki Muro, Akio Kawabata, Tomo Murakami, Mizuhisa Nihei,
Naoki Yokoyama
What causes a different behavior in the tube growth between (5,5) and (6,5) caps?
* Yohji Achiba, Takeshi Kodama, Kenro Hashimoto, Haruo Shiromaru

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㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䠚䠚䠚䠚䠚䠚䠚㻌㻯㼛㼒㼒㼑㼑㻌㻮㼞㼑㼍㼗㻌㻌㻔㻝㻜㻦㻟㻜㻙㻝㻜㻦㻠㻡㻕㻌䠘䠘䠘䠘䠘䠘䠘㻿㼜㼑㼏㼕㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㻌㻌㻔㻝㻜㻦㻠㻡㻙㻝㻝㻦㻝㻡㻕㻞㻿㻙㻡Interaction of carbon nanotube with water* Yoshikazu Homma, Shohei Chiashi, Takahiro Yamamoto㻡㻳㼑㼚㼑㼞㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㻌㻌㻔㻝㻝㻦㻝㻡㻙㻝㻞㻦㻝㻡㻕㻲㼛㼞㼙㼍㼠㼕㼛㼚㻌㼍㼚㼐㻌㼜㼡㼞㼕㼒㼕㼏㼍㼠㼕㼛㼚㻌㼛㼒㻌㼚㼍㼚㼛㼠㼡㼎㼑㼟㻌䞉㻌㻼㼞㼛㼜㼑㼞㼠㼕㼑㼟㻌㼛㼒㻌㼚㼍㼚㼛㼠㼡㼎㼑㼟㻌䞉㻌㻭㼜㼜㼘㼕㼏㼍㼠㼕㼛㼚㼟㻌㼛㼒㻌㼚㼍㼚㼛㼠㼡㼎㼑㼟
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Highly efficient purification of semiconducting single-walled carbon nanotubes using
detachable supramolecular solubilizer* Fumiyuki Toshimitsu, Nakashima Naotoshi
The effect of DNA adsorption on optical transitions in single-walled carbon nanotube* Masahiro Ito, Yuusuke Ito, Daisuke Nii, Kazuo Umemura, Hiroki Kato, Yoshikazu Homma
Mechanistic insight into the metal/semiconductor separation of single-wall carbon nanotubes
using hydrogels* Atsushi Hirano, Takeshi Tanaka, Hiromichi Kataura
Organic Film-Assisted Full-Length Electrical Breakdown for Arrays of Semiconducting
Single-Walled Carbon Nanotubes* Keigo Otsuka, Taiki Inoue, Shohei Chiashi, Shigeo Maruyama

xxiv

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㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻹㼍㼞㼏㼔㻌㻠㼠㼔㻘㻌㼀㼡㼑㻚㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䠚䠚䠚䠚䠚䠚䠚㻌㻸㼡㼚㼏㼔㻌㼀㼕㼙㼑㻌㻌㻔㻝㻞㻦㻝㻡㻙㻝㻟㻦㻟㻜㻕㻌䠘䠘䠘䠘䠘䠘䠘㻭㼣㼍㼞㼐㼟㻌㻯㼑㼞㼑㼙㼛㼚㼥㻌㻌㻔㻝㻟㻦㻟㻜㻙㻝㻠㻦㻝㻡㻕㻼㼛㼟㼠㼑㼞㻌㻼㼞㼑㼢㼕㼑㼣㻌㻌㻔㻝㻠㻦㻝㻡㻙㻝㻡㻦㻝㻡㻕㻼㼛㼟㼠㼑㼞㻌㻿㼑㼟㼟㼕㼛㼚㻌㻌㻔㻝㻡㻦㻝㻡㻙㻝㻣㻦㻜㻜㻕䚷䠄䖪䠅㻯㼍㼚㼐㼕㼐㼍㼠㼑㼟㻌㼒㼛㼞㻌㼠㼔㼑㻌㼅㼛㼡㼚㼓㻌㻿㼏㼕㼑㼚㼠㼕㼟㼠㻌㻼㼛㼟㼠㼑㼞㻌㻭㼣㼍㼞㼐㻯㼔㼑㼙㼕㼟㼠㼞㼥㻌㼛㼒㻌㼒㼡㼘㼘㼑㼞㼑㼚㼑㼟㻞㻼㻙㻝Investigation of molecular dynamics of fullernol solids by ²H NMR spectroscopy* Yoshiaki Sano, Keisuke Baba, Hironori Ogata

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Synthesis of a Novel Open-cage C60 Derivative with a Ketolactam Moiety* Yoshifumi Hashikawa, Michihisa Murata, Atsushi Wakamiya, Yasujiro Murata㻥㻠㻭㼜㼜㼘㼕㼏㼍㼠㼕㼛㼚㼟㻌㼛㼒㻌㼒㼡㼘㼘㼑㼞㼑㼚㼑㼟㻞㻼㻙㻟

A Novel Ligand-free ZnO Particle for Fullerene:Polymer Inverted Organic Solar Cell
* IL Jeon, James Ryan, Kee Sheng Yeo, Tafu Nakazaki, Yuichi Negishi, Yutaka Matsuo

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Synthesis of Penta(aryl)[60]fullerene Cobalt Dithiolene Complexes for Organic Solar Cells* Keisuke Ogumi, Takafumi Nakagawa, Yutaka Matsuo

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Characterization of surface layer of C 60 thin-film polymerized by optical vortex* Wataru Akiyama, Daiki Momiyama, Naoto Toriumi, Naoto Nakamura,
Katsuhiko Miyamoto, Takashige Omatsu, Jonathan P Bird, Yuichi Ochiai, Nobuyuki Aoki㻥㻣㻱㼚㼐㼛㼔㼑㼐㼞㼍㼘㻌㼙㼑㼠㼍㼘㼘㼛㼒㼡㼘㼘㼑㼞㼑㼚㼑㼟
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Extraction and Isolation of Missing Small-Bandgap Metallofullerenes through Exterior
Functionalization* Zhiyong Wang, Yusuke Nakanishi, Shoko Noda, Hiroyuki Niwa, Jinying Zhang,
Ryo Kitaura, Hisanori Shinohara
Supercapacitor using Lithium-Ion Endohedral Metallofullerene* Eunsang Kwon, Ken-ichirou Komatsu, Yoichi Yamada, Yuri Hasegawa, Sho Sato,
Seiji Sakai, Kazuhiko Kawachi, Kuniyoshi Yokoo, Shoichi Ono, Yasuhiko Kasama,
Shinobu Aoyagi, Tomoaki Endo, Tomoyuki Ogawa, Migaku Takahashi㻥㻤㻥㻥㻲㼡㼘㼘㼑㼞㼑㼚㼑㼟㻞㻼㻙㻤

Spin-state Tuning of Deca-Methyl C60 by an Electric Field* Kouhei Narita, Susumu Okada

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Geometric and electronic structures of two-dimensionally polymerized C32* Mina Maruyama, Susumu Okada㻝㻜㻝㻼㼞㼛㼜㼑㼞㼠㼕㼑㼟㻌㼛㼒㻌㼚㼍㼚㼛㼠㼡㼎㼑㼟㻞㻼㻙㻝㻜Electronic structure change of single-walled carbon nanotube by X-ray irradiation* Toshiya Murakami, Yuki Yamamoto, Mitsuaki Matsuda, Kenji Kisoda, Hiroshi Nishigaki,
Noriyuki Hasuike, Hiroshi Harima, Chihiro Itoh

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Anharmonic effects on phonons in single-walled carbon nanotubes* Masashi Mizuno, Riichiro Saito

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The Analysis of Exchange Reactions of Sodium Cholate and Double-Stranded DNA on Single㻝㻜㻠-Walled CNTs
* Akiko Tsuzuki, Naotoshi Nakashimaxxv㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻹㼍㼞㼏㼔㻌㻠㼠㼔㻘㻌㼀㼡㼑㻚
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Chirality Dependence of Quantum Thermal Transport in Carbon Nanotubes at Low
Temperatures: A First-Principles Study* Tomoyuki Hata, Hiroki Kawai, Tatsuhiko Ohto, Koichi Yamashita
Li-ion battery electrode property of anthraquinone molecules encapsulated in single-walledcarbon nanotubes* Shinji Kawasaki, Tomohiro Matsuura, Kosuke Tashiro, Hayong Song
Diameter dependence of RBM frequency of SWNTs in water vapor* Naoki Homma, Shohei Chiashi, Yoshikazu Homma, Takahiro Yamamoto
Optical Detection of DNA Hybridization and Denaturation on Single-Walled Carbon
Nanotube Surface* Yusuke Ito, Masahiro Ito, Daisuke Nii, Hiroki Kato, Kazuo Umemura, Yoshikazu Homma

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Observation of a gate-induced photoluminescence peak in individual carbon nanotubes* Yuto Ueda, Masahiro Yoshida, Akihiro Ishii, Takushi Uda, Yuichiro K. Kato

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Thermal Properties of SWNT Forest with Various Volume Fraction* JinHyeok Cha, Kei Hasegawa, Shohei Chiashi, Asuka Miura, Jeonyoon Lee,
Brian L Wardle, Suguru Noda, Junichiro Shiomi, Shigeo Maruyama㻝㻝㻜㻭㼜㼜㼘㼕㼏㼍㼠㼕㼛㼚㼟㻌㼛㼒㻌㼚㼍㼚㼛㼠㼡㼎㼑㼟
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In-plane conductivity of dense carbon nanotube forest on semi-insulating silicon carbide* Masafumi Inaba, Chih-Yu Lee, Kazuma Suzuki, Megumi Shibuya, Atsushi Hiraiwa,
Yoshiho Masuda, Wataru Norimatsu, Michiko Kusunoki, Hiroshi Kawarada
Systematic Conversion of Single Walled Carbon Nanotubes into n-type ThermoelectricMaterials by Molecular Dopants* Yoshiyuki Nonoguchi, Kenji Ohashi, Tsuyoshi Kawai
Evaluation of the contact resistivity and Schottky barrier height at carbon nanotubes/siliconcarbide interface* Kazuma Suzuki, Masafumi Inaba, Megumi Shibuya, Chih-Yu Lee, Miho Myodo,
Atsushi Hiraiwa, Yoshiho Masuda, Wataru Norimatsu, Michiko Kusunoki, Hiroshi Kawarada
Infra-Red Light Sensor using High-Purity Semiconducting Single-Wall Carbon Nanotube
Networks* Hikaru Kudo, Seiya Kaji, Hideki Kawai, Taishi Takenobu, Kazuhiro Yanagi
Operation Speed Improvement of Carbon Nanotube Integrated Circuits on Plastic Substrate* Toshitada Sanzen, Antti Kaskela, Patrik Laiho, Albert Nasibulin, Shigeru Kishimoto,Esko Kauppinen, Yutaka Ohno
Photovoltaic features of p-n homo-junction with position selective Cs encapsulated singlewalled carbon nanotubes thin films* Yoshihiro Abiko, Toshiaki Kato, Toshiki Akama, Rikizo Hatakeyama, Toshiro Kaneko
Molecular recognition on surfaces of metallic and semiconducting single-walled carbon
nanotubes* Wenxin Huang, Tsuyohiko Fujigaya, Naotoshi Nakashima

xxvi

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㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻹㼍㼞㼏㼔㻌㻠㼠㼔㻘㻌㼀㼡㼑㻚
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High Photovoltaic Performance of MoO3-doped Single-walled Carbon Nanotube/Si Solar
Cells* Feijiu Wang, Daichi Kozawa, Yuhei Miyauchi, Shinichiro Mouri, Yutaka Ohno,
Kazunari Matsuda
Solubility control of SWCNTs by using photofunctional dispersants* Yoko Matsuzawa, Yuko Takada, Hideyuki Kihara, Masaru Yoshida

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㻲㼛㼞㼙㼍㼠㼕㼛㼚㻌㼍㼚㼐㻌㼜㼡㼞㼕㼒㼕㼏㼍㼠㼕㼛㼚㻌㼛㼒㻌㼚㼍㼚㼛㼠㼡㼎㼑㼟
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Growth of CNT using the dip coat method as the catalyst support* Keisuke Fujii, Yoshinori Ando, Masato Ohkohchi
Chirality selective solubilization of single-walled carbon nanotubes using flavin andisoalloxazine derivatives* Masashi Fukuzawa, Fumiyuki Toshimitsu, Yuichi Kato, Naotoshi Nakashima

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Self-assembly of Highly Aligned Metallic/Semiconducting SWCNTs using Crystal Templates 㻝㻞㻞* Hideki Kawai, Kai Hasegawa, Yasuhisa Naitoh, Yuki Takagi, Yoshifumi Wada,
Taishi Takenobu, Kazuhiro Yanagi㻞㻼㻙㻟㻝Chirality selective desorption of SWCNTs using mixed surfactant gel column chromatography 㻝㻞㻟* Yohei Yomogida, Mayumi Tsuzuki, Atsushi Hirano, Shunjiro Fujii, Takeshi Tanaka,
Hiromichi Kataura

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FT-ICR Study of Chemical Reaction of Cobalt Clusters with Acetonitrile* Kazuki Ogasawara, Yuta Tobari, Shohei Chiashi, Toshiki Sugai, Shigeo Maruyama㻝㻞㻠㻱㼚㼐㼛㼔㼑㼐㼞㼍㼘㻌㼚㼍㼚㼛㼠㼡㼎㼑㼟
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Synthesis and TEM-based Structural Characterization of C 60-Flattened CNT Nanopeapods* Qing Wang, Ryo Kitaura, Yuta Yamamoto, Shigeo Arai, Hisanori Shinohara
Modulating the Electronic Properties of Multimeric Thiophene Oligomers by Utilizing
Carbon Nanotube Confinement* Takashi Yumura, Hiroki Yamashita
Energetics and Electronic Structures of Carbon Nanotubes Encapsulating Polycyclic
Aromatic Hydrocarbon Molecules* Shota Kigure, Susumu Okada

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Functionalization of Carbon Nanohorns for Targeted Photo-Thermal Cancer Therapy* Minfang Zhang, Mei Yang, Wuxiao Ding, Sumio Iijima, Masako Yudasaka
Quick charge/discharge properties of Li-ion battery using carbon-coated composites ofgraphites, vapor grown carbon fibers, and carbon nanohorns* Ryota Yuge, Noriyuki Tamura, Takashi Manako, Kaichiro Nakano, Kentaro Nakahara

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㻺㼍㼚㼛㼣㼕㼞㼑㼟㻞㻼㻙㻟㻤Synthesis and TEM structural characterizations of AgI nanowires formed inside carbon
nanospace* Shihono Naruse, Ryo Kitaura, Suguru Noda, Hisanori Shinohara

xxvii

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㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻹㼍㼞㼏㼔㻌㻠㼠㼔㻘㻌㼀㼡㼑㻚㻳㼞㼍㼜㼔㼑㼚㼑㻌㼟㼥㼚㼠㼔㼑㼟㼕㼟㻞㻼㻙㻟㻥High-yielding synthesis of graphene by supuercritical fluid* Nobuto Oka, Takaaki Tomai, Itaru Honma

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Fabrication of wide terraces on SiC (0001) for pit-free graphene growth in Ar atmosphere* Wang Chenxing , Hitoshi Nakahara, Koji Asaka, Yahachi Saito

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In situ observation of graphene formation on polycrystalline Cu* Huafeng Wang, Pei Zhao, Shohei Chiashi, Shigeo Maruyama, Yoshikazu Homma

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Interface structures between graphene and SiC formed in the nitrogen atmosphere* Yoshiho Masuda, Wataru Norimatsu, Michiko Kusunoki

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Preparation of multilayer graphene nanoribbons on very narrow graphene templates of
unzipped DWCNT* Haruki Kitakawa, Ryota Negishi, Hirofumi Tanaka, Minoru Fukumori, Takuji Ogawa,Yoshihiro Kobayashi㻝㻟㻡㻭㼜㼜㼘㼕㼏㼍㼠㼕㼛㼚㼟㻌㼛㼒㻌㼓㼞㼍㼜㼔㼑㼚㼑㻞㻼㻙㻠㻠䖪Flexible transistor and inverter of large-area WSe 2 thin film
* Kazuma Funahashi, Jiang Pu, Lain-Jong Li, Yoshihiro Iwasa, Taishi Takenobu

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Controlled doping in densely aligned graphene nanoribbons by covalent functionalization* Pablo Solís-Fernández, Mark Bissett, Masaharu Tsuji, Hiroki Ago㻝㻟㻣㻼㼞㼛㼜㼑㼞㼠㼕㼑㼟㻌㼛㼒㻌㼓㼞㼍㼜㼔㼑㼚㼑㻞㻼㻙㻠㻢Mechanism of photoluminescence in graphene oxide* Hiroyuki Yokoi, Takaaki Taniguchi, Michio Koinuma, Yasumichi Matsumoto

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Mechanisms of Near-Infrared Photoluminescence from Graphene Oxides* Daichi Kozawa, Yuhei Miyauchi, Shinichiro Mouri, Masao Ichida, Kazunari Matsuda

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Molecular dynamics simulation for water molecules between two graphene layers* Riichiro Saito, Masashi Mizuno㻝㻠㻜㻻㼠㼔㼑㼞㻌㼠㼛㼜㼕㼏㼟㻞㻼㻙㻠㻥Formation of fullerenes and polyynes by graphite laser ablation in ambient gases* Yurika Abe, Hitomi Endo, Yohji Achiba, Haruo Shiromaru

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Vibronic Interaction in the Forbidden Transition of Polyyne Molecules* Tomonari Wakabayashi㻝㻠㻞㻿㼜㼑㼏㼕㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㻌㻌㻔㻝㻣㻦㻜㻜㻙㻝㻣㻦㻟㻜㻕㻞㻿㻙㻢Chemistry of Fullerene Epoxides: Structure and Nucleophilic Substitution-Addition Reactivity
Yusuke Tajima㻢㻳㼑㼚㼑㼞㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㻌㻌㻔㻝㻣㻦㻟㻜㻙㻝㻤㻦㻟㻜㻕㻯㼔㼑㼙㼕㼟㼠㼞㼥㻌㼛㼒㻌㼒㼡㼘㼘㼑㼞㼑㼚㼑㼟䚷䞉㻌㻌㻭㼜㼜㼘㼕㼏㼍㼠㼕㼛㼚㼟㻌㼛㼒㻌㼒㼡㼘㼘㼑㼞㼑㼚㼑㼟䚷䞉㻌㻌㻌㻱㼚㼐㼛㼔㼑㼐㼞㼍㼘㻌㼙㼑㼠㼍㼘㼘㼛㼒㼡㼘㼘㼑㼞㼑㼚㼑㼟㻞㻙㻥

Anomeric effect on the ring conformation of spiro-acetalyzed [60]fullerenes* Ken Kokubo, Yu Yamazaki, Hiroyuki Masuda, Naohiko Ikuma

xxviii㻞㻢㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻹㼍㼞㼏㼔㻌㻠㼠㼔㻘㻌㼀㼡㼑㻚
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Spiro-acetalized and -thioacetalized [60]fullerene as efficient acceptor materials for bulk
heterojunction solar cells* Tsubasa Mikie, Akinori Saeki, Hiroyuki Masuda, Naohiko Ikuma, Ken Kokubo, Shu Seki㻞㻣

Dielectric Phase Transition of [Li@C 60](PF6) at Low Temperature㻞㻤* Shinobu Aoyagi, Kunihisa Sugimoto, Hiroshi Okada, Norihisa Hoshino, Tomoyuki Akutagawa
Photoinduced Electron Transfer and Photoelectrochemical Properties of SupramolecularComplexes Composed of Lithium Ion-Encapsulated Fullerene and Porphyrinoids* Kei Ohkubo, Yuki Kawashima, Hayato Sakai, Taku Hasobe, Angela Sastre-Santos,
Shunichi Fukuzumi

xxix

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㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻹㼍㼞㼏㼔㻌㻡㼠㼔㻘㻌㼃㼑㼐㻚㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻼㼘㼑㼚㼍㼞㼥㻌㻸㼑㼏㼠㼡㼞㼑㻦㻌㻠㻜㼙㼕㼚㻌㻔㻼㼞㼑㼟㼑㼚㼠㼍㼠㼕㼛㼚㻕㻌㻗㻌㻡㼙㼕㼚㻌㻔㻰㼕㼟㼏㼡㼟㼟㼕㼛㼚㻕㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻿㼜㼑㼏㼕㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㻦㻌㻞㻡㼙㼕㼚㻌㻔㻼㼞㼑㼟㼑㼚㼠㼍㼠㼕㼛㼚㻕㻌㻗㻌㻡㼙㼕㼚㻌㻔㻰㼕㼟㼏㼡㼟㼟㼕㼛㼚㻕㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻳㼑㼚㼑㼞㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㻦㻌㻝㻜㼙㼕㼚㻌㻔㻼㼞㼑㼟㼑㼚㼠㼍㼠㼕㼛㼚㻕㻌㻗㻌㻡㼙㼕㼚㻌㻔㻰㼕㼟㼏㼡㼟㼟㼕㼛㼚㻕㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻼㼛㼟㼠㼑㼞㻌㻼㼞㼑㼢㼕㼑㼣㻦㻌㻝㼙㼕㼚㻌㻔㻼㼞㼑㼟㼑㼚㼠㼍㼠㼕㼛㼚㻕㻼㼘㼑㼚㼍㼞㼥㻌㻸㼑㼏㼠㼡㼞㼑㻌㻌㻔㻥㻦㻜㻜㻙㻥㻦㻠㻡㻕㻟㻿㻙㻣

Floating catalyst CVD synthesis of SWNTs for thin film electronics applications
Esko I. Kauppinen㻣㻳㼑㼚㼑㼞㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㻌㻌㻔㻥㻦㻠㻡㻙㻝㻜㻦㻟㻜㻕㻭㼜㼜㼘㼕㼏㼍㼠㼕㼛㼚㼟㻌㼛㼒㻌㼚㼍㼚㼛㼠㼡㼎㼑㼟
㻟㻙㻝

㻟㻙㻞

㻟㻙㻟

A wet spinning method of a continuous polymer-free carbon nanotube fiber with the highelectrical conductivity* Ken Mukai, Kinji Asaka, Toshiya Murakami, Chihiro Itoh, Takeshi Saito, Motoo Yumura
Carbon nanotube 3D current collectors for lightweight, high performance and low cost
electrochemical capacitor electrodes* Ricardo Quintero, Dong Young Kim, Kei Hasegawa, Yuki Yamada, Atsuo Yamada,Suguru Noda

㻟㻜㻟㻝Green, scalable, binderless fabrication of a single-wall carbon nanotube nonwoven fabric㻟㻞
based on an ancient Japanese paper process* Kazufumi Kobashi, Tatsuya Hirabayashi, Seisuke Ata, Takeo Yamada, Don Futaba, Kenji Hata㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䠚䠚䠚䠚䠚䠚䠚㻌㻯㼛㼒㼒㼑㼑㻌㻮㼞㼑㼍㼗㻌㻌㻔㻝㻜㻦㻟㻜㻙㻝㻜㻦㻠㻡㻕㻌䠘䠘䠘䠘䠘䠘䠘㻳㼑㼚㼑㼞㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㻌㻌㻔㻝㻜㻦㻠㻡㻙㻝㻝㻦㻠㻡㻕㻭㼜㼜㼘㼕㼏㼍㼠㼕㼛㼚㼟㻌㼛㼒㻌㼓㼞㼍㼜㼔㼑㼚㼑㻟㻙㻠

Large-scale first-principles study of the electronic transport properties of graphene
nanoribbons on SiO2/Si* Hideyuki Jippo, Taisuke Ozaki, Mari Ohfuchi

㻟㻟

㻟㻙㻡

Analysis of intercalated multi-layer graphene synthesized by CVD* Daiyu Kondo, Haruhisa Nakano, Bo Zhou, Akiko I, Kenjiro Hayashi, Junichi Yamaguchi,
Makoto Takahashi, Shintaro Sato, Naoki Yokoyama

㻟㻠

㻟㻙㻢

Graphene as a Material for Next Generation Fuel Cells* Stephen Lyth, Jianfeng Liu, Thomas Bayer, Sean Bishop, Kazunari Sasaki

㻟㻡

㻟㻙㻣

Graphene enabled micromechanical switches* Shao-Wei Ma, Ya-Ping Hsieh㻟㻢㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌䠚䠚䠚䠚䠚䠚䠚㻌㻸㼡㼚㼏㼔㻌㼀㼕㼙㼑㻌㻌㻔㻝㻝㻦㻠㻡㻙㻝㻟㻦㻜㻜㻕㻌䠘䠘䠘䠘䠘䠘䠘㻼㼛㼟㼠㼑㼞㻌㻼㼞㼑㼢㼕㼑㼣㻌㻌㻔㻝㻟㻦㻜㻜㻙㻝㻠㻦㻜㻜㻕㻼㼛㼟㼠㼑㼞㻌㻿㼑㼟㼟㼕㼛㼚㻌㻌㻔㻝㻠㻦㻜㻜㻙㻝㻡㻦㻠㻡㻕䚷䠄䖪䠅㻯㼍㼚㼐㼕㼐㼍㼠㼑㼟㻌㼒㼛㼞㻌㼠㼔㼑㻌㼅㼛㼡㼚㼓㻌㻿㼏㼕㼑㼚㼠㼕㼟㼠㻌㻼㼛㼟㼠㼑㼞㻌㻭㼣㼍㼞㼐㻯㼔㼑㼙㼕㼟㼠㼞㼥㻌㼛㼒㻌㼒㼡㼘㼘㼑㼞㼑㼚㼑㼟㻟㻼㻙㻝

Thermal Bis-silylation, Carbosilylation, and Bis-germylation of Fullerenes* Daiki Inaba, Kazuya Minami, Kyosuke Miyabe, Ryosuke Iida, Masahiro Kako,
Yutaka Maeda, Michio Yamada, Tadashi Hasegawa, Takeshi Akasaka

xxx

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㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻹㼍㼞㼏㼔㻌㻡㼠㼔㻘㻌㼃㼑㼐㻚㻟㻼㻙㻞Synthesis of [60]Fullerene Derivative with 1,3-Dipolar Cycloaddition as a Novel Structure for㻝㻠㻠Bulk-Heterojunction Photovoltaic Cells* Hisashi Tokutomi, Masaru Sekido㻱㼚㼐㼛㼔㼑㼐㼞㼍㼘㻌㼙㼑㼠㼍㼘㼘㼛㼒㼡㼘㼘㼑㼞㼑㼚㼑㼟
㻟㻼㻙㻟
䖪
㻟㻼㻙㻠

Electrochemical synthesis of Li@C60 supraatom* Hiroshi Ueno, Naohiko Ikuma, Kei Ohkubo, Hiroshi Moriyama, Shunichi Fukuzumi,
Ken Kokubo
Separation of a missing small-bandgaped metallofullerene Gd@C60 by in situ
trifluoromethylation* Hiroyuki Niwa, Yusuke Nakanishi, Zhiyong Wang, Ryo Kitaura, Haruka Omachi,
Hisanori Shinohara

㻝㻠㻡

㻝㻠㻢

㻼㼞㼛㼜㼑㼞㼠㼕㼑㼟㻌㼛㼒㻌㼚㼍㼚㼛㼠㼡㼎㼑㼟㻟㻼㻙㻡

Spontaneous exciton dissociation in carbon nanotubes
Yusuke Kumamoto, Masahiro Yoshida, Akihiro Ishii, Akio Yokoyama, * Takashi Shimada,Yuichiro K. Kato

㻝㻠㻣

㻟㻼㻙㻢

Quantum interference effect in Raman spectra of metallic nanotubes and graphene* Eddwi H. Hasdeo, Ahmad R. T. Nugraha, Riichiro Saito

㻝㻠㻤

㻟㻼㻙㻣
䖪

Observation of Upconversion Photoluminescence from Single-walled Carbon Nanotubes* Naoto Akizuki, Yuhei Miyauchi, Shinichiro Mouri, Kazunari Matsuda

㻝㻠㻥

㻟㻼㻙㻤

Electronic structures of CNT with a defect under carrier accumulations* U Ishiyama, Susumu Okda

㻝㻡㻜

㻟㻼㻙㻥

㻟㻼㻙㻝㻜
䖪
㻟㻼㻙㻝㻝

Metal Deposition Effects on Photoluminescence and Raman Scattering Spectra of Suspended
Single-walled Carbon Nanotubes* Akihiko Ozao, Shohei Chiashi, Genta Yamaguchi, Yoshikazu Homma
NMR study of 13C enriched single-wall carbon nanotubes* Noboru Serita, Yusuke Nakai, Yasumitsu Miyata, Yutaka Maniwa, Takeshi Saito
Numerical study of electronic states in double-walled carbon nanotubes ---Formation of
metallic bands by covalent bridge between tubes--* Yuhei Natsume

㻝㻡㻝

㻝㻡㻞

㻝㻡㻟

㻟㻼㻙㻝㻞

Electronic Structure of Carbon and BN Nanotubes: A Comparative First Principles Study* Yuya Uchida, Takashi Koretsune, Susumu Saito

㻝㻡㻠

㻟㻼㻙㻝㻟

Photoconductivity spectroscopy of individual suspended carbon nanotubes* Takushi Uda, Yusuke Kumamoto, Masahiro Yoshida, Akihiro Ishii, Yuichiro K. Kato㻝㻡㻡㻭㼜㼜㼘㼕㼏㼍㼠㼕㼛㼚㼟㻌㼛㼒㻌㼚㼍㼚㼛㼠㼡㼎㼑㼟
㻟㻼㻙㻝㻠

㻟㻼㻙㻝㻡

Environment-friendly functionalization method to obtain water-dispersible carbon nanotubes
Mohammad Jellur Rahman, * Tetsu Mieno
A test for the growth of single-wall carbon nanotubes on the porous glass (PG) sheet by
ACCVD technique
Kyohei Nagao, * Shinzo Suzuki, Shinji Ogami, Yosuke Ito, Hiroshi Nagasawa, Yohji Achiba

xxxi

㻝㻡㻢

㻝㻡㻣

㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻹㼍㼞㼏㼔㻌㻡㼠㼔㻘㻌㼃㼑㼐㻚㻟㻼㻙㻝㻢

Molecular recognition on external grooves of bundled surfaces of single-walled carbon
nanotubes* Tsuyohiko Fujigaya, JongTae Yoo, Naotoshi Nakashima

㻝㻡㻤

㻟㻼㻙㻝㻣

Fabrication and Properties of Functionalized Multiwall Carbonnanotube/PA-6 Composite* Yoshimi Muraoka, Hiroki Sato, Masaru Sekido

㻝㻡㻥

㻟㻼㻙㻝㻤

Printed SWCNT thin film CMOS inverters based on chemically doped ion gels
* Yoshifumi Wada, Ryota Inukai, Taiyo Fujimoto, Hiroki Hamahata, Satoki Matsuzaki,
Kazuhiro Yanagi, Taishi Takenobu

㻝㻢㻜

䖪
㻟㻼㻙㻝㻥

Surface modification of multi-walled carbon nanotubes with benzyl radical derivatives
generated by photo-irradiation* Tomoya Takada, Batbuyan Munkh-od, Shigeaki Abe㻝㻢㻝”Laminated” ion-gel film as high capacitance insulator for carbon-nanotube transistor* Taiyo Fujimoto, Ryo Shimizu, Yuki Takagi, Yoshifumi Wada, Kazuhiro Yanagi,
Taishi Takenobu

㻝㻢㻞

㻟㻼㻙㻞㻝

Polyglycerol-functionalized single-walled carbon nanotubes for drug loading and delivery* Qin Hongmei, Li Zhao, Keisuke Nakamura, Takahide Kimura, Naoki Komatsu

㻝㻢㻟

㻟㻼㻙㻞㻞
䖪

Simple and loss-free printing of carbon nanotubes for flexible electronics* Hiroyuki Shirae, Dong Yong Kim, Kei Hasegawa, Suguru Noda

㻝㻢㻠

㻟㻼㻙㻞㻟

Chemical Vapor Deposition of MoS2 on Carbon Nanotube for Organic Thin Film Solar Cells* IL JEON, Dai Kutsuzawa, Yu Hashimoto, Takashi Yanase, Taro Nagahama,Toshihiro Shimada, Yutaka Matsuo

㻝㻢㻡

㻟㻼㻙㻞㻠

Dispersion of SWCNTs in Wrapping of Belt-Type pi-Conjugated Polymer* Wataru Sagawa, Masahiro Takahashi, Keiki Kishikawa, Shigeo Kohmoto

㻝㻢㻢

㻟㻼㻙㻞㻜
䖪

㻲㼛㼞㼙㼍㼠㼕㼛㼚㻌㼍㼚㼐㻌㼜㼡㼞㼕㼒㼕㼏㼍㼠㼕㼛㼚㻌㼛㼒㻌㼚㼍㼚㼛㼠㼡㼎㼑㼟
㻟㻼㻙㻞㻡

㻟㻼㻙㻞㻢
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㻟㻼㻙㻞㻣

Chirality purification of DNA-wrapped single-walled carbon nanotubes toward thin filmtransistors* Yuki Kuwahara, Fumiyuki Nihey, Shigekazu Ohmori, Takeshi Saito
Effects of pulse conditions on growth of (6,5) enriched single-walled carbon nanotubes underpulse plasma CVD* Bin Xu, Toshiaki Kato, Koshi Murakoshi, Toshiro Kaneko
Selective recognition of semiconducting single-walled carbon nanotubes with large diameters
by using polyfluorenes carrying mono-alkyl chain* Takahiro Fukumaru, Fumiyuki Toshimitsu, Tsuyohiko Fujigaya, Naotoshi Nakashima

㻝㻢㻣

㻝㻢㻤

㻝㻢㻥

㻟㻼㻙㻞㻤

Cloning Growth of Single-Walled Carbon Nanotubes from Activated Nanotube Edges* Takanori Umino, Taiki Inoue, Shohei Chiashi, Shigeo Maruyama

㻝㻣㻜

㻟㻼㻙㻞㻥
䖪

Growth of high-density carbon nanotube arrays toward thermal interface materials* Nuri Na, Kei Hasegawa, Suguru Noda

㻝㻣㻝

㻟㻼㻙㻟㻜

Selective Growth of Single-Walled Carbon Nanotubes with Specific Diameter and Chirality
by Irradiating Free Electron Laser during Growth* Keisuke Yoshida, Takumi Sagara, Yusaku Tsuda, Koji Ishii, Kenichi Yamakawa,
Hirofumi Yajima, Nobuyuki Iwata, Hiroshi Yamamoto

xxxii

㻝㻣㻞

㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻹㼍㼞㼏㼔㻌㻡㼠㼔㻘㻌㼃㼑㼐㻚㻱㼚㼐㼛㼔㼑㼐㼞㼍㼘㻌㼚㼍㼚㼛㼠㼡㼎㼑㼟
㻟㻼㻙㻟㻝
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㻟㻼㻙㻟㻞

Tuning the Seebeck coefficient of single-wall carbon nanotubes by encapsulation of guest
materials* Tomohiro Ueda, Yusuke Nakai, Yasumitsu Miyata, Yutaka Maniwa
Molecular structure of the thiophene oligomers encapsulated in single-walled carbon
nanotubes by molecular dynamics simulations* Hiromu Tabata, Akinori Sekine, Kazumi Inoue, Yousuke Kataoka, Hironori Ogata

㻝㻣㻟

㻝㻣㻠

㻳㼞㼍㼜㼔㼑㼚㼑㻌㼟㼥㼚㼠㼔㼑㼟㼕㼟㻟㻼㻙㻟㻟䖪Influence of growth substrates on chemical reactivity of CVD graphene* Ryosuke Inoue, Yasumitsu Miyata, Yutaka Maniwa

㻝㻣㻡

㻟㻼㻙㻟㻠

Synthesis and Characterization of Metal Intercalated bilayers Graphene* Kentaro Imai, Kuniharu Matsuki, Shogo Sato, Nobuyuki Iwata, Hiroshi Yamamoto

㻝㻣㻢

㻟㻼㻙㻟㻡
䖪

CVD Growth of Graphene Nanoribbons on Cu (100) Film
* Rozan Mohamad Yunus, Masahiro Miyashita, Masaharu Tsuji, Hiroki Hibino, Hiroki Ago

㻝㻣㻣

㻟㻼㻙㻟㻢

Liquid-phase exfoliation of graphene from graphite with triphenylene derivatives* Ryusuke Funahashi, Gang Liu, Shuji Aonuma, Tkahide Kimura, Naoki Komatsu

㻝㻣㻤

㻟㻼㻙㻟㻣
䖪
㻟㻼㻙㻟㻤

Plasma effects on growth of graphene nanoribbon from nickel nanobar under rapid heatingplasma CVD* Hiroo Suzuki, Toshiaki Kato, Toshiro Kaneko
Influence of electrolyte concentration for electrochemical exfoliation of graphene* Haruya Okimoto, Hiroki Kuronuma, Masahito Sano

㻝㻣㻥

㻝㻤㻜

㻭㼜㼜㼘㼕㼏㼍㼠㼕㼛㼚㼟㻌㼛㼒㻌㼓㼞㼍㼜㼔㼑㼚㼑㻟㻼㻙㻟㻥䖪High gain CMOS inverters based on transition metal dichalcogenides* Jiang Pu, Jing-Kai Huang, Yoshihiro Iwasa, Lain-Jong Li, Taishi Takenobu

㻝㻤㻝

㻟㻼㻙㻠㻜

High efficiency graphene doping* Kai-Wen Cheng, Po-shin Lin, Ya-Ping Hsieh㻝㻤㻞㻼㼞㼛㼜㼑㼞㼠㼕㼑㼟㻌㼛㼒㻌㼓㼞㼍㼜㼔㼑㼚㼑㻟㻼㻙㻠㻝Drastic Change in Photoluminescence Properties of Size-separated Graphene Quantum Dots
* Naoto Fuyuno, Daichi Kozawa, Yuhei Miyauchi, Shinichiro Mouri, Ryo Kitaura,
Hisanori Shinohara, Toku Yasuda, Naoki Komatsu, Kazunari Matsuda

㻝㻤㻟

㻟㻼㻙㻠㻞
䖪

Energetics and Electronic Structure of Graphene Edges* Ayaka Yamanaka, Susumu Okada

㻝㻤㻠

㻟㻼㻙㻠㻟

Fine Control of Oxidation of Graphitic Carbons by Oxidation of Graphite or Reduction ofHighly Oxidized Graphene Oxide
Yuta Nishina, * Naoki Morimoto㻝㻤㻡㻯㼍㼞㼎㼛㼚㻌㼚㼍㼚㼛㼜㼍㼞㼠㼕㼏㼘㼑㼟㻟㻼㻙㻠㻠Structural and magnetic changes of nanodiamond-copper composites during HPHT Sintering
Process
Fedor Shakhov, Vladimir Osipov, Sergei Kidalov, * Kazuyuki Takai, Toshiaki Enoki,
Alexander Vul’

xxxiii㻝㻤㻢㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻌㻹㼍㼞㼏㼔㻌㻡㼠㼔㻘㻌㼃㼑㼐㻚
㻟㻼㻙㻠㻡

㻟㻼㻙㻠㻢

Synthesis and characterization of Pt , Pt-Ru nanoparticles on carbon nanomaterials by onestep electrodeposition* Shohei Hayase, Haruhiko Yoshitake, Wang Zhipeng, Hironori Ogata
Hydration of Nanodiamond Surface Revisited : Intercalation Hypothesis* Ryoko Yamanoi, Amanda Barnard, Shuichi Sasaki, Eiji Osawa

㻝㻤㻣

㻝㻤㻤

㻻㼠㼔㼑㼞㻌㼠㼛㼜㼕㼏㼟
㻟㻼㻙㻠㻣

㻟㻼㻙㻠㻤
䖪
㻟㻼㻙㻠㻥
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㻟㻼㻙㻡㻜

Doping of zinc to the iron oxide nanotubes by using a poly-condensation of metal nitrate
hydrates on the surface of self-assembled surfactant* Yuta Kosugi, Shunji Bandow
Synthesis of high purity carbon nanocoils on the sheet-like carbon deposits and reduction of
byproducts using Fe fine particles* Yoshiaki Shimizu, Koji Maruyama, Tetsuo Iida, Yoshiyuki Suda, Hideto Tanoue,
Hirofumi Takikawa, Hitoshi Ue, Kazuki Shimizu, Yoshito Umeda
Synthesis and characterization of two-dimensional semiconductor heterojunction based ontransition metal dichalcogenides* Shohei Mori, Yasumitsu Miyata, Yutaka Maniwa
Electro-Chemical Doping Properties of MoS2-Single Wall Carbon Nanotube Hybrid Film
Hideaki Endo, * Hideki Kawai, Kai Hasegawa, Seiya Kaji, Kazuhiro Yanagi

㻝㻤㻥

㻝㻥㻜

㻝㻥㻝

㻝㻥㻞

㻿㼜㼑㼏㼕㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㻌㻌㻔㻝㻡㻦㻠㻡㻙㻝㻢㻦㻝㻡㻕㻟㻿㻙㻤Graphene R&D conducted in Sony
Solution-processed TFTs and CVD-grown transparent conductive films
Toshiyuki Kobayashi㻤㻳㼑㼚㼑㼞㼍㼘㻌㻸㼑㼏㼠㼡㼞㼑㻌㻌㻔㻝㻢㻦㻝㻡㻙㻝㻣㻦㻟㻜㻕㻼㼞㼛㼜㼑㼞㼠㼕㼑㼟㻌㼛㼒㻌㼓㼞㼍㼜㼔㼑㼚㼑䚷䞉㻌㻌㻭㼜㼜㼘㼕㼏㼍㼠㼕㼛㼚㼟㻌㼛㼒㻌㼓㼞㼍㼜㼔㼑㼚㼑䚷䞉㻌㻌㻳㼞㼍㼜㼔㼑㼚㼑㻌㼟㼥㼚㼠㼔㼑㼟㼕㼟㻌㻌
㻟㻙㻤

㻟㻙㻥

㻟㻙㻝㻜

Twisting angle dependence of G band Raman intensity enhancement of twisted bilayer
graphene* Kentaro Sato, Riichiro Saito
Nitrogen-containing graphene analyzed by X-ray photoelectron spectroscopy* Yasuhiro Yamada, Junpil Kim, Shintaro Matsuo, Satoshi Sato
Optical and Raman Analysis of Graphene Films Formed within Microholes on Quartz Glass
Substrates by Liquid Phase Growth Method* Hidefumi Hiura

㻟㻣

㻟㻤

㻟㻥

㻟㻙㻝㻝

Novel transfer method for clean and high mobility CVD graphene
Ya-Ping Hsieh, Mario Hofmann, * Bo-Suei Chiang

㻠㻜

㻟㻙㻝㻞

Mechanism and impact of ad-layer formation on CPCVD graphene* Yi-Wen Wang, Ya-Ping Hsieh, Mario Hofmann

㻠㻝

xxxiv

ᇶㄪㅮ₇
Plenary Lecture≉ูㅮ₇Special Lecture

1S – 1 㹼 1S – 3
2S – 4 㹼 2S – 6
3S – 7 㹼 3S – 8

1S-1
Current Status and Vision of Fullerene Business in Mitsubishi Corporation
Mikio Sasaki
Former ChairmanࠊSenior Advisor To The Board, Mitsubishi Corporation,
Japan

Tokyo 100-8086,

Mitsubishi Corporation established Frontier Carbon Corporation in Y2001 as a world’s
frontrunner, and has been persistently supplying fullerene products for the researchers anddevelopers. Approximately 20 years has passed since my encounter to fullerene which wasin Y1993. Our initial vision, our business attempts, and future vision toward nano carbon
will be presented from Mitsubishi Corporation’s perspective.
1㸬
2㸬
3㸬
4㸬
5㸬

First Encounter to Fullerene
Incubation of Fullerene Business
R&D Strategy and Fullerene Business Status of Mitsubishi Corporation
Vision of Fullerene Business
Expectation toward Researcher, Developer, and Companies

--

1S-2
Critical factors in multi-walled carbon nanotubes
in mesothelial carcinogenesisżShinya Toyokuni
Department of Pathology and Biological Responses, Nagoya University Graduate School of
Medicine, 65 Tsurumai-cho, Showa-ku, Nagoya 466-8550, Japan
Multi-walled carbon nanotubes (MWCNTs) have potential for widespread applications inengineering and materials science. However, due to their needle-like, nanoscale shape andhigh durability, concerns have been raised that MWCNTs of certain characteristics may
induce asbestos-like pathogenicity. Even though recent studies have demonstrated various
types of reactivities induced by MWCNTs, the physicochemical features of MWCNTs that
determine or trigger the cytotoxicity and carcinogenicity in mesothelial cells remain unclear.
In the present study we show that the deleterious effects of non-functionalised MWCNTs on
human mesothelial cells are associated with their diameter-dependent piercing of the cell
membrane. Thin MWCNTs with high crystallinity showed mesothelial cell piercing andcytotoxicity in vitro and subsequent mesotheliomagenicity in vivo. In contrast, thick ortangled MWCNTs were much less toxic and carcinogenic, whereas all MWCNTs affected
macrophages similarly. Furthermore, we show that the target genes for MWCNT-induced
mesothelial carcinogenesis were the same as those by asbestos. Our results suggest that
control of the diameter of MWCNTs may contribute to reduce the risks to human health. The
final results of carcinogenesis study along with those of asbestos study will also be shown.
[1] S. Toyokuni. Nagoya J. Med. Sci. 71, 1 (2009).
[2] H. Nagai et al. Proc. Natl. Acad. Sci. U.S.A. 108, E1330 (2011).
[3] L. Jiang et al. J. Pathol. 228, 366 (2012).
[4] S. Toyokuni. Adv. Drug Deliv. Rev. [Epub ahead of print] (2013).
[5] H. Nagai et al. Pathol. Int. 63, 457 (2013).
Corresponding Author: S. Toyokuni
Tel: +81-52-744-2086, Fax: +81-52-744-2091,
E-mail: toyokuni@med.nagoya-u.ac.jp

--

1S-3
Application of layered chalcogenide materials
to the aomic-layer electronics
żKeiji Ueno1
1

Graduate School of Science and Engineering, Saitama University, Saitama 338-8570, Japan

Graphene, a unit layer of graphite, is now widely and progressively studied due to its novel
physical properties. Meanwhile, other layered materials having similar stacking structures tographene are also attracting much attention. Like graphene, new properties of their single- or
few-layer flakes are actively investigated. Device fabrication is also studied using singlecrystalline films of semiconducting layered materials, which have finite band gaps unlike
graphene [1,2]. In the presentation, I will introduce kinds, properties, and thin film
preparation methods of layered chalcogenide materials. My recent studies on the fabricationof field-effect transistors (FETs) of layered chalcogenides will be also presented.
Figure 1 shows the crystal structure of 2Hb-MoS2. Its single unit-layer consists of S-Mo-S
three atomic layers connected by strong covalent bonds, and unit-layers are bound together by
weak van der Waals forces [3]. It can be easily cleaved by anadhesive tape like graphite, and single- or few-layer flakes can betransferred onto SiO2/Si gate substrates. Figure 2 is an optical imageof MoS2 FET prepared from the transferred MoS2 flake. Source anddrain electrodes were fabricated by painting gold paste onto theflake. On the SiO2 gate dielectric surface, a self-assembledMo
monolayer of hexamethyldisilazane (HMDS) was deposited toS
reduce carrier traps. Figure 3 shows a cross-sectional view of FET.
By inserting the HMDS layer, the field-effect carrier mobility was
Fig.1 Crystal structure
drastically improved to 39 cm2/Vs.
of 2Hb-MoS2.
Until now, only n-type FETs have been obtained from MoS2
MoS2
flakes. In the case of WSe2, however, both n- and p-type FETs havebeen realized by using artificial single-crystals grown by the vapor
Au
Au
transport method. N-type crystals were obtained when I2 was added
as a transport agent, and p-type ones could be grown when no50 ȝm
halogen agent was used. The carrier type and density of crystals
were determined by Hall effect measurements, and their FETs were
Fig.2 Optical image of
MoS2 FET.
fabricated like MoS2 FETs. Figure 4 shows output characteristics ofn- and p-type WSe2 FETs prepared from n- and p-type single
㻭㼡㻌
㻭㼡㻌
㻴㻹㻰㻿
㻹㼛㻿㻞㻌
crystals, respectively. Other FETs prepared from various layered㻿㼕㻻㻞㻌
chalcogenide materials will be introduced in the presentation.
㻿㼕㻌[1] M. Xu et al., Chem. Rev. 113, 3766 (2013).
[2] S. Z. Butler et al., ACS Nano 7, 2898
(2013).
[3] J. A. Wilson and A. D. Yoffe, Adv. Phys.
18, 193 (1969).
Corresponding Author: K. Ueno
Tel: +81-48-858-3388, Fax: +81-48-858-3388,
E-mail: kei@chem.saitama-u.ac.jp

Fig.3 Cross section of
MoS2 FET.
n-WSe2
ȝe = 59 cm2/Vs

p-WSe2
ȝh = 20 cm2/Vs

Fig.4 Output characteristics of n- and p-type WSe2 FETs.

--

2S-4
Structure and Property Controlled Growth of Single-Walled Carbon
Nanotubes on SubstratesżYan Li, Feng Yang, Xiaojun Qin, Fei Peng, Juan Yang
Beijing National Laboratory for Molecular Science, Key Laboratory for the Physics andChemistry of Nanodevices, State Key Laboratory of Rare Earth Materials Chemistry andApplications, College of Chemistry and Molecular Engineering, Peking University, Beijing
100871, China
Controlled growth of single-walled carbon nanotubes (SWNTs) chemical vapor deposition(CVD) on insulating substrates is a crucial issue for the application of SWNTs innanoelectronics. In the growth process, catalysts play an essential role in controlling thestructure of SWNTs. Over the years, we have systematically studied the controlled synthesisof catalyst nanoparticles and also developed some new catalysts. By careful design ofcatalysts, high quality SWNTs and the structure/property controlled growth of SWNTs wereachieved. Figure 1 shows that by using ceria as catalyst supports, we were able to growsemiconducting SWNTs at the content of >95%.

Figure 1. (a-c) Raman spectra of SWNTs synthesized with unreduced Fe/CeO2 measured with 532 nm laser (a)and 633 nm laser (b) and Fe/SiO2 measured by 532 nm laser (c), respectively. (d,e) Statistics of m-SWNTs(denoted as M) and s-SWNTs (denoted as S) by using Fe/CeO2 reduced with H2 for 0 min and 10 minutes andFe/SiO2 measured with 532 nm laser (d) and 633 nm laser (e), respectively. (f) Photoluminescence (PL) spectraof SWNTs synthesized by using unreduced Fe/CeO2 excited with 532 nm laser. The broad peaks marked withstar (*) correspond to the PL spectra of silicon.
[1] Y. Li et al., Adv. Mater. 22, 1508(2010)[2] W. Zhou et al., Nano Lett. 6, 987(2006).
[3] Z. Jin et al., Nano Lett. 7, 2073(2007).
[4] Y. Liu et al., Adv. Funct. Mater. 21, 986(2011).
[5] X. Qin et al., Nano Lett., DOI 10.1021/nl403515c
Corresponding Author: Yan Li
Tel& Fax: +86-10-6275-6773
E-mail: yanli@pku.edu.cn

--

2S-5
Interaction of carbon nanotube with waterżYoshikazu Homma1, Shohei Chiashi2, Takahiro Yamamoto3
1

Dept. of Physics, Tokyo University of Science, Shinjuku, Tokyo 162-8601, Japan
Dept. of Mechanical Engineering, The University of Tokyo, Bunkyo, Tokyo 113-8656, Japan
3
Dept. of Liberal Arts, Tokyo University of Science, Katsushika, Tokyo 125-8585, Japan2

The interaction between water molecules and a non-polar surface is of great interest.
Hydrophobicity of graphene surface is under intense debate [1]. Although the interaction of anon-polar surface with water molecules is weaker than that between water molecules, it does
exist. Single-walled carbon nanotubes (SWNTs) are ideal for the study of the interaction. The
van der Waals potential originates only from carbon atoms in a single atomic layer, and thesurface is inert and smooth owing to sp2 carbon-carbon bonds. The effect of water molecule
adsorption on an SWNT can be probed by optical measurements resonant to the
one-dimensional singular density of states of electrons, because the optical transitions in themonolayer material are strongly influenced by the surrounding environment. Furthermore, thephenomena occurring on SWNTs can be simulated with molecular dynamics (MD).
We have performed photoluminescence (PL) and Raman scattering spectroscopic
measurements using individual SWNTs suspended between micropillars and MD simulationsof the SWNT-water system to investigate the behavior of water molecules on/in SWNTs [2,3].
We found that water molecules form a stable adsorption layer of 1–2 monolayer thickness on
the outer surface of nanotube and they show rapid adsorption and desorption transition at a
critical pressure (10-2 of saturation vapor pressure). This adsorption layer is created by lateralhydrogen bonding of water molecules trapped in the weak van der Waals potential of thesurface. It is thermodynamically in equilibrium with the external vapor phase at room
temperature. MD simulation showed that the layer persists even in liquid water. Thesefeatures indicate that the condensed water layer is not a part of bulk water or a simple
adsorption layer. It is a few-layer liquid phase of water, which differs from bulk solid, liquidand vapor phases. In spite of hydration, carbon nanotubes exhibit hydrophobicity
macroscopically.
Water molecules confined in SWNTs take different configurations from that on the SWNT
surface because of the steric hindrance due to a small tube diameter. Thus, the transitionpressure and temperature of encapsulation are different from those of adsorption. Water
encapsulation can also be probed by PL and Raman scattering spectroscopic measurements.
[1] Editorial, Nat. Mater. 12, 865 (2013).
[2] Y. Homma et al. Phys. Rev. Lett. 110, 157402 (2013).
[3] S. Chiashi et al. J. Phys. Chem. Lett. 5, 408 (2014).
Corresponding Author: Y. Homma
Tel: +81-3-5228-8244, Fax: +81-3-5261-1023,
E-mail: homma@rs.tus.ac.jp

--

2S-6
Chemistry of Fullerene Epoxides: Structure and Nucleophilic
Substitution-Addition ReactivityżYusuke Tajima1,21Organic Optoelectronics Laboratory, RIKEN, Wako, Saitama 351-0198, Japan
2
FLOX Corporation, Kawasaki, Kanagawa 210-0858, Japan
Fullerene epoxides, C60On, having epoxide groups directly attached to the fullerene cage,
constitute an interesting class of fullerene derivatives. In particular, the chemicaltransformations of fullerene epoxides are expected to play an important role in thedevelopment of functionalized fullerenes. This is because such transformations can readily
afford a variety of mono- or polyfunctionalized fullerene derivatives while conserving theepoxy ring arrangement on the fullerene surface, as seen in representative regioisomericfullerene polyepoxides. The first part of this lecture addresses the synthesis and structuralcharacterization of fullerene epoxides. The formation of fullerene epoxides through different
oxidation reactions is then explored. Adequate characterization of the isolated fullerene
epoxides was achieved by concerted use of NMR and LC-MS techniques [1]. The second partof this lecture describes the substitution of fullerene epoxides in the presence of a Lewis acidcatalyst. Most major substitution products have been isolated as pure compounds and theirstructures established through spectroscopic methods [2]. The correlation between the
structure of the substitution product and the oxygenation pattern of the starting materials
allows elucidation of the mechanistic features of this transformation. This approach promises
to lead to rigorous regioselective production of various fullerene derivatives for a wide range
of applications.
O
O
O

O

O

1b (cis-1 isomer)1a1c (equatorial isomer)

Figure. Fullerene mono-epoxide and regioisomeric di-epoxides.
R1 R2
O

O

+

R1
O

R2
1a

O

Catalyst
in Toluene
75RC

2

3

Scheme. Acetalization of fullerene epoxide 1a with carbonyl compound.
[1] Y. Tajima and K. Takeuchi, J. Org. Chem. 67, 1696 (2002).
[2] Y. Tajima, et al. Molecules, 17, 6395 (2012).
Corresponding Author: Y. Tajima
Tel: +81-48-467-5499, Fax: +81-48-467-5689,
E-mail: tajima@riken.jp

--

3S-7
FLOATING CATALYST CVD SYNTHESIS OF SWNTs
FOR THIN FILM ELECTRONICS APPLICATIONS
Esko I. Kauppinen
Department of Applied Physics, Aalto University School of Science
Puumiehenkuja 2, P.O. Box 16100, FI-00076 Aalto, FINLAND

esko.kauppinen@aalto.fi
We discuss (n,m) distributions of our floating catalyst chemical vapor deposition(FFCVD) synthesis of SWCNTs from CO using Fe catalyst clusters made via direct evaporation
using hot wire generator as well as via thermal decomposition of ferrocene, and with the additionof trace amounts for CO2 and water vapor. Here both the tube diameter as well as length can be
tailored by changing the reactor temperature profile as well as CO2 concentration. Chiral i.e. (n,m)
distribution as determined with ED/TEM is biased towards large chiral angles with the maximum
population at about 23 degrees. Then we proceed to explore the effect of carbon source gas, byadding C2H4 together with CO and looking at the effect of temperature when producing catalysts
via ferrocene decomposition.
To study the effect of Fe catalyst cluster size and concentration in the floating catalyst
synthesis, we have developed a novel catalyst particle production method via physical vapor
deposition, based on arc discharge between two electrodes i.e. the spark generator. Thismethods allows to control separately both the catalyst particle size and concentration when fed
into the floating catalyst SWCNT synthesis reactor. Preliminary results show that whenreducing catalyst particle gas phase number concentration, the bundle size of the produced tubes
also is reduced, and we reduce the tube diameter below 1 nm and narrow the chiral angle
distribution towards armchair when reducing synthesis temperature and CO concentration.
Interestingly, the SWNT mean diameter does not significantly change when controlling catalyst
number mean diameter from 4 nm to 10 nm.
We present current status of transparent conducting films and field effect thin filmtransistors manufactured by direct, dry deposition of SWNTs for
G
G
G

--

3S-8
Graphene R&D conducted in Sony
Solution-processed TFTs and CVD-grown transparent conductive filmsżToshiyuki Kobayashi1
1Advanced Materials Laboratories, Sony Corporation, Kanagawa 243-0014, Japan

Sony has been engaged in nanocarbon research since early 1990s. It started with fullerene
and extended to carbon nanotube (CNT) in 2000. At that time, target applications were proton
conductors and hydrogen storage for fuel cells, solar cells, field emitters, transistors, andtransparent conductive films (TCF).
The graphene research started separately from the fullerene-CNT line. Sony has also beenworking on organic thin-film transistors (TFT) and in late 2000s, we were in search for ahigh-mobility and solution-processable alternative. The chemically-derived graphene
nanoribbon and graphene oxide were promising candidates at that time due to their reported
high mobility exceeding 100 cm2/Vs [1]. To test the possibility of using graphene for TFTs offlat panel displays (FPD), we developed a solution process which enables uniform fabricationof semiconductive graphene oxide thin film over a large area; in particular, wafer size.
Although, the fabricated TFTs showed excellent process yield that all devices show clear
transistor characteristics [2,3], the field-effect mobility (< 1 cm2/Vs) and on/off ratio (< 3)were both insufficient for FPD. The on/off ratio was improved up to 103 by controlling the
reduction of graphene oxide [4]; however, degrading mobility by increasing on/off ratio
suggested that graphene oxide is not suitable for FPD application.
In 2009, CNT team working on TCFs joined graphene research. Stimulated by a report of
30-inch roll-based production of high-quality CVD graphene [5], we started working on CVD
synthesis of high-quality graphene film from early 2010. First, we followed the CVD
synthesis of graphene on copper foil in quartz tube furnace and then tried to extend it torol-to-roll process without degrading the quality of the graphene film. We also examinedseveral different possibilities, including plasma CVD and thermal CVD with local heating of
the copper foil, and found that thermal CVD by directly Joule heating the copper foil is themost promising. After verifying graphene growth in a small glass reactor, we calculated
thermal, mechanical, and electrical specifications necessary to design a novel roll-to-roll CVD
reactor. The reactor was fabricated in the summer of 2011 and soon we succeeded in growing
a graphene film longer than 50 m. After optimizing the process conditions to growhigh-quality graphene, in early 2012, we grew graphene film longer than 100 m andtransferred it to a PET film by roll-to-roll film bonding and copper etching processes. The
obtained graphene TCF exhibited a sheet resistance as low as 150 :/sq [6], which is
sufficiently low for touch screens.
[1] C. Gomez-Navarro et al. Nano Lett. 7, 3499 (2007). X. Li et al. Science 319, 1229 (2008).
[2] T. Kobayashi et al. International Symposium on Graphene Devices. (2008).
[3] T. Kobayashi et al. small. 6, 1210 (2010).
[4] T. Kobayashi et al., MRS Fall meeting (2010).
[5] S. Bae et al., arXiv:0912.5485 (2009).
[6] T. Kobayashi et al. Appl. Phys. Lett. 102, 023112 (2013).
Corresponding Author: T. Kobayashi
Tel: +81-46-226-3708, Fax: +81-50-3809-2000, E-mail: Toshiyuki.Kobayashi@jp.sony.com--୍⯡ㅮ₇
General Lecture

1–1 䡚 1–9
2 – 1 䡚 2 – 12
3 – 1 䡚 3 – 12

1-1
Structural analysis of C60 microtube-AAO membrane joint interfaces
by FIB-SEM
żKun’ichi Miyazawa1, Shuichi Shimomura2, Takatsugu Wakahara1, Masaru Tachibana3
1

Fullerene Engineering Group, 2Carbon Composite Materials Group, Materials Processing
Unit, National Institute for Materials Science, Tsukuba, Ibaraki 305-0044, Japan3
Department of Materials System Science, Yokohama City University, 22-2 Seto,
Kanazawa-ku, Yokohama 236-0027, Japan

In 2007, it was found that C60 microtubes (C60MTs) can grow vertically on a porous anodic
aluminum oxide (AAO) membrane by slowly injecting isopropyl alcohol (IPA) into a
C60-saturated toluene solution through holes of the alumina membrane, using an electric
piston - syringe system. This method is called thediaphragm liquid-liquid interfacial precipitation
method (DLLIP). The length of C60 microtubes grownby DLLIP reaches more than 100 Pm and their outer
diameter is t ypically about 30 Pm (Fig.1).
The formation mechanism of V-C60MTs should
be known in order to control the morphology and sizeof the vertically grown C60 whiskers, since the DLLIP
method has a high potential to synthesize fullerene
nanowhiskers that are vertically grown on the othervarious conductive substrates which will be useful forelectronic applications such as solar cells.
Fig.1
SEM image of C60
In order to know the growth mechanism of microtubes vertically grown on an
V-C60MTs, longitudinal cross-sectional images of the AAO membrane.
V-C60MT - AAO membrane interfaces were
investigated by transmission electron microscopy(TEM). The V-C60MTs were machined by a
SEM-focused ion beam system (FIB-SEM, Hitachi
NB5000) at an accelerating voltage of 40 kV using a
Ga liquid metal ion source [2]. Fig.2 shows a
FIB-SEM image for a C60 microtube - AAO
membrane joint interface of a thin foil fabricated by
FIB. No cracks are observed along the joint interface,showing the good wetting and stress reduction
mechanism between the C60 crystal and the AAO
membrane.
[1]S. I. Cha, K. Miyazawa and J.-D. Kim, Chem.Mater.
20(2008)1667.
[2]K. Miyazawa, R. Kuriyama, S. Shimomura, T.
Wakahara and M. Tachibana, J. Cryst. Growth,388(2014)5.
Corresponding Author: K. Miyazawa
Tel: +81-29-860-4528, Fax: +81-29-860-4667
E-mail: miyazawa.kunichi@nims.go.jp--Fig.2 FIB-SEM image of a C60
microtube – AAO membrane joint
interface.

1-2
Photoelectron Spectra of Encapsulated Mono-metal fullerenesżTakafumi Miyazaki1, Yuuma Seino1, Noda Shoko3, Hajime Yagi1,
Hisanori Shinohara3 and Shojun Hino1
1

Graduate School of Science and Engineering, Ehime University, Matsuyama 790-8577, Japan
2
3

Institute for Molecular Science, Okazaki, 444-8585, Japan

Graduate School of Science, Nagoya University, Nagoya 464-8602, Japan

We have been measuring ultraviolet photoelectron spectra (UPS) of endohedral
fullerenes and revealed their electronic structure. Here, we present UPS and X-ray
photoelectron spectra (XPS) of Eu@C82 (I), (III) and Pr@C82 (I), (II) and discuss theirelectronic structures in conjunction with M@C82 (M= Y, Lu, Er, Tm, etc.).
The UPS were measured at UVSOR BL8B of Institute for Molecular Science withincident photon energy hv= 20㹼60 eV and the XPS were measured by a SCIENTA SES-100
electron analyzer using the Mg-KĮ (hv =1253.6eV) line.
The UPS onset energy of Eu@C82 (I) and (III) is the same 0.9 eV and that of Pr@C82(I) and (II) is 0.3 eV, which are smaller than that of empty C82 (1.2 eV). These of deeper
valence band UPS (BE >5 eV) shows good correspondence with those of other endohedral
fullerenes. The upper valence band UPS of Eu@C82 (I) are analogous to those of Tm@C82 (I)of which electronic configuration is Tm2+@C822-. The XPS Eu4d peaks of Eu@C82 appear at
higher binding energy side than those of Eu metal. The amounts of the transferred electrons
from the encapsulated Er to the C82 cage are estimated to be two electrons as was in Tm@C82.
The UPS of Pr@C82 (I) resemble those of Y@C82, Lu@C82 and Er@C82 in which
encapsulated metal atom donates three electrons to the cage. This finding suggests Pr3+@C823electronic configuration. The XPS Pr4d of Pr@C82 appears at higher binding energy side thanthose of Pr metal, which also supports above elucidation.
Present results are another example to support the empirical rule that the electronic
structure of the endohedral fullerenes is principally governed by the cage structure and thenumber of transferred electrons.
Corresponding Authors: T. Miyazaki, E-mail: miyazaki@eng.ehime-u.ac.jp, phone: 089-9279930; S. Hino, E-mail: hino@eng.ehime-u.ac.jp, phone: 089-927-9924.

- 10 -

1-3
Organic Photovoltaic Device Characteristics
using Fullerene Derivatives with a Thiophene Moiety†○Tatsuya Hayashi1, Haeseong Lee2,3, Inseob Im3, Seung Joo Lee4, Jin Jang4,
Chyongjin Pac1,5, and Hiroshi Moriyama1
1

Department of Chemistry, Toho University, Miyama2-2-1, Funabashi, Japan
TAKOMA Technology Co., Ltd., Nosung-myeon, Nonsan-city, Chungnam, Korea
3
Department of Advanced Materials Jeonju University, Wansangu Jeonju, Korea
4
Department of Information Display, Kyung Hee University, Seoul, Korea
5
Department of Materials Chemistry, Korea University, Sejong Jochiwon, Chung-Nam, Korea
2

Bulk heterojunction (BHJ)-type organic photovoltaic (OPV) cells have attracted significant
attention for next-generation solar cells because of their light weight, solution process
construction and flexibility. One of the most representative OPVs is based on a blend ofpoly(3-hexyl thiophene) (P3HT) as an electron donor and a C60 derivative,[6,6]phenyl-C61-butyric acid methyl ester (PCBM), as an electron acceptor. In this study, we
synthesized a new series of fullerene derivatives (5-HThCEB, 5-EThCEB, 3-MeOThCEB)
with a thienyl group that has potential affinity with the P3HT donor. The synthetic scheme forthese fullerene derivatives is based on that of PCBM [1]. The two fullerene derivatives(5-HThCEB and 5-EThCEB) have different alkyl chains (R1 = C2H5 and C6H13)
3-MeOThCEB has a methoxy group that is expected to raise the LUMO level.
RWefabricated
R
S
OPV
cells
R
using
P3HT
NH NHTs
NaOCH / Pyridine
RRSS
C / o-DCB
SnCl / CH Cl
R
CH OH
NNHTs
O
S
as a donorR
5-HThCEB R = C H , R = H
andthe
5-EThCEB R = C H , R = H
1
2
3
newly
3-MeOThCEB R = H, R = OCH
designedfullerene derivatives as an acceptor. The performance of the novel fullerene derivatives wasfound to be lower than that of PCBM, although the VOC of 5-EThCEB and 3-MeOThCEB ishigher than that of PCBM.
2

1

2

Cl

O

2

4

1

2

1

6

13

1

2

5

1

2

1

3

R2

2

3

1

60

2

2

2

3

Table 1. Photovoltaic parameters using new C60 derivatives.
J

V

OC

FF

PCE

(mA/cm )

(V)

(%)

(%)

PCBM

7.61

0.587

60.3

2.69

5-HThCEB

3.04

0.566

32

0.550

5-EThCEB

5.63

0.628

32.3

1.14

3-MeOThCEB

5.58

0.624

53.9

1.87

SC
2

Figure 1. J–V characteristics of the devices fabricated with P3HT and the new C60 derivatives.
[1] J. C. Hummelen, B. W. Knight, F. LePeq, F. Wudl, J. Yao, C. L. Wilkins, J. Org. Chem. 1995, 60, 532–538.

† This work is supported by Bilateral International Collaborative R&D Program (Project number: GT-2009-CL-OT-0058, Ministry of Knowledge Economy,
Republic of Korea and a MEXT-Supported Program for the Strategic Research Foundation at Private Universities, Japan.

Corresponding Author : Hiroshi Moriyama

TEL : +81-47-472-1211, FAX : +81-47-476-9449, E-mail : moriyama@chem.sci.toho-u.ac.jp- 11 -

1-4
Dispersion of Detonation Nanodiamond: A Progress Report○Shuichi Sasaki*, Ryoko Yamanoi and Eiji Ōsawa*
NanoCarbon Research Institute, AREC, Faculty of Textile Science and Engineering,
Shinshu University, 3-15-1 Tokida, Ueda, Nagano 386-8567, Japan

Probability density

Even though the primary particles of detonation nanodiamond have been observed to be of
single-nano size under TEM, dispersion of their agglutinates has been difficult and the true
picture of its primary particles still remains unknown. We succeeded in 2002 to disintegrate
the agglutinates by attrition milling into aqueous colloid with about 5 nm in diameter.
Continued improvements in the disintegration conditions eventually led to further decrease in
the diameter to 2.8 nm, which could be the final value (Fig. 1). Taguchi method ofexperimental design [1] played a
1(A)2.8nm
key role in optimizing conditions.
0.8(B)3.0nm
The most important factor is the
0.6
concentrationof
initial(C)3.8nm
0.4
agglutinates.
Mechanismof(D)4.8nm
0.2(E)5.5nm
disintegration involves not only
the attrition with zirconia beads
0
0 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15
but also self-ablation among
particle size [nm]nanodiamond particles. Stable
Fig. 1. Normalized DLS particle-size distributions of disintegrated
dispersion seems to have beendetonation nanodiamond: A Taguchi method III, 2013. B Taguchi
achieved by hydration of themethod II, 2012. C Taguchi method I, 2011. D Sonication
included, 2004. E Unoptimized attrition milling, 2002.
surface graphitic layer [2].
A
coupleofenigmatic phenomena
have been noted in thecourseofdisintegration
under
the
optimized
conditions. First, atransientpeak
appeared in the DLS
Fig. 2. Transition of size distribution in detonation nanodiamond during attrition
particle-size
milling. Left: Initial stage, DLS of aliquot from milling. Peak A dominates. Right:
distribution graphs in
After the milling, the final colloidal solution was subjected centrifugation to givethe initial stage ofthree fractions. Size-distribution of upper and middle layers shown. See text.
disintegration (Fig. 2,
left, A), which shifts
to larger size with milling time and merges into 2.8 nm range at the end. We believe 1.7 nm
corresponds to the true core size of the primary nanodiamond particle. Second, centrifugal
treatment of our final colloid at 12,000 rpm produced two additional colloidal layers aboveand below the layer of 2.8 nm particles. Surprisingly, the uppermost layer (Fig. 2, right, C)
consists of 4.8 nm particles! The nature of these larger particles is under study.
[1] Taguchi, G. et al. Taguchi’s Quality Engineering Handbook, Wiley-Interscience, 2004.
[2] Yamanoi, R. et al., presented in the poster session of this Symposium.
Particle-size distribution was determined on a DLS equipment FPAR-1000 (Otsuka Electronic Co.). Diameters
are based on volume concentration. Corresponding Authors: sasaki@bruvas.com. osawa@nano-carbon.jp, Tel:
+81-268-75-8381, Fax: +81-268-75-8551.

- 12 -

1-5
Development of Ion Mobility System with Multi-stage Ion Trap
żToshiki Sugai, Yasuhiro Hiroshiba, Ninako Mikami, and Ryota Jinnouchi
Department of Chemistry, Toho University, Miyama 2-2-1 Funabashi, 274-8510, Japan
Ion mobility measurements have been a powerful tool for analysis on structures ofnanocarbon materials. Structures of Metal-fullerenes show significant dependence on thenumber of metal atoms and the cage size and their novel structures have been also clarified[1].
To study further, we have been developing an ion trap mobility system and structural changesof polystyrene particles were monitored for more than 2 hours[2]. The measurements haverevealed the stability and the sensitivity of the system. Despite of these advantages, the trapsystem has low mobility resolution because of the small size of the trap. To improve theresolution and to research nano materials, several groups have been also developing trap
assisted IMS systems[3]. Here we present the development of an ion mobility measurement
system with multi-stage ion trap.
The system consists of a laser ionization source for polystyrene particles, an ion
funnel, and a linear ion trap for long movement and ion separation (Fig. 1). Those functions
are realized by a newly developed power supply for the system. The power supply
manipulates the particles for long distant and long-time movement with controlled RF and DC
voltage to realize efficient measurement (Fig. 2). Without this power supply the particles
cannot be hold on the center axis of the trap and eventually are lost by hitting the electrodes.
With this system, we have achieved long and stable particle movements which contribute toparticle size separation by mobility. The details of the system will be presented.

Fig. 1 Multi-stage Ion Trap IMS.

Fig. 2 RF effect on particle movements.

[1] T. Sugai et al., J. Am. Chem. Soc. 123, 6427 (2001).
[2] T. Sugai et al., The 38,44,45th symposium.
[3] F. Fernandez-Lima et al., Int. J. Ion Mobil. Spec. 14, 93 (2011).
TEL: +81-47-472-4406, E-mail: sugai@chem.sci.toho-u.ac.jp- 13 -

1-6
Vertical transport in meal/2D crystal/graphene layered heterostructures
Yoshihisa Inoue 1, Takehiro Yamaguchi 1, Sei Morikawa 1, Satoru Masubuchi 1,2
Kenji Watanabe 3, Takashi Taniguchi 3, Rai Moriya 1, and Tomoki Machida 1,2
1

Institute of Industrial Science, University of Tokyo, Tokyo 153-8505, Japan
2
INQIE, University of Tokyo, Tokyo 153-8505, Japan
3
National Institute for Materials Science, Tsukuba 305-0044, Japan

Recently, two-dimentional crystals (2DCs) such as graphene (Gr), h-BN, MoS2, WS2 andheterostructures of these materials have been revealed various extraordinal electrical andoptical properties and received lots of attention for fundamental and application point of view.
We fabricate various types of metal/2DC/Gr vertical heterostructures by using mechanicalexfoliation and dry transfer technique. This technique enables us layer-by-layer control of
2DC heterostructure fabrication at the same time realizing high quality interface. By tuning
the layer number and material of 2DC, the vertical transport of the metal/2DC/Gr structure
can be controlled between tunneling and thermionic emission.
Among then, h-BN reveals highest potential barrier height with respect to graphene and as
a result, we observed tunneling-type transport for the layer number from 1 to 4 monolayers(MLs). By fabricating Ni81Fe19/1ML h-BN/bilayer-graphene structure, we demonstrateelectrical spin injection from ferromagnetic Ni81Fe19 to graphene at room temperature [1] asshown in Fig. 1(a).
The MoS2 and WS2 exhibit lower barrier height than h-BN. In this case, we observe thetunneling-dominated transport through the 2DC layer when its thickness is 3 MLs or less. In
this regime, tunnel conductance is determined by the available density of states in thegraphene electrode. When the layer number is more than 3MLs, the tunneling conductance issuppressed and instead of this, thethermionic emission through the
Schottky barrier between Gr and 2DC
becomes dominant in the verticaltransport. Such a thermionic emission
current can be strongly modulatedwith the gate voltage VG. Withutilizing this, we demonstrated large
current modulation as well as large
current density in Ti/MoS2/Gr vertical
FET structure as shown in Fig. 1(b).
These results show the potential
high performance of the 2DC
heterostrucuture for electronics andspintronics applications.
[1] T. Yamaguchi, Y. Inoue et al., Appl.
Phys. Express 6, 073001 (2013).
Corresponding Author: Y. Inoue
Tel: +81-3-5452-6158,
E-mail: y-inoue@iis.u-tokyo.ac.jp

Fig.1 (a) Non-local magnetoresistance in
NiFe/1ML h-BN/Gr spin valve. (b) Gate voltage VG
dependence of I-V characteristics in Ti/37 ML MoS2/Gr
vertical FET.

- 14 -

1-7
Stabilities and Electronic Structures of Hexagonal Boron-Nitride Bilayers
ż<RVKLWDND)XMLPRWR, Takashi Koretsune, and Susumu Saito
Department of Physics, Tokyo Institute of Technology, Tokyo 152-8551, Japan
Two-dimensional monolayer sheet of hexagonal boron nitride (h-BN) has attracted
much attention from the viewpoint of basic nanoscience and applicable nanotechnology since
it possesses several similar properties as in a graphene sheet. On the other hand, the electronic
structure of the h-BN monolayer is quite different from that of graphene; graphene is azero-gap semiconductor, whereas the h-BN monolayer is a wide-gap semiconductor [1]. The
h-BN monolayer with the semiconducting properties is therefore the promising candidate fornext-generation nanoelectronics materials.
Strain engineering is one of the promising ways to tune the electronic properties of
two-dimensional nanomaterials such as band gap and electron transport [2-4]. For example,
the Fermi velocity of graphene can be changed by applying uniaxial strains, and it depends onthe directions of the strains [2]. It is found that the band gap of h-BN monolayer sheet can bealso changed under strains [4].
We here investigate stabilities and electronic structures of bilayer h-BN sheets using afirst-principles density-functional calculation. The energetics of the stacking patterns of h-BN
bilayers and their electronic structures are examined and carbon-impurity doping effects into
them are also studied. We show that the donor and acceptor-type states appear when boron
and nitrogen atoms are replaced by C atoms, respectively, as in the case of the h-BNmonolayer sheet. In this talk, we present strain effects on the electronic properties of h-BN
bilayers. We discuss similarities and differences between C-doped and undoped h-BN bilayer
sheets.

[1] K.Watanabe, T. Taniguchi, and H. Kanda, Nat. Mater. 3 (2004) 404.
[2] S. M. Choi, S. H. Jhi, and Y. W. Son, Phys. Rev. B 81 (2010) 081407.
[3] Y. Fujimoto, T. Koretsune, and S. Saito, JPS Conf. Proc., in press.
[4] Y. Fujimoto, T. Koretsune, and S. Saito, Submitted.
Corresponding Author: Yoshitaka Fujimoto
TEL: +81-3-5734-2368, FAX: +81-3-5734-2368, E-mail: fujimoto@stat.phys.titech.ac.jp- 15 -

1-8
Effect of Band Nesting on Optical Properties in Two-dimensional Transition
Metal Dichalcogenides○Daichi Kozawa1, Rajeev Sharma Kumar2, Alexandra Carvalho2,
Amara Kiran Kumar2, Weijie Zhao2, Minglin Toh2, Ricardo M. Ribeiro2,
A. H. Castro Neto2, Kazunari Matsuda1, and Goki Eda2
1

Institute of Advanced Energy, Kyoto University, Uji, Kyoto 611-0011, Japan
2
National University of Singapore, 2 Science Drive 3, 117542, Singapore

A[1] Weijie Zhao and Goki Eda. et al.,Nano Lett. 13, 5627 (2013).
[2] Shinichiro Mouri, Yuhei
Miyauchi and Kazunari Matsuda,
Nano Lett. 13, 5944 (2013).
Corresponding Author: D. Kozawa
Tel: +81-774-38-3465
Fax: +81-774-38-3467,
E-mail:d-kozawa@iae.kyoto-u.ac.jp

B

2

1

0
1.6

B

2.0
2.4
2.8
Excitation Energy (eV)0.5

0Figure 1 a, Simplified band structure of monolayer of MX2.
The arrows indicate the transition in A, B and the bandnesting. b, PLE spectrum for band gap emission formonolayer MoS2. The optical contrast spectrum is also shownfor comparison- 16 -

R / R

References

PLE Intensity (arb. units)

Two-dimensional (2D) crystals of semiconducting transition metal dichalcogenides (TMD)
absorb as much as 10% of incident photons in the visible frequencies despite being atomicallythin. It has been suggested that the strong absorption is due to the parallel band or “bandnesting” effect resulting in diverging joint density of states. Here, we show using
photoluminescence excitation (PLE) spectroscopy and ab initio density functional theory(DFT) calculation that the band nesting in mono- and bilayer MX2 (M = Mo, W and X = S,
Se) results in excitation-energy-dependent characteristic relaxation pathways of thephotoexcited carriers.
Since group 6 MX2 is isoelectronic, the general features of electronic structure are similar
for these compounds. For monolayer MX2, the conduction band minimum and the valenceband maximum are both at the K point of the Brillouin zone [1] as shown in Figure 1a. The
PL intensity is enhanced when the excitation energy is in resonance with the B exciton
absorption [2]. In contrast, the PLE spectrum for monolayer MoS2 shows suppressed PL
intensity at the C absorption peak (Figure 1b). In the DFT calculation, we have estimated therelaxation pathway of photoexcited carriers generated in the band nesting. Our experimental
and simulation results reveal that photoexcited electrons and holes in the nesting region of thephase space relax towards immediate local minima with opposite momentum. These effects,
which were found to be prominent in monolayer and bilayer TMD, imply that the loss ofphotocarriers due to direct exciton recombination is delayed for certain resonance conditions.
Our findings highlight thepotential for efficient hot ab
Nestingcarrier collection using these
3 1L MoS2
1.0
PLE
materials as the absorbers in
Optical Contrast
optoelectronic devices.
C1-
○Ryo Nouchi1, Nobuhiko Mitoma1,2, Morihiro Matsumoto1



Graphene is a oneatom thick material where carbon atoms are arranged into a honeycomb
lattice structure. All carbon atoms belong to its surface, and thus electronic properties ofgraphene are sensitive to surface conditions such as adsorption of foreign atoms/molecules.
Especially, adsorption of air molecules such as oxygen is of great importance due to theirubiquitousness. Oxygen adsorption onto bilayer graphene has been found to be controllable
by applying gate voltages with a fieldeffecttransistor (FET) structure [1]. In this presentation,
we connect the gatevoltage controllability of oxygen adsorption and postadsorption UV
treatment to perform gatevoltage controlled photooxidation of graphene. The oxidation
reaction is found to occur selectively at edges [2], which might offer a novel methodology tofabricate graphene nanoribbons.
Graphene layers were fabricated by mechanical exfoliation onto a Si substrate with athermal oxide layer on top of it. Cr/Au electrodes were fabricated onto the graphene layers byelectron beam lithography, vacuum deposition, and liftoff processes. UV light was irradiatedto the fabricated graphene FETs in operation in air at room temperature. Edgeselective
photochemical etching is clearly shown in Figure 1. The etching was not observed underconditions with positive gate voltages and/or low drain voltages, indicating possible
finetunability of the reaction by adjusting gate and drain voltages.


Drain current:
D



Gate voltage:G



A





Drain

voltage: D

D band intensity



Fig.1 Schematic of the experimental setup (left) and Raman  band mapping
after 20min UV irradiation with G of −60 V and D of 10 mV (right).
[1] Y. Sato, K. Takai, T. Enoki, Nano Lett. , 3468 (2011).
[2] N. Mitoma and R. Nouchi, Appl. Phys. Lett. , 201605 (2013).
Corresponding Author: R. Nouchi
Tel: +81722548394, Fax: +81722548394,
Email: rnouchi@21c.osakafuu.ac.jp- 17 -

2-1
Molecular Simulations of Single-Walled Carbon Nanotube Growth andChemical Reaction of Catalyst Cluster○Kaoru Hisama1, Tomoya Kawasuzuki1, Takuya Noguchi1, Shohei Chiashi1,
Tomofumi Tada2 and Shigeo Maruyama1

1

Department of Mechanical Engineering, The University of Tokyo, Tokyo 113-8656, Japan
2
Materials Research Center for Element Strategy, Tokyo Institute of Technology
Yokohama 226-8503, Japan
It is highly important to understand the growth mechanism of single-walled carbon
nanotubes (SWNTs) in order to develop structure-controlled growth techniques. In experiment,
the role of metal catalyst is important for SWNT growth. Thus, we performed molecular
dynamics (MD) simulation to investigate the catalyst activity. The interactions among carbon
and metal atoms (Fe and Co) are expressed by our home-made Tersoff-type potentials [1]. We
prepared metal clusters and supplied them with carbon atoms with constant number (n) in the
fully periodic cell (101010 nm3) in gas phase. We observed cap formation, cap lift-off, andelongation process of SWNTs. Chirality (n, m) of the SWNT structure can be partiallyassigned. For example, the tube structure of Fig. 1 is close to (11, 6).
We also observed two types of growth modes, ‘Octopus’ and so-called ‘VLS
(Vapor-Liquid-Solid)’ [2] depending on simulation conditions (temperature, gas carbon
density and catalyst metal species). These two modes seem to correspond to the growth modes
proposed by Loiseau group [3]. Octopus mode is ‘tangential mode’ in which SWNTs have thesame diameter as the catalyst, and the VLS mode is “perpendicular mode” in which SWNTs
have smaller diameter than catalyst. In MD simulation, Octopus mode is typically observed in
SWNTs from Co catalyst while VLS mode is shown in SWNTs from Fe catalyst at hightemperature. As the temperature is lower, SWNTs from Fe catalyst shows the Octopus mode.
These two modes show different carbon structures on the catalyst surface. Graphene sheet
structure and carbon chains appear on the metal surface in Octopus mode (Fig. 2) but muchless in VLS mode. The mechanism of chirality determination for each mode is discussed.
Furthermore, the preliminary result of ab initio simulation of chemical reaction of moleculeson small metal clusters will be discussed.
Co, 1500 K, n=3(160.0 ns)(602.0 ns)

Octopus mode

Fe, 1500 K, n=3(182.0 ns) (60.0 ns)

CNT(400.4 ns)

VLS
mode

Catalyst
sheet on metal

Chiral (11,6)

Fig. 1 Octopus growth (with local chirality assignment)
and VLS growth

Carbon chain

Fig. 2 Sheet and carbon chain structure on the
catalyst surface(Co, 1500 K, n=3)[1] T. Matsuo, et al., to be submitted. [2] M. Ribas, et al., J. Chem. Phys., 131, 224501 (2009).
[3] M. F. C. Fiawoo, et al., PRL, 108, 195503 (2012).
Corresponding Author: Shigeo Maruyama
Tel: +81-3-5841-6421, Fax: +81-3-5800-6983,
E-mail: maruyama@photon.t.u-tokyo.ac.jp- 18 -

2-2
Synthesis and transfer properties of single-walled carbon nanotubes arraywith semiconductor-type selectivityżShunsuke Sakurai1,2, Maho Yamada1,2, Hiroko Nakamura1,2, Don N. Futaba1,2, Kenji Hata1,2
1Green Nanoelectronics Center, National Institute of Advanced Industrial Science andTechnology (AIST), Tsukuba 305-8565, Japan
2
Nanotube Research Center, National Institute of Advanced Industrial Science andTechnology (AIST), Tsukuba 305-8565, Japan

Coexisting of metallic and semiconducting carbon nanotube (CNT) is one of the major
problems on the application of CNT in semiconductor electronics. Although post-synthesis
separation approaches such as electrophoresis, gel-chromatography, and selective eliminationof metallic CNTs has been reported [1], direct synthesis of semiconductor-CNT is an ideal
approach to obtain semiconductor-CNT array without impurity and damage on CNT. However,direct control of the ratio of metal/semiconductor CNT and/or chirality distribution is still oneof the biggest challenge in the field of CNT synthesis [2,3]. Here, we present our approach forthe preferential growth of semiconducting CNTs, and the properties of field-effect transistor(FET) fabricated from CNT arrays with semiconductor-type selectivity.
Selective growth has been achieved by pre-annealing the catalyst iron nanoparticle withthe small amounts of H2O and H2 as shown in Figure 1. We found out that precise control ofgas ambient is necessary to achieve the preferential growth of semiconductor-CNT, i.e., toomuch H2O amount led to no growth of CNT and too little H2O amount did not invoke thepreferential growth. These results suggest that the control of catalyst activity is important.
Importantly, performances of FET devices consisting of the as-grown CNT films aschannel layer are quite good, especially at a relatively short channel length. At a a relatively
short channel length (5 Pm), high on/off ratio (c.a. 104), and high on-current density (> 1
PS/Pm) has been obtained. We note that these performances are almost comparative to thosefabricated from the inks of the separated semiconductor CNT [3]. The relationship of FET
performances and selectivity is also presented.
Catalyst formation
H2

Water exposure

CVD
C2H4

H2O

Selective growth ofsemiconductor-CNT

Figure 1. Schematic representation of the preferential growth of semiconductor-CNT

This research is granted by JSPS through ̌Funding Program for World-Leading
Innovative R&D on Science and Technology (FIRST Program)”, initiated by CSTP.
[1] H. Liu, D. Nishide, T. Tanaka, H. Kataura, Nature Commun. 2 (2011) 309.

[2] W. H. Chiang, R. M. Sankaran, Nature Mater. 8 (2009) 882.
[3] C. Wanget al., Nano Lett., 12 (2012) 1527.
Corresponding Author: Kenji Hata
TEL: +81-29-861-6205, FAX: +81-29-861485-1169, E-mail: kenji-hata@aist.go.jp- 1 -

2-3
Low-temperature catalyst activator: Mechanism study of CNT forest
densification by “STEP” growth method using synchrotron radiation
Akito Takashima1, Yudai Izumi1, Eiji Ikenaga1, Takuo Ohkochi1, Masato Kotsugi1,
Tomohiro Matsushita1, żTakayuki Muro1,
Akio Kawabata2, Tomo Murakami2, Mizuhisa Nihei2, Naoki Yokoyama2
1

2

Japan Synchrotron Radiation Research Institute (JASRI), Hyogo 679-5198, Japan
Collaborative Research Team Green Nanoelectronics Center (GNC), National Institute ofAdvanced Industrial Science and Technology (AIST), Ibaraki 305-8569, Japan

We recently developed a thermal chemical vapor deposition method named “STEP” for thegrowth of dense carbon nanotube (CNT) forests [1]. A Ti film is used as the underlayer for an
Fe catalyst film. A characteristic point is that C2H2 feeding is begun at a low temperature of
450 °C in the course of a temperature elevation from room temperature (RT) to 800 °C. Any
pretreatments are not used for the ex-situ deposited catalyst. A growth result showed that the
CNT packing density obtained by the STEP process was 20 times higher than that obtained bya process in which C2H2 was supplied at 800 °C [1]. This suggests that the Fe layer, oxidized
due to air exposure, was reduced and transformed into nanoparticles at or near 450 °C. Thistemperature is, however, unusually low to reduce Fe oxides. It is still unknown how the STEP
process densified the CNTs. To address the mechanism, we studied the chemical andmorphological states of the Fe/Ti catalyst system (denoted by Fe/Ti) under vacuum annealing.
Fe/Ti has 2- and 1-nm-thick Fe and Ti layers, respectively, on a Si substrate. We also
prepared a comparative sample (Fe/Si) without the Ti layer. All the analyses were performed
at SPring-8. The Fe layers were analyzed at BL27SU using soft x-ray photoemission
spectroscopy (SXPES) with a probing depth of ~1.4 nm. For the buried Ti layer, hard x-ray
photoemission spectroscopy (HAXPES) with a probing depth of ~8 nm was used at BL47XU.
Surface images were observed at BL17SU using photoemission electron microscopy (PEEM).
Finally, a CNT growth experiment at 450 °C was performed at BL27SU, where the catalyst
chemical states were observed by soft x-ray absorption spectroscopy (XAS).
The result of Fe 2p SXPES showed that the Fe chemical states of Fe/Ti at 450 °C were
dominated by metallic Fe, whereas those of Fe/Si were still dominated by Fe oxides. In the Ti
2p HAXPES spectrum of Fe/Ti at 450 °C, the TiO peak, which was dominantly seen at RT,
disappeared and the TiO2 peak was solely observed. These results indicate that the Ti layer
reduced the initially oxidized Fe layer at 450 °C. An SXPES analysis also suggests that the Felayer of Fe/Ti transformed into nanoparticles on TiO2 at 450 °C. The PEEM image on Fe/Ti at
800 °C showed large Fe islands with sizes of a few 100 nm, causing sparse CNTs. We
consider that the Ti layer activated the Fe catalyst at 450 °C
in the STEP process and densified the CNTs. We will
present the CNT growth results for Fe/Ti and Fe/Si at
450 °C, which strongly support our conclusion.
This research is granted by JSPS through FIRST
Program initiated by CSTP.
[1] A. Kawabata, T. Murakami, M. Nihei, and N. Yokoyama, Jpn. J.
Appl. Phys. 52, 110117 (2013).
Corresponding Author: T. Muro
Tel: +81-791-58-0802 (ext. 3869), Fax: +81-791-58-0830,
E-mail: muro@spring8.or.jp- 20 -

Fig. 1 (a) Fe/Ti catalyst systemused for STEP.
(b) Comparative sample
without the Ti layer.

2-4What causes a different behavior in the tube growth between (5,5) and(6,5) caps? -Competition between tube and fullerene growth○Yohji Achiba, Takeshi Kodama, Kenro Hashimoto and Haruo Shiromaru
Department of Chemistry, Tokyo Metropolitan University, Hachioji, 192-0397, Japan
A semispherical cap structure consisting of 6 pentagons and infinite numbers ofhexagons has generally been believed to play an essential role on the formation of
nano-structured carbons. Actually, the chirality of a carbon nanotube is totallydependent on the cap structures formed at a very early stage in the tube growth. It has
also been generally accepted that in the tube growth process, the tube structure so called“near armchair” is the one of being the most abundant among many other structural
candidates. Particularly, the chiral tube characterized by a (6,5) chiral index is ofpossessing the high selectivity, and thus, is definitely one of the most plausible potential
candidate as a future carbon nanotube electronic device with a single chirality. On theother hand, the production yield of (5,5) tube whose diameter as well as chirality arequite similar to those of the (6,5) tube is quite low or sometimes is almost zero.
Therefore, a simple question like what causes such a significant difference between the(6,5) and (5,5) chiral structures may occur. In the present work, we will discuss thestability and reactivity of these two caps on the basis of theoretical considerations.
Although the experimental evidence whether the cap is really present or not as a
growth-reaction intermediate is still unclear, we intended to clarify the properties ofthese hypothetical structures by means of a theoretical calculation. For the purpose of
the reaction selectivity of specific cap structures, we performed density functional
calculations on many kinds of isomeric cap structures with different sizes. For example,
since the difference in the structures between (5,5) and (6,5) cap first appears upon
replacing one pentagon of the (5,5) cap by a hexagon at C30, we started to investigate
the stability and reactivity of cap structures at the size of C30 and C31 for the (5,5) and(6,5) cap structures, respectively. In order to find out the major reaction channels for thefurther growth, we extended the calculations to every sizes up to C60 including many
isomeric forms characerized by more than 200 different structures. As a result, it was
found that the highly selective reaction channels leading to the formation of IhC60
fullerene as well as (6,5) chiral tube were able to be specified.
Corresponding Author: Yohji Achiba
E-mail: achiba-yohji@tmu.ac.jp、Tel:+81-42-677-2534, Fax:+81-42-677-2525- 21 -

2-5
Highly efficient purification of semiconducting single-walled carbon
nanotubes using detachable supramolecular solubilizer○Fumiyuki Toshimitsu1, Naotoshi Nakashima1, 2, 3
1

Department of Applied Chemistry, Kyushu University, Fukuoka 819-0395, Japan
2
WPI-I2CNER, Kyushu University, Fukuoka 819-0395, Japan
3
JST-CREST, Chiyoda-ku, Tokyo 102-0075, Japan

Highly purified single-walled carbon nanotubes (SWNTs) are essential for fundamental studies
and applications toward next-generation nanotechnology 1. Especially, unique optical and electricalproperties of semiconducting-SWNTs (s-SWNTs) would be fully utilized only when they areseparated from poisoning metallic-tubes 2. Despite several technical methods have been reported
for the separation, the development of a new powerful separation method is still a greatchallenge. We have previously reported polymer wrapping techniques which efficiently
solubilize/extract semiconducting SWNTs with high chiral-selectivity by developing polyfluorene
derivatives (PFOs) 3,4. However, there are serious problems when using these solubilizing methods;that is, difficulty in the removal of the wrapping surfactants or polymers as well as their low
extraction yields.
In order to solve these problems simultaneously, here
we developed a newly designed, detachable solubilizer 1(Fig. 1) based on a supramolecular approach. Thanks to the
Figure 1. Chemical structures of ligand 1.
metal coordination bonds into PFO, the new polymers not
only recognize semiconducting chirality but also breakableso as to remove from s-SWNT surfaces. The resulted
coordination polymer of 1 and four metal ions (Co, Ni, Cu
or Zn) successfully extracted s-SWNTs (Fig. 2).
Furthermore, the extraction yield of solubilized SWNTs are
greater by ~10 times compared to conventional PFOs The
solubilized SWNT could be further purified by removing
the wrapping polymers, simply by treating in an acidic
condition. The quantitative elimination of solubilizer 1 andmetal ions were confirmed by UV-vis-Near IR, raman andtwo-dimensional PL mapping spectroscopies. The detailsof this study will be presented at the meeting.
Referneces

Figure 2. Raman spectra of extracted
s-SWNTs using coordination polymer ofligand 1. Excitation ; 633 nm.

[1] H. J. Dai, Acc. Chem. Res. 35, 1035 (2002).

[2] Cao, Q. & Rogers, J. A., Adv. Mat. 21, 29Ð53 (2009).
[3] H. Ozawa, N. Ide, T. Fujigaya, Y. Niidome, and N. Nakashima, Chem. Lett. 40, 239 (2011).

[4] K. Akazaki, F. Toshimitsu, H. Ozawa, T. Fujigaya, and N. Nakashima, J. Am. Chem. Soc., 134, 12700 (2012).
Corresponding Author: N. Nakashima
Tel: +81-92-802-2845, Fax: +81-92-802-2845
E-mail: nakashima-tcm@mail.cstm.kyushu-u.ac.jp- 22 -

2-6
The effect of DNA adsorption on optical transitions
in single-walled carbon nanotube
Masahiro Ito, Yusuke Ito, Daisuke Nii, Hiroki Kato, Kazuo Umemura, Yoshikazu Homma.

○

Department of Physics, Tokyo University of Science, Tokyo 162-8601, JapanDNA adsorption on single-walled carbon nanotubes (SWNTs) makes SWNTs solubilize
and functionalize [1,2]. The hybridization of DNA and SWNT (DNA-SWNT) is of greatinterest in chemical and biochemical fields. As a result of DNA adsorption, SWNTs are
isolated individually and photoluminescence (PL) from DNA-SWNTs can be obtained.
Because PL from an SWNT is sensitive to its environment, PL spectra should reflect the
information of adsorbed DNA. However, PL from DNA-SWNT ensemble makes spectrum
analysis difficult.
Recently, we revealed that PL could be observed even from DNA-SWNTs lying on thesubstrate i.e. under dry condition [3]. In this study, we investigated the intrinsic effect of
single stranded DNA (ssDNA) and double stranded DNA (dsDNA) adsorption on the opticaltransition in isolated DNA-SWNTs under the dry condition.
We diluted DNA-SWNT solution low enough and obtained mono-dispersed DNA-SWNTs
on the substrate as shown in Fig. 1. PL spectra from SWNT suspended between micro
structures (solid line), ssDNA-SWNT (dash line) and dsDNA-SWNT (dot line) are shown in
Fig. 2. Three spectra were obtained from the same chirality (8,6). The difference in emission
wavelength is attributed to the difference in the thickness of ssDNA and dsDNA. Figure 3
shows emission spectra under the wet and dry conditions. The emission wavelength of
ssDNA-SWNT depends on the environment. On the other hand, the emission wavelength of
dsDNA-SWNT is retained. This means that ssDNA-SWNT is more sensitive to environmental
change. The quantum yield in an isolated DNA-SWNT will also be discussed in comparison
with that of a suspended SWNT.
[1] N. Nakashima, et al.: Chem. Lett. 32 (2003) 456. [2] M. Zheng, et al.: Nature Mater. 2 (2003) 338.
[3] M. Ito, et al.: Appl. Phys. Lett. in press.
Corresponding Author: Yoshikazu Homma
Tel: +81-3-3260-4271 (ext. 2298), Fax: +81-3-5261-1023,
E-mail: homma@rs.tus.ac.jp

Fig. 1. SEM image of isolated
DNA-SWNTs.

Fig. 2. PL spectra of suspended
SWNT, ssDNA-SWNT, anddsDNA-SWNT under the dry
condition.

- 23 -

Fig 3. PL spectra under the wet
and dry conditions.

2-7
Mechanistic insight into the metal/semiconductor separationof single-wall carbon nanotubes using hydrogelsżAtsushi Hirano, Takeshi Tanaka, Hiromichi Kataura
Nanosystem Research Institute, National Institute of Advanced Industrial Science andTechnology, Tsukuba, Ibaraki 305-8562, Japan
Single-wall carbon nanotubes (SWCNTs) suspended in sodium dodecyl sulfate (SDS) are
separated into metallic and semiconducting species using hydrogel columns [1].
Understanding the mechanism helps improve the quality and quantity of the separation. In thisstudy, we provide a mechanistic model for the separation, which was derived from
pH-dependent adsorption of SWCNTs onto the hydrogels.
The adsorbability of SWCNTs on the hydrogels is reduced under acidic pH conditions. The
metallic SWCNTs are more readily desorbed from the hydrogels than the semiconducting
SWCNTs (Fig. 1). Because reversible oxidation of SWCNTs in aqueous solution depends on
O2, H+/H2O reduction potential [2], the pH dependence of the adsorption is likely ascribed tothe oxidation of SWCNTs. Based on the results, a mechanistic model of themetal/semiconductor separation is proposed as follows (Fig. 2):
1. Metallic SWCNTs is more readily oxidized because of the smaller band gaps.
2. Oxidized SWCNTs are positively charged.
3. More SDS molecules are electrostatically bound to more positively charged SWCNTs.
4. Fully coated SWCNTs with SDS result in their desorption from the hydrogel.
The metallic SWCNTs thus tend to desorbed from the hydrogel column compared withsemiconducting SWCNTs, leading to the separation [3]. This property of the adsorption isused for improvement of the quality of the separation.

Fig. 1 Photograph of the SWCNTs adsorbed onto thehydrogels at various pH values.

Fig. 2 Schematic representation of thereversible oxidation of the SWCNTs
accompanied by the SDS condensationon the SWCNTs.

Acknowledgment. This work was supported in part by KAKENHI of MEXT, Japan.
[1] T. Tanaka et al. Appl. Phys. Express 2, 125002 (2009)[2] A. Nish and R. J. Nicholas. Phys. Chem. Chem. Phys. 8, 3547 (2006)[3] A. Hirano et al. ACS Nano 7, 10285 (2013)
Corresponding Author: T. Tanaka
Tel: +81-29-861-2903, Fax: +81-29-861-2786,
E-mail: tanaka-t@aist.go.jp- 24 -

2-8
Organic Film-Assisted Full-Length Electrical Breakdown
for Arrays of Semiconducting Single-Walled Carbon Nanotubes○Keigo Otsuka, Taiki Inoue, Shohei Chiashi, Shigeo Maruyama
Department of Mechanical Engineering, The University of Tokyo, Tokyo 113-8656, Japan| Drain Current | (A)Semiconducting (s-) single-walled carbon nanotubes (SWNTs) are one of the attractive
channel materials for field-effect transistors (FETs), and highly pure s-SWNT arrays are
required for monolithic device integration. Since selective growth techniques have not yet
attained a required purity of s-SWNTs, post growth removal of metallic (m-) SWNTs is stillnecessary. Among various techniques, electrical breakdown [1] has sufficient selectivity
between s- and m-SWNTs. However, it oxidizes only small regions (~100 nm) of m-SWNTs
and most parts of m-SWNTs remain after the process, and therefore it lacks in scalability. In
this study, we propose an organic film-assisted full-length electrical breakdown of m-SWNTs
toward pure s-SWNT arrays.
Horizontally-aligned SWNTs grown on crystal quartz were transferred onto SiO2/Si
substrates and used as channels of back-gate FETs. Molecular glass, small-molecule organic
material, was deposited onto the substrates, covering the SWNTs. It was previously used asthermocapillary resists [2] but here we use it to assist oxidation of m-SWNTs. A drain voltage
was increased from 0 to 40 V at a rate of ~0.67 V/min to gradually heat up m-SWNTs, while apositive gate voltage (~10 V) was applied. After the full-length breakdown process, organic
film was removed with acetone. Transfer characteristics of an FET after the process (Fig. 1)
show improvement in on/off current ratio from ~2 to ~10,000, indicating selective removal of
m-SWNTs. Figure 2 shows scanning electron microscopy (SEM) images of the FET before andafter the process. The SWNT indicated by the arrows in Fig. 2 was removed over its full length(16.4 m) and the length is over 100 times larger than the removal length by conventional inair electrical breakdown. Removal of SWNTs was confirmed also by Raman mapping
measurement. Atomic force microscopy observations indicated that molecular glass around mSWNTs was locally involved in chemical reactions along with the SWNTs and induced thelong-length removal of m-SWNTs. Since a rate of increase of drain voltage affected the removal
length, we speculate that molecular glass heated up by Joule heating of SWNTs prevented rapid
cooling of the SWNTs after the breakdown, thus increasing the removal length.
Before
10

−6

10

−8

10

−10

After

Drain Voltage = −1 V

−10Fig. 10Gate Voltage (V)10Transfer characteristics of the FET
before and after the process.

[1] P. G. Colins et al., Science 292, 706 (2001).
[2] S. H. Jin et al., Nat. Nanotechnol. 8, 347 (2013).
Corresponding Author: S. Maruyama
Tel: +81-3-5841-6421, Fax: +81-3-5841-6983,
E-mail: maruyama@photon.t.u-tokyo.ac.jp

Fig.2 SEM images of an SWNT array (a) before and(b) after the breakdown process.

- 25 -

2-9
Anomeric effect on the ring conformation of spiro-acetalyzed [60]fullerenes○Ken Kokubo, Yu Yamazaki, Hiroyuki Masuda, Naohiko Ikuma
Division of Applied Chemistry, Graduate School of Engineering, Osaka University,
2-1 Yamadaoka, Suita, Osaka 565-0871, Japan.
The anomeric effect is a kind of stereoelectronic effect that is originally observed inpyranose rings with heteroatomic substituents adjacent to an oxygen atom within atetrahydropyran ring. The substituent, generally hydroxyl or alkoxy group, prefers the axial
position instead of the sterically less hindered equatorial position. In the present study, we
first found such anomeric effect in specially designed fullerene derivatives, such as
spiro-acetalyzed [60]fullerenes, on the steric conformation of exo- and endo-isomers.
Spiro-acetalyzed fullerenes were synthesized by TiCl4-mediated acetalization of
cyclohexanone-fused fullerene, which was prepared by Diels-Alder reaction of C60 with
2-trimethylsilyloxy-1,3-butadiene followed by hydrolysis, with various diols [1]. While
simple diols HO(CH2)nOH (n = 2, 3, 4) gave the corresponding 5-, 6-, and 7-membered ringspiro-acetalyzed fullerenes as a single product, respectively, 2-substituted-1,3-propanediol
HOCH2CHRCH2OH (R = Me, Ph) gave the two separable isomers. By 1H and 13C NMR
spectroscopy along with X-ray structural analysis, the structures of major and minor products
were determined as exo- and endo- ring-flipped isomers, respectively. The DFT calculations
revealed that endo-isomer is more stable than exo-isomer, although the former seems to be
more sterically hindered. This result can be well explained by the anomeric effect.

[1] Kokubo, K.; Masuda, H.; Ikuma, N.; Mikie, T.; Oshima, T. Tetrahedron Lett. 2013, 54, 3510.
Corresponding Author: K. Kokubo
Tel: +81-6-6879-4592, Fax: +81-6-6879-4593, E-mail: kokubo@chem.eng.osaka-u.ac.jp- 26 -

2-10
Spiro-acetalized and Ðthioacetalized [60]fullerene as efficient acceptor
materials for bulk heterojunction solar cells○Tsubasa Mikie, Akinori Saeki, Hiroyuki Masuda, Naohiko Ikuma, Ken Kokubo, Shu Seki
Department of Applied Chemistry, Graduate School of Engineering, Osaka University,
2-1 Yamadaoka, Suita, Osaka 565-0871, Japan.
Although functionalized fullerene derivatives are the most promising electron acceptor
materials in organic photovoltaics (OPV), the successful examples have been limited in[6,6]-phenyl-C61-butylic acid methyl ester (PC61BM) and indene C60 bis-adducts (ICBAs).
This is due to the difficulty in simultaneous achievement of solubility, miscibility with p-type
polymer, and electron accepting and transporting ability. Besides, simplified schemes ofsynthesis and purification are strongly required in the practical applications.
Herein, we report a systematic study on OPV of spiro-acetalized and -thioacetalized[60]fullerene derivatives as a n-type materials and poly(3-hexylthiophene) (P3HT) as a p-typematerial. The spiro-acetalized [60]fullerene having 7-membered ring synthesized by two-stepreactions (3c in Fig.1a) demonstrates the power conversion efficiency (PCE) of 4.04%, whichis comparable to that of PC61BM. Interestingly the PCEs are increased linearly with thesolubility of the mono-adduct fullerenes and saturated at > 5 mg/ml (Fig. 1b), indicating the
PCE is primarily dominated by the solubility relating to the film morphology. Accordingly wemeasured hole and electron mobilities (µhand µe) for the fullerenes showing > 2.5%
PCE

byspace-charge

limitedcurrent(SCLC) technique. As shown in Fig. 1c, it

was found that the balance between µh andµe scales with the PCE, revealing that µe/µh

is

the

secondarydominant

factor,inaccordance with the reported simulation
result. To our surprise, 3c showed perfectly

balanced mobilities, which may evolve
further advancement in PEC by extra

molecular engineering of spiro-acetalized
fullerene family.

Figure 1. a) Structure of spiro-acetalized andÐthioacetalized[60]fullerene
derivatives.
Correlation of the PCE if P3HT:fullerenes OPV
with b) solubility of fullerenes in toluene andwith c) log (µe/µh).

[1] Kokubo, K.; Masuda, H.; Ikuma, N.; Mikie, T.; Oshima, T. Tetrahedron Lett., 2013, 54, 3510.
*Corresponding Author: Shu Seki
Tel: +81-6-6879-4586, Fax: +81-6-6879-4586, E-mail: seki@chem.eng.osaka-u.ac.jp- 27 -

2-11
Dielectric Phase Transition of [Li@C60](PF6) at Low Temperature○Shinobu Aoyagi1, Kunihisa Sugimoto2, Hiroshi Okada3,
Norihisa Hoshino4, Tomoyuki Akutagawa4
1

Department of Info. and Bio. Sciences, Nagoya City University, Nagoya 467-8501, Japan
2
SPring-8/JASRI, Kouto, Sayo, Hyogo 679-5198, Japan3
Department of Chemistry, The University of Tokyo, Tokyo 113-0033, Japan
4
Institute of Multidisciplinary Research for Advanced Materials and Graduate School ofEngineering, Tohoku University, Sendai 980-8577, Japan
Endohedral lithium fullerene Li+@C60 can have a dielectric polarization by theoff-centered location of the Li+ cation inside the C60 cage. The x-ray structure analysis of thePF6− salt [Li@C60](PF6) revealed that the Li+ cation occupies two off-centered equivalent
positions at 20 K and hence the crystal is non-polar [1]. The disordered structure at low
temperature is explained by a static orientation disorder of polar Li+@C60 cations and/or adynamic tunneling of the Li+ cation inside the C60 cage. The Li+ tunneling would be
suppressed by an intermolecular interaction at lower temperature and a dielectric phasetransition might be induced. We reveal the dielectric property and crystal structure of[Li@C60](PF6) below 20 K in this study.
The temperature dependence of the dielectric permittivity was measured for the single
crystal down to 9 K. The dielectric permittivity increases with decreasing temperatureaccording to the Curie-Weiss law. Such a behavior was also observed in H2O@C60 crystal but
not in empty C60 crystal [2]. No dielectric phase transition was observed in H2O@C60 down to
8 K. In contrast, a dielectric anomaly suggesting a phase transition was observed in[Li@C60](PF6) around 18 K. The x-ray diffraction experiment below 20 K was also performed
at SPring-8 BL02B1. The crystal has a cubic structure at 20 K [1]. The temperaturedependence of the cubic lattice constant shows no anomaly around 18 K. However, diffraction
peaks that are forbidden for the given structure appear below 18 K. Thus the crystal symmetryis lowered by the dielectric phase transition. We present the result of the crystal structure
analysis of the newly discovered low-temperature phase.
[1] S. Aoyagi et al. Angew. Chem. Int. Ed. 51, 3377 (2012).
[2] S. Aoyagi et al. Chem. Commun. 50, 524 (2014).
Corresponding Author: S. Aoyagi
Tel: +81-52-872-5061,
E-mail: aoyagi@nsc.nagoya-cu.ac.jp- 28 -

2-12
Photoinduced Electron Transfer and Photoelectrochemical Properties ofSupramolecular Complexes Composed of Lithium Ion-Encapsulated
Fullerene and Porphyrinoids○Kei Ohkubo 1, Yuki Kawashima 1, Hayato Sakai 2, Taku Hasobe 2, Ángela Sastre-Santos 3,
Shunichi Fukuzumi 1
1

Department of Material and Life Science, Graduate School of Engineering, Osaka
University, ALCA, Japan Science and Technology Agency, Osaka 565-0871, Japan2
Department of Chemistry, Faculty of Science and Technology, Keio University, Yokohama,223-8522, Japan
3
División de Química Orgánica Instituto de Bioingeniería, Universidad Miguel Hernández,
Elche 03202, Spain
Photoelectrochemical cells (PECs) have been widely investigated as a next-generation solar
cell because of their simple structures. The photoinduced charge separation between the
excited state of dye and the electrode plays an important role in improvement of PEC
performance. Extensive efforts have so far been devoted to design and synthesize electron
donor-acceptor linked molecules to achieve efficient photoinduced charge separation for
applications to PECs. Porphyrins and the related macrocyclic molecules such asphthalocyanines and chlorins are widely used as the electron donor due to the efficientelectron transfer and light harvesting properties. We have recently designed and synthesized
simple electron donor-acceptor supramolecular complexes composed of lithium ion
encapsulated fullerene (Li+@C60) and sulfonated zinc meso-tetraphenylporphyrin (ZnTPPS4–).
Photoexcitation of the supramolecule exhibited extremely slow charge-recombination of the
CS state (τ = 0.3 ms) in benzonitrile (PhCN).[1] The driving force of photoinduced electrontransfer from ZnTPPS4– to the triplet excited state of Li+@C60 is highly positive (–ΔGET =0.98 eV) in polar PhCN,[1] which is large enough to afford the CS states even under the
non-polar environment in nanoclusters. We report herein photovoltaic cells using
Li+@C60/ZnTPPS4– nanoclusters, which areassembled on optically transparent electrode(OTE) of nanostructured SnO2 (OTE/SnO2) asshown in Scheme 1.
The maximum IPCE value attained in theseexperiments was 77% at 450 nm [2]. WhenZnTPPS4– is replaced by anionic zincphthalocyanine and zinc chlorin derivatives [3],efficient photocurrent generation behaviours were
Scheme1
Schematic
imageofalso observed under the similar experimental
photoelectrochemical
cellof
OTE/SnO2/ZnTPPS4–/Li+@C60
conditions.
[1] Ohkubo, K.; Kawashima, Y.; Fukuzumi, S. Chem. Commun. 2012, 48, 4314
[2] Ohkubo, K.; Kawashima, Y.; Sakai, H.; Hasobe, T.; Fukuzumi, S. Chem. Commun. 2013, 49, 4474.
[2] Kawashima, Y.; Ohkubo, K.; Mase, K.; Fukuzumi, S. J. Phys. Chem. C 2013, 117, 21166.
Corresponding Author: K. Ohkubo
Tel: +81-6-6879-7369, Fax: +81-6-6879-7370,
E-mail: ookubo@chem.eng.osaka-u.ac.jp- 29 -

3-1
A wet spinning method of a continuous polymer-freecarbon nanotube fiber with the high electrical conductivity○Ken Mukai 1, Kinji Asaka 1, Toshiya Murakami 2 , Chihiro Itoh 2,
Takeshi Saito 3, 4, Motoo Yumura 3, 4
1

Health Research Institute, National Institute of Advanced Industrial Science and Technology(AIST), Ikeda 563-8577, Japan2
Department of Materials Science and Chemistry, Wakayama University, Wakayama
640-8510, Japan
3
Nanotube Research Center, National Institute of Advanced Industrial Science andTechnology (AIST), Tsukuba 305-8565, Japan
4
Technology Research Association for Single Wall Carbon Nanotubes (TASC), Tsukuba
305-8562, Japan

Fibers composed of carbon nanotubes (CNTs) have the potential to form high strength,
lightweight, thermally and electrical conducting materials.
As one of typical methods to fabricate CNT fiber, wet spinning method is widely known.
In an established method of fabricating CNT fiber by wet spinning method, coagulating
solution contains a polymer in order to allow easy fabrication and structural stability. [1] On
the other hand, the insulating characteristics of polymer in the CNT fiber results in a loweringof the electrical conductivity.
We have successfully developed a novel wet-spinning method of a continuous
polymer-free CNT fiber. We here shows remarkably high electrical conductivity, more than7000 Scm-1 of the polymer-free CNT fiber.
This achievement was possible due to the CNT alignment in CNT fiber by stretching thestrong CNT fiber composed of `the enhanced direct injection pyrolytic synthesis method(e-Dips)’ CNTs during drying process.

Two AA
Batteries(3 V)

Fig. 1

Diode Midget
Lamp
CNT fiber(50 cm in Length)

Lighting up of Midget Lamp.

Fig. 2 SEM photograph of CNT fiber after
stretching process.

[1] B. Vigolo, et al., Scinece 290, 1331 (2000).
Corresponding Author: K. Mukai
Tel: +81-72-751-8376, Fax: +81-72-751-8370,
E-mail: mukai-ken@aist.go.jp- 30 -

3-2
Carbon nanotube 3D current collectors for lightweight, high performanceand low cost electrochemical capacitor electrodes○ Ricardo Quintero1,2, Dong Young Kim2, Kei Hasegawa2, Yuki Yamada1, Atsuo Yamada1
and Suguru Noda2,*
1

Department of Chemical System Engineering, The University of Tokyo, 7-3-1 Hongo,
Bunkyo-ku, Tokyo 113-8656, Japan2
Department of Applied Chemistry, Waseda University, 3-4-1 Okubo, Shinjuku-ku, Tokyo
169-8555, Japan
In the electrochemical capacitor (EC) field, extensive research has been made toincrease the specific capacitance of active materials. These materials often lack enoughelectrical conductivity and the addition of conductive fillers is necessary in practicalapplication, with the trade-off of reduction of maximum specific capacitance of devices.
Metal current collectors account for a significant part of the weight of practical devices, andby replacing them with lightweight materials, the performance of an entire capacitor device
can be further improved [1]. We propose here the development of simpler electrodearchitecture in order to achieve higher performances. By capturing activated carbon (AC), a
low cost capacitive material, inside a matrix made using a small amount of FWCNTs, lightweighted hybrid electrodes were fabricated [2].
Self-supporting electrodes were obtained throughthe systematic combination of AC with sub millimeterlong FWCNTs (6–10 nm diameter, 0.4 mm length, 99
wt% purity, 3 walls on average) [3]. To evaluate theperformance of the FWCNT 3D collector matrix, different
configurations of a Ti mesh connected to the carbon
electrodes were prepared (Fig. 1). Long FWCNTs provide
mechanical stability and less contact/junction resistances,making possible to produce electrodes featuring no
additional binder materials and able to contain capacitiveFig.1 Schematic of proposed electrodeparticles at a weight 9 times as much as its own weight. architecture and metal collector
The FWCNT matrix effectively improved the capacitance connections.
of the inexpensive, high surface area AC to 169 F/g at aslow scan rate of 5 mV/s, and to 131 F/g at a fast scan rateof 100 mV/s, in fairly thick (~200 mm) electrodes.
Connection to a metallic collector at the film edge only,
which significantly reduced the use of metal, retainedmuch larger capacitance for the AC-FWCNT hybrid film
(107 F/g) than for the conventional AC electrode withbinder (PTFE) and conductive filler (AB) (3.9 F/g) at apractical voltage scan rate, 100 mV/s (Fig 2).
[1] P. Simon, Y. Gogotsi, Nat Mater 7 (2008) 845.
[2] R. Quintero, et al., RSC Adv., in press.
[3] D.Y. Kim, et al., Carbon 49 (2011) 1972.
Corresponding Author: Suguru Noda
Tel/Fax: +81-3-5286-2769, E-mail: noda@waseda.jp- 31 -

Fig.2 Rate capability of AC-FWCNT
and AC-AB-PTFE electrodes indifferent metal collector configurations.

3-3
Green, scalable, binderless fabrication of a single-wall carbon nanotube
nonwoven fabric based on an ancient Japanese paper process○Kazufumi Kobashi 1,2, Tatsuya Hirabayashi 2, Seisuke Ata 1,2, Takeo Yamada 1,2, Don N.
Futaba 1,2, Kenji Hata 1,2
1

Technology Research Association for Single Wall Carbon Nanotubes (TASC), Tsukuba,
305-8565, Japan
2
Nanotube Research Center, National Institute of Advanced Industrial Science andTechnology (AIST), Tsukuba, 305-8565, Japan

We propose a fabrication method for carbon nanotube (CNT) nonwoven fabrics based on
an ancient Japanese papermaking process where paper is made from natural plant fibers [1].
In our method, CNT nonwoven fabrics are made by a scalable process of filtering binder-free,aqueous suspensions of CNTs. The aqueous suspension of these entangled single-wall carbon
nanotube (SWNT) aggregates enabled smooth filtration through a cellulose filter with large
pores (8um). The “wet SWNT cakes,” which comprised solely of SWNT and water andobtained after filtration, were press dried to fabricate a SWNT nonwoven fabric. This
environmentally friendly process employs water and the raw CNT material alone, anddemonstrates a great advantage over conventional CNT nonwoven fabric (Buckypaper)
manufacturing technology which utilizes large quantities of organic solvent and binders,which must subsequently be disposed and removed, respectively. Moreover, the scalability ofthis process was demonstrated by manufacturing a large area (A3, 30x42 cm, thickness,
40–150 µm), self-supporting SWNT nonwoven fabric with a density of 0.4 g/cm3, basis
weight of 0.2 g/m2 , porosity of 63%, and specific surface area of 740 m2/g. This SWNT
nonwoven fabric is anticipated to find application as functional particle-supported sheets,
electrode materials, filters.
Filter100 mDisperse
SWNT forest
in water by
wet-jet mill

SWNT nonwoven fabricA3 size (30x42 cm)

100 mEntangled aggregate
of long SWNTs

Figure 1 Green, scalable, binderless fabrication of nonwoven fabric (A3 size) from aqueous
suspension of entangled SWNT aggregates.
[1] K. Kobashi et al. ACS Appl. Mater. Interfaces. 5, 12602 (2013).
Corresponding Author: Kenji Hata
Tel: +81-29-861-4654, Fax: +81-29-861-4851,
E-mail: kenji-hata@aist.go.jp- 32 -

3-4
Large-scale first-principles study of the electronic transport properties ofgraphene nanoribbons on SiO2/Si○Hideyuki Jippo1, Taisuke Ozaki2, Mari Ohfuchi1
1

Fujitsu Laboratories Ltd., 10-1 Morinosato-wakamiya, Atsugi, Kanagawa 243-0197, Japan
2
JAIST, 1-1 Asahidai, Nomi, Ishikawa 923-1292, Japan

Graphene is normally supported on insulators such as SiO2 in electronic devices. The
electronic transport properties of graphene on SiO2 are remarkably different from those ofsuspended graphene [1,2]. The surface treatment of SiO2 even changes the electric transport
properties [3]. In this article, we investigate the electronic transport properties of armchairgraphene nanoribbon (AGNR) transistors on SiO2/Si with long channel lengths of 9.91 and15.1 nm. We also show the difference between O- and OH-termination of the SiO2 surface.
The models of AGNRs on SiO2/Si with the channel
length of 9.91 nm are shown in Fig. 1. The channel of
AGNRs is sandwiched between semi-infinite AGNR
leads. The numbers of atoms for the models with channel
lengths of 9.91 and 15.1 nm amount to 1974 and 3030,
respectively. For transport calculations, we employ thenonequilibrium Green’s function method implemented inFig. 1. (a) Top view and (b)(c) side
the density functional theory code, OpenMX [4].
Figure 2 shows currents evaluated by integrating the views of the left edge of the model of
AGNRs on SiO2/Si with a channeltransmission at a bias voltage of 0 V over the energy length of 9.91 nm.
The SiO2 surfaces
regime of 0.5 eV with respect to the center energy of the are terminated by (b) O and (c) OH.
integration region. For freestanding AGNRs [(a) and (b)], The dotted rectangles represent thethe on/off current ratio for the longer channel (15.1 nm) unit cell of leads.
is larger by a factor of 107 than that for the shorter
channel (9.91 nm). On the other hand, for AGNRs on
O-terminated SiO2/Si [(c) and (d)], the ratio does notdepend on the channel length. The current gaps are
shifted by 0.7 eV, indicating p-type conduction. The
current on/off ratio 105 is significantly smaller than thosefor freestanding AGNRs. The value 105 is consistent with Fig. 2. Currents for (a)(b) freestanding
AGNR, (c)(d) AGNR on O-terminatedthe experimental data for GNRs on SiO2 [1]. We also SiO /Si, and (e) AGNR on
2
investigated AGNRs on OH-terminated SiO2/Si [5]. The OH-terminated SiO2/Si. The channel
on/off current ratio for the OH-terminated surface (e) is lengths are 9.91 nm for (a)(c)(e) andsmaller on the p side than that for the O-terminated 15.1 nm for (b)(d).
surface (c). We found that the OH groups have broad states around the valence band
maximum of AGNRs and more holes are injected from OH-terminated SiO2 to AGNRs thanO-terminated SiO2. This is considered to contribute the smaller on/off current ratio and may
relate to the Dirac point shift and the degraded mobility found in the measurements forgraphene on OH-terminated SiO2 [3].
[1] X. Li et al., Science 319, 1229 (2008). [2] M.-W. Lin et al., Nanotechnology 22, 265201 (2011).
[3] K. Nagashio et al., J. Appl. Phys. 110, 024513 (2011).
[4] http://www.openmx-square.org/ [5] H. Jippo et al., Appl. Phys. Express, to be published.
Corresponding Author: H. Jippo
Tel: +81-46-250-8843, Fax: +81-46-250-8274, E-mail: jippo.hideyuki@jp.fujitsu.com- 33 -

3-5
Analysis of intercalated multi-layer graphene synthesized by CVDżDaiyu Kondo, Haruhisa Nakano, Bo Zhou, Akiko I, Kenjiro Hayashi, Junichi Yamaguchi
Makoto Takahashi, Shintaro Sato and Naoki Yokoyama
Collaborative Research Team Green Nanoelectronics Center (GNC), AIST, 16-1 Onogawa,
Tsukuba 305-8569, Japan
Nano-carbon materials including graphene [1] are one of promising electronic materials
for future LSIs due to their excellent physical properties. Especially their tolerance to a highcurrent density might make them replace cupper (Cu) as future interconnect materials, since
the reliability of Cu interconnects decreases with their line width. However, nano-carbon
materials have generally indicated a resistivity higher than that of Cu. For instance, theresistivity of high-quality graphene peeled off from HOPG is an order of magnitude higher
than Cu. Recently, we reported that intercalated MLG interconnects synthesized by chemical
vapor deposition (CVD) had a resistivity of the same order as that of Cu [2]. On the other
hand, the amount of FeCl3 intercalated into MLG grown by CVD was not as large as thatintercalated into MLG peeled off from HOPG reported previously, according to Raman
spectroscopy [3]. To find the origin of these differences, we analyzed the distribution of FeCl3
molecules in the MLG by using EELS, EDX and(a)
PEEM measurements.
MLG was synthesized on a 200-nm cobalt
MLG
catalyst film sputtered on a sapphire c plane by
SiO2°
thermal CVD at around 1000C . As process gases,
20nm(b)CH4, H2 and Ar were utilized. After MLG
interconnects were fabricated by the conventional
photo lithography, the intercalation of FeCl3 into
MLG interconnects was performed at 310C°.
Figure 1 shows a cross sectional STEM imageof the intercalated MLG interconnect and the line
profile of EELS spectra. From the line profile, it is Figure 1 Cross sectional STEM image ofclear that Fe and Cl have nonuniform distributions the intercalated MLG interconnect and theacross the MLG interconnect, implying nonuniform line profile of EELS spectra measured
intercalation into MLG. The details will be discussed along blue dot lines.
in the presentation.
This work was supported by JSP through the “FIRST Program,” initiated by CSTP. A
part of this work was conducted at the Nano-Processing Facility, supported by IBEC
Innovation Platform, AIST. The synchrotron radiation experiments were performed at theBL17SU of SPring-8 with the approval of the Japan Synchrotron Radiation Research Institute(JASRI) (Proposal No. 2012B1029 and 2013A1017).
[1] K.S. Novoselov et al., Science 306, 666 (2004).
[2] D. Kondo et al., IEEE International Interconnect Technology Conference 2013, pp 190.
[3] W.J. Zhao et al., J. Am. Chem. Soc. 133, 5941 (2011).
Corresponding Author: D. Kondo
Tel: +81-29-849-1074, Fax: +81-29-849-1186,
E-mail: kondo.daiyu@aist.go.jp- 34 -

3-6
Graphene as a Material for Next Generation Fuel Cells
Stephen Matthew Lyth1, Jianfeng Liu2, Thomas Bayer1, Sean Bishop1, Kazunari Sasaki1,2
1
1International Institute for Carbon-Neutral Energy Research, Fukuoka 819-0395, Japan
Department of Mechanical Engineering, Kyushu University, Fukuoka 819-0395, Japan

Graphene is an extremely promising material for use in fuel cells, due to its high strength,
large surface area, and excellent thermal and electronic conductivities.. Fuel cells are
extremely efficient energy conversion devices which react fuel (e.g. hydrogen) and oxygen in
an electrochemical process to produce electricity. They have high energy density, are quite,
durable, and can be carbon-neutral if renewably sourced hydrogen is used as a fuel.
We are exploring the application of graphene in polymer electrolyte membrane fuel cells(PEMFCs) as high surface area platinum electrocatalyst supports; as metal-free non-precious
catalysts; and we are utilizing graphene oxide as a new proton-conducting material.
We synthesize large surface area, defective graphene foam (GF) by combustion of sodium
ethoxide, followed by several high-temperature treatment steps to reduce oxygen content,
increase crystallinity, and improve electronic conductivity (Figure 1a). This is decorated withplatinum nanoparticles and applied as a cathode catalyst for PEMFCs. Our results arepromising, with Pt/GF having a higher mass activity (the catalytic activity normalized to themass of platinum) than the industry standard; Pt-decorated carbon black. (Figure 1b).
However, we are still working on improving durability and PEMFC power density.
We also make nitrogen-doped defective graphene foam (GFN). We apply this as a
non-precious catalyst for electrochemical oxygen in PEMFCs. By virtue of the large surface
area, we observe very high current density despite absence of metal. We use these results toshed insight on the catalytic mechanism of electrochemistry on nitrogen-doped carbons.
Graphene oxide (GO) is produced by acid treatment of graphite. It is an electronicallyinsulating, water dispersible analogue of graphene. The surface oxygen functionalities and theaffinity for water make GO a potential material for ionic membranes in PEMFCs. We haveprobed the fundamental ionic conductivity of graphene oxide membranes, and successfully
made GO membrane fuel cells that operate at elevated temperature (Figure 1c).

Figure 1. (a) Scanning electron microscopy image of our defective graphene foam. PEMFC voltage and power
density using (b) a Pt/GF electrocatalyst layer and (c) a GO proton-conducting membrane.
[1] J. Liu, K. Sasaki, S. M. Lyth, ECS Transactions 58, 1751 (2013)[2] J. Liu, K. Sasaki, S. M. Lyth, ECS Transactions 58, 1529 (2013)[3] S. M Lyth, et al, International Journal of Hydrogen Energy 39 (1), 376-380
Corresponding Author: S. M. LythTel: +81-92-802-6742, Fax: +81-92-802-6742. E-mail: lyth@i2cner.kyushu-u.ac.jp- 35 -

3-7
Graphene enabled micromechanical switches
Shao-Wei Ma1, Ya-Ping Hsieh *1

Graduate of Institute of Opto-Mechatronics, National Chung Cheng University, ROC*corresponding email: yphsieh@ccu.edu.tw

Power consumption is the major technical problem affecting the development andapplication of electronic devices. Especially leakage currents in the off-state are afundamental issue of semiconductor devices. Micro-electromechanical switches havedemonstrated significantly lower leakage currents due to their dissimilar underlying operation
mechanism. Their high complexity, large scale and low switching speed, however, make them
unsuitable for universal integration in electronics.
We here demonstrate the application of graphene, a single-atomic layer of graphite.
Graphene’s low mass density and high strength make it ideally suited for high switching
speed while its chemical and mechanical stability allows the application of high current
densities.
We developed a novel three-terminal device layout where suspended graphene-membranes
are forced into contact with a bottom electrode by application of a gate bias, resulting in the
micromechanical equivalent of a transistor. Using facile self-assembly techniques, large
arrays of these switches are produced at low cost and with easy scalability. The use of large
scale switch arrays allows the control of high current values.
The presented results highlight the potential of graphene-enabled microswitches and open
up new opportunities for mobile and ubiquitous electronic devices.

- 36 -

3-8
Twisting angle dependence of G band Raman intensity enhancement of
twisted bilayer graphene○Kentaro Sato 1, Riichiro Saito 2
1

2

Sendai National College of Technology, Sendai 989-3128, Japan
Department of Physics, Tohoku University, Sendai 980-8578, Japan

Twisted bilayer graphene (TBG) is a kind of bilayer graphene. When the first or second
graphene layer of bilayer graphene rotates about an axis perpendicular to the graphene surface,a structure with a much larger unit cell than that of graphene appears at a twisting angle. Since
the physical properties of TBG depends on the twisting angle [1], it is important to estimate
the angle in order to understand its physical properties.
Several groups have reported that G band Raman intensity of TBG is enhanced more than
30 times as large as that of monolayer graphene at specific excitation laser energy (Elaser) andtwisting angle because of singularity in density of states [2-5]. Since resonance Raman spectra
give us information to characterize not only the number of graphene layers but also thestacking structure, we can estimate the angle of TBG sample from the Raman spectra.
In this presentation, we study the G band Raman intensity of TBG as a function of twistingangle for more than 150 samples with different twisting angles and Elaser. The intensity of
TBG is enhanced at a specific twisting angle and Elaser because the density of states of TBG isdivergent and the energy difference between the singular points in the density of statescorrespond to Elaser. We calculate density of states and Raman intensity of TBG as a functionof twisting angle in order to compare experimental results with calculation directly and study
the relation between Raman intensity and twisting angle [6]. The density of states iscalculated based on the tight binding method. The Raman intensity is given by calculating
electron-photon and electron-phonon matrix elements.
[1] G. Trambly et al., Nano Lett. 10, 804 (2010).
[2] Z. Ni et al., Phys. Rev. B 80, 125404 (2009).
[3] R. W. Havener et al., Nano Lett. 12, 3162 (2012).
[4] K. Kim et al., Phys. Rev. Lett. 108, 246103 (2012).
[5] K. Sato et al. Phys. Rev. B 86, 125414 (2012).
[6] G.S.N. Eliel, H.B. Ribeiro, K. Sato et al. unpublished.
Corresponding Author: K. Sato
Tel: +81-22-391-5575
E-mail: kentaro@sendai-nct.ac.jp- 37 -

3-9
Nitrogen-containing graphene analyzed by X-ray photoelectron
spectroscopy○Yasuhiro Yamada, Jungpil Kim, Shintaro Matsuo, Satoshi Sato
Graduate School of Engineering, Chiba University, 1-33 Yayoi, Inage, Chiba 263-8522,
Japan
X-ray photoelectron spectroscopy (XPS) is among the most commonly used analyticalmethods for N-containing graphene. However, mainly three unclear problems such as C1sshifts, sp2- or sp3-hybridized carbon, and quaternary N (Q-Ns) still exist. In this work, XPS
spectra of N-containing graphene were simulated using density functional theory (DFT).
Peak shifts and FWHMs of C1s and N1s XPS spectra of N-containing graphene such as
pyridinic, sp2C-NH2(Fig. 1a), sp3C-NH2, pyrrolic, sp2C-CN, sp3C-CN, and valley quaternary
N (Q-N) on edges and sp3C-NH2, center amine (Fig. 1b), and center Q-N in the basal plane
were simulated using DFT calculation (B3LYP/6-31g(d) pop=full gfprint, Gaussian 09), andour recently developed method [1]. Binding energies of these model structures were obtainedusing an approximation based on the modified Koopmans theory (Fig. 2).
Assignments of N1s shifts were well fitted with reported shifts (Fig. 3), and assignments of
C1s and N1s shifts of various unreported functional groups could be obtained. Three major
problems could be mostly solved. For example, the shifts of main peaks of C1s spectra ofgraphene with various N-containing functional groups were revealed. There were clear
differences of C1s and N1s shifts between sp2C-NH2 and sp3C-NH2 on edges. Also,
assignments of amine groups and Q-Ns at valley and center positions were obtained. N1s
shifts revealed that shifts of center Q-Ns were different from valley Q-Ns, valley amine, andcenter amine. This type of fine XPS analysis of N-containing functional groups using C1s andN1s shifts, and FWHMs has not been conducted elsewhere.
(a)

Fig.1

(b)

N1s

Modeled structures of N- containing graphene
C-C

C-H
C-N

Fig.2

Simulated spectra of graphene in Fig. 1a[1] Y. Yamada et al. J. Mater. Sci. 48, 8171 (2013).
Corresponding Author: Y. Yamada
Tel: +81-43-290-3376, Fax: +81-43-290-3376,
E-mail: y-yamada@faculty.chiba-u.jp

Fig.3 Correlations between calculated binding
energies and averaged binding energies fromreferences of N1s spectra- 38 -

3-10
Optical and Raman Analysis of Graphene Films Formed within Microholeson Quartz Glass Substrates by Liquid Phase Growth MethodżHidefumi Hiura
1

Smart Energy Research Laboratories, NEC Corporation, Tsukuba, Ibaraki 305-8501, Japan
(a)

(b)

Since graphene has unique and excellent properties, many applications have been proposed sofar. In particular, graphene is promising fornext-generation electronics as a channel of transistors because it has extremely high field-effectmobility of more than 200,000 cm2 V௅1s௅1 even at(d)room temperature. In the future when fabricating (c)graphene devices in an industrial scale, it will benecessary to develop graphene-on-insulator substrates. In the past Symposia, we reported a novel
production method of graphene using liquid
phase growth (LPG), thereby making it possible
to synthesize graphene films directly on many (e)(f)
kinds of insulating substrates from many kinds ofsolid carbon materials [1, 2].
As reported in [2], the LPG method enables us
to form graphene films selectively within the microholes on the surface of a quartz substrate. An
example is shown in Fig. 1. An optical analysis
based on the multilayer and multiple reflection Fig.1 Images of graphene films formed withinmodel [3, 4] reveals that the number of graphene a 10-ȝm-side square microholes, (a) opticalreflection image, (b) color plot of the number
layers is distributed from 1 L up to 8 L as depict- of graphene layers, (c) Raman intensity
ed in Fig. 1(b). Raman mapping analyses clearly mapping image of G band, (d) Raman intendemonstrate that both G band and 2D band tend sity mapping image of 2D band, (e) Raman
to increase in intensity as the number of graphene frequency mapping image of G band, (f) Ralayers increases as shown in Fig. 1 (c) and (d). On man frequency mapping image of 2D band.
the contrast, there is no apparent correlation between the number of graphene layers and Raman frequencies both of G and 2D bands as shown in Fig 1(e) and (f), respectively. As awhole, the closer graphene films lie to the circumference of the microhole, the lower Raman
frequencies both of G and 2D bands are: the lowest G band frequency is around 1560 cm௅1and can be found in the cutting edge of the microhole. These observations may be explainedin part by differences in strain of graphene films. Namely, the graphene films in the central
part become strained due to the firm contact with the bottom of the microhole, while the graphene films in the peripheral have no strain because they are suspended in the air.
Distribution of Number of Layers

Optical Image

8L
7L
6L
5L
4L
3L
2L
1L

0 0.1 0.2 0.3
Abandance / 

1 ȝm

G Band Raman Intensity Image

Raman Intensity / Counts

0

0

1590

2D Band Raman Frequency Image

2696

2D Band Raman Shift / cm௅1

G Band Raman Shift / cm௅1

1585

2690

1580

2684

1575

2678

1570

2672

1565

2666

1560

2660

[1] H. Hiura et al. The 40th Commemorative Fullerene-Nanotubes General Symposium, 3-7 (2011).
[2] H. Hiura et al. The 42nd Fullerene-Nanotubes-Graphene General Symposium, 3-2 (2012).
[3] P. Blake et al. Appl. Phys. Lett. 91, 06124 (2007).
[4] H. Hiura et al. NEW DIAMOND, 27(3), 42-46 (2011).
Corresponding Author: H. Hiura
Tel: +81-29-850-1116, Fax: +81-29-856-6139,
E-mail: h-hiura@bq.jp.nec.com- 39 -103

Raman Intensity / Counts

G Band Raman Frequency Image

2D Band Raman Intensity Image

103

3-11
Novel transfer method for clean and high mobility CVD graphene○Ya Ping Hsieh1, Mario Hofmann 2, Bo Suei Chiang 3
1

2

Department of Opto-Mechatronics, National Chung Cheng University, Taiwan
Department of Materials Science and Engineering, National Cheng Kung University,
Taiwan3.
Department of Opto-Mechatronics, National Chung Cheng University, Taiwan

Using Chemical vapor deposition (CVD) to synthesis graphene is known to produce highquality and large area graphene. The employed conductive catalytic substrate necessitates atransfer process after graphene growth. Surface contamination of graphene with polymer
residues has been a significant problem in graphene transfer. Various reports show that theincomplete bond-scission and covalent bonding of Poly(methyl methacrylate)(PMMA) withgraphene will deteriorate the quality and thus limit the achievable carrier mobility.
Here we report a new method of transferring graphene using alkane-based polymer supports.
XPS, FTIR and Raman analysis show that these polymers produce less defects in thegraphene which attributed to the absence of oxygen functional groups. The lower thermal andchemical stability of the alkenes used furthermore assists in the cleaner removal as confirmed
by Atomic force microscopy. These advantageous properties result in a higher carrier mobility
in graphene after transfer as determined by both Hall-effect and field effect mobility
measurements.
Our approach makes transferring graphene cheaper and easier and opens up a route toenhance the mobility of graphene for future electronic applications.

Corresponding Author: Ya Ping Hsieh
Tel: 05-2720411, Fax:
E-mail: yphsieh@ccu.edu.tw- 40 -

3-12
Mechanism and impact of ad-layer formation on CPCVD graphene
Yi-Wen Wang1, Ya-Ping Hsieh1, Mario Hofmann 2
1

2

Graduate of Institute of Opto-Mechatronics, National Chung Cheng University, ROC.
Department of Material Science and Engineering, National Cheng Kung University, ROC.

Graphene, a two-dimensional carbon allotrope, has the potential to revolutionize
transparent optical conductors (TOCs) for use as electrodes in solar cells and novel electronics.
controlled chamber Chemical vapor deposition (CPCVD) has emerged as a promisingsynthesis method of large scale and high quality graphene. The conductance of one layer ofgraphene, however, is too low for many applications. Therefore, multi-layer graphene
formation is being investigated to improve electrical performance of TOCs.
We here present a study on the formation of a second layer during graphene CPCVD. From
the dependence of ad-layer growth rate, grain shape, and nucleation density on CPCVD
parameters such as pressure and carbon feedstock concentration we extract the formation
mechanism and its energetics.
We furthermore demonstrate that depending on the extent and density of this ad-layer, anenhancement or deterioration of the single-layer carrier mobility is observed. Theseobservations are explained by the competition of scattering interactions and parallel
conduction pathways.
The presented findings provide both methods and guidelines for further optimization ofgraphene morphology for TOC applications.
Corresponding Author: Ya-Ping Hsieh
Tel: +886-52720411#23601
E-mail: yapinglab@gmail.com- 41 -

࣏ࢫࢱ࣮Ⓨ⾲
Poster Preview

1P – 1 㹼 1P – 50
2P – 1 㹼 2P – 50
3P – 1 㹼 3P – 50

1P-1
Semiempirical molecular orbital estimation of the relative stability ofsulfated fullerenes○Naoki Noji2, Yosiaki Sano2, Kazumi Inoue1,2, Yosuke Kataoka1 , Hironori Ogata1,2,
Graduate School of Engineering, Hosei University , Tokyo 113-8656, Japan
Department of Faculty of Biosci Applied Chem., Hosei University ,Tokyo 113-8656, Japan
1

2

Polyhydroxylated fullerenes (C60(OH)x:fullerenols) have been thought to have potential
applications in a variety of areas, including optoelectronics, medical therapeutics,
biochemistry, polymer materials science, and electrochemistry, owing to its high solubility inlarge variety of solvents (depending on the number of hydroxyl groups x). The structure andsolid state properties of fullerenol solids composed of a single fullerenol element are very
interesting. However, fullerenols obtained by the normal synthetic procedures are all mixturesof various compositions and structural isomers. Figure 1 shows the typical MALDI TOF mass
spectrum of fullerenol(C60(OH)x, x=4-9) sample. Fullerenols were synthesized via hydrolysisof polycyclosulfted fullerene precursors1). So, the stable molecular structure of fullerenols canbe speculated from the molecular structure of the polycyclosulfted fullerenes.
In this work, the energies and heats of formation of C60(SO4)n (n=1-6) molecules were
calculated by using AM1 semi-empirical Molecular Orbital (MO) calculations. Table 1 shows
the results of heats of formation about most stable sulfated fullerene molecules.
In this presentation, the possible stable molecular structures of C60(OH)x will be discussed.
8000

6000

4000

2000

0
700

800

900

1000

M/z

Figure 1. MALDI TOF mass spectrum of the fullerenol C60(OH)x(x=4-9).
Table 1. Heats of formation of C60(SO4)n (n=1-6) molecules.
Substance
Heats of formation[kcal/mol]

C60SO4

C60(SO4)2

C60(SO4)3

C60(SO4)4

C60(SO4)5

C60(SO4)6

807

640

472

306

136

-28

[1] L. Y. Chiang et al. ,J. Org. Chem.59(1994) 3960.
[2] Zhongfang Chen et al. Journal of Molecular Structure (Theochem) 498 (2000) 227.
[3] Bo-Cheng Wang et al. Journal of Molecular Structure (Theochem) 391 (1997) 179-187
Corresponding Author:Hironori Ogata hogata@hosei.ac.jp, Tel. &Fax: 81-42-387-6229- 43 -

1P-2
Excited State Electronic Interactions inPushÐPull-ChromophoreÐ[60]Fullerene Conjugates○Michio Yamada1, Francesca Tancini2, Michael Sekita3, Dirk M. Guldi3, Mariza N. Alberti2,
W. Bernd Schweizer2, François Diederich2
1

Department of Chemistry, Tokyo Gakugei University, Koganei, Tokyo 184-8501, Japan
2
Laboratorium fŸr Organische Chemie, ETH ZŸrich, ZŸrich, Switzerland
3
Department of Chemistry and Pharmacy and Interdisciplinary Center for MolecularMaterials, Friedrich-Alexander-UniversitŠt Erlangen-NŸrnberg, Erlangen, Germany

A variety of pushÐpull-chromophoreÐ[60]fullerene conjugates was successfully synthesized
by applying Òclick chemistryÓ to the corresponding acetylene-appended fullerene precursors(see below). When the C60 units and pushÐpull motifs were linked through pyrrolidine rings,
no interactions occurred between the two moieties in the ground states. Instead, an electrontransfer proceeded upon light excitation, giving the charge-separated states, which wascorroborated by time-resolved transient absorption measurements.1
NEt2
Me
N

Me
N

(±)-7
NC
Me
N

(±)-8
NC

CN
CN

Me
N

CN

Fe

CN

NC

NEt2

Me
N

NC

CN
CN

Me
N

CN

CN
Fe

Fe
Et2N

NC

(±)-9

NC

CN

(±)-10
Et2N

CN(±)-11

CN

CN
CN

13

CN

CN

Et2N

CN

(±)-12

CN
Fe

CN
CN

CN

CN
Fe
CN
CN

CN

CN

14

15

List of compounds for this study.

[1] M. Yamada et al. Fullerenes, Nanotubes, Carbon Nanostruct., in press (2014).
Corresponding Author: M. Yamada
Phone & Fax: +81-(0)42-329-7493
E-mail: myamada@u-gakugei.ac.jp- 44 -

16

CN

1P-3
Synthesis of C60-C70 Two-Component Fullerene NanowhiskersżToshio Konno, Takatsugu Wakahara, Kun’ichi Miyazawa
Fullerene Engineering Group, Materials Processing Unit, National Institute for Materials
Science, Tsukuba, Ibaraki, 305-0044, Japan
Fullerene nanowhiskers (FNWs) are thin single crystal nanofibers composed of fullerene
molecules. Since FNWs are dissoluble in organic solvents, fullerene molecules can be reusedby redissolving FNWs into organic solvents. For this recyclability of FNWs, FNWs have avariety of material applications.
Various combinations of fullerene molecules are possible in FNWs. In this study, we attempt
to synthesize C60-C70 two-component FNWs with C70 molecules uniformly solid-soluted inmother phase of C60, since these have absorption bands of both C60 and C70, and are available
as new unique semiconductors with a wide wavelength range of light absorption.
We synthesized C60-C70 two-component FNWs by the liquid-liquid interfacial precipitation
method[1] at 288 K with toluene as a good solvent for fullerene and isopropyl alcohol as a poor
solvent for fullerene, shifting the ratio of C70 to C60. We conducted chemical composition
analyses on C60-C70 FNWs redissolved toluene solution by high-performance liquid
chromatography. As the result, from 9 to 14 mass% C70 is solid-soluted in C60-C70 FNWs. We
conducted Raman spectroscopic analyses on C60-C70 FNWs and particles. As the result, C70
peak area ratios of C60-C70 FNWs are from 15 to 27 % and C70 peak area ratios of particles arefrom 58 to 86 %. That is, the excess C70 molecules over the solid solubility limit to C60 motherphase form particles. We conducted Raman spectroscopic analyses on the surface and the insideof C60-C70 FNWs. As the result, C70 peak area ratios of the surface of C60-C70 FNWs are from15 to 27 % and C70 peak area ratios of the inside of C60-C70 FNWs are from 60 to 81 %. Thatis, there are more C70 on the inside of C60-C70 FNWs than on the surface of C60-C70 FNWs.
Using a focused ion beam system (Hitachi NB5000), we cut a C60-C70 whisker along thedirection normal to the growth axis by gallium ion beams, and obtained a cross-section of C60C70 whisker. We observed the cross-section of C60-C70
whisker by scanning electron microscopy. Figure 1
shows the micrograph of the sample. We conducted Xray diffraction analyses on C60-C70 FNWs and
C60NWs. As the result, C60-C70 FNWs contain a small
amount of rhombohedral phase, and have a lattice
constant of face-centered cubic phase that is larger by
0.77% than that of C60NWs. We conducted ultravioletvisible spectroscopic analyses on C60-C70 FNWs and
C60NWs. As the result, C60-C70 FNWs show thestronger visible light absorption than C60NWs, Fig.1 SEM image of the cross-section of
C60-C70 whisker.
especially at 600 nm.
[1] K. Miyazawa, Y. Kuwasaki, A. Obayashi, and M. Kuwabara, J. Mater. Res., 17, 83-88(2002).
Corresponding Author: K. Miyazawa
Tel: +81-(0)29-860-4528, Fax: +81-(0)29-860-4667
E-mail: miyazawa.kunichi@nims.go.jp- 45 -

1P-4
Transport Characteristics of Fullerene Nano-Whisker
Field Effect Transistor using Ionic Liquid Gate
○Naoto Toriumi1, Yoshiaki Ito1, Daiki Momiyama1, Wataru Akiyama1, Naoto Nakamura1,
Taishi Takenobu2, Jonathan P. Bird3, Yuichi Ochiai1, and Nobuyuki Aoki1
1

Graduate School of Advanced Integration Science, Chiba University,
Chiba, 263-8522 Japan2
3

Department of Applied Physics, Waseda University, Shinjuku 169-8555, Japan

Department of Electrical Engineering, University at Buffalo, SUNY, Buffalo, NY 14260-1920, USA

Ionic liquid (IL) shows highly polarized and low melting point at around room temperature.
Recently, the application to the electrical device is actively carried out. Using IL as a gate
dielectric layer of the field effect transistor (FET), electric double layer can be formed at theinterface of the semiconductor and the IL by applying a bias voltage. Since the thickness of thelayer is approximately 1 nm, extremely high electric field can be realized even by applying a
few voltages. Consequently, a low voltage operation is achieved in organic FETs [1]. In thisstudy, we applied the technique to an FET composed of fullerene nano-whisker (FNW) andobserved the transport characteristics.
The FNWs were prepared by liquid-liquid interfacial precipitation (LLIP) [2] and then weused m-xylene or toluene as the rich solvent. The FNW-FETs were put on preformed Au
electrodes on a SiO2/n++-Si substrate to form a bottom-contact structure. Observations of thetransport characteristics were carried out using a probe station in vacuum (~10-6 torr) afterthermal annealing at 440 K for 12 hours. IL (EMIM-TFSI) was dropped on FNW using one ofthe probes in vacuum after cooled down to room10
3.0x10
forward
V =1V
10
3.0x10backward
temperature and then the probe was used as an (a)2.5x10
forward
V =1V
backward
10
2.5x10electrode for the top-IL gate.
2.0x1010
2.0x10
Typical transfer and output characteristics of
10
1.5x1010
1.5x10the FNW-FET using the IL gate is shown in Fig.
1.0x1010
1.0x101 (a) and (b), respectively. Using the IL, a low
10
5.0x105.0x10threshold voltage (Vth = 0.13 V) was achieved.
0.0
10
-0.5
0.0
0.5
1.0
1.5
0.0
10
The mobility is estimated as 4.1 × 10-2 cm2/Vs.
-0.5
0.0
1.0
1.5
V G0.5(V)V (V)The detail of the characteristics of the FNW-FETV=0V(b) 40 0.30.6 VV
will be discussed in the presentation.
30
-7

-4

-7

-4

SD

-8

-4

SD

-4

-4

-8

-9

-4

-4

SD

-9

√I √I (A1/2)(A1/2)SD

I SD (A)I SD (A)

-4

-4

-10

-4

-5

-10

-5

-11

-11

G

G

[1] S. Ono et al., Appl. Phys. Lett. 92 103313 (2008)[2] K. Miyazawa et al., J. Mater. Res. 17 83 (2002)

I SD (nA)

20

0.9 V
1.2 V
1.5 V

10
0

-10

Corresponding Author: N. Toriumi
Tel: +81-43-290-3430, Fax: +81-43-290-3427,
E-mail: n.toriumi@chiba-u.jp- 46 -

-20
-30
-0.5

0.0

0.5

V SD (V)

1.0

1.5

Fig. 1. (a) Transfer and (b) output
characteristics of FNW-FET using IL-gate.

1P-5
Photoinduced Charge Separation in Supramolecules between
Lithium-ion-encapsulated PCBM Fullerene and Anionic Porphyrins○Yuki Kawashima1, Kei Ohkubo1, Hiroshi Okada2, Yutaka Matsuo2, Shunichi Fukuzumi1
1

Department of Material and Life Science, Graduate School of Engineering, Osaka
University, ALCA, Japan Science and Technology Agency, Osaka 565-0871, Japan2
Department of Chemistry, School of Science, The University of Tokyo, Tokyo, 113-0033,
Japan
Various supramolecular donor-acceptor compounds composed of lithium-ion-encapsulated
C60 (Li+@C60) as an electron acceptor have merited special attention, because Li+@C60 has
much more efficient electron acceptability as compared with pristine fullerene.[1] Non-polar
solvents have usually been employed to construct supramolecular electron donor-acceptor
compounds with strong binding. In contrast,
O
SO
O S
supramolecules composed of Li+@C60 and anionicO
porphyrinoids can be formed by utilizing ionic
N
Li
N M N
interaction in a polar solvent, which stabilizes theNcharge-separated (CS) state by solvation. When
4Ð
anionic porphyrins (MTPPS : M = Zn, H2, Fig. 1)
SO
O S
MTPPS4Ð
were employed as electron donors, the supramolecules
Li+@PCBM(M = Zn, H )exhibited long lifetimes of the CS state (ca. 300 Fig. 1 Chemical structure of Li+@PCBMµs).[2] However, the energy of the CS state is low and MTPPS4Ð (M = Zn, H ).
because the LUMO level of Li+@C60 is significantly lower than that of C60. When an electron
acceptor with higher LUMO level is employed to the donor-acceptor supramolecule, theenergy of the CS state can be increased. We report herein construction of supramoleculecomposed of MTPPS4Ð and lithium-ion-encapsulated [6,6]-phenyl-C61-butyric acid methyl
ester (Li+@PCBM, Fig. 1),[3] which has a higher LUMO level than that of Li+@C60.
UV-vis absorption spectra of ZnTPPS4Ð in PhCN at
3.0
298 K are changed upon addition of Li+@PCBM, where(ZnTPPS4Ð)¥+
2.5
670 nmthe Q band at 558 and 599 nm are red-shifted to 562 nm
2.0+¥Ð
and 602 nm, respectively. The formation constant (K)Li @PCBM
995 nm1.5
was determined from the titration to be 9.3 ×104 MÐ1.
1.0This results exhibit that strong supramolecular binding
between ZnTPPS4Ð and Li+@PCBM occurs by ionic
0.5
interaction in PhCN. The transient absorption spectrum
0of the ZnTPPS4Ð/Li+@PCBM supramolecular complex
was measured by nanosecond laser flash photolysis as
600
800
1000
1200
Wavelength, nm
shown in Fig. 2. The absorption band at 670 and 995 nm
Fig. 2 Transient absorption spectrum
can be assigned to [ZnTPPS4Ð]¥+ and Li+@PCBM¥Ð,4Ð
Ð5of ZnTPPS (2.5  10 M) andrespectively. This clearly indicates formation of the CS
Li+@PCBM (5.0  10Ð5 M) in
state. The lifetime of the CS state in the supramolecular
PhCN measured at 30 µs after laser
complex was determined to be 560 µs at 298 K.
excitation at 450 nm.
Ð

3

3

Ð

+

Ð

3

3

Ð

3

10 ∆Abs

2[1] Aoyagi, S. et al. Nature Chem. 2010, 2, 678Ð683. [2] Ohkubo K. et al. Chem. Commun. 2012, 48, 4314Ð4316.
[3] Matsuo, Y. et al. Org. Lett. 2012, 14, 3784Ð3787.
Corresponding Author: S. Fukuzumi,
Tel: +81-6-6879-7369, Fax: +81-6-6879-7370, E-mail: fukuzumi@chem.eng.osaka-u.ac.jp- 47 -

1P-6
Formation mechanism of metallofullerenes suggestedby the distribution of empty fullerenes
�Tatsuki Kobayashi1, Takeshi Kodama2, Wataru Fujita2, Koichi Kikuchi2, Yohji Achiba2
12School of Science, Kitasato University, Sagamihara, 252-0373, Japan
Department of Chemistry, Tokyo Metropolitan University, Hachioji, 192-0397, Japan

Normalized Intensity (arb. units)

Recently, we have found that some kinds of dimetallofullerenes such as Y2@C80 and
Sc2@C80 are extracted as a Òsoluble and stableÓ fullerene when we choose a mixed solvent oftriethylamine (TEA) and acetone for extraction[1,2]. This fact strongly suggested that, ingeneral, the metallofullerenes that have never been extracted by a conventional organic solvent
like 1,2,4-trichlorobenzene or CS2 are generated in growth process, but are insoluble due to theelectronic properties induced by the metal atoms inside. Furthermore, it was also found that themixed solvent works well on the stabilizing even some kinds of empty fullerenes such as C74
and C80 in solution. These phenomena can be rationalized by a charge transferring effect on theÒinsolubleÓ fullerenes from TEA. Therefore, the more systematic experiments by varying
metal atoms combined with use of the mixed solvent for both empty- and metallo-fullerenes
seem to shed a new light on understanding the growth properties of fullerenes in more detail.
Soot containing metallofullerenes wasproduced by direct-current (typically 60 A) arc** **discharge of M/C composite rods (atomic ratio***
M:C=2:98, M=Ba, Gd, Lu, or Sc) under a 500 Torr***
* *He atmosphere. As a reference, pure carbon rods*
were also arc discharged at the same condition.
** *The raw soot was extracted for 8 h with a mixed
solvent of TEA and acetone (volume ratio 1:3).
Figure 1 shows the LD-TOF-MS spectra of
the extracts. It is clearly shown that the MS Fig. 1 LD-TOF-MS spectra of extracts by amixed solvent extraction. Intensity is normalized
intensity of C60-C90 region significantly decreases by setting the peak height of C140 (m/z=1680)
stndby adding metals, and these intensity changes same for all the spectra. The sum of 1 and 2
ionization potentials is shown in parenthesis. The
depend on the sum of 1st and 2nd ionization peaks with asterisk are assigned toenergies of the metals used. We will discuss in metallofullerenes, MCn or M2Cn.
more detail in the symposium.
[1] T. Kodama, et al. The 41st Fullerenes-Nanotubes-Graphene General Symposium 31 (2011).
[2] A. Togashi, et al. The 44th Fullerenes-Nanotubes-Graphene General Symposium 144 (2013).
Corresponding Author: Takeshi Kodama
E-mail: kodama-takeshi@tmu.ac.jp
Tel:+81-42-677-2530, Fax:+81-42-677-2525- 48 -

1P-7
Energetics of water molecules encapsulated into C60 dimer○Kazuya Nomura and Susumu Okada
Graduate School of Pure and Applied Sciences, University of Tsukuba
1-1-1 Tennodai, Tsukuba, Ibaraki 305-8571, Japan
Fullerenes are known to accommodate forging molecules and atoms within their sphericalinner space with the diameter of about 1 nm. For instance, the metal atoms can beaccommodated within several fullerene cages resulting in the metalofullerenes which exhibit
interesting diversity in their physical properties. In addition to atoms, recently, molecules
such as hydrogen and water are also encapsulated into C60 by molecular surgery schemes.
Since the interaction between host C60 and guest molecule are important to form thesecomplexes, the physical properties of these materials are not the simple sum of those of
constituent units. Therefore, detailed energetic stability and electronic structures of thesecomplexes are still unclear. In this work, we study the energetics and electronic structures of
C60 dimer encapsulating water molecules by first-principles total-energy calculations in theframework of density functional theory. In particular, we elucidate the dipole-dipole
interaction between two H2O molecules encapsulated into C60. In the calculation, C60 dimer
possesses [2+2] intermolecular covalent bonds and each C60 contains H2O molecule withvarious mutual dipole directions to the adjacent H2O molecule.
Figure 1 shows the geometric structure of C60 dimer encapsulating H2O molecules.
Calculated encapsulation energy of H2O is -1.1eV/molecule indicating that the encapsulation
reaction is exothermic. We find that the dipole moment of H2O points to the intermolecularbonds of C60 dimer under their ground state dipole arrangement as shown in Fig. 1 in sharp
contrast to the ground state configuration for two dipole moments in the classicalelectrodynamics. The fact indicates that the π electrons in C60 dimer decisively affect theenergetics of encapsulated H2O molecules and sufficiently screen the dipole moment of H2O.

Fig1: An optimized structure of ground state of C60
dimer encapsulating H2O molecules. Large and small
gray circles denote O and H atoms, respectively.

Corresponding Author: K. Nomura
Tel: +81-29-853-5600(ext. 8233), Fax: +81-29-853-5924,
E-mail: sokada@comas.frsc.tsukuba.ac.jp- 49 -

1P-8
High-Resolution Transmission Electron Microscopic Study ofElectron-Beam-Irradiated C60 Single Crystal Films○Hideki Masuda1, Hidehiro Yasuda2, and Jun Onoe1*
1

2

Research Laboratory for Nuclear Reactor, Tokyo Institute of Technology, Tokyo 152-8550
Research Center for Ultra-High Voltage Electron Microscopy, Osaka University, Osaka 567-0047

We reported that one-dimensional (1D) uneven peanut-shaped C60 polymer is formed byelectron-beam (EB) irradiation of a pristine C60 film [1], and exhibits novel physicalproperties such as the geometric curvature effects on the Tomonaga-Luttinger liquid states [2].
Although in situ infrared spectra and density-functional calculations suggest that the 1D
polymer has a cross-kinked structure close to the waist structure of the P08 C120 isomer
obtained from the general Stone-Wales transformation, the exact structure is not still
understood at this stage. In the present study, we examined the structure of the 1D polymer
formed from a C60 single crystal film, using HRTEM and electron diffraction (ED).
The 1D C60 polymer film was formed on a mica substrate in an UHV chamber. Afterconfirming the formation of the 1D polymer using in situ infrared spectroscopy [3], we ripped
the film off the mica by putting it into pure water and mounted the film on a Cu micro-gridunder the atmospheric condition, and observed the film by HRTEM.
Figure 1 (a) and (b) show a HRTEM image and ED pattern of the pristine C60 film (20 nm
thick), respectively. This film is oriented along [111] and main spots of ED are spot-A
corresponding to (220) series of FCC. Since thefilm contains some twins as stacking faults on(111), spot-B appears at 1/3 of (422) series(spot-C).
Figure 1 (c) and (d) show the HRTEM andED pattern of the EB-irradiated C60 single
crystal film (20 nm thick). Main spots of ED
are spot-B. The increase in reflection intensityof spot-B indicates the increase in stacking
faults. Namely, a part of the FCC molecular
crystalline [111] stacking structure changes into
the HCP [001] stacking.
Comparison between (b) and (d) showssome other differences such as doubleness andcircular form of spot-A. These can be well
explained using an HCP lattice model with adecrease in the closest C60-C60 distance, which Fig. 1. HRTEM images (insets: FFTis the same as for the P08 isomer, along one patterns) and ED patterns of pristine C60 (a,b) and 1D C60 polymer (c, d) formed fromgiven direction.
single crystal films.
[1] J. Onoe et al., Appl. Phys. Lett. 82, 595 (2003).
[2] J. Onoe et al., Europhys. Lett. 98, 27001 (2012), and references therein.
[3] A. Takashima, T. Nishii, and J. Onoe, J. Phys. D: Appl. Phys. 45, 485302 (2012).
*Corresponding Author: J. Onoe, E-mail: jonoe@nr.titech.ac.jp- 50 -

1P-9
X-ray irradiation effect on the electric conductivity of single-walled carbon
nanotube films
Takuma Araki1, Toshiya Murakami1, Kenji Kisoda2, and Chihiro Itoh1
1

Department of Materials Science and Chemistry, Wakayama University, Wakayama
640-8510, Japan2
Department of Physics, Wakayama University, Wakayama 640-8510, Japanln(σ(Τ)/σ(300Κ))Single-walled carbon nanotubes (SWNTs) have many attractive properties because of their
quasi-one-dimensional structure. In particular, the strong correlation between the electricalproperty and the geometric structure, so-called chirality, gives flexibility of controlling theelectronic properties of SWNTs. We have shown that the X-ray irradiation generates defects
efficiently and that the defect formation eventually leads to the structural change of
SWNTs.[1] We concluded that the X-ray-induced defect is a pair of an interstitial and avacancy (Frenkel pair) based on the results of thermal annealing study.[2] In order to clarify
the irradiation effect on the electric conductivity of SWNT, we have measured thetemperature dependence of the electric conductivity of SWNT films.
SWNTs grown by chemical vapor deposition were dispersed in 1wt%- aqueous solution of
sodium dodecyl sulfate. In order to enrich each of the metallic (m-) or the semiconducting(s-) SWNTs, we processed the solution by gel-column-chromatographic technique.[3] The
enriched SWNTs were collected by filtering the processed aqueous dispersion by a membranefilter and shaped into the film on silicon substrates by removing the filter with organic solvent
vapor. The SWNT films were irradiated with 277-eV X-ray in vacuum. The electricalconductivities of X-ray irradiated films were measured at 160-300 K in vacuum (4 × 10-5 Pa).
Figure 1 shows the semilogarithmic plot
0.0
of the normalized electrical conductivity vs
T-1/4 for pristine and the irradiated films. The-0.1
evident linear relation suggests that theelectrical conductivities of the SWNT films
are governed by the hopping conduction. We-0.2
also found that the irradiation made the slopeof the temperature dependence of both films
steep. On the basis of these results, it is-0.3
conceivable that the carriers in SWNTs tend to
localize by the formation of defects.
-0.4

    
  


[1] C. Itoh et al. Nucl. Instr. Meth. B 266 (2008) 2772.
[2] M.Matsuda, et al., 45th FNTG symposium, 2P-16.
[3] T. Tanaka, et. al., App. Phys. Exp.2 (2009) 125002.

-0.5
0.24

   
 

0.25

0.26
-1/4

T

Corresponding Author: T. Araki,
Tel: +81-73-457-8532,
E-mail: s143001@center.wakayama-u.ac.jp

0.27

0.28

Fig.1 Temperature dependence of theelectric conductivity of pristine andthe irradiated SWNT films.

- 51 -

1P-10
Fluidized Bed CVD of Submillimeter-Long Carbon Nanotubes
Using an Internal Heat-Exchange Reactor○Zhongming Chen1,2, Kei Hasegawa 2, Dong Young Kim 2, Toshio Osawa 2, Suguru Noda 2*
1
2

Department of Chemical System Engineering, The University of Tokyo, Japan
Department of Applied Chemistry, Waseda University, Tokyo 169-8555, Japan

Low cost production of carbon nanotubes (CNTs) will open many opportunities for the practicalapplications such as batteries/capacitors. Fluidized bed chemical vapor deposition (FBCVD) has
realized mass production of multi-wall CNTs (MWCNTs) at several hundred tons annually per plant,
but suchCNTs are short, thick, entangled, and thus less conductive. Large-scale, low-cost productionof long and thin CNTs are of highly demanded. We previously developed an original FBCVD andrealized semi-continuous production of submillimeter-long few-wall CNTs from C2H2 at a high yield 70% and short gas residence time ～ 0.3 s [1]. But the high gas feed causes insufficient heating of
the bead bed when scaled up (Fig. 1a). This time, we designed and developed a new FBCVD reactor
having an internal heat-exchange and preheating zone (Fig. 1b) and examined its performance inproducing submillimter- long CNTsusing a reactor with three-times enlarged cross sectional area.
All processes for catalyst (re-)deposition, catalyst reduction, CNT growth, CNT separation, andremoval of residual carbons were performed in a single fluidized bed reactor (Fig. 1b). All the gases
except for the catalyst vapor were fed to the outer tube, flown down and preheated by the furnace andthe hot effluent gas in the inner tube, and then flown into the inner tube through the distributor at thebottom. Catalyst vapors (aluminum-isopropoxide and ferrocene, carried by 4 vol% O2/Ar at 20 slm)
were fed directly to the bed through the catalyst line penetrating the distributor from the bottom.
After catalyst deposition for 4 min, the catalyst was reduced by flowing 26 vol% H2/ 0.06 vol% H2O/
Ar at 9.48 slm for 10 min. CVD was performed by flowing 1.1 vol% C2H2/ 26 vol% H2/ 600 ppmv
H2O/ Ar at 9.48 slm for 20 min. CNTs were separated
from the beads by vigorously fluidizing the bed by Ar for
10 min. The residual carbon on the beads was removed byflowing 20 vol% O2/Ar for 5 min. These processes wererepeated at 745 C by changing the gas flow.
The bead bed expanded from 3 cm (Fig. 1c) to 12 cm(Fig. 1d) after CVD for 20 min. The CNT yield wasincreased from 0.25 to 0.81 g/cycle (Fig. 1e) while
CNTs retained the submillimter- long array structure (Fig.
1f). From the transmission electron microscopy (TEM)
analysis, we found that the average diameter of the CNTs
is 11 nm. We reduced the total supply of Ar carrier for
ferrocene to one fifth and the concentration of C2H2 to
0.73 vol%, and realized the diameter reduction to 6.5 nm
in average. The FBCVD reactor with the internal heatexchanger will realize further scale-up for practical mass Fig. 1. Structures of the old (a) and new (b)reactors, photos of the bead-bed before (c) andproduction.
after (d) CVD, photo of CNTs collected in[1] D Y Kim, et al., Carbon 49, 1972 (2011).
container (e), and SEM images of the CNTs (f).
Corresponding Author: S. Noda
Tel: +81-3-5286-2769, Fax: +81-3-5286-2769, E-mail: noda@waseda.jp- 52 -

1P-11
Coherent G-band phonons in single wall carbon nanotubes○ Ahmad R.T. Nugraha, Eddwi H. Hasdeo, Riichiro Saito
Department of Physics, Tohoku University, Sendai 980-8578, Japan
In this work, we discuss the probe energy dependence of the coherent G-band phonon
intensity. In a single wall carbon nanotube (SWNT) sample, ultrashort laser pulses (~10 fs)
are known to induce coherent lattice vibrations. The coherent phonon motions are been
observed as oscillations of optical constants (such as reflectivity or transmittance) as afunction of time in the pump-probe spectroscopy measurement, which is directly related to themodulations of absorption coefficient [1,2]. Using Fourier transform of the reflectivity ortransmittance, we obtain a power spectrum as a function of phonon frequencies. The peaks inthe power spectrum correspond to the coherent phonon frequencies. Some important SWNT
phonon modes can be observed from this spectrum, such as the radial breathing mode (RBM)with frequency of 100-200 cm-1 and the G-band with frequency of about 1580 cm-1 [1]. For
the RBM, oscillations of optical constants are already understood as a result of adiameter-dependent bandgap [2, 3]. On the other hand, while the G-band phonons can also
modify absorption coefficient of SWCNTs, a previous theoretical calculation predicted thatthe modulations of absorption coefficient due to G-band phonons are about 1000 times
smaller than those caused by the RBM [4].
However, a recent experimental measurement showed that the coherent G-band signal iscomparable to the RBM signal [5]. Therefore, it indicates that a different mechanism isnecessary. We recently notice that the previous theory calculated the change of absorption
coefficient due to the G-band phonons by considering the same concept of energy-gap
modulations as induced by RBM phonons. Instead of the energy gap modulations, here we
expect that the modulations of electron-photon (or exciton-photon) interaction as a function oftime should be responsible for the coherent G-band intensity. The coherent G-band vibration
could cause larger change in the optical matrix elements than the RBM vibration, in which thetime-dependence of optical matrix elements was not necessary.
[1] A. Gambetta et al., Nat. Phys. 2, 515-520 (2006).
[2] Y.-S. Lim et al., Nano Lett. 6, 2696-2700 (2006); J.-H. Kim et al., Phys. Rev. Lett. 102, 037402 (2009).
[3] A. R. T. Nugraha et al., PRB 84, 174302 (2011).
[4] G. D. Sanders et al., PRB 79, 205434 (2009).
[5] J.-H. Kim et al, PRB 86, 161415 (2012).
Corresponding Author: A. R. T. Nugraha
TEL: +81-22-795-6442, FAX: +81-22-795-6447, E-mail: nugraha@flex.phys.tohoku.ac.jp- 53 -

1P-12
Photochemical Behavior of Single-walled Carbon Nanotubes in the
Presence of Propylamine
Yutaka Maeda,1 Yuhei Hasuike,1 Michio Yamada,1 Tadashi Hasegawa,1Takeshi Akasaka1,2
1

Department of Chemistry, Tokyo Gakugei University, Koganei, Tokyo 184-8501, Japan
Life Science Center of Tsukuba Advanced Research Alliance, University of Tsukuba, Ibaraki
305-8577, Japan

2

Single-walled carbon nanotubes (SWNTs) have excellent mechanical and electricalproperties that are desirable in many potential applications. SWNTs are typically grown asbundles of metallic and semiconducting SWNTs, hindering the widespread application of
SWNTs. Therefore, practical use of SWNTs requires exfoliation of the bundles and separationof the metallic and semiconducting SWNTs. Various types of interactions of SWNTs withorganic compounds have been studied in order to understand not only the properties of
SWNTs, but also their dispersion and separation. The dispersion and separation of metallic
SWNTs or semiconducting SWNTs have been achieved by sonication with various organic
compounds, such as porphyrins, aromatic compounds, flavin, and so on, followed bycentrifugation. We have studied the dispersion and separation of SWNTs in organic solvent
using amines.1 Interestingly, metallic SWNTs were extracted selectively from pristine
SWNTs into THF containing an aliphatic amine. In recent years, much interest has been
directed toward the photochemical properties of SWNTs because of the evolution of their
possible applications, e.g., photovoltaic cells. Photochemical reactions of unsaturatedhydrocarbons such as benzene, stilbene, and fullerene with amines are well known to afford
the corresponding adducts via an electron transfer process. However, the interaction of
SWNTs with amines in the excited state has not been clarified. We report here thephotochemical behavior of SWNTs in the presence of propylamine. Optical and Raman
spectroscopic analyses and ESR experiments reveal that the photoinduced electron transferfrom the amine to the excited SWNTs causes the sidewall functionalization of small-diameter
SWNTs.

SWNTs + H 2NCH 2CH2CH3 nhνnSWNTs + H 2NCH 2CH2CH3nfunctionalized SWNTs
O2
O2

SWNTs
+
decomposed product of amine[1] Maeda, Y. et al. Nano. 2012, 7, 1130001.
Corresponding Author: Y. Maeda
Tel: +81-42-329-7512, Fax: +81-42-329-7512
E-mail: ymaeda@u-gakugei.ac.jp- 54 -

1P-13In-situ Photoluminescence-spectroelectrochemistry of
Oxygen-doped Single-walled Carbon Nanotubes
Tomonari Shiraishi1, Naoto Akizuki2, Yuhei Miyauchi2,3, Kazunari Matsuda2,
Naotoshi Nakashima1,4,5
1 Department of Applied Chemistry, Graduate School of Engineering, Kyushu University, 744

Motooka, Fukuoka 819-0395, Japan

2 Institute of Advanced Energy, Kyoto University, Uji, Kyoto 611-0011, Japan

3 PRESTO, Japan Science and Technology Agency, 4-1-8 Honcho Kawaguchi, Saitama

332-0012, Japan

4 WPI-I2CNER, Kyushu University, 744 Motooka, Fukuoka 819-0395, Japan
5 CREST, Japan Science and Technology Agency, 5 Sanbancho, Chiyoda-ku,

Tokyo 102-0075, Japan

Local luminescent states in single-walled carbon nanotubes (SWNTs) have been of greatinterest due to the bright photoluminescence (PL) from such states promising for theirapplications in optoelectronics and bioimaging. Recently, Miyauchi et al. [1] have reported
the extraordinary exciton brightening in such local states generated by oxygen-doping [2] andclarified the mechanism of the PL enhancement induced by dimensionality modification of
excitons. However, detailed electronic structure of the oxygen-derived local states has been
still unclear. To investigate the origin of the local states, it is important to evaluate the electron
potentials in conduction and valence bands of the oxygen-doped SWNTs. We have reported
that electronic potentials of (n,m)SWNTs can be determined based on in situ PL
spectroelectrochemistry [3]. Here, we used this method to determine the electronic potentialsof the oxygen-doped SWNTs dispersed in a carboxymethylcellulose (CMC) film.
Oxygen-doped SWNTs in a sodium dodecyl benzene sulfonate (SDBS) solution wereprepared according to the previous paper [1], and the SDBS molecules were replaced with
CMC. A CMC film containing the oxygen-doped SWNTs was formed on an ITO plate andused for the PL spectroelectrochmical measurements in an aqueous solution.
Fig. 1 shows a 2D-PL map obtained from the oxygen-doped SWNTs in a CMC film. The
clear spot at around 1000 nm is the PL of the (6,5) SWNTs. The broad spot found at around1150-1270 nm is the new band generated by the oxygen doping [2]. The PL intensities of the
new band were found to change by applying the electrochemical potentials to the ITO
electrode; thus the oxidation and reduction potentials of
the local states in the oxygen-doped (6,5) SWNTs could bedetermined. In the meeting, we will provide detailed
results of the electronic states of the oxygen-doped
SWNTs.
[1] Y. Miyauchi et al. Nat. Photonics, 7, 715 (2013).
[2] S. Ghosh et al., Science 330, 1656 (2010)[3] N. Nakashima et al. Angew. Chem. Int. Ed. 48, 7655 (2009); N.
Nakashima et al. Scientific. Reports, 3, art. no. 2959 (2013).
Fig. 1. 2D-PL mapping of a film of theCorresponding Author: Naotoshi Nakashima
oxygen-doped SWNTs on an ITO
E-mail: nakashima-tcm@mail.cstm.kyushu-u.ac.jp
Tel&Fax: +81-92-802-2840
electrode.

- 55 -

1P-14Far-Infrared and THz Spectroscopy of Multi-Walled Carbon Nanotubes○Keijiro Sakai,1 Takahiro Morimoto1 and Toshiya Okazaki,2,1,*
1

Technology Research Association for Single Wall Carbon Nanotubes (TASC), c/o Nanotube
Research Center, AIST, Tsukuba 305-8565, Japan
2

Nanotube Research Center, AIST, Tsukuba 305-8565, Japan,

Carbon nanotubes (CNTs) show very unique optical properties associating with their
low-dimensionality over wide spectral ranges. Even in the far infrared (FIR) and terahertz (THz)frequency ranges, there is a broad absorption peak around a few 100 cm-1. Recently, we reported the
FIR-THz spectroscopic study of various SWCNT samples of different tube lengths [1]. Each SWCNT
was cut via strong sonication with a different duration. Importantly, the sonication processes did notaffect the diameter distribution, which was confirmed using resonance Raman and UV-Vis-NIR
absorption spectroscopy. The obtained FIR-THz absorption frequencies exhibited a linear correlation
with the inverse of the tube length, which agrees well with the one-dimensional (1D) dispersion
relation. Moreover, the different effects of doping on the FIR-THz spectra between metallic andsemiconducting SWCNTs indicate that the motion of the photo-induced carriers predominantly
accounts for the optical response. It was also found that the observed resonance peaks were very
sensitive to the presence of defects on the tube wall and correlated with the electric resistance of thesamples. These observations suggest that the 1D current path length of the SWCNTs determines theplasmon resonance conditions.
Here we report the FIR-THz study of various multi-walled CNT (MWCNT) samples having
different tube diameter and quality. Some MWCNTs show the intense peak in the FIR-THz region
whereas the other exhibit no signal. Detailed characterization including the tube length dependence
will be discussed in the symposium.

Reference[1] T. Morimoto, S.-K. Joung, T. Saito, D. N. Futaba, K. Hata, T. Okazaki, submitted.
Corresponding author: Toshiya Okazaki
toshi.okazaki@aist.go.jp- 56 -

1P-15Prediction of Redox Potentials of Semiconducting Single-Walled Carbon
Nanotubes○Gergely Juhász1, Yasuhiko Hirana1, Naotoshi Nakashima 1
1

Department of Applied Chemistry, Graduate School of Engineering, Kyushu University,
Fukuoka 819-0395, Japan

Semiconducting single-walled carbon nanotubes (SWNTs) are promising candidates forconstruction of nanoelectronics for their diverse semiconducting properties. Nanotubes witheach chirality have well defined electronic properties which uniquely determined by thechirality index (n,m). For practical application, the determination of the precise value of theseproperties are essential.
We have previous reported a spectroelectrochemical method based on photoluminescence(PL) spectroscopy to determine the precise value of redox potentials of (n,m)SWNTs
embedded in a film of carboxymethylcellulose sodium salt. [1] Such method allowed theaccurate determination of a large set of nanotubes (tube diameters (d) = 0.75 -1.10 nm).
However, the methods is limited by the effectiveness of dispersant can be used and it can beused only with nanotubes with well observable PL peaks. These limitations highlight theimportance of empirical and theoretical predictions of electronic properties.
In this study, an empirical formula is derived from the experimentally determined redox
properties of semiconducting SWNTs, and compared to a theoretical calculation on the band
structure of the nanotubes. The calculations were performed on periodic models using Density
Functional based Tight Binding (DFTB) method, without considering the effect of thepolymer matrix. This method is capable to handle systems of several hundreds or thousands
atoms, therefore it is possible to extend the calculations more complex electrochemicalsystems.
Experiments showed that chirality family
behavior is clearly observable in the
reduction potentials (Ered), however hardly
effects the oxidation potentials (Eox). In
agreement with the experiments, the family
behavior is more pronounced in the
conducting band energies and it has small
effect on valence band energies around theband gap. The results suggest that accurate
prediction of redox / electronic properties ofnanotubes is possible even with moderatecomputational resources.
[1] Y. Tanaka et al. Angew. Chem. Int. Ed. 48, 7655
(2009)[2] Y. Hirana et al. Sci. Reports 3, 2959 (2013)[3] M. Elstner et al. Phys. Rev. B 58,7260 (1998)
Corresponding Author: N. Nakashima
Tel: +81-92-802-2840, Fax: +81-92-802-2840,
E-mail: nakashima-tcm@mail.cstm.kyushu-u.ac.jp- 57 -

Fig.1 The calculated electronic properties andexperimental redox potentials (Ered, Eox) plotted asa function of the inverse nanotube diameter (1/d).

1P-16
Photoluminescence Spectroelectrochemistry of a Single SWNT
Molecule○Liu Hong1, Shinichiro Mouri2, Yuhei Miyauchi2,
Kazunari Matsuda2, Naotoshi Nakashima1, 3, 4
1

Department of Applied Chemistry, Graduate School of Engineering, Kyushu University,
Fukuoka 819-0395, Japan
2
Institute of Advanced Energy, Kyoto University, Uji 611-0011, Japan
3
International Institute for Carbon Neutral Energy Research (WPI-I2CNER), Fukuoka
819-0395, Japan
4
JST-CREST, Tokyo 102-0075, Japan

Many attempts have been made to investigate the electronic properties of single-walledcarbon nanotubes (SWNTs) by means of scanning tunneling spectroscopy, chemical doping
and Raman spectroelectrochemistry [1]. We have developed a photoluminescence (PL)spectroelectrochemical method in determining redox potentials of individual SWNTs [2].
Here we report our trial study on the PL spectroelectrochemical measurement of a single
SWNT molecule, which is expected to open up a new way in characterizing electronic statesof SWNTs.
CoMoCAT-SWNTs
were
dispersedinatoluenesolutionofpoly[(9,9-dioctylfluorenyl-2,7-diyl)-alt-co-(6,6’-{2,2’-bypyridine})] (PFO-Bpy) by sonication,
and a diluted supernatant after centrifugation was
spin-cast on an ITO substrate so that the SWNT could
be isolated. The fluorescence from single nanotube has
been successfully observed by means of fluorescenceimaging. PL spectroelectrochemical measurement of
single nanotube was carried out with a conventional
three-electrode setup (Fig. 1) in aqueous electrolyte. It
has been observed that fluorescence of single nanotube
was gradually quenched as the applied potential to ITO
substrate increased, and this quenching behavior was inagreement with the plots of PL response frommacroscopic SWNTs sample against potentials as
previously reported. Detail will be reported at themeeting.
Fig.1 setup of PL spectroelectro[1] a) J. W. G. Wildoer et al. Nature. 391, 59 (1998); b) M. J.
chemical measurement
O’Connell et al. Nat. Mater. 4, 412 (2005); c) K. Okazaki et al.
Phys. Rev. B. 68, 035434 (2003).
[2] a) Y. Tanaka et al. Angew. Chem. Int. Ed. 48, 7655 (2009); b) Y. Hirana et al. J. Am. Chem. Soc. 132,
13072 (2010).
Corresponding Author: N. Nakashima
Tel: +81-92-802-2840, Fax: +81-92-802-2840,
E-mail: nakashima-tcm@mail.cstm.kyushu-u.ac.jp- 58 -

1P-17
Electric Characterization of Chirality Controlled
Single-Walled Carbon Nanotubes○Yusaku Tsuda1, Takumi Sagara1, Keisuke Yoshida1, Koji Ishii2, Kenichi Yamakawa1,
Hirofumi Yajima2, Nobuyuki Iwata1 and Hiroshi Yamamoto 1
1

Department of Electronics & Computer Science,College of Science & Technology,
Nihon University, 7-24-1 Narashinodai, Funabashi, Chiba 274-8501 Japan2
Department of Applied Chemistry, Faculty of Science, Tokyo University of Science, 1-3
Kagurazaka, Shinjyuku-ku, Tokyo 162-0826, Japan
Single-walled carbon nanotubes (SWNTs) have been regarded as one of the best
candidates for future applications in nanoelectronic devices due to its high mobility,
high current-carrying capacities, and so on.
In our previous report, position selective
growth of single-walled carbon nanotubes (SWNTs) is carried out on a surface treated
SiO2 (300nm)/Si substrate between electrodes by cold-wall chemical vapor deposition(CC-CVD) method in μm-scale.
In addition, chirality controlled growth of the
SWNTs is also done by irradiating free electron laser (FEL) with the wavelength of 800
The grown SWNTs are all semiconducting
nm during CC-CVD growth [1].
investigated by a multi excited laser Raman analysis.
However, the grown SWNTs
direction is random on SiO2 (300nm)/Si substrate.
The remained issue forapplications of the field effect transistor (FET) using just one SWNTs is the in-planealignment synthesis process. In addition, chirality controlled and semiconducting
SWNTs growth is expected by just Raman spectra.
The purpose of this study is not
only to align the SWNTs but also to clarify the semiconducting property by electricmeasurement. The CC-CVD growth was carried out on the SiO2/Si and annealed r-cut
sapphire substrate for the purpose of the in-plane alignment [2]. The Co/Mo catalysts
were adhered by dipping technique followed by firing.
The electrodes will bedeposited before and/or after the CVD process with the FEL irradiation.
Thechirality controlled electric property will be discussed.
[1] K. Sakai, S. Doi, N. Iwata, H. Yajima, and H. Yamamoto, IEICE Trans. Electron. E94-C(2011) 1861-1866.
[2]H. Ago, K. Imamoto, N. Ishigami, R. Ohdo, K. Ikeda and M.Tsuji, “Competition andcooperation between lattice-oriented growth and step-templated growth of aligned carbon
nanotubes on sapphire”, Applied Physics Letters 90, 123 (2007).

- 59 -

1P-18
Hydrogen evolution from benzene with single-walled carbon nanotubes as aphotocatalyst○Naoki Kohno 1, Kei Ohkubo 1, Shunichi Fukuzumi 1
1

Department of Material and Life Science, Graduate School of Engineering, Osaka
University, ALCA, Japan Science and Technology Agency, Osaka 565-0871, Japan

104 H2 evolved, µmol sÐ1

Hydrogen is regarded as a clean fuel for the next generation but most hydrogen supplied
for industries is produced from fossil fuels by the steam-reforming reaction at hightemperature. To solve this problem, extensive efforts have been devoted to the developmentof various photocatalytic hydrogen production. So far, noble metals such as Pt or
semiconductors have been used as a photocatalyst. However, there is no report on
photocatalytic hydrogen evolution using organic compounds as a photocatalyst. Single-walledcarbon nanotubes (SWNTs) have merited great interest because of their unique opticalproperty and large hydrogen storage capacity[1]. We report herein the use of SWNTs as ahydrogen evolution photocatalyst by laser irradiation in aromatic solvent.
Hydrogen evolution occurred in a deaerated benzene solution (2.5 mL) containing SWNTs(0.15 mg) under laser irradiation (λ =532 nm, 500 mW). The amount of hydrogen evolved
reached 102 µmol and yield based on benzene used as a solvent was 0.40% by laser
irradiation for 2 hours. The quantum yield of hydrogen evolution was determined as 0.34.
When benzene was replaced by deuterated benzene, the deuterated hydrogen molecules suchas HD and D2 were evolved efficiently. This Scheme 1
result suggests that the hydrogen source is
SWNTs
H2
2
Laser irradiation
benzene used as a solvent. Hydrogen was
λ= 532 nm, 500 mW
also evolved in substituted benzene such as
400
toluene, 1,4-dimethylbenzene or benzonitrile
as solvents. The evolved H2 amounts were66.0, 60.2 or 39.2 µmol by laser irradiation
300
for 2 h, respectively. The products frombenzene were determined by GC-MS and
HPLC to be biphenyl and terphenyls. Thus,
200
hydrogen was evolved via the condensation
reaction of benzene in the photocatalytic
reaction.
100
The initial rates of hydrogen evolution areproportional to the fourth power of laser
intensity as shown in Figure 1. This result
0
0
5
10
15
20
25
indicates that a multiphoton absorption
Ð4
Ð1 4
10 (Intensity, mJ pulse )process is involved in this photochemical
Figure 1. Plot of rate of H2 evolution vsreaction.
the fourth power of laser intensity inbenzene containing SWNTs (2.5 mL, 0.15
[1] Dilon, A. C. et al. Nature 1997, 386, 377.
mg) by laser irradiation (λ = 532 nm).
Corresponding Author: S. Fukuzumi
Tel: +81-6-6879-7369, Fax: +81-6-6879-7370,
E-mail: fukuzumi@chem.eng.osaka-u.ac.jp- 60 -

1P-19High-throughput fabrication of carbon nanotube thin-film transistors withflexographic printing process: Fabrication of short channel top-gate devices○Michihiko Maeda1, Kentaro Higuchi1, Shigeru Kishimoto1, Yuta Nakajima2,
Takuya Tomura2, Masafumi Takesue2, Katsuhiko Hata2, and Yutaka Ohno1
Department of Quantum Engineering, Nagoya University, Nagoya 464-8603, Japan
Research and Development Center, Bando Chemical Industries, LTD., Kobe 650-0047,
Japan
1

2

Among many kinds of thin-film transistors (TFTs), carbon nanotube (CNT) TFTs haveattractive properties such as high mobility, flexibility, transparency, printability, and so on. In
the previous work, we introduced flexographic printing technique, one of high speed printing
methods, in the fabrication of CNT TFTs on a plastic film, and achieved a high mobility of
157 cm2/Vs by the fully lithography-free and ambient-pressure processes. [1] In this work, wehave improved the resolution of the printing technique to realize top-gate CNT TFTs with ashort channel length of sub-10 µm.
The plate for high-resolution flexographic printing was made of PDMS withmicro-fabrication process. Top-gate TFTs were fabricated on a polyethylene naphthalate(PEN) film with a thickness of 100 µm. First, a thin film of semiconductor CNTs was formedon the film by transfer process. The CNTs
were patterned by printing resist ink
subsequent etching with ambient pressureplasma with O2/Ar. Then, the source anddrain electrodes, gate insulator, and gateelectrode were printed. Silver nanoparticle
ink and polyimide ink were respectively used
for the electrodes and insulator.
Figure 2(a) shows the fabricated CNT
Fig. 1 Device fabrication process
TFTs. The channel length is about 8 µm as(b)shown figure 2(b), which is about(a)one-fourteenth of our previous device. [1]This work was partially supported by Õ08
NEDO Grant, ALCA-JST, SICORP-JST,and Grant-in-Aid of MEXT.
[1] K. Higuchi et al., Appl. Phys. Express 6, 085101(2013).
Corresponding Author: Y. Ohno
Tel: +81-52-789-5387, Fax: +81-52-789-5387
E-mail: yohno@nuee.nagoya-u.ac.jp

Fig. 2 (a) Printed CNT TFT on PEN substrate. (b)Printed source and drain electrodes with channel
length of 8 µm.

- 61 -

1P-20Evaluation of Dynamic Performance of CNT Random Network Transistors
Noriyuki Tonouchi1,4, Hiroyuki Endoh1,4, Takashi Manako1,4
Fumiyuki Nihey , Hideaki Numata2, Tomoyuki Yokota3, Tsuyoshi Sekitani3, and Takao Someya3,421

Smart Energy Research Laboratories, NEC Corporation, Tsukuba 305-8501, Japan
Phone: +81-29-850-1157 E-mail: n-tonouchi@ab.jp.nec.com
2
Technology Research Association for Single Wall Carbon Nanotubes (TASC), Tsukuba 305-8565, Japan3
Department of Electrical Engineering, School of Engineering, The University of Tokyo, Tokyo 113-8656, Japan
4
Institute for Nano Quantum Information Electronics, Tokyo 153-8505, Japan

1. Introduction

We have promoted research and development on carbon nanotube transistors (CNT-TFTs) as
promising devices toward achieving applications for printed electronics [1–2]. CNTs have highelectrical properties and the mobility of CNT-TFTs has achieved 1–10 cm2/Vs or more even though
their channels have been fabricated with printing processes [3–4]. Therefore, CNT-TFTs are expected
to have the potential to achieve printed devices that are high performance such as those that require
operating frequencies over 100 kHz (e.g., scanning line drivers for display panels). Until now,
CNT-TFTs have been evaluated by only focusing on their static performance. Therefore, there havebeen few researchers who have actually evaluated their dynamic performance. In the present work, weevaluated the dynamic performance of CNT-TFTs whose channels had been fabricated with a printing
process. We aimed at demonstrating switching action over 100 kHz.

2. Experiments and Results

First, we fabricated a CNT-TFT having vapor-deposited source-drain electrodes. Figure 1 has across-sectional view of the CNT-TFT. The width of the source-drain electrodes was 100 um. Generally,
TFTs have parasitic gate capacitance due to the overlap between gate and source-drain electrodes. The
parasitic capacitance conducts the displacement current, or the background noise superimposed on theon-off switching signal. Since the amplitude of the background noise has positive dependence on thegate frequency, the background masks the on-off signal of the CNT channel at higher frequency. We
measured the amplitude of the background and found that it was 100-1000 times larger than that of the
on-current of the CNT-TFT at 100 kHz. So no reliable verification of switching action could beachieved at the higher frequency. That is, verification of on-off action over 100 kHz requires animproved S/N ratio.
There are two main methods of improving the S/N ratio: (1) Reducing the gate capacitance; (2)Enhancing the on-current. We examined making the drain electrode narrower as a method of (1). We
patterned the source-drain electrodes with super inkjet (SIJ) technology to make them narrower. The
width of the electrodes was confirmed to be 2–3 μm from the SEM image. Compared to the case of the
TFTs having vapor deposited electrodes, the amplitude of the background was suppressed to ~1/10. As
a method of (2), we examined increasing CNT density. We fabricated the channel with CNT ink
that had been treated to reduce the surfactant through dialysis to increase the CNT
density. Reducing the surfactant enabled us to increase the relative content of CNTs. The
on-current of the fabricated CNT-TFT was about 100 times larger than that of the
CNT-TFT having vapor-deposited electrodes. Figure 2 shows the actual switching actionof this improved CNT-TFT. Clear switching action can be identified even at 500 kHz. This
study confirmed the superiority of CNTs as
printable channel materials and suggested thepossibility of pioneering fields of application
for printed electronics by using CNT-TFTs.
References[1] H. Numata et al., Appl. Phys. Express 5 (2012) 055102.
[2] H. Endoh, J.Photopoly.Sci.Tech 25 (2012) 281.
[3] P. Beecher et al., J. Appl. Phys. 102 (2007) 043710.
[4] T. Takenobu et al., Appl. Phys. Express 2 (2009) 025005.

Fig. 1. Cross section of TFT- 62 -

Fig. 2. Switchingaction at 500 kHz (SIJ)

1P-21
Preparation of Al-CNT Nanocomposites using Mechanical Alloying○Takumi Goto, Kouki Terashima, Mitsuhiro Takeda, Masaru Sekido
Department of Material Science and Engineering, Sendai National College of Technology,
Natori 981-1239, JapanDue to their combination of outstanding mechanical characteristics, extremely large inter-facial contact area, high aspect ratio, and low mass density, CNTs are considered as the ideal
reinforcement fillers for the nanocomposite materials. Among various nanocomposites
CNT–metal matrix composites are expected to assume the role of structural materials in thenext-generation. However, CNT–metal matrix composites are currently falling behind in bulk
fabrication due to the difficulty of dispersing the CNTs. In this work we used mechanicalalloying (MA) and spark plasma-sintering (SPS) technique to prepare Al-CNT
nanocomposites with homogenous distribution and excellent dispersion of CNTs.
Briefly MWCNTs powder (0.5 -2.0 wt%) and Al powder were suspended in Acetone andsonicated for 30 min. After removing solvent the obtained powder was dried under reducedpressure for 12 h to give MWCNTs/Al powder with good dispersion. MWCNTs/Al powder
was then placed into stainless steel mixing jars containing 25 stainless steel milling balls of
10 mm diameter (ball-to-powder weight ratio (BPR) = 10:1). The jars were filled with argon
and were then agitated using a planetary ball mill at 300 rpm for 6 h. Microstructure
characterizations were performed using scanning electron microscope (SEM).
The obtained MWCNTs/Al powder was sintered in a carbon mold using a spark
plasma-sintering (SPS) device. The sintering conditions were maximum temperature 500 oC,
holding time 20-30 min., and pressure of 10 MPa.
We will also report and discuss the improvement of tensile strength of Al-CNT
nanocomposites, prepared by MA and SPS technique.

Corresponding Author: M. Sekido
Tel: +81-22-381-0329, Fax: +81-22-381-0329
E-mail: sekido@sendai-nct.ac.jp- 63 -

1P-22Multi-walled carbon nanotubes and carbon black supported platinum
nanoparticles for catalyst of polymer electrolyte membrane fuel cells○ Zehui Yang 1, M. R. Berber1, Tsuyohiko Fujigaya1,2, and Naotoshi Nakashima1,2,3
1 Department of Applied Chemistry, Graduate School of Engineering, Kyushu

University, 744 Motooka, Nishi-ku, Fukuoka 819-0395, Japan

2 International Institute for Carbon Neutral Energy Research (WPI-I2CNER), Kyushu

University, 744 Motooka, Nishi-ku, Fukuoka 819-0395, Japan

3 JST-CREST, 5 Sanbancho, Chiyoda-ku, Tokyo, 102-0075, Japan

50

Potential / V

0.2

2

References[1] N. Nakashima, et al., Adv. Mater. 25 (2013)
1666-1681.
[2] N. Nakashima, et al., Sci. Rep. 3 (2013) 1764.
Corresponding Author: N. Nakashima
TEL: 092-802-2840, FAX: 092-802-2840
E-mail:nakashima-tcm@mail.cstm.kyushu-u.ac.jp

0.4

Power density / mW/cm

Investigating alternating energy is one of the biggest challenges for the 21st century.
Owing to high energy density, high efficiency and green emissions, polymer electrolyte
membrane fuel cells (PEMFCs) are recognized as one of the promising solutions.
Platinum (Pt) is selected as the catalyst due to the high catalytic activity among othermetals and alloys. However, Pt nanoparticles still suffer from low durability due to the
corrosion of carbon supports, Pt dissolution, Ostwald ripening, aggregation and migration.
The low durability and high price blocks widespread commercialization of PEMFCs.
To reduce the cost and enlarge the catalytic activity, Pt loading on carbon supporting
materials has been studied. Multi-walled carbon nanotubes (MWNTs) due to highelectron conductivity and chemical stability are ideal supporting materials for Platinum.
Carbon black (CB) has been widely used as the supporting material because of its low
price. The pyridine-containing polybenzimidazole (PyPBI) can be used as a dispersant of
CNTs to make them homogeneously dispersed. In this study, PyPBI wrapped CB and
MWNTs were used as a hybrid support for the Pt-based PEMFCs catalyst.
Different ratios between the MWNTs and CB are investigated. Based on the durability
measured by CV cycling and fuel cell
1200
performance, when the mount of MWNTs
reaches to 10wt%, the durability and fuel0.8
150
cell performance are similar to that of
100wt%-MWNTs. Typical result is shown
0.6
in Fig. 1.
100
Details will be reported at the meeting.

0

0

0.2

0.4

0.6

0.8

1

0

2

Current density / A/cm

Figure 1. Polarization of I-V and power density curvesof different MEAs for PyPBI/10%MWNTs-90%CB/Pt(dotted line), PyPBI/MWNTs/Pt (solid line), and
PyPBI/CB/Pt ( dashed line)- 64 -

1P-23Low-voltage carrier injection into semiconductor thin film from CNT thinfilm utilizing field enhancement effect○Tatsuya Yamada 1, Shigeru Kishimoto 1, and Yutaka Ohno 1
1Department of Quantum Engineering, Nagoya University, Nagoya 464-8603, Japan

CNT thin films are attractive material for transparent conductors of various semiconductor
devices such as OLEDs because of their flexibility and processability. In this work, we haveinvestigated carrier injection from sparse CNT thin films into a semiconductor thin film bymeans of device simulation. As the result, we have found that it is possible to inject carriers at
low voltage by utilizing field concentration onto CNTs.
Figure 1 shows a device structure examined in the simulation. CNTs were placed as theanode on the top surface of a p-type semiconductor thin film (Eg = 1.1e V, NA = 1017 cm-3)
with a thickness of 300 nm. Here, a simple metal wire with a diameter of 1 nm was assumed
as the CNTs. The interface between the CNTs and semiconductor assumed to be a Schottky
junction with a barrier height of 0.56 eV for a hole. A flat cathode electrode was placed on thebottom of the semiconductor layer. Ohmic contact was assumed for the cathode.
Figure 2 shows the hole current injected fromthe CNTs into the semiconductor film as a functionof spacing between the CNTs () at a bias voltageof 1 V. Here,  = 0 corresponds to a plate electrode.
The hole current increased with , and showed apeak at around  = 125 nm. Figure 3 shows theFig. 1 Device structure examined in simulation.
calculated energy band structure at 1 V for twocases; the plate anode and the CNT anode with  =125 nm. In the case of the CNT anode, theSchottky barrier was bent strongly, and thethickness of the barrier was decreased. This isbecause the electric field was concentrated to thethin CNT electrodes. As the consequence, thetunneling probability of holes was increased. The
hole current increased about four orders ofmagnitude in the low voltage region as comparedto the plate anode. For  > 125 nm, the current
Fig. 2 Calculated hole current versus  at 1 V.
decreased due to a decrease in effective area of theanode electrode. By utilizing the fieldenhancement effect, it can be expected to reduce
the operation voltage of devices such as OLEDs.
This work was partially supported by
ALCA/JST, SICORP/JST, and Grant-in-Aid of
MEXT.
Corresponding Author: Y. Ohno
Tel: +81-52-789-5387, Fax: +81-52-789-5387,
E-mail: yohno@nuee.nagoya-u.ac.jp

Fig. 3 Calculated energy band structures at 1 V
for two cases; the plate anode and the CNT
anode with  = 125 nm..

- 65 -

1P-24Highly durable membrane electrode assembly consists ofpoly(vinylphosphonic acid)-polybenzimidazole electrolyte and carbon
nanotubes based-electrocatalyst○Mohamed R. Berber1,2, Tsuyohiko Fujigaya1,3, Naotoshi Nakashima1,3,4
1International Institute for Carbon Neutral Energy Research (WPI-I2CNER),
Kyushu University, Fukuoka 819-0395, Japan2
Department of Chemistry, Faculty of Science, Tanta University,
Tanta 31527, Egypt
3
Department of Applied Chemistry, Graduate School of Engineering,
Kyushu University, 744 Motooka, Nishi-ku, Fukuoka 819-0395, Japan
4
JST-CREST, 5 Sanbancho, Chiyoda-ku, Tokyo, 102-0075, JapanLow durability of polymer electrolyte fuel cell (PEFC) is a major drawback that should be
solved. Recent studies have revealed that leaching of liquid phosphoric acid (PA) from bothpolymer electrolyte membrane (e.g. polybenzimidazoles; PBIs) and catalyst layers causes
inhomogeneous PA distribution and into membrane electrode assembly (MEA), leading to a
deterioration of PEFC performance during long-term operation [1].
In this study, in order to prevent acid leaching from the high temperature PEFC system, weused poly(vinylphosphonic acid) (PVPA) in place of PA because PVPA is a polymeric acidand is stably bound to the PBIs via multipoint acid-base reactions [2]. Also, It forms ahydrogen-bonding network with the neighboring phosphonic acid groups [3]. Consequently, it
forms an effective proton pathway after blending with PBI [4]. Typically in this study, wefabricated a novel fuel cell electrocatalyst by using carbon nanotubes (CNTs), PVPA-doped
PBI and platinum (Pt) nanoparticles as an electron-conducting supporting material, electrolyte
and metal catalyst, respectively (figure 1). The fabricated electrocatalyst was used beside a
PVPA-PBI membrane to prepare the MEA. The assembled MEA was used to test the fuel cell
performance and the durability at a non-humidified operating. The fuel cell performance of
the assembled MEAs was measured at atmospheric pressure under flowing dry hydrogen(flow rate; 100 mL/min) and dry air (flow rate; 200 mL/min) at the anode and cathode,respectively. The polarization curves were recorded at 120° C under non-humidified operating
conditions. Subsequently, the assembled MEA were subject to accelerating potential
durability test.
Successfully, the assembled MEA showed a remarkable high durability (single cell test:>400,000 cycling) together with a high power density of 252 mW/cm2 at 120˚C under anon-humidified condition. Such a high performance PEFC opens the door for the
next-generation PEFC for “real world” use.
[1] Y. Oon et al. J. Power Sources 189, 943(2009).
[2] Ü. Akbey et al, Aust. J. Chem. 62, 848 (2009).

[3] Y. J. Lee et al. J. Phys. Chem. B 111, 9711(2007).

[4] O. Acar et al. Int. J. Hydrogen Energy 34, 2724(2009).
Corresponding Author: M. R. Berber
Tel: +81-92-802-2845, Fax: +81-92-802-2845,

Fig. 1 schematic illustration of
the prepared electrocatalyst

E-mail: mrberber@mail.cstm.kyushu-u.ac.jp- 66 -

1P-25Single-Walled Carbon Nanotubes/Poly(Ionic Liquids) Nanocomposites
for Extremely High Thermovoltage○Motohiro Nakano, Yoshiyuki Nonoguchi, Takuya Nakashima, Tsuyoshi Kawai
Graduate School of Materials Science, Nara Institute of Science and Technology,
Nara 630-0192, Japan[1] J. C. Grunlan et al.
Energy Technol. 1, 265-272 (2013).
[2] T. Aida et al. Small 2, 554 (2006).
R MOE-200 purchased[3] TREKSTAR○
from PIOTREK was used.
Corresponding Author: Y. Nonoguchi
E-mail: nonoguchi@ms.naist.jp

Seebeck coefficient [μV/K]

Most flexible thermoelectric polymer composites with carbon nanotubes (CNTs) [1] haveever lacked practical Seebeck coefficient comparable to that of conventional inorganic
materials. The effective procedure for enhancing the Seebeck coefficient has not yet been
established. On the other hand, Aida et al. discovered that polymerizable ionic liquids (PILs)
enable single-walled carbon nanotubes (SWNTs) to be exfoliated from their bundles, which
formed highly-conducting polymer composites. [2] This well-dispersed SWNT material
inspired us to investigate effects of the interaction between SWNT and PIL on their
thermoelectric properties. We here-in report thethermoelectric properties of SWNT/PIL nanocomposites,
using CNTs synthesized by supergrowth chemical vapor
deposition (SG-CNT from AIST), and commercial ones
purchased from KH-Chemicals Co., Ltd. (KH-CNT) and
R1
Southwest Nanotechnologies (CoMoCAT). PILs were
[2]
Methacryloyl Acryloyl
synthesized following the modified procedure except[3]for MAEMAM(Fig.1). These PILs and SWNTs
MAEMAM AEMAM
were mixed with radical initiators at various
concentrations and the mixtures were heated at 330 K
for 2 hours, forming polymerized solids. We evaluated
MAEMIM
AEMIM
R2
Seebeck coefficient and electrical conductivity of all theeighteen composites at 310 K. A SG-CNT/MAEMAMAEMPYMAEMPY
composite possessed an extremely high Seebeckcoefficient (135 µV/K) at 310 K. This composite
showed roughly 5-fold increase in Seebeck coefficientFig.1 Chemical structures of ionic liquid
based thermoelectricin comparison with previous CNT-basedmaterials. We also found that thecomposite showed the highest
Seebeck coefficient with 1% ofweight fraction of SG-CNT. We will
discuss temperature dependence ofSeebeck coefficient and electricalconductivity.

Fig.2 Seebeck coefficient of SWNT/PIL nanocomposites at 310 K- 67 -

1P-26Large-scale separation of eDIPS for application to TFTs
Shunjiro Fujii1,2, Takeshi Tanaka1,2, Tomoko Sugita2, Satoshi Asano2,
Masaharu Kiyomiya2,Takeshi Saito1,2, żHiromichi Kataura1,2
12

National Institute of Advanced Industrial Science and Technology (AIST)
Technology Research Association for Single Wall Carbon Nanotubes (TASC)

Semiconducting single-wall carbon nanotubes (s-SWCNTs) have a great potential asa channel source of thin film transistors (TFTs) because of their excellent electricaltransport properties, for example, carrier mobility and high current carrying capacity.
Recently, we achieved performance enhancement of solution-processed TFTs by using a
network of s-SWCNTs obtained by gel separation method [1]. For further improvementsof the performance, a use of higher quality s-SWCNTs is desirable. In this work, we
separated eDIPS-SWCNTs [2] by gel column chromatography method [3] andfabricated TFTs using the separated high quality s-SWCNTs.
A liquid chromatography system equipped with a column filled with ~400 ml ofdextran-based gel beads were used for large-scale separation. About 40 mg of SWCNTs
were separated into metallic and s-SWCNTs in 2 hours. Figure 1 shows atomic force
microscopy (AFM) image of the separated s-SWCNTs. The lengths of s-SWCNTs were
1-2 Pm. TFTs using this s-SWCNTs exhibited high-performance transportcharacteristics. The on-off current ratio and the hole mobility calculated by a parallel
plate model were larger than 105 and 100௒cm2/V, respectively. Figure 2 shows the output
characteristics of the TFT. Detailed separation methods and device characteristics will
be discussed.
-2x10-4-4

Drain Current (A)-1.5x10

2 Pm

-4

-1x10

-5x10-500

7.4 nm

Fig.1 AFM image (10 x 10 Pm2) of s-SWCNTs.

0-5-10 -15 -20 -25
Drain Voltage(V)Fig.2 Output characteristics measured
at gate voltages from í40 (top) in
2.5ௗV step.

[1] S. Fujii et al., Appl. Phys. Express (2009), 2, 071601.
[2] T. Saito et al., J. Nanosci. Nanotechnol. (2008), 8, 6153.
[3] T. Tanaka et al., Phys. Status Solidi RRL (2011), 5, 301.
Corresponding Author: Hiromichi Kataura E-mail: h-kataura@aist.go.jp, Tel: +81-29-861-2551- 68 --30

1P-27
Evaluation of the ratio of metal/semiconductive single-wallcarbon nanotubes separated in two immiscible aqueous solution
phases by utilizing Raman spectroscopy technique
Naoki Kanazawa1, żShinzo Suzuki1, Yu Tanaka1, Akira Yamasaki1,
Daiki Miyazaki1, Akira Ono2
1

2

Department of Physics, Kyoto Sangyo University, Kyoto 603-8555, Japan
Department of Engineering, Kanagawa University, Yokohama 221-8686, Japan

PEG_532nm
DX_532nm*

PEG phase*DX phase

Raman Intensity / arb. unit

Raman Intensity / arb. unit

In 2013, C.Y. Khripin et al. reported about spontaneous partition of single-wall carbon
nanotubes (SWNTs) in polymer-modified aqueous solution phases [1], wheremetal/semiconductive SWNTs of large diameter (> 1.2 nm) are shown to be easily separated
in two immiscible aqueous solution phases, i.e., polyethylene glycol (PEG) and dextran (DX)aqueous solution.
In this presentation, Raman spectroscopy technique was applied to each aqueous solution
phase, in order to evaluate the ratio of metal / semiconductive SWNTs by changing excitation
photon energy (532 nm and 633 nm). Briefly, mono-dispersed sodium cholate (SC) solution(2wt%) of SWNTs produced by arc-burning of Ni/Y-carbon composite rod in helium
atmosphere was utilized for two immiscible aqueous solution, following the recipe by C.Y.
Khripin et al. [1]. After recognizing that PEG sand DX solution phases show different colors
because of the difference in the ratio of metal/semi-conductive SWNTs, Raman spectra ofeach phases were obtained by different excitation photon energy (532 nm and 633 nm).
Typical example of Raman spectra (G-band region) by excitation photon energy (532 nm
and 633 nm) for PEG and DX solution phase were shown in Figures 1 and 2. It was clearly
indicated that the ratio of semiconductive SWNTs to metallic ones was higher in PEG
solution phase than that in DX solution phase.

1400 1450 1500 1550 1600 1650 1700 1750 1800

Raman Frequency / cm

-1

Figure 1. Raman spectra obtained by 532 nm
photon energy (* indicates the reference signal
due to the sample tube).

**

1400 1450 1500 1550 1600 1650 1700 1750 1800

Raman Frequency / cm

-1

Figure 2. Raman spectra obtained by 633 nm
photon energy (* indicates the reference signal
due to the sample tube).

[1] C.Y. Khripin et al., J. Am. Chem. Soc., 135, 6822-6825(2013).

- 69 -DX phase

PEG_633nm
DX_633nm

References:

Corresponding Author: Shinzo Suzuki
Tel: +81-75-705-1631, Fax: +81-75-705-1631,
E-mail: suzukish@cc.kyoto-su.ac.jp

PEG phase1P-28Single Chirality Separation and Optical Properties of Small-diameter
Single-Wall Carbon Nanotubes○Xiaojun. Wei1, Yasuhiro. Ito1, Takuya. Hirakawa1, Atsushi. Hirano1, Shunjiro. Fujii1, Yuhei.
Miyauchi2,3, Kazunari. Matsuda2, Takeshi. Tanaka1 and Hiromichi. Kataura1
1

2

Nanosystem Research Institute, AIST, Tsukuba, Ibaraki 305-8562, Japan
Institute of Advanced Energy, Kyoto University, Uji, Kyoto 611-0011, Japan
3
PRESTO, JST, Kawaguchi, Saitama 332-0012, Japan

Single-wall carbon nanotubes (SWCNTs) are one-dimensional nanostructures that offer
great potential for application to novel optoelectronic devices due to large exciton binding
energies. Because current SWCNTs products are mostly composed of various structures,
structure sorting is necessary to obtain single chirality SWCNTs. Our group has successfully
separated 13 different single-chirality SWCNTs using multicolumn gel chromatographymethod two years ago [1].
Recently, we have improved the multicolumn method and optimized it for the small
diameter SWCNTs. In this work, (5,4) SWCNTs, which have the smaller diameter than C60
are successfully separated for the first time. In addition, high-purity (6,4) SWCNTs have also
been successfully separated at room temperature using the same separation method. Here, thepurity of (6,4) is much higher than that of our former separations by thetemperature-controlled gel chromatography at 10 degree (66%) [2]. Moreover, both of (5,4)
and (6,4) SWCNTs, show many bright photoluminescence (PL) peaks in an excitationemission PL map (shown as Figure 1). All these peaks can be assigned to the emissions fromonly one type SWCNTs by considering oxide states probably produced in the heavy
dispersion process before the separation [3].

Figure 1. Contour maps of PL intensity of (5,4) SWCNTs (left) and (6,4) SWCNTs (right) as afunction of the excitation and emission wavelength.
[1] H. Liu et al. Nat. Commun. 2, 309 (2011).
[1] H. Liu et al. Nano Lett. 13, 1996 (2013).
[3] Y. Miyauchi et al., Nat. Photonics 6, 2013547 (2013).
Corresponding Author: H. Kataura
Tel: +81-29-861-2551, Fax: +81-29-861-2786, E-mail: h-kataura@aist.go.jp- 70 -

1P-29Fabrication of metal nanorods for the synthesis of short-carbon nanotubes○Takao Sada1, Tsuyohiko Fujigaya1,2, Naotoshi Nakashima 1,2,3
1 Department of Applied Chemistry, Graduate School of Engineering, Kyushu University

Motooka, Fukuoka 819-0395, Japan, 2WPI-I2CNER, Kyushu University,
3JST-CREST,5 Sanbancho, Chiyoda-ku, Tokyo, 102-0075, Japan

Carbon nanotubes (CNTs) are nanomaterials that possess remarkable electrical,
mechanical and thermal properties and have been explored for biological applications [1].
One of the obstacles for the biological application of CNTs is the toxicity. The use of CNTs iscurrently considered with apprehension owing to their carcinogenic risks, especially comefrom their structural similarity to asbestos. To apply the CNTs to the biological applications,several groups have investigated the way to reduce their toxicity and reported long CNTs
were found to trigger an inflammatory response [2]. Therefore, the demand for thelength-controlled CNTs, especially short-CNTs is increasing. In this report, we describe thefabrication of metal nanorods as the new template catalyst for the synthesis of short-CNTs
which is expected to be formed by the graphene around metal nanorods.
Fabrication of metal nanorods
were conducted by the pulsed
electrodepositon in anodic aluminumoxide (AAO) template thus forming
Ni as the catalyst and Ag as thesacrificial layer alternatively withregulated pulse duration (τNi = 10 s,
τAg = 120 s) to control respective
segment length (Fig. 1a). The
scanning
transmission
electronmicroscope (STEM) image andEnergyDispersive
X-ray
spectroscopy (EDX) analysis in Figs.
1b, 1c and 1d indicated that Ni-Ag
nanowires with 75 ±9 nm in Ni
segment were successively formed insingle nanopore of AAO template.
We have also confirmed Ni segment Fig. 1 (a) Schamatic illustration of the fabrication of Ni-Ag
is easily controlled by the pulse nanowires by pulsed electrodeposition. (b) STEM andduration. In the future, we are going corresponding Ni-Ag intensity profile along its growth
to show the utility of the Ni nanorods direction. (c) STEM image of Ni-Ag nanowires after Ag
as the metal catalyst for the synthesis etching. (d) Length histogram of Ni segment.
of short-CNTs.
[1] H. Dai et al., Nano Res. 2009, 2, 85.
[2] H. Boucetta et al., Angew. Chem. Int. Ed.. 2013, 52, 2274.
Corresponding Author: N. Nakashima
Tel: +81-92-802-2840, Fax: +881-92-802-2840,
E-mail: nakashima-tcm@mail.cstm.kyushu-u.ac.jp- 71 -

1P-30
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   ! "#$  ! %#  "&'#(&)" *

                                       !"   #       $     
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 9 : 0 $# ; ": <4)25**44*33 (,: <4)25*%))&*2=: > $?

- 72 -

1P-31
Rapid separation of high-purity and micrometer-long semiconducting
carbon nanotubes by gel filtration○Boanerges THENDIE1, Yasumitsu MIYATA2,3, Haruka OMACHI1, Ryo KITAURA1, Yuhei
MIYAUCHI3,4, Kazunari MATSUDA4, and Hisanori SHINOHARA1
1

Department of Chemistry and Institute for Advanced Research, Nagoya University,
Nagoya, 464-8603, Japan2
Department of Physics, Tokyo Metropolitan University, Tokyo, 192-0397, Japan
3
JST, PRESTO, Tokyo, 102-0075, Japan
4
Insititute of Advanced Energy, Kyoto University, Uji, Kyoto, 611-0011, Japan

Single-wall carbon nanotubes (SWCNTs) hold promising applications for high performanceelectronic devices due to their excellent carrier mobility, flexibility, and solution processability.
So far, realizing high performance nanotubes-based devices requires a sophisticated techniqueto prepare high purity and micrometer-length semiconducting SWCNTs. In the past, we havereported that the multi-stage gel filtration is capable to provide 99% high purity semiconducting
and micrometer-long SWCNTs [1]. However, this multi-stage process is time-consuming (morethan 24 hours per run) which limits the scalability of the method.
In the present study, we develop a fast, one-stage gel filtration method to obtain micrometerlong and high-purity semiconducting SWCNTs [2]. The present method utilizes fractionation
process during the elution of semiconducting
SWCNTs as illustrated in Fig. 1. The
semiconducting SWCNTs fraction evaluated by
optical absorption and Raman spectra shows thepurity of semiconducting SWCNTs is as high as
99%, whereas the evaluation of SWCNTs length byphotoluminescence imaging and atomic force
microscopy provides the simultaneous length-based
separation of micrometer-long SWCNTs.

Figure 1 Schematic of the simultaneous single-[1] Y. Miyata et al. Nano Res. 4, 963 (2011)stage separation of micrometer-long and high-[2] B. Thendie et al. Appl. Phys. Express 6, 065101 (2013)

purity semiconducting SWCNTs

Corresponding author: Hisanori Shinohara
Tel: (+81) 52-789-2482, Fax: (+81) 52-747-6442,
E-mail: noris@nagoya-u.ac.jp- 73 -

1P-32
Efficiency Synthesis of Double Wall Carbon Nanotubes by Pressure
Control of High-temperature Pulsed-arc Discharge○Hayato Kikuchi1, Katsuhide Terada2, Toshiki Sugai 1
1

2

Department of Chemistry, Toho University, Chiba 274-8510, Japan
Faculty of Pharmaceutical Sciences, Toho University, Chiba 274-8510, Japan

G-band Intensity / a.u.

Speed of Vaporization / mg / hConcentration of DWCNTs / %Concentration of CNTs / %A high-temperature pulsed-arc discharge (HTPAD) has been developed to produce carbon
nanotubes (CNTs). The system utilizes width controlled pulsed arc discharge for thevaporization of electrodes in a temperature controlled ambient gas. With this width andtemperature control, novel materials have been produced such as high-quality double wall
carbon nanotubes (DWCNTs)[1]. We have also optimized the production processes of CNTsby high-pressure discharge up to in 5 atm with controlling vaporization and condensation
processes[2]. Here, we present TGA and TEM evaluation of product CNTs as well as Raman
spectroscopy with getting optimal condition not only for SWCNTs but also for DWCNTs.
The system consists of a furnace with a ceramic tube inside, an Ar gas flow and pressure
control system, an HV pulse voltage controller, and a water cooling trap. Electrodes made ofgraphite containing catalytic metals (Ni/Y 4.2/0.5 and 4.2/1.0 at. %:Toyo Tanso Co. Ltd.)
were located in the ceramic tube. The pulsed arc discharges (0.6 ms, 50 Hz, and 100 A)
vaporized the electrodes and produced CNTs in the high-temperature (1250 °C) and a wide
pressure range of Ar (0.2-5 atm) in the ceramic tube. The products were collected on the trap
and were characterized by Raman spectroscopy with excitation laser of 633 nm, TGA, andTEM.
Figure 1 shows the pressure dependence of concentration of CNTs by TGA. The obtained
optimal pressure is 1.5 atm which is the same as that15
Y = 1.0 %obtained with the Raman and TEM observations. The
Y = 0.5 %analysis on the optimal pressure of various production
10
methods such as laser and steady arc methods have shownthat the production processes are dominated by cooling and5condensation processes[3]. Our optimal condition is exactly
Y = 1.0 %corresponding to those analyses[2], which shows that theY = 0.5 %0cooling processes are also crucial for HTPAD.
0
1
2
3
4
5
Figure 2 shows the pressure dependence of thePressure / atm
Fig. 1 Pressure Dependence of theconcentration of DWCNTs obtained by TEM and the speed
Concentration of CNTs by TGAof electrodes vaporization. Clearly, the lower the pressure,the high the concentration. The different pressure
Y = 1.0 %Y = 0.5 %20
dependence shows that the production processes are
Vaporization
dominated not by the cooling processes but by different
processes. The correspondence of the concentration of
10
DWCNTs and the speed of the electrodes vaporizationsuggests that the vaporization process is the crucial process0on the production of DWCNTs.
0
1
2
3
4
5
[1] T. Sugai et al., Nano Lett. 3, 769 (2003).
Pressure / atm[2] H. Kikuchi et al. The 43th FNTG General Symposium. 1P-24.
Fig. 2 Pressure Dependence of[3] O. Jost, A. A. Gorbunov, J. Moller, W. Pompe X. Liu, P. Georgi, L.
Concentration of DWCNTs
Dunsch, M. S. Golden, and J. Fink, J. Phys. Chem. B. 106, 2875 (2002).
Corresponding Author: T. Sugai Tel: 047-472-4406 E-mail: sugai@chem.sci.toho-u.ac.jp- 74 -

1P-33Synthesis and Evaluation of Single-Walled Carbon Nanotubes
Using Metal Catalyst Ni-Y-Mo○Bo Sun, Sakae Inoue, Tomoko Suzuki, Takayuki Yamamoto,
Chihiro Yanagi, Yoshinori Ando
Department of Materials Science and Engineering, Meijo University, Nagoya
468-8502, Japan
In the past decades, extensive works have been done in order to improve the purity
and quality of single-walled carbon nanotubes (SWNTs) structure such as chirality,
diameter by varying its growth conditions [1–3]. This paper focuses on the influence ofMo on the growth of SWNTs in arc discharge. Mo with different concentrations isincorporated in Ni-Y/He system. The yield, purity, ease of purification and diameter
distribution of as-grown samples are characterized, and used to evaluate the effects of
Mo. Based on analyses of yield and purity, we found the best concentration of Mo is 0.5
at% in Ni-Y/He system.
Figure 1 shows yield of SWNTs. For this system, the incorporation of Mo has
dramatically increased the yield of soot in their best concentrations. Thermal
gravimetric analysis showed that after purification, only negligible impurities remain in
the sample for Ni-Y-Mo/He system. Figure 2 shows TGA plot of as-grown SWNT and
purified SWNTs. Considering on these experimental results, we prove that Mo plays apositive role in arc discharge for the enhancement of SWNTs growth.

Fig. 1

Yield of SWNTs

Fig. 2

TGA plot of as-grown and purified SWNTs[1] C. Journet, W. K. Maser, P. Bernier, A. Loiseau, M. Lamyde la Chapelle, S. Lefrant, P. Deniard, R.
Lee, and J. E. Fischer, Nature 388, 756 (1997).
[2] X. Zhao, S. Inoue, M. Jinno, T. Suzuki, and Y. Ando, Chem. Phys. Lett. 373, 266 (2003).
[3] Y. Ando, X. Zhao, K. Hirahara, K. Suenaga, S. Bandow, and S. Iijima, Chem. Phys. Lett. 323, 580(2000).
Corresponding Author: B. Sun
E-mail: louiskoo2518@hotmail.com- 75 -

1P-34
Studies on Chemical Reactions of Cobalt Clusters
with Water and Oxygen by FT-ICR Mass Spectrometer○Yuta Tobari 1, Kazuki Ogasawara 2, Shohei Chiashi 2, Shigeo Maruyama 2, Toshiki Sugai 1
1

2

Department of Chemistry, Toho University, Chiba 274-8510 Japan
Department of Mechanical Engineering, The University of Tokyo, Tokyo 113-8656, Japan

Cobalt nano particles and clusters are a popular catalyst
for carbon nanotube (CNT). However, reactions on Co
clusters associated with CNT growth are not well known.
To investigate these reactions, time of flight (TOF) and
quadrupole mass spectrometers have been utilized asconventional methods but most of the studies are
performed on hot (~2000 K) clusters with short term (~ms)
observation, which is far from the realistic catalyzed
reactions. Here we present studies on room temperature
reactions of Co clusters with water and oxygen with longterm (~10 s) observation by Fourier transform ion
cyclotron resonance mass spectrometer (FT-ICR).
Experimental details have been described elsewhere[1]. Co clusters were produced by a laser vaporization
cluster source and were introduced and trapped in a cellunder a magnetic field of 6 T. The trapped clusters are
Fig. 1 Mass spectra of pristine andthermalized in several seconds and are then exposed toreacted Co clusters with H2O & O2.
water and dry air for several seconds. Finally ICR signalsof product ions were observed and analyzed as mass spectra.
Figure 1 shows mass spectra of pristine Co clusters and their reactants with water and dry
air. Pristine Co clusters are observed with negligible contamination. In the water reactions, up
to 4 adducts with dehydrogenation of Con(OH)m(H2O)l (m+l=1~4) are observed. Those multiple
adducts have not been observed with TOF because of the hot production condition and the shortterm observation. Dehydrogenation is more significant as the number of water molecules
increase. Tetra-water adducts are always more significant than tri-water adducts indicating that
their stoichiometry is not Con(H2O)2O2 but Con(OH)4. On the contrary of the water adducts
indicating weak interaction, the products with dry air are observed as Co oxide clusters ofConOm (n=m+1 or m+2) with much stronger interaction between Co clusters and oxygen. In the
hot TOF condition, much complicated and statistical distribution of n and m are observed [2].
In these oxide clusters, Co13O8 cluster is obtained as the same magic number cluster of those in
the TOF hot condition [2]. Those results show the special stability of Co13O8 and much smaller
stability of other ConOm. The intensity of Co13O8 is much larger than that of pristine Co13
showing dissociation from larger oxide clusters of ConOm (n>13) to Co13O8 [3]. Those salient
differences between our results and those obtained with TOF show that our FT-ICR reaction
condition is mild enough to have the final products with the highest stabilities. Thoseadvantages of FT-ICR will contribute to reveal the catalyst reactions.
[1] S. Maruyama, et al., Fullerene Sci. Technol. 7 (1999) 621. [2] Q. Sun, et al., Phys. Rev. B 62 (2000) 8500.
[3] M. L. Anderson, et al., J. Chem. Phys. 130 (2009) 064305.
Corresponding Author: T. Sugai, Tel: +81-47-472-4406, E-mail: sugai@chem.sci.toho-u.ac.jp- 76 -

1P-35
Encapsulating Carborane within Aligned and Dense Carbon Nanotubes
on SiC Substrate○H. Fujita1, W. Norimatsu1, and M. Kusunoki1,2
1

Department of Applied Chemistry, Nagoya University, Nagoya 464-8603, Japan2
Eco Topia Science Institute, Nagoya University, Nagoya 464-8603, Japan

Carbon nanotube (CNT) has been studied for various applications based on its specificproperties since its discovery. Especially, encapsulation into CNTs has recently attracted agreat attention for control of their properties. The encapsulation within CNTs has beendeveloped from the first report of encapsulating fullerene which is called a peapod, andrecently expands to various endohedral metallo-fullerene, metals, molecules and so on.
In this study, we focused on the boron cluster called carborane (C2B10H12) as a newmaterial instead of fullerene. The carborane has super aromatic series and cage type structures
similar to fullerene and the constituent element is based on boron. It is well known that cluster
materials inside the CNT could form one dimensional crystal and the carbon material such as
the CNT and diamond becomes superconductive by doping boron [1][2]. We then expect thatappearance of boron clusters into CNT’s exhibits new properties. Here we report results about
the carboranes encapsulated in the CNTs film on SiC substrate.
Firstly, we prepared the CNTs film about 160 nm thick synthesized by the SiC(000-1)
surface decomposition [3]. The CNTs has a well aligned and highly dense structure, whichmight contribute to the formation of densely-aligned encapsulated CNTs. Secondly we opened
the CNT’s end-cap by oxidation using hydrogen peroxide solution. Finally we encapsulated
carboranes into CNTs by exposing the CNTs film to the vapor of carboranes in the quartz tube.
Observation of the CNTs film was carried out using transmission electron microscopy (TEM)and electron energy loss spectroscopy (EELS). Figure1 shows the CNTs film on SiC substrate
after encapsulating carboranes into CNTs at 350 ˚C. Figure 1 (a) and (b) show that the CNTs
were formed with a well aligned and highly dense film structure on SiC substrate. Figure 1(c)shows EELS boron K-edge mapping image in the area of Fig.1(b). That image indicates thatmany boron atoms existed in the CNTs film not that surface and lined along the CNTs axis.
Furthermore, it was estimated from the intensity of each spectra in Fig.1(d) that the CNTs film
included boron atoms about 4 at.% compared with carbon atoms.

Fig.1(a) TEM image of the CNTs film on the SiC substrate and (b) the CNTs film within
the white squire in (a), (c) boron K-edge mapping in the same area and (d) the EELS spectrum[1] N, Murata et al, Phys. Rev. Lett. 101, 027002(2008)[2] M. Nesladek et al, Appl. Phys. Lett. 88, 23211 (2006)[3] M. Kusunoki et al, Appl. Phys. Lett. 77, 531-533(2000)
Corresponding Author: H. Fujita
Tel: +81-52-789-5859, Fax: +81-52-789-5859,
E-mail: fujita.hayato@f.mbox.nagoya-u.ac.jp- 77 -

1P-36
Synthesis of a carbon nanotube filled with solid-phase separating
stainless alloy by liquid and solid interfacial arc discharge method○Takuya Sagara 1, Satoshi Kurumi 1, Ken-ichi Matsuda 1, Kaoru Suzuki 1
1

Department of Electrical Engineering CST, Nihon University, Tokyo 101-8308, Japan

Metal-filled carbon nanotube (CNT) which is filled the DC power supply Electrodehollow with various metal materials has been reported by S.
Iijima and P. M. Ajayan [1]. In previous our work, we reported
on controlling elongation and growth mechanism of Ni-filled
SUS304 mesh
CNT that is directly synthesized on Ni mesh by liquid andsolid interfacial arc discharge method [2]. The method is basedon liquid-phase deposition invented by M. Gamo-Nishitani etal [3]. Here we report on the structure of a CNT filled withSi substrate
Ethanol solution
stainless alloy separating solid-phase or crystalline phase by a
Fig.1 Schematic ofsimilar technique.
experimental set-up
Figure 1 shows schematic diagram of liquid and solidinterfacial arc discharge method. A sectorally processed
stainless mesh (original diameter 3mm, 200 grid per an inch,
SUS304) is set between Si substrate and cathode connected toa direct current power source (3.0 A, 70 – 80 V) as in fig.1.
This electrically closed circuit is submerged in ethanol
solution (99.5%). Then, arc discharge takes place between the
SUS mesh of cathode and Fe rod of anode by applying direct
current to the circuit. Figure 2 is the close-up photograph of Cathode spot SUS304 mesh ElectrodeFig.2 Appearance of cathode spot
cathode spot at the apex of the SUS mesh.
Figure 3 (a) is the scanning transmission electron microscope dark field image of typical
CNT filled with stainless alloy. White contrast appears in the part of CNT’s hollow, whichindicates evidence for filling. Figure 3 (b) - (d) are elemental mapping images with energy
dispersive X-ray spectroscopy. These images showed
the filler in the CNT is stainless alloy that consists of(b)(a)
homogeneous Fe and Ni. However, difference inconcentration of Cr is appears in fig.3 (d), and we
suppose that solid-phase separation is attributed tothis distribution of Cr.
Acknowledgement
A part of this work was supported by"Nanotechnology Platform" (project No.12024046) of(c)(d)
the Ministry of Education, Culture, Sports, Scienceand Technology (MEXT), Japan.
[1] P.M. Ajayan and S. Iijima, Nature 361(1993) 333.
[2] T. Sagara et al. Appl. Surf. Sci. in press APSUSC-26712[3] M. Nishitani-Gamo et al, Jpn. J. Appl. Phys. 46 (2007) 6329.
Corresponding Author: K. Suzuki
Fig.3 STEM and EDX elemental mapping images ofTel: +81-3-3259-0770, Fax: +81-3-3259-0770,
a CNT filled with stainless alloy. (a) dark fieldE-mail: kaoru@ele.cst.nihon-u.ac.jp
image, and signal from: (b) Fe; (c) Ni; (d) Cr.

- 78 -

1P-37
Containment method for transmission electron microscopy of gas molecules
within the inner space of carbon nanotubes under high vacuumżKeita Kobayashi 1, Takeshi Saito 2,3, Masaharu Kiyomiya 3, Hidehiro Yasuda 1
1

Research Center for Ultra-High Voltage Electron Microscopy, Osaka University, Ibaraki,
Osaka 567-0047, Japan
2
Nanotube Research Center, National Institute of Advanced Industrial Science andTechnology (AIST), Tsukuba, Ibaraki 305-8565, Japan
3
Technology Research Association for Single Wall Carbon Nanotubes (TASC), Tsukuba,
Ibaraki 305-8562, Japan

The inner space of carbon nanotubes (CNTs) provides a suitable nanospace for molecules
storage, and CNTs have thus been widely used as nanoscale test tubes for transmission
electron microscopy (TEM) observation of isolated molecules and unstable low-dimensional
crystals. The TEM observation of guest materials encapsulated within CNTs clarifies both thestructure of the guest materials and their behavior within a confined nanospace, making this apowerful method for research on nanomaterials. However, since CNTs used as test tubes areprepared by removing the end-caps to provide a pathway for the guest molecules, containmentof highly volatile molecules and gases in the inner space is problematic in the TEM specimen
chamber, which is kept at high vacuum (~10-5 Pa). For this reason, TEM observation of gas
molecules has not yet been reported, whereas the behavior and structure of various molecules(fullerenes [1], metal complexes [2], polycyclic aromatic hydrocarbons [3], etc [4].) havebeen observed directly by TEM using CNTs as test tubes. Therefore, the development of anovel method for the containment of gas molecules in CNTs during TEM observation isnecessary for discovering the unique behavior and structures of such confined gas molecules.
Against this background, we aimed to observe guest gas molecules encapsulated within CNTsby blocking the escape pathways. A typical EDX spectrum of Xe encapsulated in CNTs withblocked pathways shows a peak at 4.1 keV corresponding to the LĮ line of Xe, whichindicates that Xe gas was contained within the inner space of the CNTs even under highvacuum.
In this presentation, we will introduce the details of the method and discuss the uniquebehavior of gases confined within nanospaces.
This work was supported by KAKENHI (#25790003) from JSPS. KK thanks Prof. R.
Kitaura and Prof. H. Shinohara for valuable discussion.
[1] R. Kitaura & H. Shinohara, Chem. Asian J. 1, 646 (2006).
[2] L.-J. Li et al., Nature Mater. 4, 481 (2005).
[3] T. Okazaki et al., Angew. Chem. Int. Ed. 50, 4853 (2011).
[4] M. Koshino et al., Science 316, 853 (2007).
Corresponding Author: K. Kobayashi
Tel: +81-6-6879-7941, Fax: +81-6-6879-7942,
E-mail: kobayashi-z@uhvem.osaka-u.ac.jp

Fig.1 typical EDX spectrum of Xe
encapsulated CNTs

- 79 -

1P-38Light-assisted in-situ polymer formation on carbon nanohorns
Mei Yang1, ○Minfang Zhang1, Masao Kunioka1, Sumio Iijima1, 2, Masako Yudasaka1
2

1 National Institute of Advanced Industrial Science and technology 5-2, Tsukuba, Japan

Department of Material Science and Engineering, Meijo University, Nagoya, Japan

Carbon nanomaterials have attracted tremendous interest in the basic and application
sciences. For example, carbon nanomaterials absorb light in a wide range from UV to IR andconvert the light energy to thermal energy. The photothermal conversion has been shown to be
useful for photothermal tumor therapy by animal tests [1]. Among the carbon nanomaterials,
carbon nanohorns (CNHs) present higher photothermal conversion efficiency than othercarbon nanomaterials, such as carbon nanotubes [2]. Here we report a method for in-situ
polymer formation by using CNHs. In this method, by light irritation, CNHs worked as“molecular heater” to raise the local temperature, which helped selectively forming thepolymers just on the surface of CNHs. This method may be quite useful for synthesis of
nanocarbon-polymer composites and surface functionalization of carbon nanomaterials.
Polycaprolactone (PCL) is aliphatic polyester composed of hexanoate repeat units. It is an
important biocompatible and biodegradable polymer. Due to its multiple biomedical
applications, the synthesis of PCL or PCL/nanocarbon composites has received increased
attention. In this study, irradiating NIR light (808nm) for 1 hour, the local temperature around
CNH increased and the ring of cyclic monomer caprolactone was opened, leading to thepolycaprolactone (PCL) formation on the CNHs surface. The number average molecularweight (Mn) and polydispersity (Mw / Mn) of the obtained PCL were 6982 and 1.235. As acontrol, without CNHs, the Mn of PCL is only 555.
Biological origin molecule of polydopamine (PDA) has served as a universal coating tonanoparticles for various biomedical applications. With the light irradiation, dopamine
quickly self-assembled to the PDA and selectively coated the surface of CNHs. The coating
amount can be controlled by the reaction time and light intensity.
All of these data suggested that the photothermal effect of CNHs is useful for polymer
synthesis on the surface of carbon nanomaterials.
[1] M. Zhang et al. Proc. Natl. Acad. Sci. U. S. A. 105, 14773 (2008).
[2] E. Miyako et al. Proc. Natl. Acad. Sci. U. S. A. 109, 7523 (2012).
Corresponding Author: M. Zhang and M. Yudasaka.
TEL/Fax: +81-29-861- 6290
E-mail: m-zhang@aist.go.jp (M. Zhang), m-yudasaka@aist.go.jp (M. Yudasaka).

- 80 -

1P-39Selective carboxylation of graphite-like thin sheet edges in carbon
nanohorn aggregates○Maki Nakamura 1, Michiko Irie 1, Ryota Yuge 2, Toshinari Ichihashi 2, Sumio Iijima 1,3,
Masako Yudasaka 1
1

National Institute of Advanced Industrial Science and Technology (AIST),
Tsukuba 305-8565, Japan
2
NEC Corporation, Tsukuba 305-8501, Japan
3
Meijo University, Nagoya 468-8502, Japan

Single-walled carbon nanohorns (CNHs) are expected to have many applications in thefields of electrochemistry, biomedicinal chemistry, and so on. Chemical functionalization of
CNHs is important for their various applications. Especially, carboxylation is useful forchanging hydrophobic CNHs to hydrophilic ones that are dispersible in aqueous solutions.
Usually, as-prepared CNHs assemble by the thousands to form the spherical aggregates (~100nm) containing graphite-like thin sheets (GLSs) [1]. We previously reported that several
oxygenated groups, such as carboxyl, quinone, carbonyl, and hydroxyl groups wereintroduced into the CNH-GLS aggregates by the mild oxidation with hydrogen peroxide atroom temperature for a certain period (from 1 hour to 56 days) [2,3]. In this report, we showthat the GLS edges in CNH-GLS aggregates can be selectively carboxylated by 1 hour
immersion in hydrogen peroxide at room temperature [4].
CNH-GLS aggregates were prepared by CO2 laser ablation of graphite in Ar (~760 Torr)
without auxiliary heating. For selective oxidation of the GLS edges, CNH-GLS aggregateswere immersed in a 30% hydrogen peroxide aqueous solution for 1 hour at room temperature.
After immersion, the oxidized CNH-GLS aggregates were filtered and washed with water.
The types of the generated oxygenated groups were determined by using temperatureprogrammed desorption mass spectrometry (TG-MS). To visualize the location of carboxylgroups in the oxidized CNH-GLS aggregates, they were stained with Pt-ammine complexes,
and observed using a transmission electron microscope (TEM) and a scanning transmission
electron microscope (STEM).
According to the TG-MS results of the oxidized CNH-GLS aggregates, the presence ofcarboxyl groups was confirmed with the emission of m/z = 44 at 100-300 °C. In TEM and
STEM observations, the Pt-ammine complexes that reacted with the carboxylic groups in theoxidized CNH-GLS aggregates were visible at the edges of GLSs, but not so on the basal
planes of GLS and on CNHs. The selective carboxylation of GLS edges in CNH-GLS
aggregates would enable unique chemical functionalization of CNH-GLS aggregates andcould expand their application possibilities.
[1] M. Irie, M. Nakamura, M. Zhang, R. Yuge, S. Iijima, M. Yudasaka. Chem. Phys. Lett. 500, 96 (2010).
[2] M. Nakamura et al. The 42th Fullerenes-Nanotubes-Graphene General Symposium, 2012.
[3] M. Nakamura, T. Kawai, R. Yuge, S. Bandow, S. Iijima, M. Yudasaka. Carbon in press.
[4] M. Nakamura, M. Irie, R. Yuge, T. Ichihashi, S. Iijima, M. Yudasaka. PCCP 15, 16672 (2013).
Corresponding Author: M. Nakamura and M. Yudasaka
Tel: +81-29-861-4604, Fax: +81-29-861-6290,
E-mail: ma-ki-nakamura@aist.go.jp (M.N.) and m-yudasaka@aist.go.jp (M.Y.)- 81 -

1P-40Topological Controlled Synthesis of Graphene Sheet
Chozo Inoue,11Professioal Engineer,(Department of Chemistry) ,Chigasaki city Kanagawa Japan
E-mail:choinoue@nifty.com

1. Introduction.
There are many problems in the application of the graphene sheet. In order to enable an excellentalignment control, the development of a simple precursor to continue to grow into a sheet on the spotat the time of use is desirable. When synthesizing SWNT using a raw material decalin, sometimes
graphene sheets extend laterally from the tube as a by-products . [1] By considering the mechanism of
avoiding the winding of graphene, I found conditions under which the graphene grows into sheet.
Using the raw material of armchair type and π-topological controlled catalysis of graphene edges, atwo-step process were developed.
2. Experiment
Chemicals and feedstock are listed in comparative table 1. Zirconocene is a π-polymerization
catalyst which is difficult to produce a CNT . Dibenzo-thiophene is the source of unit structure of thearmchair type edge because having fixed rotational plane of the biphenyl structure by cross-linking of
sulfur,. Paraffin was used for aliphatic carbon source, having higher boiling point than decaline.
Table1. Comparison of Catalyst, Radical-source, Raw material and Process Condition.
CNTprocess

Ferrocene

Thiophene

Benzene

1step

Graphene

Zirconocene

Dibenzothiophene

Paraffin

2step① First step: .At 100 ℃ or more , dissolve the zirconocene and dibenzothiophene in paraffin.
Stirring and changed the red purple color of the solution , the creamy solution to cool to room
temperature.
② Second step: Schmear the cream thinly on a filter paper of quartz wool to facilitate
sublimation .Then its slowly inserted into the electric furnace of 900 ℃ under a stream of argon.
After the sublimation are finished, agglutinate graphene soot gather on the expanded graphite
substrate placed at the exit. [3] Fig 1. SEM Photograph

3. Result and Discussion
These graphene soot can be dispersed to sheet easily inalcohol. This indicate to prevent the byproduct of CNT andthe like, by setting to remain at the start point the
impurities that can not be sublimated. Each step ismonitored by Raman spectrum and was analyzed by SEM,
TEM, STEM, EDX. [2] For future tasks, optical
microscope should use to evaluate of graphene sheet.
So nano-graphene precursor in the first stage is a PAH
meso-phase having a terminal hydrogen, it is possible toalign on device. Coating method is very important final
step for the improvement of orientation and performanceof the graphene sheet.

Fig.1[1] Mauricio Terrones et al, Nano Lett., 2008, 8 (9), pp 2773–2778[2] Andrey L. Chuvilina et al , Carbon 4 7 ( 2 0 0 9 ) 3 0 9 9 –3 1 0 5[3].C.Inoue et al, P2011-219372- 82 -

Map

of

Hongo

campus,1P-41
Direct growth of graphene on dielectric substrates
by etching-precipitation method○Masaki Kosaka1,2, Kei Hasegawa 2, Suguru Noda 2
1

Department of Chemical System Engineering, The University of Tokyo, Japan2
Department of Applied Chemistry, Waseda University, Japan

Chemical vapor deposition (CVD) on catalyst metals is considered as the most promising
method to synthesize graphene because of its potential for high scalability [1]. For many
applications, it is necessary to fabricate graphene on dielectric substrates. However, wettransfer process easily causes impurities and damages to graphene. The synthesis of graphenewith fair quality and uniformity directly on dielectric substrates is still challenging.
We have realized metal-free graphene directly on dielectric substrates by
etching-precipitation method [2,3], in which carbon precipitates as graphene by removing thesolvent metal by dry etching from carbon-metal solid solution on the substrates (Fig. 1).
In this work we used the Fe-C mixture film of various thickness (20-200 nm) sputter
deposited on SiO2/Si or quartz glass substrates. The samples were heated to 400-700 oC under
25 vol% H2/ Ar at 100 Torr and kept for 10 min in the tubular reactor, and the etching of Fe
was carried out under 0.05 vol% Cl2/ Ar at the same temperature and 5 Torr for 1-90 min toyield graphene directly on the substrates. Typical results are shown in Fig. 2. The photographof the sample shows the uniform gray color over the substrate, suggesting the uniform
formation of graphene. Its optical transmittance was 86%, indicating the average layer
number of 6~7. In the AFM image taken near the voids, the height difference between thegraphene and void surfaces were ~ 2 nm, which is consistent with the layer number evaluatedfrom the optical transparency. The Raman spectrum showed a G-band peak and a relatively
small D-band peak with the G to D intensity ratio (IG/ID) of 20, suggesting the fair quality ofthis graphene. The plan-view SEM image had some contrast difference, suggesting some layer
number distribution, and small holes
Heating Cl2 Fe2Cl6 Etchingsuggesting some voids in the graphene film.
at high temp.
30.00
Fe-C
From this image the grain size and graphene
Fe-C
[nm]
Substrate
coverage were estimated to be 4~5 µm andover 99%, respectively. This film had a sheet
Fig.1 Schematic of etching-precipitation method
resistance of 340~460 Ω/sq., corresponding(a)(b)
I /I = 20
1.5 cmto the volume resistivity of 70~90 μΩ cm
which is similar to that of HOPG (20~50 μΩcm). Our etching-precipitation method is apractical route to synthesize graphene directly
1000
1500
2000
2500
3000
1000 1500 2000 2500 3000
on device substrates of arbitrary sizes.
Raman shift / cm
Intensity / -

G D

-1

(d)

(c)

[1] S.Bae, et al. Nat. Nanotechnol. 5, 574 (2010).
[2] S. Takano and S. Noda, The 40th FNTG General
Symposium, 2P-38 (2011).
[3] M. Kosaka, et al., The 44rd Fall Meeting of theSociety of Chemical Engineers, Japan, G315 (2012)*Tel&Fax: 03-5286-2769, E-mail: noda@waseda.jp- 83 -

30
[nm]

7.9
[nm]
0

Void

30.00
[nm]

Graphene

50 µm

2 µm

0

Fig. 2 (a) A photograph, (b) Raman
spectrum,
0.00(c)2.00SEM
and
(d)
AFM
image
of
the
sampleµm
5.00 x 5.00 µm
synthesized at 650 oC on a quartz substrate
2.00 µm

5.00 x 5.00 µm

0.00

1P-42CVD-growth of nitrogen-doped grapheneusing tetraphenyl porphyrin as a solid precursor○Yuma Sugisaki, Ryo Kitaura*, Haruka Omachi and Hisanori Shinohara*
Department of Chemistry & Research Center for Materials Science, Nagoya University,
Nagoya 464-8602, Japan
Graphene, the two-dimensional monolayer form of sp2-hybridized carbon, has
attracted widerange interests due to its novel physical properties and promising
applications in electronic devices and composite materials.

While graphene canreadily be p-doped by adsorbates, n-doped graphene, which is indispensable for device
applications, is more difficult to achieve. Nitrogen doping is one of the most polularmethods to dope electrons into graphene, but it is still a challenging topic to prepare
large-area nitrogen-doped graphene with a controlled way. Here, we report the growthof large-area nitrogen-doped graphene using a chemical vapor deposition (CVD) with asolid precursor such as tetraphenyl porphyrin(TPP).
Figure 1 shows electron diffraction pattern and a corresponding TEM image ofgraphene using tetraphenyl porphyrin (TPP-G). 12 spots with 6-folded symmetry
appears in the diffraction pattern, which clearly demonstrates a formation of hexagonal
network of carbon. Figure 2 shows an intensity profile along the white line shown in
Fig.1. The intensity ratio of two types of spots is 1:1, which is consistent with aformation of single-layer graphene. In the presentation, we will discuss details ofsynthesis and characterizations of structure and electronic properties of TPP-G.
0-110

1-210

0-110

1-210

Fig.1 Electron diffraction pattern of

Fig.2 Intensity profile along the white line in

TPP-G Inset : TEM image of TPP-G

Fig.1

Corresponding Author: Hisanori Shinohara
Tel: 052-789-2482, Fax: 052-747-6442
E-mail: r.kitaura@nagoya-u.jp and noris@nagoya-u.jp- 84 -

1P-43In situ doping of Electrochemical foliation- Mechanismof intercalation,exfoliation and doping
Shang-Lin Tsai1, Mario Hofmann 2, Ya-Ping Hsieh1
1

Graduate of Institute of Opto-Mechatronics, National Chung Cheng University,
ROC.
2
Department of Material Science and Engineering, National Cheng Kung University,
ROC.
In the last few years graphene has become an important material in many
application areas due to its unique properties such as transparency, high thermal
conductivity, great mechanical resistance and excellent electronic conduction. Among
all of these applications the use of graphene as a transparent optical conductor (TOC)
has been considered the most promising.
To become a suitable replacement for current TOCs, a scalable production method
and higher performance of graphene TOCs are required. Common fabrication
methods rely on the chemical exfoliation of graphite which typically requires many
complicated process steps and decreases the graphene quality.
Electrochemical exfoliation has been demonstrated to be a simple, low cost andfast route for synthesizing graphene. However, the reported quality and conductivityof exfoliated graphene has not met the criteria for transparent conductive thin film
application and the mechanism of electrochemical exfoliation and intercalation is still
not well understood.
We here present an approach to combine electrochemical exfoliation withsimultaneous doping. A detailed analysis of the interaction between dopant andgraphene was performed. Intercalation of dopant between graphene planes was
confirmed through X-ray diffraction. X-ray photoelectron spectroscopic and EDS
were used to characterize the effect of electrochemical parameters on the doping
process. Raman analysis shows that under optimized exfoliation condition graphene
could maintain its high quality while being highly doped.
This work opens a route to enhance the scalability and quality of graphene
production which improves the commercial appeal of graphene for TOC applications.
Corresponding Author: Ya-Ping Hsieh
Tel: +886-52720411#23601
E-mail: yapinglab@gmail.com- 85 -

1P-44
CVD Growth of Millimeter-Sized Graphene Grains on Heteroepitaxial Cu
Kenji Kawahara,1 Tasuku Iwaizako,2 Masaharu Tsuji,1,2 and ٤Hiroki Ago1,2,3,*
1

Institute for Materials Chemistry and Engineering, Kyushu University, Fukuoka 816-8580
2Graduate School of Engineering Sciences, Kyushu University, Fukuoka 816-8580
3
PRESTO-JST

Graphene has been attracting great interest as a new type of two-dimensional atomic sheet
owing to its high carrier mobility, optical transparency, mechanical flexibility, and thermal
conductivity, which promise applications in many electronic devices. Recent progress ofchemical vapor deposition (CVD) growth offers a promising route to produce large-areagraphene with low cost. To bring out the graphene’s potential, the large-area andhigh-quality graphene growth is necessary. We have developed our original “heteroepitaxial
CVD method” to grow high-quality single-layer graphene with controlled hexagon orientation[1-5]. In this method, the graphene hexagon orientation is defined by the surface lattice ofheteroepitaxial metal films [4]. To realize the CVD growth of a single-crystalline graphenesheet, seamless connection of neighboring grains is important, but it is still under discussion[6]. Another approach is to increase the graphene’s grain size to fully cover the Cu surface.
Recently, a great progress has been achieved along this research direction [7,8].
In this presentation, we report our recent progress of large-area graphene grain growth on
crystalline Cu films deposited on single crystalline
substrates. Owing to the high Cu crystallinity andsurface flatness, we can reproducibly synthesize
mm-sized graphene grains on heteroepitaxial Cu
films by ambient pressure CVD, as shown in
Figure 1. We will also report transport propertiesof our CVD graphene. High performanceelectronic applications are expected for these large
single-crystalline graphene grains.
Figure 1 Photograph of mm-scale
References:graphene grains on the epitaxial Cu films.
[1] H. Ago et al., ACS Nano, 4, 7407 (2010). [2] B. Hu et al.,ArrowsindicategraphenegrainsCarbon, 50, 57 (2012). [3] C. M. Orofeo et al., Carbon, 50,
visualized by weak oxidation of the Cu
2189 (2012)., [4] Y. Ogawa et al., J. Phys. Chem. Lett., 3,
catalysts. Left substrate has a number of219 (2012). [5] H. Ago et al., Appl. Phys. Exp., 6, 75101
mm-sized grains, while right substrate has(2013). [6] Y. Ogawa et al., submitted. [7] Z. Yang et al.,single mm-grain on the 1 cm Cu film.
ACS Nano, 6, 9110 (2012). [8] Y. Hao et al., Science, 342,
720 (2013).
Acknowledgments:
This work was supported by JSPS-NEXT Funding Program (GR075).
Corresponding Author: Hiroki Ago (Tel&Fax: +81-92-583-7817, E-mail: ago@cm.kyushu-u.ac.jp)

Ƒ- 86 -

1P-45
Quantum interference in a ballistic graphene n-p-n junction:from Fabry-Perot to edge channel interference○Sei Morikawa1, Satoru Masubuchi1,2, Rai Moriya1,
Kenji Watanabe3, Takashi Taniguchi3, Tomoki Machida1,21Institute of Industrial Science, The University of Tokyo, Tokyo 153-8505, Japan
2
Institute of Nano Quantum Information Electronics,
The University of Tokyo, Tokyo 153-8505, Japan
3
National Institute for Material Science, Tsukuba 305-0044, Japan

We studied transport properties of a ballistic graphene n-p-n junction. The graphene was
sandwiched between two hexagonal boron-nitride (h-BN) crystals in order to eliminate themobility degradation. By tuning the back gate and top gate bias voltages, a n-p-n junction
with tunable polarity and doping levels (nb-nt-nb, respectively) was formed [Fig. 1(a)] and it
showed two types of characteristic quantum interference.
First, we studied the Fabry-Perot interference of charge carriers within the n-p-n cavity in
low magnetic fields (B < 0.5 T) [Fig. 1(b,d)]. This observation indicates the charge carriers
travelled ballistically and coherently in the cavity [1]. When a small magnetic field wasapplied, the oscillation phase was shifted by , indicating the observation of Klein Tunneling,which is the intrinsic phenomenon of Dirac fermions.
Second, we studied the anomalous magnetoresistance oscillations in the quantum Hall
regime [2]. Fig. 1(c) shows a color plot of two-terminal resistance R as a function of nt andmagnetic field B with fixed nb. Aperiodic resistance oscillations as a function of B were
emerged. These oscillations were neither periodic in 1/B (SdH oscillation) nor in B (ABoscillation), indicating the observation of novel quantum interference. We will discuss thisresult in terms of a new commensurability between the magnetic flux enclosed within the
co-propagating edge channels and the flux quantum. This is the first observation ofinterference between the edge channels along p-n interfaces [Fig. 1(e)].
(a)(d) Fabry-Perot interference

(c)

(b)

(e) Edge channel interference

Fig. 1: (a) A schematic of our h-BN/Graphene/h-BN device. (b) The Fabry-Perot interference in low magnetic
fields. (c) The edge channel interference in the quantum Hall regime. The experimental result (left) shows good
agreement with the simulated result (right). (d,e) Schematics of the two types of interference.
[1] S. Masubuchi, S. Morikawa et al., Jpn. J. Appl. Phys. 52, 110105 (2013).
[2] S. Morikawa et al., in preparation.
Corresponding Author: S. Morikawa
Tel: +81-3-5452-6158, Fax: +81-3-5452-6157, E-mail: morikawa@iis.u-tokyo.ac.jp- 87 -

1P-46
Exciton-Exciton Annihilation in Monolayer Transition-Metal
Dichalcogenides○Satoru Konabe1,2 and Susumu Okada1,2
1Graduate School of Pure and Applied Sciences, University of Tsukuba, Tsukuba, Ibaraki

305-8571, Japan

2Japan Science and Technology Agency, CREST, 5 Sanbancho, Chiyoda, Tokyo 102-0075,

Japan

Monolayer transition metal dichalcogenides (TMDs) are atomically thin layeredmaterials, which have been attracting much interest because of their remarkable electronic
and optical properties [1Ð3]. TMDs are direct-gap semiconductors with the energy gaps
within the range of visible light. Interestingly, TMDs show peculiar valley-dependent opticalselection rules; the circular polarized light can selectively excite electrons in one of the twovalleys. These valley-related phenomena make TMDs possible candidates for emerging
materials for spintronics and valleytronics devices. In addition to these striking properties,
many-body effects play a crucial role in TMDs since the screening effect is less effective in
TMDs due to their atomically thin structures, resulting in enhanced Coulomb effects.
Generally, the strong Coulomb interaction profoundly affects the excited state dynamics in
low-dimensional nanomaterials and induces the interesting nonlinear phenomena.
In the present paper, we theoretically investigate the optically excited states in TMD
and their dynamical properties focusing on the exciton-exciton annihilation by the Auger
recombination process in TMDs. Solving the Bethe-Salpeter equation based on the effectivemass theory, we first calculate the absorption spectra of TMDs, which shows the good
agreement with both the experimental observation and the previous theoretical calculations.
We then evaluate the exciton-exciton annihilation rate by the exciton Auger recombination
process using the FermiÕs golden rule with the obtained exciton states.

References:[1] A. Splendiani et al. Nano Lett. 10, 1271 (2010).
[2] K. F. Mak et al. Phys. Rev. Lett. 105, 136805 (2010).
[3] Q. H. Wang et al. Nat. Nanotechnol. 7, 699 (2012).
Corresponding Author: Satoru Konabe
E-mail: konabe@comas.frsc.tsukuba.ac.jp
Tel: +81-2-9853-5600 ext.8233- 88 -

1P-47
Edge-Roughness Effect on Electronic Transport in Semiconductor Graphene
Nanoribbons○Kengo Takashima1, Hiromu Fujii1, Takahiro Yamamoto1,2
1

Dept. of Electrical Engineering, Tokyo Univ. of Science, Niijuku-ku, Tokyo 125-8585, Japan

2

Dept. of Liberal Arts, Tokyo Univ. of Science, Niijuku-ku, Tokyo 125-8585, Japan

Graphene is expected to be a channel material of field effect transistors (FETs) because of their highcarrier mobility. However no band gap of the graphene is a serious problem for its FET application. One
possible way to overcome the gap-opening problem is to process it in the form of a nanometer width
ribbon, referred as graphene nanoribbons (GNRs). They have been successfully applied to FETs with highon-off ratio. However, the GNR-based FETs have not yet provided the best performance. A recent
experiment reported that the resistance of GNRs increases exponentially with their length even at theroom temperature [1]. This non-Ohmic behavior is due to the edge-roughness of GNRs. The effects ofedge-roughness become more remarkable when the ribbon width becomes narrower in the future.
However the electronic transport properties of such narrow GNRs have not been clarified yet.
In this study, we have computationally investigated the coherent electronic transport in narrowedge-disordered armchair GNRs (ED-AGNRs) using the nonequilibrium Green’s function method
combined with a tight-binding model. In our model, the edge roughness is modeled by removing pairs ofcarbon atoms at the armchair-type edges and ED-AGNR is connected to semi-infinite armchair GNR
leads without disorder. We calculated the conductance with various edge-disorder configurations withchanging the electron energy from -2eV to 2eV, the amount of edge carbon-pair vacancies from 4% to
30% and the ribbon-width from 0.74nm to 2.95nm.
We confirmed that the averaged conductance of ED-AGNRs decreased exponentially with their lengths,
which is consistent with a previous experimental report [2]. We also examined (i) a relation between thelocalization length ξ and the edge-vacancy concentration, and (ii) the ribbon-width dependence of ξ. As is
expected, ξ increases with decreasing the edge-vacancy concentration and with increasing the ribbon
width. Furthermore, we found ξ for holes is longer than that for electrons, i.e., the electrons tend to be
more localized than holes. The electron-hole symmetry breaking on the localization will be discussed indetail at the symposium.
[1] Xu et al., Nano Lett. 11, 1082 (2011).
[2] K. Takashima and T. Yamamoto (submitted)
Corresponding Authors: Takahiro Yamamoto
TEL&FAX: +81-3-5213-0990
E-mail: takahiro@rs.tus.ac.jp- 89 -

1P-48Temperature dependence of polarization-resolved photoluminescencein monolayer WSe2
○Lizhong Zhou1, Yuhei Miyauchi1, 2, Shinichiro Mouri1, Minglin Toh3, Goki Eda3and Kazunari Matsuda1
12Institute of Advanced Energy, Kyoto University, Uji, Kyoto 611-0011, Japan
Japan Science and Technology Agency, PRESTO, 4-1-8 Honcho Kawaguchi, Saitama
332-0012, Japan3
Department of Physics, National University of Singapore, 2 Science Drive 3,
Singapore 117542

Atomically-thin transition metal dichalcogenides (TMDs) such as MoS2 and WSe2
have attracted much attention as novel 2D semiconductors with remarkable physicalproperties [1-3]. In contrast to graphene with no band gap and centrosymmetricstructure, monolayers of the TMDs are non-centrosymmetric materials with a direct
band-gap located at the energy-degenerate K and K’ valleys in momentum space. The
structural inversion asymmetry in the 1L(monolayer)-TMDs gives rise to coupling ofelectron spin and valley degree of freedom; this characteristic enables valley-selective
optical excitation in these materials using circular-polarized incident photons [1].
Therefore, the 1L-TMDs are promising materials for “Valleytronics”, future
optoelectronics technology using valley degree of freedom of electrons.
Here we study temperature dependence of polarized photoluminescence (PL) in
1L-WSe2 [2] to understand spin-valley relaxation mechanism between the degenerate K
and K’ valleys. In the experiment, circular polarization of the incident photons was set
to beσ+ polarization (corresponding to selective excitation of K’ valley), andσ+ andσcomponents of the PL signals were separately detected.
Figure 1 shows the polarization-resolved PL spectra at
15 K. The PL intensity of theσ+ emission is larger thanthat of σ- emission under theσ+ excitation condition,suggesting spin-valley polarization in 1L-WSe2 at 15 K.
Temperature dependence of the observed valley
polarization and its mechanism will be discussed.
[1] K. F. Mak et al., Nature Nanotech. 7, 494 (2012).
[2] W. Zhao et al., ACS Nano 7, 791 (2013).
[3] S. Mouri, Y. Miyauchi, and K. Matsuda, Nano Lett. 13, 5944 (2013).
Corresponding Author: L. Zhou

Fig.1 Polarization-resolved PL
spectra of 1L-WSe2 at 15 K.

E-mail: zhou.lizhong.46a@st.kyoto-u.ac.jp- 90 -

1P-49Nonlinear Photoluminescence Properties
in Monolayer Transition Metal Dichalchogenides
Shinichiro Mouri1, Lizhong Zhou1, Yuka Tsuboi1, Yuhei Miyauchi1,2, Minglin Toh3,
Satoru Konabe4, Goki Eda3, Susumu Okada4, and Kazunari Matsuda1
1Institute of Advanced Energy, Kyoto University, Uji, Kyoto 611-0011, Japan
Japan Science and Technology Agency, PRESTO, 4-1-8 Honcho Kawaguchi, Saitama
332-0012, Japan3
Department of Physics, National University of Singapore, 2 Science Drive 3, Singapore
4Graduate School of Pure and Applied Sciences, University of Tsukuba, Tsukuba, Ibaraki
305-8571, Japan
2

Monolayer transition metal dichalcogenides (TMDs) have been attracted much attention as anovel two-dimensional direct band gap semiconductor [1], and are also a promising candidate
to realize the ultra-thin opto-electronic devices [2]. Strong Coulomb interactions due to thequantum confinement effect in ultra-thin materials would give rise to intriguing many-bodyeffects among optically generated carriers [3,4]. In this study, we investigated theexciton-exciton interactions in TMDs through optical nonlinearity and exciton dynamics.
Figure 1 (a) shows the photoluminescence (PL) spectraof monolayer (1L) WSe2 with increasing excitation power
density. The peak around 1.66 eV is originated fromexciton (X) PL. As shown in the inset of Fig. 1 (a), theintegrated exciton PL intensity is gradually saturated withincreasing excitation power density. Exciton PL decay
profiles at each excitation power density are plotted inFig. 2. The exciton recombination time of 1L-WSe2 isestimated as ~3 ns from the data of weak excitation
region (0.0085 ȝJ/ȝm2). On the other hand, rapid decay
component (<500 ps) due to exciton-exciton annihilation
Fig. 1 Excitation power density(EEA) becomes dominant with increasing excitation
dependent PL spectra of 1L
1L-WSe2.
power density. From these results, we will discuss thedetail mechanism of exciton-exciton scattering in TMDs
based on the Monte-Calro simulation and the EEA rate
calculated using Bethe-Salpeter-equations.
[1] A. Splendiani et.al. Nano Lett. 10, 1271 (2010).
[2] Q. H. Wang et.al. Nat. Nanotechnol. 7, 699 (2012).
[3] K. F. Mak et.al. Nat. Mater. 12, 207 (2012).
[4] S. Mouri et.al. Nano Lett. 13, 5944 (2013).
Corresponding Author: Shinichiro Mouri
Tel: +81-774-38-3463,
Fax: +81-774-38-3467,
E-mail: iguchan@iae.kyoto-u.ac.jp

Fig.2 Decay profile of exciton PL of
1L-WSe2 at each exciton power.

- 91 -

1P-50
Photoluminescence Imaging of Monolayer MoS2 Synthesized by
Chemical Vapor Deposition Method
1

1

1,2

1

○Yuka Tsuboi , Daichi Kozawa , Yuhei Miyauchi , Shinichiro Mouri ,Kazunari Matsuda1
12Institute of Advanced Energy, Kyoto University, Uji, Kyoto 611-0011, Japan
Japan Science and Technology Agency, PRESTO, 4-1-8 Honcho Kawaguchi, Saitama
332-0012, Japan
Two-dimensional transition metal dichalcogenide, MX2 (M=Mo,W, S=S,Se) has

been extensively studied from the viewpoint of fundamental physics and optoelectronic
applications. The atomically-thin monolayer MoS2 is a direct band-gap semiconductor
showing photoluminescence (PL). Very recently, the fabrications of large scalemonolayer MoS2 by chemical vapor deposition (CVD) have been reported [1]. However,the PL properties of these CVD grown MoS2 have not been fully understood. In thisstudy, we investigated PL properties of monolayer MoS2 synthesized by CVD.
Monolayer MoS2 with a triangle shape on SiO2 substrate was fabricated by CVD
method [1]. The fabricated monolayer MoS2 shows PL around 1.8 eV [2]. The obtained
PL images in the insets of Figure 1(a) and 1(b) clearly show the triangular shapes
reflecting the shape of monolayer MoS2. There are two types of triangle MoS2 flakes inthe spatial PL mapping; one shows stronger PL at the edge of triangle flake in Fig. 1(a)and the other shows that at the inside of flake in Fig. 1(b). The PL spectra at various
positions of the triangular flakes are also shown. It is found that PL peak energy in Fig.
1(a) slightly changes. We will discuss the physical mechanism of difference of PL
properties depending on the
432
(b)
(a)
4 32
flakes based on detail PL1
1
1
imaging measurement.
[1] C. Cong, J. Shang, X. Wu, et al.,arXiv:1312.1418 (2013).
[2] S. Mouri, Y. Miyauchi, and K.
Matsuda, Nano Lett. 13, 5944,(2013).

+11

Corresponding Author: Y. Tsuboi
Tel: +81-774-38-3465
Fax: +81-774-38-3467
E-mail:tsuboi.yuka.72w@st.kyoto-u.ac.jp

[10

]

PL Intensity (arb. units)

[10

+11

]

2

4
3
2

3

4

1
0

1.7
1.8
1.9
Photon Energy [eV]0

2.0 1.7
1.8
1.9
Photon Energy [eV]2.0

Fig. 1(a),(b) Normalized PL spectra measured at various
points of the flakes. The insets show the PL images ofmonolayer MoS2 flake (scale bar: 10 m).

- 92 -

2P-1
Investigation of molecular dynamics of fullernol solids by ²H NMR
spectroscopy○Yoshiaki Sano1, Keisuke Baba 2, Hironori Ogata 1,2
Graduate School of Engineering, Hosei University, Tokyo 184-8584, Japan2
Department of Faculty of Biosci. and Applied Chem.,Hosei University,Tokyo184-8584, Japan
1

Fullerenols (Polyhydroxylated Fullerene: C60(OH)x) have been a subject of intense
research in many fields with the claim of possible applications in a variety of areas, including
optoelectronics, medical therapeutics, biotechnology, chemical mechanical polishing, and fuelcells, owing to their high solubility in a large variety of solvents (depending on the number ofhydroxyl groups, x). It was reported that C60(OH)n (n~12) show proton conductivity and theirapplications for the proton conducting membrane of a polymer electrolyte fuel cell (PEFC)
is proposed. However, their proton conduction mechanism has not been thoroughly studied
yet. We previously reported the proton dynamics in both C60(OH)13.5 and C60(OH)38.7(O)1.6
solids by means of 1H-solid-state NMR[4] and it was clarified that the formation of bothinteramolecular and intermolecular hydrogen-bond networks had a large influence on their
proton dynamics at low temperature. In this study, we investigated to get more detailed proton
dynamics by using 2H-NMR of deuterated fullerenols.
The detailed results about their proton dynamics will be presented.

References:[1] Hinokuma et. al., Chem. Phys. Lett., 341, 442 (2001)[2] Chiang et al., Org. Chem. 59, 3960 (1994).
[3] Kokubo et al., Nano Res., 4, 204 (2011)[4]K.Baba et al, Proc.of the 44th Fullerene-Nanotubes-Graphene General Symposium(1-5).
Corresponding Author: H. Ogata
Tel: +81-42-387-6229, Fax: +81-42-387-6229,
E-mail: hogata@hosei.ac.jp- 93 -

2P-2
Synthesis of a Novel Open-cage C60 Derivative with a Ketolactam MoietyżYoshifumi Hashikawa1, Michihisa Murata1, Atsushi Wakamiya1, Yasujiro Murata1,21Institute for Chemical Research, Kyoto University, Uji, Kyoto 611-0011, Japan
2
JST, PRESTO, 4-1-8 Honcho, Kawaguchi, Saitama 332-0012, Japan

Open-cage fullerene derivatives1 have been attracting considerable attention because they
are interesting molecules for host-guest chemistry and can be used as precursors forendohedral fullerenes encapsulating an atom or small molecules. However, reports on theirsynthesis are still limited. We have previously synthesized several open-cage C60 derivatives,
which can encapsulate a He atom, H2 molecules, and an H2O molecule.2 Ketolactam 1, one of
the reported open-cage C60 derivatives,3 is known as a precursor for azafullerenes such as(C59N)2.4 However, the size of the opening is too small for insertion of even a He atom.
Herein, we studied its reaction in order to enlarge the opening.
Novel open-cage C60 derivative 4 was
obtained in 40% yield by the reaction of 1 with
N-methylmorpholine N-oxide (NMO) ino-dichlorobenzene (ODCB) in the presence ofa small amount of water (Scheme 1). The
structural assignments of 4 were conducted by
APCI MS, 1H and 13C NMR, UV-vis, and IR
spectra, in addition to theoretical calculations.
It is supposed that the epoxidation of 1, as thepossible first step of this reaction, takes place
at one of the C=C double bonds a, b, c, or d.
Thetheoretical
calculationsatthe
B3LYP/6-31G* level of theory demonstrated
that the LUMO is relatively localized at the
butadiene unit (C1=C2–C3=C4) including
bonds a and b, and that epoxide 2 formed by reacting on a is 9.0 kcal/mol more stable thananother epoxide formed by reacting on b. Then, compound 2 is thought to react with thesecond NMO to give 3, which affords 4 by the addition of an H2O molecule.5
The chemical reactivity of 4 was studied. The reaction of 4 with 20-fold trifluoroacetic
anhydride at room temperature for 3 h gave tetraketo derivative 3. In addition, 4 wasconverted to original 1 in 70% yield by treatment with triphenylphosphine in toluene.
Structures and encapsulation behaviors of these open-cage C60 derivatives will be presented indetail.
[1] Vougioukalakis, G. C.; Roubelakis, M. M.; Orfanopoulos, M. Chem. Soc. Rev. 2010, 39, 817.
[2] Murata, M.; Murata, Y.; Komatsu, K. In Organic Nanomaterials: Synthesis, Characterization, and Device
Applications; Torres, T., Bottari, G., Eds.; John Wiley & Sons: West Sussex, U.K, 2013, pp 225–239.
[3] Hummelen, J. C.; Prato, M.; Wudl, F. J. Am. Chem. Soc. 1995, 117, 7003.
[4] Hummelen, J. C.; Knight, B.; Pavlovich, J.; González, R.; Wudl, F. Science 1995, 269, 1554.
[5] Kurotobi, K.; Murata, Y. Science 2011, 333, 613.
Corresponding Author: Y. Murata
Tel: +81 774-38-3172, Fax: +81 774-38-3178,
E-mail: yasujiro@scl.kyoto-u.ac.jp- 94 -

2P-3
A Novel Ligand-free ZnO Particle for Fullerene:Polymer Inverted Organic
Solar Cell
○ Il Jeon1, James W. Ryan1, Kee Sheng Yeo1, Tafu Nakazaki2, Yuichi Negishi2 and Yutaka
Matsuo1
12

Department of Chemistry, The University of Tokyo, Tokyo 113-0033, Japan
Department of Applied Chemistry, Tokyo University of Science, Tokyo 162-8601, Japan.

Organic solar cells are drawing much attention as thenext-generation solar cells on account of their cost effectiveness,lightweight, and flexibility with its high power conversion
efficiency. [1] Its shortcoming of low stability is now resolved byapplying the inverted structure. [2] Recently, zinc oxide (ZnO)
nanoparticles have been a popular choice for use as interlayers in Fig. 1. Inverted Organic Solar
Cell with ZnO layer
organic thin film solar cells, due to its favorable energy levels, aswell as its solution-processability. The ZnO nanoparticles not only
possess a work function that matches well with acceptor materials(e.g. PCBM)[3] but also exhibit high electron mobility. In addition,
ZnO is not as dependent on UV light activation like in the case of
TiO2.[4] Unlike conventional ZnO thin film fabrication, where highenergy and high temperature are required, ZnO nanoparticles can beapplied to device with much mild conditions. However, current Fig. 2.TEM image at 150,000x
magnification
ZnO nanoparticles synthesis needs ligands to stabilize them and in
turn, requires higher temperature around 150 ûC to remove the insulating ligand remnants. In
our research we introduce a novel ZnO nanoparticle synthesis, which is ligand free andconsequently leading to ZnO film with no annealing temperature required, making theflexible device application more facile.
For generation of ZnO, following the heating of zinc acetate precursor in amino-ethanol
under reflux, the reaction mixture is centrifuged, to separate the precipitate that contains
larger ZnO particles. Table 1. Optimal OSC Device performance both ZnO sol-gel (ref.) and ZnO
The supernatant in nano particles based devices according to their annealing temperatures
Annealing
this case will contain
ECL
VOC (V) JSC (mA/cm2)
FF
Rs(Ω)
Rsh(Ω)PCE (%)
Temperature
well-dispersed ZnO
200 ¡C
0.60
9.42
0.56
5.71
2.23E+04
3.2
nanoparticlesof ZnO sol-gel
average size of 2.5 ZnO sol-gel No Anneal
0.01
0.03
0.25
280
3.54E+02
0.0
nm, as observed via
ZnO np
No Anneal
0.61
9.08
0.56
8.29
1.66E+04
3.1
TEM. (Fig. 2) The
ZnO np120 ¡C
0.62
9.13
0.53
8.43
1.54E+04
3.0
experimental results
ZnO np150 ¡C
0.62
8.65
0.53
8.35
1.27E+04
2.9
compared to theconventional sol-gel
ZnO np180 ¡C
0.61
7.98
0.45
9.77
1.22E+04
2.2
method are given in
ZnO np210 ¡C
0.59
6.91
0.34
20.11 1.12E+04
1.4
Table 1.
[1] X. Yang et al., Adv. Mater. 24 1202 (2012), [2] A.K.K. Kyaw et al., Appl. Phys. Lett. 93 2211071 (2008), [3]L. Dou et al., Nature Photon. 6, 180 (2012), [4] J. You et al., Adv. Mater. 24, 5267 (2012)
Corresponding Author: Professor Y. Matsuo
Tel: +81-3-5841-1476
E-mail: matsuo@chem.s.u-tokyo.ac.jp- 95 -

2P-4
Synthesis of Penta(aryl)[60]fullerene Cobalt Dithiolene Complexes
for Organic Solar Cells○Keisuke Ogumi, Takafumi Nakagawa, Yutaka Matsuo
Department of Chemistry, The University of Tokyo, Tokyo 113-0033, Japan
Introduction
The transition metal fullerene complexes frequently have been studied because of theirinteresting chemical properties. Cobalt trisulfide fullerene complex 1 had 4-membered ringfrom cobalt and trisulfide [1]. This organometallic ring exhibited an aromatic 6π-electron
system. Thus, this complex possessed antithetical properties, the stability from aromaticity
and the reactivity from distortion of 4-membered ring. This complex also showed distinctive
structure which has bowl-shape derived from fullerene and five substituents. Cobalt trisulfide
fullerene complex 1 was consequently prominent starting material because of specificreactivity and structure [2].
This work
Novel cobalt dithiolene complexes Scheme 1. Synthesis of cobalt dithiolene complexes.
2-8 were obtained from starting material
penta(aryl)[60]fullerene cobalt trisulfide[C6H5S]222827%
complex and corresponding disulfides
]
2
50%
S
[4H4
FC
through a process of SÐS bond cleavage
C6
6H
2
O
4 S]
N
2
2
[
and CÐH bond activation (Scheme 1).
1
Their electrochemical properties were
7
3
19%
15%
tuned by the dithiolene ligand moiety(Figure 1).
64Complexes
2-8
showedlong
32%
16%
wavelength absorption and the stability
5
due to aromaticity in pentagonal cobalt
21%
dithiolene rings. These properties
suggested complexes 2-8 were suitablematerials for organic solar cells.
Photovoltaic devices using complexes
2-8 acted as electron acceptors inorganic solar cells. AFM observations
revealed that the dithiolene ligand
moiety influenced on film morphology
and device performance. Complex 8
having bulky naphthalene dithiolene
Figure 1. HOMO-LUMO levels of 2-8.
ligand moiety gave 0.59% PCE. These
complexes will expand organometallic
fullerene chemistry in organic solar
cells.
S[4-tBuC6H4S]2
S[1] M. Maruyama. et al. J. Am. Chem. Soc. 2011, 133, 6890Ð6893.
[2] M. Maruyama. et al. Angew. Chem. Int. Ed. 2013, 52, 3015Ð3018.
Corresponding Author: Y. Matsuo
Tel: 03-5841-1476, Fax: 03-5841-1476, E-mail: matsuo@chem.s.u-tokyo.ac.jp- 96 -S
Co
C60Ar5S] 2

SCo
C60Ar53S

S
Co
C60Ar5

F

C 6H
-F 2

NH
Co
C60Ar5

S

[3,4

S

6H
11 S
]2

S
Co
C60Ar5

[C

S

S
S S
Co

F

F

S

S
Co
C60Ar5S

S
Co
C60Ar5

2P-5
Characterization of surface layer of C60 thin-film polymerized by
optical vortex○Wataru Akiyama1, Daiki Momiyama1, Naoto Toriumi1, Naoto Nakamura1,
Katsuhiko Miyamoto1, Takashige Omatsu1,2, Jonathan P. Bird3, Yuichi Ochiai1,
and Nobuyuki Aoki1,41

Graduate School of Advanced Integration Science, Chiba University,
Chiba, 263-8522 Japan
2
JST-CREST, 4-1-8 Honcho Kawaguchi, Saitama 332-0012, Japan3
Department of Electrical Engineering, University at Buffalo, SUNY, Buffalo, NY
14260-1920, USA
4
JST-PREST, 4-1-8 Honcho Kawaguchi, Saitama 332-0012, Japan
Recently, a state of the art photo-polymerization of a C60 thin film has been realizedby irradiation of topological laser beam namely optical vortex (OV). Since the beam has
a helical wavefront and a torque appears along the tangential direction, a confinement
force can be expected along the peripheral direction of the beam and the polymerization
takes a progress with a compressive photon-pressure under a high-beam-power density.
Therefore, it can be expected to achieve unusual photo-polymerization mechanism in a
C60 thin film. Moreover, combining with circular polarization, total angular momentumof light can be controlled [1].
In our study, thermally evaporated C60 thin film was deposited 100 nm on a SiO2
layer on top of a heavily doped Si substrate. A continuous-wave laser beam (λ = 532nm) was used for the optical source. The OV was produced by using a spiral phase plateand irradiated onto the sample through an objective lens. The photo-polymerization was
done at high-vacuum condition.
In the observation of the surface of the C60 thin film by atomic force microscope, verythin layers having a thickness of 5~6 nm covering the grains of C60 were observed after
the OV irradiation. Taking care of the fact, in-situ transport characteristics (top-contact
condition) were observed in a vacuum probe station after the irradiation of the OV. The
transfer characteristic after a dose of 30 MJ/cm2 shows a linear current-voltage
characteristic and no dependence on the sweep of the back gate voltage, which isdifferent from the usual semiconducting characteristic of a C60 photo-polymer. It
suggests that a metallic layer might be realized on the top of the thin-film after theheavy dose of OV irradiation.
[1] T. Omatsu et al., Opt. Express 18 (2010) 17967.
Corresponding Author: W. Akiyama
Tel: +81-43-290-3430, Fax: +81-43-290-3427,
E-mail: adsa3781@chiba-u.jp- 97 -

2P-6
Extraction and Isolation of Missing Small-Bandgap Metallofullerenes
through Exterior Functionalization○Zhiyong Wang, Yusuke Nakanishi, Shoko Noda, Hiroyuki Niwa, Jinying Zhang, Ryo
Kitaura, Hisanori Shinohara
Department of Chemistry and Institute for Advanced Research, Nagoya University, Nagoya
464-8602, Japan
C60 and C70 are the most stable members in the fullerene family. However, thecorresponding endohedral fullerenes M@C60 and M@C70 (M = rare-earth metal) are missing
in conventional extract of arc-produced fullerene soot. Besides M@C60 and M@C70, there area large number of other missing, the so-called small-bandgap (or small HOMO-LUMO gap)
metallofullerenes such as M@C72, M@C74, etc. These metallofullerenes are chemicallyunstable due to their open-shell electronic configurations or small bandgaps, and they tend toform insoluble polymerized solids in the raw soot.
Here, we report in situ exterior functionalization of the small-bandgap metallofullerenes
using a modified arc-discharge method [1]. Solid polytetrafluoroethene (PTFE) is used as asource for the functional groups. A series of trifluoromethyl derivatives of small-bandgap
metallofullerenes M@C2n(CF3)m (2n = 60, 70,
72 or 74; m = 1 or 3) are formed effectively.
Surprisingly, these derivatives, including thoseof M@C60 and M@C70, are totally soluble andstable in conventional fullerene solvents (Fig.
1). A C70-based metallofullerene (Y@C70) is
solvent extracted and isolated for the first timeever since the first macroscopic synthesis of
metallofullerenes
in1991.
Theoretical
calculations demonstrate that trifluoromethyl
functionalization of Y@C70 induces a large
bandgap opening and thereby gives rise to astable metallofullerene.
This method can be applied to any rare-earth
metals. Similar results have been obtained in
the present laboratory for metals of Y, La, Gd,
and Dy.
[1] Z. Y. Wang et al. Angew. Chem. Int. Ed. 52,
11770-11774 (2013).
Corresponding Author: H. Shinohara
Fax: +81-52-747-6442,
E-mail: noris@nagoya-u.jp

Fig. 1. Laser desorption time-of-flight mass
spectra for (a) o-xylene extracted mixture and (b)separated metallofullerenes (the observed Y@C2nions are actually fragments of Y@C2n(CF3)m).
DFT-optimized

molecular

Y@C70 and (d) Y@C70(CF3)3.

- 98 -

structures

of

(c)

2P-7
Supercapacitor using Lithium-Ion Endohedral Metallofullerene○Eunsang Kwon1, Ken-ichirou Komatsu1, Yoichi Yamada2, Yuri Hasegawa2, Sho Sato2, Seiji
Sakai3, Kazuhiko Kawachi4, Kuniyoshi Yokoo4, Shoichi Ono4, Yasuhiko Kasama4, Shinobu
Aoyagi5, Tomoaki Endo6, Tomoyuki Ogawa7, Migaku Takahashi71

Research and Analytical center for Giant Molecules, Graduate School of Science, Tohoku
University, Sendai, 980-8578, Japan
2
Institute of Applied Physics, University of Tsukuba. 1-1-1 Tennodai, Tsukuba, Ibaraki,305-8573, Japan
3
Advanced Science Research Center, Japan Atomic Energy Agency, Japan
4
Idea International Co., Ltd, 981-0922, Japan
5
Nagoya City University, Nagoya 467-8601, Japan
6
Sendai National College of Technology, 981-1239, Japan
7
NICHe, Tohoku University, Sendai 980-8579, Japan

Since the synthesis and characterization of (a)(b)
lithium cation endohedral metallofullerene (licfullerene) [1], several investigations have been
performed on the application of the “lic fullerene”
to the functional materials [2]. However, there has
been no study on the application of the “licFig. 1. (a) A photograph of an interdigital Au
fullerene” to the energy storage systems.
In the present work, we investigated the energy electrode. (b) AFM image of thestorage characteristics of Li+@C60 capacitor. The Au(111)/-Al2O3(0001) electrode showing
ortho-dichlorobenzene (o-DCB) solution of surface roughness of Au.
Li+@C60•PF6- in different concentrations, ranging
from 0.1 to 1.0 mmol/L, and interdigital Au
electrode (Fig. 1) were used for the measurements.
The o-DCB solution of TBA+•PF6- was used forcomparison under the same experimental
conditions.
As shown in Fig. 2, the energy stored by
Li+@C60/o-DCB capacitor was greater by several
times than that stored by TBA+/o-DCB capacitor
under the same conditions. This result indicatedthat TBA+ ions undergo solvation and the size of Fig. 2. Charge versus voltage plot of Li+@C60
the solvated TBA+ would be larger than that of • PF6-/o-DCB (1.0 mmol/L) capacitor
Li+@C60 ions. Moreover, the charging speed of (triangles), TBA+•PF -/o-DCB (1.0 mmol/L)
6
Li+@C60/o-DCB capacitor was faster than that of
TBA+/o-DCB capacitor. This would originate from capacitor (squares) and o-DCB (circles).
the shape of Li+@C60 ion having a spherical structure.
[1] S. Aoyagi et al., Nature Chemistry, 2, 678 (2010). [2] For recent reports, see: K. Ohkubo et al., Chem.
Commun., 49, 7376 (2013); K. Kokubo et al. Nanoscale, 5, 2317 (2013); K. Ohkubo et al. Chemical Science, 4,1451 (2013).
Corresponding Author: E. Kwon
Tel: +81-22-795-6752, Fax: +81-22-795-6752, E-mail: ekwon@m.tohoku.ac.jp- 99 -

2P-8
Spin-state Tuning of Deca-Methyl C60 by an Electric Field○Kohei Narita and Susumu Okada
Graduate School of Pure and Applied Sciences, University of Tsukuba
1-1-1 Tennodai, Tsukuba, Ibaraki 305-8571, Japan
Electronic structure of carbon allotropes with the three-fold coordination depends on theirmorphology, dimensionality, size, and boundary condition. Indeed, chemical modifications on
fullerenes result in interesting π electron systems on the spherical networks. For instance,deca-organo C60 possesses interesting geometric and electronic structures arisen fromchemical modification on C60 by ten aromatic molecules [1]. Attached aromatic molecules
divide spherical π electron system into three parts: a short armchair nanotube and two
pentagonal rings surrounded by molecules. According to these two pentagonal rings, this C60
derivative has two radical spins localized at these pentagonal rings, which are coupled in ananti-parallel manner in their ground state [2]. In this work, we explore the possibility of thespin-state tuning of the radical spins in deca-methyl C60 by an external electric field in theframework of first-principles electronic structure calculations.
By applying the normal electric field to the pentagonal rings surrounded by the methylgroups, we find that the energy difference between the total energies of the parallel andantiparallel spin states gradually decrease with increase of the electric field (Fig. 1). Finally,at the electric field of 0.07 V/A, the total energy of the parallel state is the same as that of the
antiparallel arrangement indicating that the spin-flip process occurs in terms of the external
electric field. In(a)(b)
sharp contrast, suchspin-flip
process
does not occur
under the parallel
electric field to thepentagonalrings
possessing radical
spins. Based on the
result, we conclude
the possibility ofmagnetic-statetuning of the radical
spin in deca-methyl
C60 by the electric Fig. 1 (a) Geometric structure of deca-methyl C60 sandwiched by two electrons.
(b) Energy difference between the total energies of the parallel and antiparallel
field..
spin configuration.

References[1] E. Nakamura, et al. J. Am. Chem. Soc. 125 (2003) 2834.
[2] H. Nitta et al. Appl. Phys. Express. 6 (2013) 045102
Corresponding Author: K. Narita
Tel: +81-29-853-5921, Fax: +81-29-853-5924
E-mail: sokada@comas.frsc.tsukuba.ac.jp- 100 -

2P-9
Geometric and electronic structures of two-dimensionally polymerized C32!Mina Maruyama and Susumu Okada
Graduate School of Pure and Applied Sciences, University of Tsukuba, Tennodai, Tsukuba 305-8577, Japan

Fullerenes are kwon to form covalent networks of C atoms with one-, two-, andthree-dimension in which the fullerenes are tightly bound each other via covalent bonds
between adjacent molecules by introducing the four-fold coordinated C atom. According to
the intermolecular covalent bonds, these condensed phases of fullerenes could be classified asa novel carbon allotropes consisting of both sp2 (three-fold coordinated) and sp3 (four-foldcoordinated) C atoms. Electronic structures of these sp2 - sp3 hybrid carbon allotropes
strongly depend on their dimensionality and morphologies leading to peculiar electronic
structure at/around Fermi level. Among the possible fullerenes, small fullerenes whose cluster
sizes are smaller than C60 are also regarded as possible constituent units for such covalent
networks of sp2 and sp3 carbon atoms because of their remarkable chemical reactivity arisingfrom the large curvatures. Indeed, in our previous calculations, we demonstrated that the C26
and C28 fullerenes form two and three-dimensional covalent networks, respectively, as theirstable condensed forms with interesting diversity in their electronic structures. In the present
work, we theoretically design two-dimensional covalent networks with hexagonal symmetrycomprising small fullerene C32 with D3h symmetry based on the first-principles total-energy
calculations in the framework of the density functional theory (DFT).
Figure 1 (a) shows an optimized structure of two-dimensionally polymerized C32. As
shown in figure, C32 forms a two-dimensional honeycomb network with covalent bond
between C32 as in the case of graphene sheet. We find that polymerized C32 is asemiconductor with a direct energy gap of 1.3 eV. For this sheet, we examine the possibilityof molecular doping of the other small fullerene C36 [Fig. 1 (b)]. The doped structure isenergetically stable and is a metal with relatively small dispersion band at the Fermi level.
!$#

!"#

Fig. 1 Geometric structures of (a) the polymerized C32 and (b) the two-dimensional networkof polymerized C32 with additional C36.
Corresponding Author: M.Maruyama
Tel: +81-29-853-5600, Fax: +81-29-853-5924,
E-mail: mmaruyama@comas.frsc.tsukuba.ac.jp- 101 -

2P-10Electronic structure change of single-walled carbon nanotube
by X-ray irradiation  ○Toshiya Murakami1, Yuki Yamamoto1, Mitsuaki Matsuda1, Kenji Kisoda2,
Hiroshi Nishigaki3, Noriyuki Hasuike3, Hiroshi Harima3, Chihiro Itoh1

1

Department of Materials Science and Chemistry, Wakayama University, Wakayama,640-8510, Japan2
Department of Physics, Wakayama University, Wakayama, 640-8510, Japan3
Department of Electronic, Kyoto Institute of Technology, Kyoto, 606-8585, Japan

Because of strong correlation of the electronic structure with geometric structure of
single-walled carbon nanotubes (SWNTs), structural modification by ionizing radiation canbe utilized as a tool to modify the SWNTÕs electronic structure. We have shown that X-ray
irradiation gives rise to the formation of vacancy and interstitial pairs (Frenkel defects) in
SWNTs, which eventually leads to their structural change.[1] The formation efficiency andthermal stability of X-ray-induced defects were shown to depend on the number and helicityof layer of tubes.[2] However, the irradiation effects on the SWNTÕs electronic structure has
been left to be ambiguous. In this report, we have shown the results of the multi-probe
resonant Raman spectra of the X-ray-irradiated SWNTs and discuss the irradiation effect on
the electronic structure of SWNT.
SWNTs grown by chemical vapor deposition were irradiated by X-ray (Kα line of Mg) in
vacuum. Resonant Raman spectra were measured with the excitation wavelengths of 532,
561, 568, 647, and 660 nm.
Figure 1(a) shows the radial breathing modes (RBMs) in Raman spectra of the SWNTs
before X-ray irradiation. Figure 2 is an RBM map of pristine SWNT drawn based on theexperimental spectra shown in Fig. 1 with simulating the spectral features according to theprevious reports. The resonant Raman spectra of the X-ray-induced samples can be
reproduced from Fig. 2 by considering that the optical transition energy contributing theresonance is reduced by 0.05 eV by the X-ray irradiation. The simulated resonant Raman
spectra thus obtained are shown by dotted curves in Fig. 3. This result is consistent with theresults of optical absorption measurements. On the basis of these results, we have concluded
that the X-ray irradiation modifies electronic structure of SWNTs.

[1] Murakami, et. al., Eur. Phys. J. B 86,187 (2013)[2] Murakami, et. al., J. Appl. Phys. 114, 114311 (2013)

Corresponding Author: T. Murakami, Tel: +81-73-457-8532, E-mail: murakami@sys.wakayama-u.ac.jp- 102 -

2P-11Anharmonic effects on phonons in single-walled carbon nanotubes○Masashi Mizuno,1 Riichiro Saito1
1

Department of Physics, Tohoku University, Sendai 980-8578, Japan

Graphene and carbon nanotubes are promising materials for their outstanding physicalproperties, i.e., thermal conductivity, etc. [1]. However, the analytical forms of theseproperties are not well understood yet [2-4]. To calculate thermal conductivity accurately, we
have to take anharmonicity (cubic or higher order terms) of interatomic potential [5,6] into
account [7], so the problem is non-linear. With anharmonicity, phonon states are no longer the
eigenstates of crystal and phonons have finite lifetimes, which make the thermal conductivity
a finite value. The main purpose of this research is to understand anharmonic effects onphonons in carbon nanotubes for getting better understanding of thermal conductivity and line
broadening in phonon spectra.
There are two approaches for this study: classical and quantum method. Classical way issolving the classical equations of motions for crystal atoms numerically and applying Fourier
analysis to observe phonons’ behavior. Quantum way is to treat anharmonic interactions as
perturbations, but this research is at an early stage now.
From study on classical one-dimensional chain with anharmonic potential, it is found thatthe frequencies and wavenumbers of scattered phonons are mixing of those of initial phonons,
and these mixing rules can be found formally in equations of motions as cross-terms.
Also looking at the shape of the potential, it is found that the hexagonal lattice is relevant
to anharmonicity especially for bond-stretching mode, which determines the mean free pathsof in-plane phonons. Therefore, thermal conductivity may depend on crystal direction or
chirality of a carbon nanotube. In the presentation, we show how to make anharmonic
potential terms and some preliminary calculations.
[1] R. Saito, et al., Physical Properties of Carbon Nanotubes, Imperial College Press, London (1998).
[2] J. Shiomi, et al., Int. J. Thermophys. 31, 1945–1951 (2008).
[3] L. Paulatto, et al., Phys. Rev. B. 87, 214303 (2013).
[4] Chen S, et al., Nat. Mater. 11, 203 (2012).
[5] L. Lindsay, et al., Phys. Rev. B 81, 205441 (2010).
[6] V. K. Tewary, et al., Phys. Rev. B 79, 075442 (2009).
[7] G. P. Srivastava, The Physics of Phonons, Taylor & Francis, New York (1990).
Corresponding Author: M. Mizuno
E-mail: mizuno@flex.phys.tohoku.ac.jp- 103 -

2P-12The Analysis of Exchange Reactions of Sodium Cholate andDouble-Stranded DNA on Single -Walled CNTs
○Akiko Tsuzuki1 and Naotoshi Nakashima1,2,3
1

Department of Applied Chemistry, Graduate School of Engineering, Kyushu University,
744 Motooka, Nishi-ku Fukuoka, 2 WPI I2CNER, 3 JST-CREST,

Deoxyribonucleic acid (DNA) is one of the well-known solubilizers of single-walled carbon
nanotubes (SWNT). The DNA-SWNT hybrids have attracted much research. There are many
applications of the hybrids. Bio-sensors, electron (A)(B)
transfer, length fractionation, and chirality separationof SNWTs are the typical examples. Previously, we
reported quantitative evaluation of the exchange
reactions between sodium cholate (SC) andsingle-stranded DNA (ssDNA) on SWNTs [1,2]. In
this work, the interaction of ssDNA anddouble-stranded DNA (dsDNA) on SWNTs was
Figure 1 Equilibrium constants (A) andstudied.
thermodynamic parameters (B) of exchanges of
CNTs were solubilized by sonication in a SC
SC for the d(A)20, d(T)20, d(G)20, d(C)20.
solution (2 mM). After centrifugation (120,000 ×g, 3h), the supernatant was used as a solubilized-CNT(B)solution. Two ssDNA solutions, NF-B decoy sense (A)
that
have
such
nucleotide
sequence,
5’-CCTTGAAGGGATTTCCCTCC-3', and NF-B
decoy anti-sense which have the complementary
sequence of NF-B decoy sense, were mixed andstored for one hour at 80 °C to prepare dsDNA. The
CNT solution with TE buffer was mized with various
concentrations of DNAs (20-mers, d(A)20, d(T)20,
Figure 2
Equilibrium constants (A) andd(G)20,d(C)20, NF-B decoy sense, NF-B decoy
thermodynamic parameters (B) of the exchanges
anti-sense, 0-800 M, and dsDNA of NF-B decoy,of SC for the double stranded (ds) NF-B and its
0-400 M). The solutions were stored for three days
single strands.
at a temperature of 15, 20, 25, 30, 35, or 40 °C, andthen absorption spectra were measured using a UV-vis spectroscopy with a temperature
controller. The equilibrium constants (), enthalpy change (H), and entropy change (S) of
the solubilizer exchanges were evaluated.
Figure 1-(A) and Figure 2-(A) indicate the value of Kagainst each of the kinds ofnucleobasesand Figure 1-(B) and Figure 2-(B) indicate the value of H against the values ofTS (T = 298 K) which of the exchange reaction. We found the behavior of this reaction canbe seen from these data, d(G)20 and dsDNA (NF-B decoy) is similar. We have already done
also discussed about the discussion of this, on the behavior of the other.
[1] Y. Kato, Y. Niidome, N. Nakashima, Chem. Lett., 2011, 40, 730.
[2] Y. Kato, A. Inoue, Y. Niidome, N. Nakashima, Scientific Reports, 2012 2,733.
Corresponding Author: N. Nakashima
Tel: +81-92-802-2841, Fax: +81-92-802-2841
E-mail: nakashima-tcm@mail.cstm.kyushu-u.ac.jp- 104 -

2P-13Chirality Dependence of Quantum Thermal Transport in Carbon
Nanotubes at Low Temperatures: A First-Principles StudyżTomoyuki Hata, Hiroki Kawai, Tatsuhiko Ohto, Koichi Yamashita
Department of Chemical System Engineering, The University of Tokyo, Tokyo 113-8656, Japan
I. OBJECTIVE
Understanding the structural dependency of the physical properties of low dimensional
systems is one of the challenges in the design of potential material. Single-walled carbon
nanotubes (SWCNTs) are among the most promising candidates for materials of
nano-electronic devices because of their high thermal conductivity. We investigate the thermal
properties of single-walled carbon nanotubes (SWCNTs), focusing the chirality dependency.
II. COMPUTATIONAL DETAILSFor calculations of thermal properties, the nonequilibrium Green’s function (NEGF)
method based on lattice dynamics is chosen in this work. This method includes the quantum
nature of phonons adequately and reliable at the low temperatures where the thermal
conductances have quantized plateau.
Moreover, to evaluate the transmission coefficients and the thermal conductances from theperspective of the coupling properties of each normal mode, we project the dynamical matrix
renormalized by the interactions with the semi-infinite leads onto the normal mode basis of
the center region. This allows us to evaluate the effect of the coupling and the energy shift
from the phonon-phonon interaction [1].
III. RESULTS AND DISCUSSION
We applied our methods to three SWCNTs with different
chiralities (3, 3), (5, 0) and (4, 2) (Fig. 1), and found thethermal conductance varies significantly with the chirality,
at both low and high temperatures (Fig. 2) [2,3]. Such
differences are attributed to the dependence on the chiralityof the frequency of optical modes and phonon-phonon
interaction with the semi-infinite leads.
Our result indicates that high optical mode frequency andweak phonon coupling on the SWCNT (3, 3) are the origin Fig. 1 Atomic structures of SWCNTs
of slow rise of the thermal conductance at low temperature.
On the other hand, the suppression of the (5, 0)
thermal conductance at high temperature resultsfrom the fact that the transmission coefficient isreduced greatly in the vicinity of 50-70 meV.
[1] T. Hata, et al. J. Chem. Phys. 139, 044711 (2013)[2] N. Mingo, et al. Phys. Rev. B 77, 033418 (2008)[3] T. Yamamoto, et al. Appl. Phys. Express 2, 095003(2009)
Corresponding Author: K. Yamashita
Tel: +81-í-7228, Fax: +81-í-5012,
E-mail: yamasita@chemsys.t.u-tokyo.ac.jp- 105 -

Fig. 2 Thermal conductances of SWCNTs

2P-14Li-ion battery electrode property of anthraquinone molecules
encapsulated in single-walled carbon nanotubes
żS. Kawasaki, T. Matsuura, K. Tashiro, H. Song
Nagoya Institute of Technology
Gokiso,Showa, Nagoya 466-8555, Japan+

Potential (V vs Li/Li )Li-ion battery (LIB) whose energy density is the highest among the secondary batteries has
been widely used for cell phones, notebook computers and so on. Recently it has come to be
used for electric vehicles including plug-in hybrid cars. However, it should be noted that LIB
is facing today serious problems related to safety concerns and resource costs. The latterproblem is caused by the use of what we call “rare metals” in the cathode active materials
such as LiCoO2 and LiNiO2.
Organic electrode active materials are expected for the replacement of the expensive rare
metal oxides. However, it is generally very difficult for LIB using the organic electrode active
materials to show good cyclability because organic materials tend to dissolve in theelectrolyte during charge-discharge cycles. If the dissolution can be restricted, we could
obtain cheap and flexible LIBs. For that purpose we tried to use organic electrode active
materials encapsulated in single-walled carbon nanotubes. Here, we show the electrodeproperty of anthraquinone molecules encapsulated in SWCNTs.
The encapsulation of anthraquinone was carried out by exposing the SWCNT sample toanthraquinone gas in an evacuated glass tube. The open-end SWCNT sample and the organic
molecule powder sample in the evacuated glass tube were heated at 200ºC for 10 hours. Afterthe heat-treatment, the SWCNT sample
Anthraquinone in SO(O) (26.4wt%)
was washed several times with ethanol inorder to remove the physically adsorbed
organic molecules on the SWCNT surface.
3
The encapsulation was confirmed by XRD
and N2 adsorption experiments. For theelectrochemicalmeasurements,
we
prepared a test cell consisting of the
SWCNT working electrode and Li metal
counter electrodes. A mixture ofethylene-carbonate: diethyl-carbonate = 1:1
2
containing 1 M LiClO4 was used as the
3rd
2nd
1st
electrolyte solution. Charge-discharge
measurements were performed in an Ar
drybox in a potential range of 1.5-3.2 V vs.
Li/Li+.
0
100
200
300
As shown in Fig. 1, the capacity drop by
Capacity (mAh/g)
cycling is effectively restricted by the useof SWCNTs.
Fig.1
Charge-discharge
curvesofanthraquinone encapsulated in SWCNTs.

- 106 -

2P-15
Diameter dependence of RBM frequency of SWNTs in water vapor○Naoki Homma1, Shohei Chiashi2, Yoshikazu Homma1, and Takahiro Yamamoto3
1

Dept. of Physics, Tokyo University of Science, Shinjuku, Tokyo 162-8601, Japan
Dept. of Mechanical Engineering, The University of Tokyo, Bunkyo, Tokyo 113-8656, Japan
3
Dept. of Liberal Arts, Tokyo University of Science, Katsushika, Tokyo 125-8585, Japan

2

Radial breathing mode (RBM) is one of the most important vibrational modes ofsingle-walled carbon nanotubes (SWNTs), because the measurement of RBM frequency ωRBM
enables us to uniquely assign the chirality of an individual SWNT by combining it with thetheory of resonant transitions.
In FNTG44, we reported the molecular dynamics (MD) simulation on (i) the distribution
structure of water molecules around an SWNT and (ii) ωRBM of SWNTs in water vapor [1].
The water molecules are condensed around an SWNT surface due to the van der Waals
interactions between water molecules and an SWNT. The condensed water molecules formed
the hydrogen-bond network parallel to the SWNT surface and eventually they construct a
few-layer structure. In addition, we showed that the diameter dependence of ωRBM of thin
SWNTs with the tube diameter dt~1nm is approximately represented as ωRBM=A/dt+B referred
to as the 1/dt law, where A and B are estimated as A=227.9 cm-1nm and B=7.5±2.5 cm-1 by
MD simulation.
In this symposium, we report tube-diameter dependence of ωRBM in a wider range of dt up
to 2 nm on SWNTs in water vapor. In the wider range, the tube-diameter dependence of ωRBM
𝐴𝐴
no longer obeys the 1/dt law, but it can be well fitted by ωRBM= 𝑑𝑑 √1 + 𝐶𝐶e 𝑑𝑑t2 . In ourtsimulation, the environment parameter Ce was estimated as Ce=0.057±0.005nm-2 for thewider range of dt<2nm. Table 1 shows various values of Ce for carbon nanotubes in different
environments [2].
Table 1. Environment parameter Ce [2].

Ce (nm-2)

Sample0.05

HiPCO@SDS

0.059

Alcohol-assisted CVD

0.065

SWNT@SiO 2

0.067

Free-standing

0.057

SWNT in water vapor (This work)[1] N. Homma, et al., Abstract book of 44th FNG symposium, p.22.
[2] A. Jorio, R. Saito, G. Dresselhaus, M. S. Dresselhaus. “Raman Spectroscopy in Graphene Related Systems”
Wiley-VCH (2011), pp.205, and references therein.
Corresponding Author: Takahiro Yamamoto,Tel&FAX: +81-3-5876-1486,
E-mail: takahiro@rs.tus.ac.jp- 107 -

2P-16
Optical Detection of DNA Hybridization and Denaturationon Single-Walled Carbon Nanotube Surface○

Yusuke Ito, Masahiro Ito, Daisuke Nii, Hiroki Kato, Kazuo Umemura, Yoshikazu Homma.
Department of Physics, Tokyo University of Science, Tokyo 162-8601, JapanDNA is one of the functional dispersant of single-walled carbon nanotubes (SWNTs) [1,2].
The combination of DNA and SWNT (DNA-SWNT) is expected to have application for abiosensor. For example, Heller et al. revealed a conformation change of the DNA from B-type
to Z-type adsorbed on the SWNT surface by photoluminescence (PL) spectroscopy [3].
Double stranded DNA (dsDNA) transforms single stranded DNA (ssDNA) when heatedapproximately 94°C in solution. Gradually decreasing the temperature causes transition from
ssDNA to dsDNA. However, ssDNA does not transform dsDNA when rapidly cooled. These
reactions are known as hybridization (ssDNA to dsDNA) and denaturation (dsDNA to
ssDNA). In this study, we investigated hybridization and denaturation of DNA adsorbed on
SWNT surface by PL spectroscopy.
First, we investigated hybridization on SWNT. The combination of oligo(dT)30 and SWNT
(T30-DNA-SWNT) is prepared, and then T30-DNA-SWNT and oligo(dA)30 are mixed insolution and heated to cause the hybridization. Schematic illustration of experimental
procedure and PL spectrum of each process are shown in Fig. 1 and Fig. 2. The redshift of PL
spectra is attributed to the change of dielectric constant surrounding SWNT, i.e. hybridization
occurred on SWNT surface. Then, we investigated denaturation of dsDNA on SWNT. The
dsDNA derived from salmon testes was used. The combination of dsDNA and SWNT in
solution was heated to cause denaturation and rapidly cooled to prevent hybridization. In thiscase, any change of PL spectrum was not observed. This result shows existence of strong
interaction between DNA and SWNT surface. This interaction inhibits detachment of DNA
from the SWNT surface.
In conclusion, we revealed that the transition of DNA between ssDNA and dsDNA on
SWNT is non-reversible. Based on these results, we will discuss mechanism and structure of
DNA adsorption on SWNT surface.
[1] N. Nakashima, et al.: Chem. Lett. 32 (2003) 456.
[2] M. Zheng, et al.: Nature Mater. 2 (2003) 338.
[3] D. Heller, et al.: Science. 311 (2006) 508.
Corresponding Author: Yoshikazu Homma
Tel: +81-3-3260-4271 (ext. 2298), Fax: +81-3-5261-1023,
E-mail: homma@rs.tus.ac.jp

Fig. 1. schematic illustration of experiment.

- 108 -

Fig. 2. PL spectrum of each process.

2P-17
Observation of a gate-induced photoluminescence peakin individual carbon nanotubes
żY. Ueda, M. Yoshida, A. Ishii, T. Uda, Y. K. Kato
Institute of Engineering Innovation, The University of Tokyo, Tokyo 113-8656, Japan
We perform photoluminescence spectroscopy on individual air-suspended carbon
nanotubes within field effect transistor structures [1,2]. The devices are fabricated by etching
trenches on Si substrates with a 100-nm-thick oxide layer, and Ti/Pt are deposited aselectrodes. Single-walled carbon nanotubes are grown by chemical vapor deposition, and we
perform photoluminescence microscopy at room temperature under high vacuum.
Photoluminescence imaging and excitation microscopy are used to identify individual
nanotubes, and spectra are collected as a function of gate voltage. As the gate voltage isincreased, we find that a new peak appears at an energy lower than the bright exciton
emission, consistent with the expected behavior for trion luminescence.
Work supported by KAKENHI, KDDI Foundation, and the Photon Frontier Network
Program of MEXT, Japan.
[1] S. Yasukochi, T. Murai, S. Moritsubo, T. Shimada, S. Chiashi, S. Maruyama, and Y. K. Kato, Phys. Rev. B
84, 121409(R) (2011).
[2] Y. Kumamoto, M. Yoshida, A. Ishii, A. Yokoyama, T. Shimada, and Y. K. Kato, arXiv:1307.5159 (2013).
Corresponding Author: Y. K. Kato
Tel: +81-3-5841-7702, Fax: +81-3-5841-7772
E-mail: ykato@sogo.t.u-tokyo.ac.jp- 109 -

2P-18
Thermal Properties of SWNT Forest with Various Volume Fraction○JinHyeok Cha1, Kei Hasegawa2, Shohei Chiashi1, Asuka Miura1, Jeonyoon Lee3, Brian L
Wardle3, Suguru Noda2, Junichiro Shiomi1, Shigeo Maruyama1
1

Department of Mechanical Engineering, The University of Tokyo, Tokyo 113-8656, Japan2
Department of Applied Chemistry, Waseda University, Tokyo 169-8555, Japan3
Department of Aeronautics and Astronautics, Massachusetts Institute of Technology,
Cambridge, MA 02139, U.S.A.

CNTs on squeezer

Cover CNTs

3 mm

Densified SWNT forest

Another-direction

Densify one-direction

3 mm

Fig. 1 Densification process of vertically aligned SWNT
forest by mechanical squeezing.

10

40

6
4

20

2
0

0

5

10

15

Volume Fraction (%)

20

0
25

Fig. 2 Thermal conductivity of SWNT forest andthe calculated thermal conductivity equivalent toa single SWNT.

[1] Y. Won et al., PNAS, 110, 20426 (2013).
[2] K. Hasegawa et al., ACS Nano 5, 975-84 (2011).
[3] B. L. Wardle et al., Adv. Mater. 20, 2707-2714 (2008).
Corresponding Author: S. Maruyama
Tel: +81-3-5841-6408, Fax: +81-3-5841-6408, E-mail: maruyama@photon.t.u-tokyo.ac.jp- 110 -

60

Forestan SWNT

8

Thermal Conductivity of an SWNT (W/mK)

VASWNTs w/o Si sub.

Thermal Conductivity of Forest (W/mK)

Needs of a material for thermal management in reduced-sized electronic devices drive
single-walled carbon nanotubes (SWNTs) to be one of the most expected materials due to theoutstanding flexibility and thermal conductivity [1]. Therefore, many numerical andexperimental studies to understand thermal property of SWNTs have been reported to be usedin the applications.
In present study, we have investigate thermal diffusivity and thermal conductivity of
mm-long SWNT forest [2] with various volume fraction using laser flash technique. Our
primary aim here is to understand thermal properties of SWNT forest, and to identify thedifference from that of an individual SWNT which potentially explains lower thermal
property than expected when composing forest.
Figure 1 shows the densification process of SWNT forest that various volume fraction [3] of
mm-long vertically aligned SWNT forest [2] were obtained by mechanical squeezing. We
measured the thermal diffusivity of SWNT forests and calculate thermal conductivity using
additional information such as density and specific heat of the forest. Through the estimationof numbers of SWNTs in the forest and the density of SWNTs, we derived the apparent
thermal conductivity equivalent to a single SWNT. The result reveals that thermal diffusivity
and thermal conductivity of SWNT forest increased with at high volume fraction of the
SWNT forest, which is considered to give additional channels for thermal transport. In
particular, apparent thermal conductivity equivalent to a single SWNT is found to be greaterat higher volume fraction. We potentially considered that densification of the forest made aninterstitial distance between SWNTs, hence the thermal boundary resistance between them isrelieved.

2P-19In-plane conductivity of dense carbon nanotube forest
on semi-insulating silicon carbide○Masafumi Inaba1, Chih-Yu Lee1, Kazuma Suzuki1, Megumi Shibuya1, Atsushi Hiraiwa1,
Yoshiho Masuda2, Wataru Norimatsu2, Michiko Kusunoki2, Hiroshi Kawarada1
1
Graduate School of Advanced Science and Engineering, Waseda University, Tokyo
169-8555, Japan2
Eco Topia Science Institute, Nagoya University, Aichi 464-8603, Japan

Sheet conductivity (S/sq)

Carbon nanotube forest formed by silicon carbide surface decomposition method (CNT on
SiC) consists of nearly ideally close-packed CNTs with a surface density of ~1013 cm-2[1].
Generally, CNT conducts in its on-axis direction, yet such highly dense CNT forest may cause
high in-plane direction conductivity. Previously, we revealed the Schottky barrier height of
CNT/SiC interface for CNT new application as heat dissipating ohmic electrode of SiC powerdevices[2]. Here we report on the in-plane conductivity evaluation of CNT forest on
semi-insulating SiC.
On-axis C-face (000-1) of semi-insulating SiC substrates (< 10-8 S/cm) were annealed at
1500~1600 oC in vacuum (~10-3 Pa). The in-plane conductivity was measured by van der
Pauw method. Fig.1 shows (a) the schematic image of sheet conductivity measurement and(b) its equivalent circuit. Four parts which may contribute to CNTs on SiC in-plane
conductivity are considered, CNT caps, CNT bulk, CNT/SiC interface, and SiC bulk. To
determine which part(s) is/are dominant
Point probe(a)in conduction, CNT lengths were varied(b)by controlling decomposition time to CNT cap
Conductance Gcapchange CNT bulk conductivity.
CNT
bulk
Fig.2 shows the relationship between
Conductance Gcnt
CNT on SiC sheet conductivity and CNT CNT/SiC
length. The slope corresponds to the CNT interface
Conductance Gint
SiC Substratebulk conduction. The in-plane CNT bulk SiC bulk(<10-8 S/cm)
Conductance Gsic
conduction is calculated to be ~50 S/cm.
The intercept of Fig.2 corresponds to the Fig. 1 (a) Schematic image of sheet conductivity
conduction of the others. The SiC bulk measurement and (b) its equivalent circuit-3
conduction is negligible, since the
3x10
conductivity of initial SiC substrate isextremely as low as 10-7 S/cm. The
conductivity of CNT/SiC interface was-3
2x10
checked by removing CNTs and is alsosufficiently small. Therefore, theintercept indicates the sheet conductivity
CNT bulk conduction-3
1x10
of CNT caps as ~7×10-4 S/sq. If the~ 50 S/cm
thickness of CNT caps is presumed to be
CNT cap conduction
5 nm, the room temperature conductivity~ 7×10-4 S/sq (~1.4×103 S/cm)
3
is evaluated to be ~1.4×10 S/cm.
0[1] M. Kusunoki et al., Appl. Phys. Lett.77, 531 (2000)[2] M. Inaba, H. Kawarada et al., to be submitted
Corresponding Author: M. Inaba
Tel&Fax: +81-3-5286-3391
E-mail: inaba-ma@ruri.waseda.jp

0

100

200

300

400

CNT length (nm)Fig. 2 Relationship between CNT sheet conductivity
and CNT length- 111 -

2P-20
Systematic Conversion of Single Walled Carbon Nanotubes into n-type
Thermoelectric Materials by Molecular Dopants○Yoshiyuki Nonoguchi1, Kenji Ohashi1, Tsuyoshi Kawai1
1Graduate School of Materials Science,Nara Institute of Science and Technology,
Ikoma, Nara 630-0192, Japan

Thermoelectrics is a challenging issue for modern and future energy conversion andrecovery technology. Carbon nanotubes are promising active thermoelectic materials owing totheir narrow band-gap energy and high charge carrier mobility, and they can be integrated into
flexible thermoelectrics that can recover any waste heat. Pristine single walled carbon
nanotubes (SWNTs) exhibit p-type majority charge carriers because of oxygen impurity, andfew examples of their controlled n-type doping has
been exploited.[1] We here report air-stable n-type
SWNTs with a variety of weak electron donors in therange of HOMO level between ca. -4.4 eV and ca.
-5.6 eV, in which partial uphill electron injection fromthe dopant to the conduction band of single walledcarbon nanotubes is dominant.[2]We demonstrated that a Seebeck coefficient ofpristine SWNT buckyapers (+49 V/K) can be
drastically converted into negative values by doping
SWNT buckypapers with a wide range of electron
donors. All the dopants altered the Seebeckcoefficients ranging from +90 V/K to -80 V/K.
Among them, a lot of dopants listed in Fig.1
successfully switched the majority carriers of SWNT
materials from p- to n-type (Fig.2). We assumed that
this conversion was due to charge transfer dopingfrom Lewis bases to SWNTs. This methodology was
not limited for previously-known dopants such as PEI,
Fig.1 Dopants for n-type SWNTs
and versatile electron donors are here available todope SWNTs into n-type materials. To generalize
these phenomenon, we obtained the trend of highest
occupied molecular orbital (HOMO) of dopants for
n-type doping of SWNT materials. Dopants with
HOMO energy above roughly -5.6 eV against thevacuum level successfully altered the sense ofmajority carriers from holes in pristine SWNTs toelectrons.
[1] H. Dai et al. J. Am. Chem. Soc. 123, 11512 (2001).
[2] Y. Nonoguchi et al. Sci. Rep. 3, 3344 (2013).
Corresponding Author: Y. Nonoguchi
Tel: +81-743-72-6028, Fax: +81-743-72-6179,
E-mail: nonoguchi@ms.naist.jp- 112 -

Fig.2 Seebeck coefficient of doped
SWNT films

2P-21
Evaluation of the contact resistivity and Schottky barrier heightat carbon nanotubes/silicon carbide interface○Kazuma Suzuki1, Masafumi Inaba1, Megumi Shibuya1, Lee Chih Yu1,
Miho Myodo1, Atsushi Hiraiwa1, Yoshiho Masuda2,
Wataru Norimatsu2, Michiko Kusunoki2, Hiroshi Kawarada 1
1School of Science and Engineering, Waseda University, Tokyo 169-8555, Japan2
Eco topia Science Institute, Nagoya University, Aichi 464-8603, Japan
1. CNT on SiC
Carbon nanotube forest synthesized with silicon carbide
surface decomposition method (CNT on SiC)[1][2] exhibits
the most densely packed CNT forest (~1013 cm-2) and issuitable for electrodes with high current density durability.
CNTs can be important material for SiC, which is promisingmaterials of power semiconductors, in cooperation with its
high thermal conductivity. It is necessary for application aselectrodes to evaluate the contact resistivity.
2. The contact resistivity at CNT/SiC interface
As shown in Fig.1, lateral conduction also coexists in the
CNT on SiC because of its high tube density. To restrict thecontact area of CNT forest on SiC, electrically isolatedareas was formed with focused ion beam schematicallyshown in Fig.1. The electric properties of isolated areas
with different size were measured by conductive AFM toobtain size dependence of total resistance composed of top
and bottom contact resistances and CNT intrinsic resistance.
Fig. 2 shows the relationship between reciprocal conduction
area and total resistance of the measurement system (Fig.1)
at each donor density. Since the contact resistance of
CNT/SiC interface is inversely proportional to the
conduction area, the slope of the graph corresponds to thecontact resistivity. In addition, contact resistivity decreases
as donor density of SiC substrate increases.
3. Schottky barrier height at CNT/SiC interface
Fig. 3 shows the results of plotting the contact resistivityof the each donor density(5×1017 cm-3, 1×1018 cm-3, 1×1019
cm-3) SiC. Each curve is the theoretical relationship between
donor density and contact resistivity of the metal and 4H-SiC
when Schottky barrier height varies from 0.3 to 1.5 eV.
Contact resistivity of donor density of 5×1017 cm-3, 1×1018
cm-3 corresponds to Schottky barrier height of 0.5 ~ 0.6 eV. At
donor density of 1×1019 cm-3, however, lower contact
resitivity than 2×10-4Ωcm2 is difficult to measure in thepresent technique, the estimated Schottky barrier height
deduced from the contact resistivity was 0.8 eV. The realcontact resistivity at donor density of 1×1019 cm-3 might belower than this value.

[1] M. Kusunoki et al., Appl. Phys. Lett.77, 531 (2000)[2] M. Kusunoki et al., Appl. Phys. Lett. 87, 103105 (2005)
Corresponding Author: K. Suzuki
Tel: 03-5286-3391, Fax: 03-5286-3391, E-mail: gloria-274@asagi.waseda.jp- 113 -

Fig.1 Schematic image ofcurrent paths in CNT/SiC system

Fig.2 Relationship between reciprocal
conduction area and total resistanceFig.3 Relationship of the dopant
density and the contact resistivity

2P-22
Infra-Red Light Sensor using High-Purity
Semiconducting Single-Wall Carbon Nanotube Networks○Hikaru Kudo1, Seiya Kaji1, Hideki Kawai1, Taishi Takenobu2, Kazuhiro Yanagi1
1. Department of Physics, Tokyo Metropolitan University, Tokyo 192-0397, Japan
2. Waseda University, Tokyo 169-8555, Japan
There is a lot of demand for un-cooled infrared (IR) light image sensors for security andhealth industries. Micro-bolometers are the most popular high-performance un-cooled far-IR
detectors and are widely used for night-vision cameras, and thermography applications.
However, they are considerably expensive due to their fabrication costs. A diaphragm
structures with vacuum thermal isolation is used in the cell, which requires complicatedsemiconductor MEMS processes and vacuum packaging, and this makes it very difficult to
reduce costs. Therefore, there is a large demand for IR detection sensors which are fabricatedthrough other const effective processes. Single-wall carbon nanotubes (SWCNTs) have IR
optical absorption. Thus the uses of SWCNTs for IR detection have been proposed. The valueof temperature coefficient ratio (TCR) is a very important parameter to evaluate theperformance of bolometer. In the mixture of metallic and semiconducting SWCNTs, previous
study has revealed almost zero TCR value at room temperature, 1,2 suggesting that SWCNTs intheir mixture state cannot be used as un-cooled IR detectors. However, in high-purity
semiconducting SWCNTs networks, a large temperature dependence is expected. 2 Here weclarified that the high-purity single-chiral SWCNTs has - 2.6% K-1 TCR value (Figure 1),
which is the larger than typical VOx bolometer, andwas the largest TCR value in SWCNTs. We
clarified the TCR value can be controlled throughcarrier injection using ion gel. We demonstrated IR
detection
using
semiconducting
SWCNTsfabricated on plastic substrate. Figure 2 shows 28%
of resistance change under IR radiation from black
body source at temperature of 150 ℃ (in thissituation, peak emission wavelength is 7μm). Our
sensors displayed approximately 1 % of resistancechanges to the IR radiation from our body,suggesting semiconducting SWCNTs are useful for
un-cooled IR sensors.
Acknowledgment:
KY thanks for discussion with Dr. Narita (NEC) and
Komatsubara (Nippon Avionics Co.). This work is partially
supported by JST A-step program.
Reference:[1]Itkis et al., Science 312, 413 (2006)[2]Yanagi et al., ACS Nano 4, 4027 (2010)
Corresponding Author: Kazuhiro Yanagi
Tel: +81-42-677-2494
E-mail: yanagi-kazuhiro@tmu.ac.jp- 114 -

Figure 1 Temperature dependence ofresistance of semiconducting SWCNTs
networks.

Figure 2 IR responses of semiconducting
SWCNTs networks

2P-23Operation Speed Improvement of Carbon Nanotube Integrated Circuits
on Plastic Substrate○Toshitada Sanzen1, Antti Kaskela2, Patrik Laiho2, Albert G. Nasibulin2,
Shigeru Kishimoto1, Esko I. Kauppinen2, and Yutaka Ohno1
1

Department of Quantum Engineering, Nagoya University, Nagoya 464-8603, Japan2
Department of Applied Physics, Aalto University, Espoo, Finland

Carbon nanotube thin-film transistors (CNT TFTs) are expected to realize
high-performance flexible devices. In the previous works, we realized CNT TFTs andintegrated circuits (ICs) on a flexible plastic substrate [1,2]. However, the speed of theprevious ICs, which was evaluated using a ring oscillator, was lower than that expected fromthe carrier mobility. It was considered that the parasitic overlap capacitances between the gate
and source/drain electrodes degraded the switching speed of the inverters. In this work, wereport the improvement of operation speed by reducing the overlap capacitances. The
operation speed has been enhanced by reducing the overlap capacitances by a factor of 7.4.
We have also measured the gate capacitances of the devices to discuss the effect of parasitic
capacitances on the operation speed.
We fabricated three types of 21-stage ring oscillators consisting of bottom-gate TFTs (a)with 20-m overlaps (same as the previous work), (b) with 2-m overlaps, and (c) without
overlap on PEN substrates as shown in Fig. 1. Conventional photolithography-based
processes were used for the fabrication. A 40-nm-thick Al2O3 insulator was deposited by anatomic layer deposition technique. A CNT thin film
was grown by floating-catalyst chemical vapor
deposition, collected on a membrane filter, andtransferred on the substrate as our previous works.
Chemical doping with F4TCNQ was carried out toadjust the logic threshold voltage and reduce parasitic
resistances of the non-overlap regions in device (c).
Figure 2(a)-(c) show the photograph of thefabricated devices, the micrograph, and the output
wave form of the ring oscillator with device (c). The
Fig.1 Schematic device structures (a)with 20-m overlaps, (b) with 2-moscillation frequencies (f) were 1.4, 3.6, and 10 kHz
overlaps, and (c) without overlap.
for devices (a), (b), and (c), respectively.
Corresponding delay times ( = 1/2Nf, N = 21 stages)
were 17, 6.6, and 2.3 s, respectively. The switching
speed was enhanced by a factor of 7.4 by reducing
the parasitic overlap capacitances. The results will be
discussed on the basis of the results ofcapacitance-voltage measurements in the TFTs.
[1] D.-M. Sun et.al., Nature Nanotech. 6, 156 (2011).
Corresponding Author: Y. Ohno
Tel: +81-52-789-5387, Fax: +81-52-789-5387,
E-mail: yohno@nuee.nagoya-u.ac.jp- 115 -

Fig.2 (a) Photograph of devices on PEN
substrate. (b), (c) Optical micrograph andoutput wave form of a ring oscillator with
device (c).

2P-24
Photovoltaic features of p-n homo-junction with position selective
Cs encapsulated single-walled carbon nanotubes thin films○Yoshihiro Abiko, Toshiaki Kato, Toshiki Akama, Rikizo Hatakeyama, Toshiro Kaneko
Department of Electronic Engineering, Tohoku University, Sendai, 980-8579, Japan
Single-walled carbon nanotube (SWNT) is one of the most attractive material for futurehigh performance solar cells due to their flexible filament-like structure, high carrier mobility,
tunable bandgap energy by controlling the diameter. In addition, multiple exciton generation(MEG) in SWNT has demonstrated experimentally and theoretically [1, 2]. For the fabricationof p-n homo-junction based SWNTs thin film, it is necessary to fabricate both p- and n-type
SWNTs thin film. It is well known that pristine SWNTs shows p-type transport property.
Recently, we have demonstrated very stable n-type SWNTs-thin film transistors (TFTs) by Cs
encapsulation into SWNTs by a plasma ion irradiation method [3].
Here we report the fabrication of p-n homo-junction based on position selective Cs
encapsulated SWNTs thin film. The half channel area of a pristine SWNTs-TFT fabricated bya conventional photolithography technique is covered with polymer to prevent Cs plasma
irradiation and position selective Cs encapsulation is realized. Cs encapsulation is carried out
by the plasma ion irradiation method. Finally, Cs
irradiated SWNTs thin film is rinsed by purified waterto remove the Cs atoms adsorbing on the outside of
SWNTs. In this study, the electrical transport properties
are investigated without or with light illumination
using a solar simulator.
It is found that the clear rectifying drain-source
current (IDS) vs. drain-source voltage (VDS)
characteristics can be observed after the position
selective Cs encapsulation into SWNTs thin film.
Furthermore, a short-circuit current and an open-circuit
voltage can be detected under light illumination using asolar simulator, as shown in Fig. 1. This indicates thatp-n homo-junction based on SWNTs thin film can beapplicable to solar cells. Our finding is important as a Fig.1 IDS-VDS characteristics of position
crucial step for the fabrication of high performance selective Cs encapsulated SWNTs thinfilm without and with light illumination.
SWNTs solar cells.
[1] S. Konabe and S. Okada, Phys. Rev. Lett. 108 (2012) 227401.
[2] N. M. Gabor et al., Science 325 (2009) 1367.
[3] R. Hatakeyama et al., J. Phys. D: Appl. Phys. 44 (2011) 174004.
Corresponding Author: Y. Abiko
Tel: +81-22-795-7046, Fax: +81-22-263-9225,
E-mail: abiko12@ecei.tohoku.ac.jp- 116 -

2P-25
Molecular recognition on surfaces of metallic and semiconducting singlewalled carbon nanotubes○Wenxin Huang1, Tsuyohiko Fujigaya1,2, and Naotoshi Nakashima1,2,3
1Department of Applied Chemistry, Graduate School of Engineering, Kyushu University,

744 Motooka, Fukuoka 819-0395, Japan

2World Premier International (WPI), International Institute for Carbon-Neutral Energy

Research, Kyushu University 744 Motooka, Nishi-ku, Fukuoka 819-0395, Japan

3Japan Science and Technology Agency, CREST, 5 Sanbancho, Chiyoda-ku, Tokyo,

102-0075, Japan

Introduction
Single-walled carbon nanotubes (SWNTs) are produced as a mixture of metallic SWNTs (mSWNTs) and semiconducting SWNTs (s-SWNTs). Since both of them are promising materials
especially for electronics in next generation, their separation (MS separation) is necessary. Up
to date, many MS separation methods such as gel chromatography and selective oxidation havebeen reported. However, these methods involve problems that are either time consuming or
causing damages to SWNTs. It is expected the process become very simple if only dispersion
process realizes the MS separation. For that purpose, the first requisite is to find out themolecule that can recognize the m- or s-SWNTs. In this study, we utilized the newly developed
affinity chromatography technique [1] to search for a type of molecule that can make MS
separation possible by solubilization, in which m- or s-SWNT were employed as a stationary
phase. As analytes, polyaromatic hydrocarbons were used to obtain the preliminary data.
Experiment
As a stationary phase, m-SWNTs are coated on silica gel. The silica gel coated with mSWNTs was fabricated by a simple mixing of m-SWNTs (0.733 mg NanoIntegris) dispersed in
N-methyl-2-pyrrolidinone (NMP) at a concentration of 0.01 mg mL-1 (73.3 mL) and aminofunctionalized silica gel (NH2-silica) with a 3.5 μm diameter (733 mg). Green blue power wascollected after filtration. The m-SWNT-silica-gel slurry prepared from m-SWNT-silica (323mg) was packed in a 2.1 mm×125 mm empty column (CE-402, Waters) using a slurry packing
apparatus (Model 124A, Chemco Scientific) to fabricate a packed column (m-column). The
column having s-SWNTs as a stationary phase (s-column) was made in similar fashion using sSWNTs instead of m-SWNTs.
Results and discussion
Fig. 1 shows the chromatographs forpolyaromatic hydrocarbons obtained from m(Fig. 1A) and s-columns (Fig. 1B) using
tetrahydrofuran (THF) as an eluent. Four
samples showed different retention times
depending on the magnitude of the interaction.
Interestingly, we found the elution orders of
the four samples in m- and s-columns are
identical (Fig.1). The result suggests that thesemolecules showed no clear recognition for mor s-SWNTs, which agreed well with thegeneral understanding for these molecules
showing no MS separation ability.
[1] J. Yoo et al., Nanoscale 2011, 3, 2517.
Corresponding Author: Naotoshi Nakashima
E-mail: nakashima-tcm@mail.cstm.kyushu-u.ac.jp
Tel & Fax: +81-92-802-2842

Fig. 1 Chromatograms of PAHs using (A) m- and(B) s-SWNT-silica as stationary phases at flow rates
of 0.1 mL min-1; eluent: THF.

- 117 -

2P-26
High Photovoltaic Performance of MoO3-doped Single-walled Carbon
Nanotube/Si Solar Cells
Feijiu Wang1, Daichi Kozawa1, Yuhei Miyauchi1,2,
Shinichiro Mouri1, Yutaka Ohno3, and Kazunari Matsuda1
1Institute of Advanced Energy, Kyoto University, Uji, Kyoto 611-0011, Japan
Japan Science and Technology Agency, PRESTO, 4-1-8 Honcho Kawaguchi, Saitama
332-0012, Japan3
Department of Quantum Engineering, Nagoya University, Furocho, Chikusa-ku, Nagoya
464-8603, Japan
2

2

Current Density (mA/cm )Single-walled carbon nanotubes (SWNT) have attracted a great deal of attention forphotovoltaic applications due to their excellent physical and electronic properties. Recently,
the heterostructures of SWNT and Si has been extensively studied for photovoltaic cells [1]. It
was found that the key to realize the highly efficient solar cell is the use of high quality anddoped SWNTs network film [2-4]. In this study, we have fabricated the SWNTs/Si solar cells
using the high quality and MoO3 doped SWNTs network film and evaluated the photovoltaic
properties of the cells.
The high quality SWNTs network films fabricated by the floating catalytic CVD method
were used for the cells. The dotted line and solid line of Figure 1 show the current density
voltage (J-V) characteristics of pristine SWNT/Si and MoO3-doped SWNT/Si heterojunction
solar cells, respectively. From the J-V curve of pristine SWNT/Si solar cell, the conversion
efficiency (), current density (Jsc), fill factor (FF) and open circuit voltage (Voc) are 11.1%,
27.9 mA/cm2, 69% and 0.57 V, respectively. In contrast, the photovoltaic properties are muchenhanced in MoO3-doped SWNT/Si solar cell. The high values of Jsc (=38.4 mA/cm2), Voc(=0.59 V), and FF (=0.59 V) cause very high value of photovoltaic conversion efficiency of
17.6 %. The obtained value of 17.6 % is the highest
10
one in the carbon nanotube based solar cells. The
0physical mechanism of drastic enhancement ofphotovoltaic properties in MoO3-doped SWNT/Si−10will be discussed.
−20[1] D. D. Tune et al., Adv. Energy Mater. 2, 1043 (2012).
[2] D. Kozawa et al., Appl. Phys. Express 5, 042304 (2012).
[3] F. Wang et al., Appl. Phys. Express 6, 102301 (2013).
[4] F. Wang et al., submitted for publication.

−30

SWNT/Si η = 11.1%−40

MoO3-SWNT/Si η = 17.6%−50

Corresponding Author: Feijiu Wang

0

0.2

0.4

Voltage (V)0.6

Fig. 1: J–V curves of SWNTs/Si solar cell
before and after coating MoO3

Tel: +81-774-38-3465, Fax: +81-774-38-3460
E-mail: wang.feijiu.75w@st.kyoto-u.ac.jp- 118 -

2P-27
Solubility control of SWCNT by using photofunctional dispersants○Yoko Matsuzawa, Yuko Takada, Hideyuki Kihara, Masaru Yoshida
Nanosystem Research Institute,
National Institute of Advanced Industrial Science and Technology,
Tsukuba 305-8656, Japan
Solubilization of the single-walled carbon nanotubes (SWCNTs) is important for
fundamental studies and industrial applications of SWCNTs. Especially, precise tuning of thedispersibility of the SWCNTs is necessary in advanced applications including switching
devices, sensors, and drug delivery systems.
Recently, we have reported dispersibility tuning of SWCNTs by applying photochemical
reaction of a water-soluble stilbene 1 as a dispersant [1]. Due to the rigid and nearly coplanar
structure of 1, it can interact with the SWCNTs via  interactions, resulting in a stabledispersion of the SWCNTs in water without bundling. In contrast, the photocyclized product 2
having a highly twisted and bent structure is unfavorable for the  interactions with the
SWCNTs. Since such drastic change in the molecular structure of the dispersant affects theaffinity between the dispersant and the SWCNT surfaces, on-off switching of thedispersibility control of the SWCNTs has been successfully demonstrated by in-situ
photoreaction of the 1/SWCNTs dispersion. Further, it has been found that thephotofunctional dispersant 1 is useful for purification of raw-SWCNT by combination
procedure with high-speed centrifugation [2].
In this study, we have investigated photochemical reaction of the dispersant 1 in
1/SWCNTs hybrid films. The films were prepared by casting of the 1/SWCNT dispersion on
fused silica. Upon UV-light irradiation, photoreaction of 1 progressed even in the hybrid films,
and we found that the solubility of the SWCNT films was altered by the photoirradiation. The
1/SWCNTs hybrid films without photoirradiation easily dissolved into water. In contrast, theUV-exposed films remained on the glass substrate, while only photoreacted dispersant 2 wasrinsed off from the SWCNT surface using water.
H3C N

CH3

1
N
H

2

N

O
H
N
2Cl

O

H3C

Isomerization

H
N

H
N

O

hv

hv

E

O

N CH3

N

2Cl

Cyclization

Z

Oxidation

Fig.1 Structures of the photoresponsive dispersant (up). Photoreaction of stilbene (bottom).
[1] Y. Matsuzawa et al., Adv. Mater., 23, 3922 (2011)[2] Y. Matsuzawa et al., J. Phys. Chem. C submitted.
Corresponding Author: Yoko Matsuzawa
Tel: +81-29-861-2958, Fax: +81-29-861-4673
E-mail: yoko-matsuzawa@aist.go.jp- 119 -

2P-28Growth of CNTs using the dip coat method as the catalyst support
Keisuke Fujii, Yoshinori Ando, Masato Ohkohchi

Dept. of Materials Science and Engineering, Meijo University, Nagoya,Japan
Dip coat method [1] is well known as a simple method for supporting thecatalyst. This method only includes pulling the substrate that is placed in the
catalyst solution. So, no special equipment is needed in the process, and it ispossible to reduce the waste of the catalyst.
In this experiment, Fe / Co was used as the catalyst, and camphor [2] wasused as the carbon source. The catalyst was supported on the substrate by
dip coat method (drawing speed 3cm/min). Carbon nanotubes (CNTs) weregrown up using chemical vapor deposition (CVD). Camphor was sublimed at
200℃ in an electric furnace, and the temperature of the substrate was set to
750℃.
In the experiments by the dip coat method, CNTs which are arranged on
the entire surface of the substrate have been synthesized (Fig.1). The G/Dratio obtained from Raman measurements was 1.26. CNTs did not

sometimes grow up even if the experiments had been done under the same
conditions. Formation of the liquid film on the substrate is to be influenced
by slight fluctuations of the vibration, temperature, and humidity. Dip coatmethod has so poor reproducibility, further improvement is needed.

[1] F. Iskandar, M. Abdullah, H. Yoden, K. Okuyama,
J. Sol-Gel Sci. Tech.: 29, 41-47 (2004)[2]M. Kumar, Y. Ando, J. Physics: Conference Series
61, 643–646 (2007)
10μm

Corresponding Author: K. Fujii
E-mail: 133434028@ccalumni.meijo-u.ac.jp

Fig 1- 120 -SEM image of the oriented carbon nanotubes

2P-29Chiral selective solubilization of single-walled carbon nanotubes
using flavin and isoalloxazine derivatives
Masashi Fukuzawa1, Fumiyuki Toshimitsu1, Yuichi Kato1, Naotoshi Nakashima1, 2, 3
1

Department of Applied Chemistry, Kyushu University, Fukuoka 819-0395, Japan
2 WPI-I2CNER, Kyushu University, Fukuoka 819-0395, Japan
3 JST-CREST, Chiyoda-ku, Tokyo 102-0075, Japan

SWNTs are classified into metallic or semiconducting tubes according to their chirality.
However, the coexistence of tubes with various chiralities in the raw SWNT materialinterferes fundamental researches and development of devices. Despite several technicalmethods have been developed for the separation, the development of a new powerful
separation method is still a great challenge.
Here we report a selective recognition and extraction of semiconducting SWNTs(s-SWNTs) using flavin and isoalloxazine derivatives. We previously revealed that dmC12(Fig. 1), the compound that has been reported to disperse SWNTs [1], can selectively solubilize
s-SWNTs [2]. In order to explore the origin of such chiral selectivity, we here synthesized
several flavin and isoalloxazine derivatives (Fig. 1), and examined their s-SWNTs
solubilization ability. Fig. 2 shows the absorption spectra of the HiPco-SWNTs dissolved intoluene using such derivatives, in which we observe that dmC12, dmC18 and 7mC12 areable to solubilize s-SWNTs selectively. On the other hand, C12 and NmdmC12 did notsolubilize any SWNTs. These results strongly suggested that the imidyl hydrogen and methylgroup(s) on the aromatic rings are essential for selective solubilization/extraction of thes-SWNTs. A possible mechanism for such selective dissolution/separation will be presented at
the meeting.
dmC12/HiPco
dmC18/HiPco
7mC12/HiPco

R1, R2, R3, R4 =a) Me, Me, C12H25, H (dmC12)b) H, H, C12H25, H (C12)c) Me, Me, C18H37, H (dmC18)d) H, Me, C12H25, H (7mC12)e) Me, Me, C12H25, Me (NmdmC12)
Fig. 1 Chemical structures of flavin andisoalloxazine derivatives.

NmdmC12/HiPco
C12/HiPco

Fig. 2 Vis-near IR absorption spectra of SWNTs
dissolved by flavin and isoalloxazine deraivatives.

[1] F. Papadimitrakopoulos et al., Science. 323, 1319 (2009).
[2] Y. Kato et al., the 44th FNTG symposium, 2P-25 (2013).

Corresponding Author: N. Nakashima
Tel: +81-92-802-2840, Fax: +81-92-802-2840;
E-mail: nakashima-tcm@mail.cstm.kyushu-u.ac.jp- 121 -

2P-30Self-assembly of Highly Aligned Metallic/Semiconducting
SWCNTs using Crystal Templates○H. Kawai1, K. Hasegawa¹, Y. Naitou2, Y. Takagi3, Y. Wada3, T. Takenobu3, K. Yanagi1
1

Tokyo Metropolitan Univ., 2AIST, 3Waseda Univ.

Single Wall Carbon Nanotubes (SWCNTs)
have various electronic structures dependingon their chirality. Recent progress of
separation technique enables us to extract
metallic, semiconducting and single chiralstate of SWCNTs from the mixed state
sample. It is expected that fabrication ofdevices exploiting their intrinsic excellent
electrical transport property. However,Fig. 1 (a) Assembly process of aligned SWCNT
typical devices fabricated as random(b) Removal of the surfactans crystal
networks in which the SWCNTs are
randomly oriented and connected. Random
interfaces work as scattering centers,
thereby localizing conducting carriers thus,
the device performance of such networks isinferior to that expected in a single rope of
SWCNTs. Therefore, controlling thealignment of SWCNTs is an essential stepto achieving superior macroscopic device
performance. We previously reported Fig. 2 (a) Metallurgical microscope image of assembly of SWCNTs
after washing.(b) Polarized micro-Raman measurement.
string-like assembly of aligned SWCNT in asingle-chiral state, which induced by self assemble process in temperature controlled solutionof SWCNTs, and the assembly exhibit good field effect performance[1].
In this study, we introduce another unique technique to control alignment of SWCNTs,
which utilize self-assemble processes of SWCNTs upon the crystal surfaces of surfactants.
Fig. 1 illustrates our method for assembling SWCNTs on the surfaces of needle-like crystalsof deoxycholate (DOC). SWCNTs dispersed in solution with surfactants were dropped on theneedle, and SWCNTs were self-assembled on the crystal surfaces during the gradualevaporation of the solutions. Then the surfactant crystals were removed by soaking thesubstrate in aceton for 20h, as a result aligned SWCNT assemblies were left on the substrates.
Micro -Raman measurement and scanning electron microscopy (SEM) measurements clearlyshow that the SWCNTs were highly aligned parallel to needle axis in the assembly. Angle
distribution evaluated from SEM image indicates about 65% of SWCNTs are aligned parallel
to needle axis within ±5°and about 85% are aligned within ±10°, which is better alignment
than that we previously reported and on the same level with aligned SWCNTs horizontallygrown on specific substrate.
[1]Kawai et al., Appl. Phys. Express 6 (2013) 065103.
Corresponding Author: K. Yanagi
Tel: +81-42-677-2494, Fax: +81-42-677-2483, E-mail: yanagi-kazuhiro@tmu.ac.jp- 122 -

2P-31Chirality selective desorption of SWCNTs using mixed surfactant gelcolumn chromatography○Yohei Yomogida, Mayumi Tsuzuki, Atsushi Hirano, Shunjiro Fujii, Takeshi Tanaka,
Hiromichi Kataura
Nanosystem Research Institute, National Institute of Advanced Industrial Science andTechnology, Ibaraki 305-8562, Japan

Absorbance (a.u.)Single-wall carbon nanotubes (SWCNTs) show great promises of future applications inelectronics and optoelectronics. Because the band structure of SWCNT is highly depending
on its structure, chirality separation from the structure-mixed raw soot is very important for
both fundamental research and further application of SWCNTs. Recently, we have developed
a multicolumn gel chromatography method for single chirality separation that is based on thechirality-dependent interaction between sodium dodecyl sulfate (SDS)-wrapped SWCNTs andthe gel.[1] In this method, however, we had to prepare a huge amount of SWCNT solution to
get a tiny amount of single-chirality SWCNTs. To accelerate SWCNT research, we still needmore effective separation method for the single-chiralities.
To improve the selectivity, in this work, we tried small amount of sodium deoxycholate(DOC) as a co-surfactant that is well known to be effective for diameter selective desorption
in agarose gel chromatography. [2]Figure 1 shows typical optical5
absorption spectra of SWCNTs
obtained by stepwise elution changing
wt% SDS,
4 10.06
DOC concentration from 0.04 to 0.12
wt% DOC
wt%, in addition to 1 wt% SDS
aqueous solution. These spectra clearly
3 1 wt% SDS,
(6, 5)
show chirality selective desorption.
0.10 wt% DOC(6, 5)The second upper spectrum shows(9, 1)(9, 1)
prominent (6,5) peak while the upper2
and lower most spectra never show
1 wt% SDS,
(6,5) peak. This strong selectivity is
0.12 wt% DOC
1(8, 3)
very useful for large scale chirality(8, 3)
sorting despite less selectivity in large
S
S
diameter part (1100 - 1300 nm). We
22
110
can combine another diameter sorting
400 600 800 1000 1200 1400
process to get single chirality
Wavelength (nm)SWCNTs.
This work was supported by
Fig. 1 Optical absorption spectra of the SWCNTs eluted
KAKENHI No. 25220602.
from gel columns by the stepwise elution with various DOC
concentrations in the presence of 1 wt% SDS[1] H. Liu et al. Nat. Commun. 2, 309 (2011).
[2] H. Liu et al. J. Phys. Chem. C 247, 9270 (2010).
Corresponding Author: Hiromichi Kataura,
Tel: +81-29-861-2551, Fax: +81-29-861-2786
E-mail: h-kataura@aist.go.jp- 123 -

2P-32
FT-ICR Study of Chemical Reaction of Cobalt Clusters with Acetonitrile○Kazuki Ogasawara 1, Yuta Tobari 2, Shohei Chiashi 1, Toshiki Sugai 2, Shigeo Maruyama 1
1

Department of Mechanical Engineering, The University of Tokyo, Tokyo 113-8656, Japan2
Department of Chemistry, Toho University, Chiba 274-8510, JapanThe chemical vapor deposition (CVD) method is currently regarded as one of the most
expected techniques for the industrial or commercial production of single walled carbon
nanotubes (SWNTs). In CVD method, SWNTs grow from carbon source molecules such as
CH4 or alcohol on nanoscale catalytic metal particles, therefore understanding surface chemical
reaction is critically important. Recently, Thurakitseree et al.[1] reported that changing thecarbon feedstock from pure ethanol to a few % mixture of acetonitrile (CH3CN) in ethanol
during CVD drastically reduces the average diameter of the SWNTs from approximately 2 to 1
nm, and the feedstock-dependent change is reversible and repeatable. The role of nitrogen in
reducing the diameter is suggested to be the surface impeding of SWNT formation, whichcauses the growth mode change from ‘Octopus’ to ‘VLS (vapor-liquid-solid)’, but the detailed
mechanism of the surface impeding is still not clear.
In this work, chemical reaction of small cobalt cluster cation with acetonitrile was observed
by Fourier Transform Ion Cyclotron Resonance (FT-ICR) mass spectrometer [2,3]. Cobalt
clusters composed of 7-17 atoms were directly trapped within the FT-ICR cell. Subsequently,
acetonitrile was introduced into the ICR cell via pulsed leak valve. Figure 1 shows the typicalmass spectrum of the reaction products from Co11+ clusters. Dotted line indicates simple
chemisorption of acetonitrile, and we can also observe dehydrogenated chemisorption such as+(CCN)2 or +(CCN)2(HCCN). Figure 2 shows the Co cluster size dependence of the reaction
products. Con+ clusters smaller than Co10+ show no dehydrogenate reaction and thechemisorption rate monotonically increases with cluster size. On the other hand, Con+ clusters
larger than Co10+ shows almost the same dehydrogenate rate and hence the chemisorption rate.
The efficient full dehydrogenate process leading to +(CCN)2 will be discussed.
911

Number of Cobalt atoms
10
12

0.8

1113
+

Intensity (arb. unit)* indicates peaks originated from Co12 or Co13+HCCN

+CH3CN+(CCN)2

Pure Con++(CCN)2(HCCN)

0.6

*

*

*

*

React. ratio+5[10 ]

0.4

+

+HCCN
+CH3CN+(CCN)2+(CCN)3
+(CCN)2(HCCN)

0.2

0
0

0

50
100
Relative Mass (amu)

1015Number of Co clusters

Fig. 1 Chemisorption on Co clusters of 11 atoms.

Fig.2 Cluster size dependence of the reaction products.

[1] T. Thurakitseree et al., ACS Nano, 7 (2013), 2205./[2] S. Maruyama et al., Rev. Sci. Instrum., 61 (1990),
3686./[3] S. Inoue, S. Maruyama, Jpn. J. Appl. Phys., 47 (2008) 1931.
Corresponding Author: S. Maruyama, Tel: +81-3-5841-6421, Fax: +81-3-5841-6983,
E-mail: maruyama@photon.t.u-tokyo.ac.jp- 124 -

2P-33Synthesis and TEM-based Structural Characterization of
C60-Flattened CNT Nanopeapods○Qing Wang1, Ryo Kitaura1*, Yuta Yamamoto2, Shigeo Arai2, Hisanori Shinohara1*
1

Department of Chemistry & Institute for Advanced Research, Nagoya University, Nagoya
464-8602, Japan
2
High Voltage Electron Microscope Laboratory, Ecotopia Science Institute, Nagoya
University, Nagoya 464-8602, JapanThe fully flattened carbon nanotube (FNT), a graphene nanoribbon analogue, provides aunique low-dimensional nanospace with an extremely wide dumbbell-like cross section that issignificantly different from that of carbon nanotubes [1]. This new type of nanospace provides
the ability to align atoms or molecules in not only one-dimensional but also two-dimensionalway, creating a brand new class of FNTs-based hybrid nanostructures such as FNTnanopeapods. In this study, we report synthesis of FNTs-based C60 nanopeapods and theirstructure characterization using transmission electron microscopy (TEM).

Fig.1 Structure models of one-dimensional (left) and two-dimensional (right) packing of
C60 molecules inside of FNTs

TEM images and electron energy loss spectroscopy (EELS) spectra of FNT show a clear-cut
evidence of the hollow space at the edges. The encapsulation of C60 molecules into the edge
space provides new hybrid material (C60@FNT) with one-dimensional C60 alignment at theedge. In addition, we also synthesized C60@FNT that possesses two-dimensional packing of
C60. These structures were characterized by TEM observation and image simulation based on
the multi-slice method. While the observed one-dimensional C60 chains along the edges of
FNTs are almost identical to that already reported for C60-peapods, the two-dimensional
packing of C60 molecules in FNT has been revealed for the first time in the present study.
Further investigation on structure and properties of C60@FNTs is currently underway and will
be presented in future.
[1] D. H. Choi et al. Scientific Reports 3 1617 (2013).
Corresponding Author: Ryo Kitaura and Hisanori Shinohara
TEL: (+81) 52-789-2482, FAX: (+81) 52-789-6442,
E-mails: r.kitaura@nagoya-u.jp and noris@ nagoya-u.jp- 125 -

2P-34Modulating the Electronic Properties of Multimeric Thiophene Oligomers
by Utilizing Carbon Nanotube ConfinementżTakashi Yumura1, Hiroki Yamashita 1
1

Department of Chemistry and Materials Technology, Kyoto Institute of Technology,
Matsugasaki, Sakyo-ku, Kyoto, 606-8585, Japan

We investigated the arrangement of methyl-terminated terthiophenes inside a nanotube byusing density functional theory (DFT) including dispersion corrections.
The DFT
calculations aim at obtaining atomistic information of thiophene oligomers inside nanotubes,
which were reported experimentally [1]. After conducting DFT calculations, a variety ofarrangements of the inner terthiophene chains was found, depending on host-tube diameters
and the number of chains [2,3]. Because of the various inner thiophene arrangements, theterthiophene chains interact differently. The interactions are stronger in a smaller nanotube
compared to within a larger nanotube, indicating importance of nanotube confinements to theinterchain couplings. The interchain interactions split the orbitals of the multimeric
terthiophene chains, which are built from single-chain frontier orbitals, to broaden theirenergy levels. Therefore, nanotube confinements are key factors in determining the energy
levels of the frontier orbitals of contained multimeric terthiophenes. As a result, theirelectronic transitions are affected by the encapsulation into a restricted nanotube space.
According to time-dependent DFT calculations, a specific electronic transition occurs from a
HOMO-built orbital to a LUMO-built orbital. The broadening of the orbital energies by theaggregation of terthiophene chains in a nanotube leads to a widened range of excitationenergies (Ex) in their electronic transitions relative to the single-chain. With respect to thestrongest transition of multimeric terthiophenes, the excitation energy is enhanced byconfinement to a nanotube. The Ex enhancement within a smaller nanotube is moresignificant than within a larger nanotube due to the stronger interchain interactions in asmaller nanotube. Therefore, it is proposed from the DFT calculations that nanotube
confinements can modulate electronic and absorption properties of multimeric terthiophene
chains by changing the interchain interactions.

Fig. 1 Modulating the electronic properties of thiophene
multimers by utilizing carbon nanotube confinement.
[1] (a) M. A. Loi et al., Adv. Mater. 22, 1635 (2010). (b) L. Alvarez et al., J. Phys. Chem. C 115, 11898 (2011).
[2] H. Yamashita and T. Yumura, J. Phys. Chem. C 116, 9681 (2012).
[3] T. Yumura and H. Yamashita, submitted for publication.
Corresponding Author: Takashi Yumura
Tel: +81-75-724-7571, Fax: +81-75-724-7571
E-mail: yumura@chem.kit.ac.jp- 126 -

2P-35
Energetics and Electronic Structures of Carbon Nanotubes Encapsulating
Polycyclic Aromatic Hydrocarbon Molecules○Shota Kigure and Susumu Okada
Graduate School of Pure and Applied Sciences, University of Tsukuba,
1-1-1 Tennodai, Tsukuba, Ibaraki 305-8571, Japan
Single-walled carbon nanotubes (SWCNTs) can accommodate molecules or atoms within
their interior space. Tubular space inside CNT with the nanoscale diameter leads to unusual
ordered arrangements of encapsulated molecules and atoms. Indeed, C60s form
one-dimensional van-deer Waals chain inside the CNTs with interesting electronic properties
those are not expected from the simple sum of the constituent units [1]. Recently, polycyclicaromatic hydrocarbon (PAH) molecule, coronene, is also encapsulated into the SWCNT in
which the coronene molecules are coaxially aligned along the tube axis [2]. In this work, we
aim to elucidate the energetics and electronic properties of PAH molecules (coronene,sumanene, and coranulene) encapsulated into SWCNT based on density functional theory
with local density approximation.
Figure 1 shows an energy gain upon the encapsulation of PAH molecules inside the
SWCNTs as a function of the tube diameter. We found these molecules can be encapsulated
within SWCNTs with appropriate diameter: Optimum tubes for encapsulation is (17,0)CNT
for sumanene and coranulene, while the tube is (19,0)CNT for coronene, depending on the
diameter of these PAH molecules. The calculated encapsulating energies for the optimum
structures are about 1 eV per molecules
irrespective to the molecule species. The large
encapsulation energy is ascribed to the substantial
interaction between CH bond of PAH moleculesand π states of CNT. Indeed, the energy depends
on the number of CH bonds of PAH molecules.
We also check the stable mutual angle associatedto the tube axis and find that the encapsulated
PAH molecules are not tilted for the case of
coranulene and sumanen in contrast to thecoronene inside the CNT.
[1] S. Okada et al. Phys. Rev. Lett. 86, 3835 (2001)[2] T. Okazaki et al. Angew. Chem. Int. Ed. 50, 4853 (2011)
Corresponding Author: S. Kigure
Tel: +81-29-853-8233, Fax: +81-29-853-5924,
E-mail: skigure@comas.frsc.tsukuba.ac.jp- 127 -

Figure.1 Encapsulation energy (∆E) of PAH
within (n,0) CNT(n = 16~20).

2P-36Functionalization of Carbon Nanohorns
for Targeted Photo-Thermal Cancer Therapy○Minfang Zhang1*, Mei Yang1, Wuxio Ding1, Sumio Iijima 1, 2, Masako Yudasaka1*
1

National Institute of Advanced Industrial Science and technology 5-2, Tsukuba
Department of Material Science and Engineering, Meijo University, Nagoya

2

Carbon nanomaterials such as nanotubes and nanohorns have been extensively
investigated for applications in drug delivery system and photo-thermal cancer therapy.
Recently, the functionalization of single-wall carbon nanotubes (SWNTs) by coating with 90
kDa amphiphilic poly(maleic anhydride-alt-1-octadecene)-methoxy poly(ethylene glycol)(C18-PMH-mPEG) have shown a longer blood circulation and higher tumor accumulation due
to EPR effect in vivo [1]. The modification of SWNTs with a targeting agent, epidermal
growth factor (EGF) exhibited high active targeting efficiency to squamous cancer cells thatoverexpress EGFR [2]. Herein, we multiply functionalized carbon nanohorns (CNHs) with
C18-PMH-mPEG and EGF to realize a targeted photo thermal cancer therapy.
CNHs labelled by Gd2O3 particles [3] were non-covalently coated with C18-PMH-mPEG
and DSPE-PEG-EGF (named as p-CNH-EGF) as reported previously [1-2]. Gd2O3@CNHs
coated only with C18-PMH-mPEG (p-CNHs) was also used for control. The obtained samples
were dispersed in phosphate buffered saline and intravenously injected into mice that had
subcutaneously transplanted tumor. After samples injection for 24 h, the tumor on the flank ofeach mouse was irradiated with 808-nm laser for about 5 min every day for 7 days. The laser
irradiation markedly suppressed the tumor growth of mice with p-CNHs-EGF injected. These
results indicated that the EGF modification had efficiency on targeted photo-thermal cancer
therapy. However, the quantity of p-CNHs-EGF and p-CNHs in tumors were similar, about
2% of injection dose. This means that the quantity was not the reason for the high anti-tumor
effect of p-CNHs-EGF. We infer that the accumulation site of p-CNHs-EGF in tumor might
be different from that of p-CNHs, thereby caused the different effects of photo-thermal
therapy.
[1] J.T. Robinson, et al. J. Am. Chem. Soc. 134, 10664 (2012).
[2] A. A. Bhirde, et al. ACS Nano 3, 307 (2009).
[3] J. Miyawaki et al. ACS Nano 3, 1399 (2009)
Corresponding Author: M. Zhang and M. Yudasaka.
TEL/Fax: +81-29-861- 6290
E-mail: m-zhang@aist.go.jp (M. Zhang), m-yudasaka@aist.go.jp (M. Yudasaka).

- 128 -

2P-37
Quick charge/discharge properties of Li-ion battery using carbon-coatedcomposites of graphites, vapor grown carbon fibers, and carbon nanohorns○Ryota Yuge, Noriyuki Tamura, Takashi Manako, Kaichiro Nakano, and Kentaro Nakahara
Smart Energy Research Laboratories, NEC Corporation, Tsukuba 305-8501, JapanThe lithium-ion battery (LIB) is the most remarkable rechargeable battery for portableelectronics, electric vehicles (EVs), and plug-in hybrid electric vehicles (HEVs) [1]. Recently,
their applications in EVs and HEVs have been demanded especially, leading to increases inbattery size and capacity [2-3]. The demand for quicker charging of EVs has been increased
drastically for very long charge time. Therefore, the LIB operating at high-rates needs to be
developed to realize the above industrial applications [4-5]. In this study, we tried to preparenovel composites of graphite, vapor grown carbon fibers (VGCFs), and carbon nanohorns(CNHs) covered by carbon films (C-graphite/VGCF/CNH) for quick charge-discharge of LIB.
We also investigated the relationship between the structure of C-graphite/VGCF/CNH andelectrochemical rate-properties.
Graphite (1g), VGCFs (20 mg), and CNHs (20 mg) were dispersed in ethanol (40 ml) andstirred at room temperature for about 10 min. The mixture was filtered, and black powder was
obtained on the filter paper (graphite/VGCF/CNH). The mixture of graphite, vapor growncarbon fibers (VGCFs), and carbon nanohorns (CNHs) was heat-treated in Ar atmosphere andcarbon-coated by using a chemical vapor deposition (CVD) method.
Scanning electron microscopy observation showed that the graphite and/or VGCF in
C-graphite/VGCF/CNH had a smoother and rounder surface structure than those ofgraphite/VGCF/CNH. Thermogravimetric analysis also indicated that carbon film formed by
the CVD method combusted at 550ºC and the quantity of carbon film was about 4 wt%. The
C-rate properties of half-cell for C-graphite/VGCF/CNH were superior to those for the
mixture of graphite, VGCF, and CNHs (C-graphite/VGCF/CNH (discharge) : 3C/0.1C, 85%,
graphite/VGCF/CNH (discharge) : 3C/0.1C, 50%), accelerating a promising application for
quick charge-discharge of LIB. The details are shown in the presentation.
[1] M. Endo et al. Carbon 38, 183 (2000).
[2] Y. E. Hyung et al. J. Power Sources 81-82, 842 (1999).
[3] T. Horiba et al. J. Power Sources 97-98 719 (2001).
[4] H. Fujimoto, J. Power Source 195, 5019 (2010).
[5] R. Krishnan et al. Nano Lett. 11, 377 (2011).
Corresponding Author: R. Yuge
Tel: +81-29-850-1566, Fax: +81-29-856-6137
E-mail: r-yuge@bk.jp.nec.com- 129 -

2P-38Synthesis and TEM structural characterizations of AgI nanowires
formed inside carbon nanospace○Shihono Naruse1, Ryo Kitaura1.*, Suguru Noda2, Hisanori Shinohara1,*
1

Department of Chemistry & Institute for Advanced Research,
Nagoya University, Nagoya 464-8602, Japan2
Department of Applied Chemistry & School of Advanced Science and Engineering,
Waseda University, Tokyo 169-8555, Japan
α-phase of silver iodide (α-AgI) is one of the most promising candidates for solid-stateelectrolytes for various electrochemical devices due to its superionic conductivity. α-AgI
cannot exist, however, below 420 K, thereby limiting their applications. Recently, it wasreported that AgI nanoparticles with a diameter of 10 nm can retain α-phase even at 313 K,
where size and morphology of AgI presumably play an important role in this α-AgI
stabilization [1]. Low-dimensional AgI nanostructures thus can act as a superionic conductor
at room temperature that is potentially important in the field ofelectrochemical devices.
To synthesize low-dimensional AgI nanostructures, we haveused one-dimensional (1D) nanospace of carbon nanotubes(CNTs). CNTs have unique 1D nanospace ranging in diameterfrom 0.4 to 50 nm, which can stabilize otherwise unstablephases of nanomaterials. Here, we present a high yield
synthesis and TEM structural characterization of AgI nanowires
that are formed in nanospace of CNTs with various diameters.
We have synthesized AgI nanowire encapsulated in CNTs
(hereafter designated as AgI@CNTs) by the sublimation
method reported previously [2]. Figures 1 (a) and (b) show
low-magnification high resolution transmission electron
microscope (HR-TEM) images of CNTs and AgI@MWCNTs [3].
In contrast to empty CNTs, the image of AgI@MWCNTs
clearly shows dark areas overlapping with the CNTs. An
estimated filling ratio of AgI is as high as ca. 80 %. Figure (c)shows high magnification HR-TEM images of AgI nanowire
synthesized wthin MWCNT with an inner diameter of 9.0 nm.
The figure clearly shows dark spots aligned in the MWCNT ina perfectly regulated fashion.
In the presentation, we will discuss the details on the synthesisof various AgI nanowires and characterizations of theirstructure using HR-TEM and HAADF observations.
[1] R. Makiura, et al., Nature.Mater. 8, 476 (2009).
[2] R. Kitaura, et al., Angew.Chem.Int.Ed. 48, 8298 (2009).
Fig. 1 HR-TEM images of[3] R. Kitaura, et al., Nano Res. 1, 152 (2008).
(a) empty MWCNTs(b) (c) AgI@MWCNTs
Corresponding Author: Hisanori Shinohara
TEL: (+81)52-789-2482, FAX: (+81)52-747-6442, E-mail: r.kitaura@nagoya-u.jp, noris@ nagoya-u.ac.jp- 130 -

2P-39High-yielding synthesis of graphene by supuercritical fluid○Nobuto Oka 1, Takaaki Tomai 1, Itaru Honma 1
1

Institute of Multidisciplinary Research for Advanced Materials, Tohoku University,
Sendai 980-8577, Japan

Graphene is a monolayer of sp2-bonded carbon atoms arranged in a dense honeycomb
crystal structure, which exhibits remarkable electronic, optical, thermal, and mechanicalproperties. These absorbing properties make graphene the most promising candidate forvarious applications in many fields, such as electronic and optical devices, and energy storage
in batteries. A mass production technique of high-quality graphene is indispensable for manyof these applications. Recently, we have reported a novel supercritical fluid (SCF) method forthe exfoliation of graphite to obtain high quality and high yield graphene sheets [1-3]. SCF
has unique characteristics such as a low interfacial tension, excellent surface wetting, and highdiffusion coefficients. Solvent molecules in SCF state diffuse between the graphene layers inbulk graphite and expand the interlayer distance. Consequently, graphene sheets are exfoliatedfrom graphite crystals.
In this study, the flow-through reactor for graphite flakes dispersed in ethanol has beendeveloped for the purpose of mass production and much higher yield, as shown in fig. 1 [4]. A
repeat of specific temperature profile, temperature rise and rapid quench, leads to bettersynthetic efficiency of graphene, amounting to improvement by one digit or more ascompared to before. On the other, the conventional chemical exfoliation method, known as
modified Hummers' method, is widely used as the mass production technique. It involves anoxidation process, resulting in the formation of defective graphene sheets. The supercriticalfluid exfoliation method, developed in this study, denotes the direct conversion from graphite
crystals into much less defective graphene since this method does not require the oxidation
process. This mass production technique of high-quality graphene should contribute to thedesirable growth of various industrial applications.
[1] D. Rangappa, K. Sone, M. Wang, U. K. Gautam, D.
Golberg, H. Itoh, M. Ichihara and I. Honma, Chem.
Eur. J. 16, 6488- 6494 (2010).
[2] J.-H. Jang, D. Rangappa, Y.-U. Kwon and I. Honma,
J. Mater. Chem. 21, 3462-3466 (2011).
[3] T. Tomai, Y. Kawaguchi and I. Honma, Appl. Phys.
Lett. 100, 233110 - 233110-4 (2012).
[4] http://www.sdk.co.jp/assets/files/news/2013/sdkrelea
se20130110.pdf

Fig.1 Schematic diagram of flow-throughsupercritical fluid method

Corresponding Author: N. Oka, I. Honma
Tel: +81-22-217-5816, Fax: +81-22-217-5828,
E-mail: n.oka@tagen.tohoku.ac.jp,
i.honma@tagen.tohoku.ac.jp- 131 -

2P-40Fabrication of wide terraces on SiC (0001) for pit-freegraphene growth in Ar atmosphere○Wang Chenxing, Hitoshi Nakahara, Koji Asaka, and Yahachi Saito
Department of Quantum Engineering, Nagoya University, Furo-cho, Nagoya 464-8603, Japan

Average width of terraces (μm)

According to the current experimental studies on thermal decomposition of SiC (0001)
surfaces, morphology of SiC substrate surfaces after graphene growth depends on annealing
conditions, such as inert gases and their pressure, and annealing temperature and duration. In
the present study, the SiC substrates are annealed at various temperatures and at variouspressures of argon (Ar) atmosphere, and the processes of annealing the SiC substrates areinvestigated by in situ scanning tunneling microscope (STM) to reveal the most appropriate
annealing condition for forming wide terraces and pit-free graphene on SiC.
Before the forming of graphene layers on SiC surfaces, the terraces keep growing due
to the step bunching. Figure 1 shows the temporal evolutions of the average width of terraces
at different temperatures at 0.1 atm of Ar atmosphere, and the largest increasing rate of terrace
widths was observed at 1400℃. In the annealing processes at 0.5 and 1atm of Ar atmosphere,
the largest increasing rate of terrace widths was also observed at 1400℃. The temperatureappropriate for promoting step bunching was found to be 1400℃, while Ar pressure did notshow any significant effect on this process.
On the other hand, we observed that Ar pressure played an important role forsuppressing the formation of pits after graphene growth. The density of pits decreases
dramatically with increasing the pressure of Ar atmosphere. Figure 2 shows a STM image ofgraphene on SiC substrate which was heated at 1400℃ for an hour, and then graphene wasgrown at 1 atm of Ar atmosphere. The uniform graphene covered almost the whole surface ofthe 4-μm-width terrace without the growth of pits.
5

1500℃
1450℃

4
3

1400℃

2

1300℃

1
0

10

20

30

40

50

Annealing time (min)Fig. 1 Average width of terraces versus annealing

1μmtime for various annealing temperatures. Ar
pressure during annealing was 0.1 atm.

Fig. 2 STM image of graphene grown on
SiC surface. The substrate was annealed atCorresponding Author: Wang Chenxing
Tel: +81-52-789-3714, Fax: +81-52-789-3703,
E-mail: cx-wang@surf.nuqe.nagoya-u.ac.jp

1400℃ for an hour, and then graphene
was grown at 1 atm of Ar atmosphere.

- 132 -

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+0&1+        2                     $%'34   

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$&'7 #    -5*&556,$-'"(89 89:8; <8! 

$/'> ?7    /@A6*&5%-,!  

# B<  C                 (BD=%-E&&==&//; 2BD=%-E&A%%5&-. B  F    G- 133 -

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2P-42
Interface structures between graphene and SiC
formed in the nitrogen atmosphere○Yoshiho Masuda, Wataru Norimatsu and Michiko kusunoki
1

Department of Applied Chemistry, Nagoya University, Nagoya 464-8603, japan
2
Eco Topia Science Institute, Nagoya University, Nagoya 464-8603, Japan

Introduction
Epitaxial graphene on silicon carbide (SiC) is synthesized by Si sublimation of the SiC
substrates in a vacuum at high temperature, which is a very promising method forhomogeneous large scale production with a high crystalline quality [1]. In particular, higher
quality graphene was obtained when the decomposition process is progressed in the Ar
atmosphere, which suppresses the sublimation of Si [2]. However, the carrier mobility ofgraphene grown on SiC (0001) is reduced by the influence of the SiC substrate. So, it isimportant to modify the interface structure between graphene and SiC for obtaining the higher
mobility. In this study, we aimed to grow homogeneous graphene in the atmosphere ofanother inert gas, N2, and investigated its interface structure.
Experimental Procedures
Single-crystal wafers of 6H-SiC (0001) were heated to 1600~1800 °C and held at thistemperature in the mixed gas of N2 and Ar. For comparison, the substrates were also heated in
the Ar atmosphere. The observations were carried out using Topcon EM-200B andARM200F-type transmission electron microscopes.
Results and Discussion
After heated at 1700 °C in the mixed gas of N2 and Ar, few layers graphene was formed on
SiC surface. Interestingly, periodic contrasts were also observed at the interface between thegraphene and the SiC substrate [Figure 1(a)], which had never been observed for graphene
formed in the Ar atmosphere [Figure 1(b)]. And we also discovered that two types of nitrided
interface structure were formed by decomposed SiC in the presence of nitrogen gas. In thepresentation, we will report the origin of the periodic contrasts and introduce these two typesof nitrided structures.

Figure 1 TEM images of graphene formed in (a) the Ar and (b) the mixed gas of N2 and Ar.
[1] W. Norimatsu and M. Kusunoki. Phys. Rev. B 81, 161410 (2010).
[2] K. V. Emtsev et al. Phys. Rev. B 77, 155303 (2008).
Tel: +81-52-789-5859, Fax: +81-52-789-5859,
E-mail: masuda.yoshiho@a.mbox.nagoya-u.ac.jp- 134 -

2P-43
Preparation of multilayer graphene nanoribbons on very narrow graphene
templates of unzipped DWCNTs○H. Kitakawa1, R. Negishi1, H. Tanaka2, M. Fukumori2, T. Ogawa2, Y. Kobayashi1
1Department of applied physics, Osaka University, Suita 565-0871, Japan2
Department of Chemistry, Osaka University, Toyonaka 560-0043, Japan
Corresponding Author: E-mail: negishi@ap.eng.osaka-u.ac.jp

References: [1] Y. Ouyang, et al., Nano Research 3 (2010)8. [2] S. R.
Dhakate et al., Carbon 49 (2011) 4170. [3] X. Li, et al., Science 319(2008)1229. [4] R. Negishi, et al., Thin Solid Films 519 (2011)6447.
Acknowledgement: Authors would like to thank Prof. K. Matsumoto(Osaka Univ.) for supporting AFM measurements.

- 135 -CountsCountsHeight(nm)Multilayer graphene nanoribbons (M-GNRs) with weak interlayer coupling such as
turbostratic structures are promising candidates for channel materials in field effect transistors(FETs) because the multilayer channels lead to high-current gain [1] in addition to band gap
opening between graphene Dirac cones due to the electron confinement. M-GNRs can besynthesized by unzipping multi-wall carbon nanotubes (CNTs), but their width becomes
relatively large [2]. As a result, it is difficult to observe the band gap opening and control thelayer numbers. In this work, we report the M-GNR synthesis by graphene growth on narrowdouble-layer GNRs with several nanometers width, which are prepared by unzipping
double-wall CNTs (DWCNTs).
GNRs as growth templates were obtained from unzipping of DWCNTs [3]. Graphene
layers were grown by chemical vapor deposition (CVD) using a furnace with threetemperature zones, in which temperatures for carbon feedstock decomposition and graphene
growth can be controlled individually[4]. The temperatures used for thermal decomposition
and graphene growth were 900 ºC and 720-735 ºC, respectively. Thickness of the growngraphene was evaluated by atomic force microscopy (AFM).
Figure 1 shows the AFM images obtained from the GNR (a) before and (b) after CVD
growth, and (c) height profiles of the GNR along L-L’. Before the growth, the layer numbersof the GNR estimated from the AFM image is mono or bilayer [3]. The height of the GNR
increases from ~0.7 to ~1.7 nm after growth. This result indicates that the multilayer GNR
with 2~3 layers is formed by the growth. Figure 2 shows
(a)
(b)
L
L
the height and width distributions of the GNR before andL’
L’
after growth. The median height and width of M-GNRs
increase from 1.2 to 1.6 nm and 25 to 50 nm after growth,
200nm
200nm
respectively. These results indicate that the growth rate at
3 (c)Beforeedge sites is higher than that at terrace sites of GNR
After
2
L’
templates, and that the edge sites are active sites forL1
adsorption of carbon species compared with terrace sites.
In addition to that, the surface roughness on the GNR is
00
100
50
150
not changed before and after growth, and is atomicallyDistance(nm)flat. This result means that the growth of graphene layers Fig.1 AFM images of GNR (a) before(b) after growth. (c) Height profiles
is proceeded via layer-by-layer mode, and is consistent andalong L-L'.
with the graphene layer growth on the graphene prepared8(a)Before12 (b)
Beforeby mechanical exfoliation[4]. More works are necessary
6
After
After
for elucidation of the growth mechanism of the M-GNRs
84
to control the layer number and width.
CNT
4
2

0
0

1

2

Height(nm)

3

0

0

20

40

60

Width(nm)Fig.2 (a)Height and (b)width
distributions of GNRs before andafter growth estimated from AFM
observations.

2P-44
Flexible transistor and inverter of large-area WSe2 thin film
○Kazuma Funahashi1, Jiang Pu 1, Lain-Jong Li 2, Yoshihiro Iwasa 3,4, Taishi Takenobu 1,5
12

Department of Applied Physics, Waseda University, Shinguku 169-8555, Japan
Institute of Atomic and Molecular Sciences, Academia Sinica, Taipei 11529, Taiwan
3
Department of Applied Physics, The University of Tokyo, Tokyo 113-8656, Japan
4
RIKEN Center for Emergent Matter Science (CEMS), Wako 351-0198, Japan
5
Kagami Memorial Laboratory, Waseda University, Tokyo 169-0051, Japan

Atomically thin films of transition metal dichalcogenides (TMDCs) are promising
candidates for flexible devices complementing graphene due to their extraordinary properties
such as high on/off switching ratio, sizable bandgap, and flexibility. Actually, highly flexible
transistors based on molybdenum disulfide (MoS2), one of the TMDCs, have been reported[1-3] and proved the usefulness of TMDCs in flexible electronics. Although logic circuit (e.g.
CMOS inverter) is strongly required for further application, commonly-used MoS2 is notsuitable because of their n-type unipolar conduction. For logic application, p-type orambipolar flexible transistors are additionally necessary. Therefore, in this study, we focus ontungsten diselenide (WSe2) which is known as ambipolar TMDC semiconductor [4]. Usingchemically grown WSe2 and electrolyte-gating method, we fabricate flexible ambipolartransistors and CMOS-like inverters.
WSe2 thin film was synthesized by chemical vapor deposition [4] and was transferred onto
flexible polyimide substrate. We fabricated WSe2 electric double layer transistors (EDLTs)
using flexible gate insulator, ion gel, and they showed ambipolar operation as reported [4].
This realization of WSe2 ambipolar transistors allowed us the development of CMOS-likeinverters because the inverters can be achieved by combining two identical ambipolartransistors together, as shown in Fig. 1 [5]. We applied this method into WSe2 ambipolar
flexible transistors and realized flexible inverters (Fig. 2). The device revealed gain ~17,
which is sufficient to drive next stage components in a logic circuit.
In summary, we have demonstrated flexible inverter based on WSe2 ambipolar EDLTs,
which is important first step for the next-generation flexible devices.

Fig.1 Schematics of WSe2 flexible inverter (left) and equivalent circuit (right)

Fig.2 Inverter characteristic[1] J. Pu, T. Takenobu et al. Nano Lett. 12(8), 4013–4017 (2012), [2] G. H. Lee et al, ACS Nano 7(9), 7931–7936 (2013),[3] H. Y. Chang et al, ACS Nano 7(6), 5446–5452 (2013), [4] J. K. Huang, J. Pu, T. Takenobu et al., ACS Nano, DOI: 10.1021/nn405719x,[5] E. J. Meijer et al, Nat. Mater. 2, 678–682(2003)
Corresponding Author: Taishi Takenobu, Tel&Fax: +81-3-5286-2981, E-mail: takenobu@waseda.jp- 136 -

2P-45
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'1)    3   1)  1  3 &'  1'1)     3'2  37 8     1'  '+)  3    3'   '   '         '     )  '  ' ''  56    02   ' ''  56&  1'2 3       '1      ' '2 ) 1 211'01  '
   '1 32-'     ' 
2 1 ' 3       9 '    '' 3 1' '1)  1'2  1' 01
 ,   & *)                 
11  '       -'3 '    '''   1 1 215 2161' '        
56 -)      ' 
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1' 212.             12 4'  01    '   
31   4! 3  ' 


7*8$!%&'( ,3 ):;: 5 <*=6
7 8,  ,!)*<==;5 <*=6               
''1, ' /,         !"    - >?*@ ;?=A?*A)&0 >?*@ ;?=A?*A) "  B +2.1

- 137 -

2P-46
Mechanism of photoluminescence in graphene oxideżHiroyuki Yokoi1,2, Takaaki Taniguchi1,2, Michio Koinuma1,2, Yasumichi Matsumoto1,2
1

Graduate School of Science and Technology, Kumamoto University, Kumamoto, 860-8555,
Japan
2
JST, CREST, K’s Gobancho 6F, 7 Gobancho, Chiyoda-ku, Tokyo, 102-0076, Japan

Graphene oxide (GO) is graphene-like material which can be produced through oxidationof graphite. Carbon atoms in the basal plane or on the edges of GO are partially modified withfunctional groups containing oxygen. One of the interesting features of this material is toexhibit photoluminescence (PL) in a wide spectral range between near-infrared and blue
depending on the degree of oxidation or reduction [1]. A lot of researches have been
conducted to investigate the PL properties and mechanisms. However, the PL mechanisms
have not been clarified fully yet. In a recent model, for example, it is thought that excitation
occurs between SS* bands, and that red and blue
emissions are induced through defect levels induced bymodification with functional groups and quantum levelsin sp2 quantum dot produced by reduction, respectively[1]. However, it is inexplicable with this model that PL
excitation spectra for red and blue emissions are different.
In this work, we aim to clarify the PL mechanisms
through ab initio calculations with realistic structuralmodels for GO, where an sp2 quantum dot is embedded infully epoxidated area. We arranged the relative
configuration of the epoxy groups as stably as possible[2]. In the calculations of structure relaxation andelectronic states, we have employed the Vienna Ab Initio
Simulation Package (VASP) [3]. Figure 1 shows theelectronic structure of a GO sheet with a coronene-type
sp2 quantum dot (Region A in Fig. 2). HOMO and LUMO Fig. 1 Band structure of GO with awere Sand S* states localized in the quantum dot. We coronene-type sp2 quantum dot.
have found that a state locating at around 1.2 eV above
LUMO spreads both in the quantum dot and in thespecific epoxidation structure, where all epoxides arearranged outward from a six-membered carbon ring as
shown in Fig. 2. This structure appears in the fully
epoxidated area inevitably. We have considered that it
could work as an excitation site in the blue emission. We
will also report a model for the red emission, andexperimental results to examine these models.
[1] C.-T. Chien et al. Angew. Chem. Int. Ed. 51, 6662 (2012).
[2] G. Kresse and J. Furthmüller, Phys. Rev. B 54, 11169 (1996).
[3] M.-T. Nguyen et al. Phys. Rev. B 86, 115406 (2012).
Corresponding Author: H. Yokoi
Tel: +81-96-342-3727, Fax: +81-96-342-3710,
E-mail: yokoihr@kumamoto-u.ac.jp- 138 -

Fig. 2 The employed structure modeland partial charge density of a state
above LUMO by 1.2 eV. A: quantum
dot area; B: six-membered ring area
where epoxides are arranged outward.

2P-47
Mechanisms of Near-Infrared Photoluminescence from Graphene Oxides○Daichi Kozawa1, Yuhei Miyauchi1,2, Shinichiro Mouri1, Masao Ichida3,
and Kazunari Matsuda1
1Institute of Advanced Energy, Kyoto University, Uji, Kyoto 611-0011, Japan
Japan Science and Technology Agency, PRESTO, 4-1-8 Honcho Kawaguchi, Saitama
332-0012, Japan
3
Faculty of Science and Engineering, Konan University, 8-9-1 Okamoto, Higashi-Nada-ku,
Kobe 658-8501, Japan
2

PL Intensity (arb. units)

Graphene oxide (GO) is one of the graphene related materials, and has attracted interests
because of a finite band gap[1]. The availability of oxidation and reduction for GO enables
tunable photoluminescence (PL) in the broad range of UV–visible–near-infrared (NIR) as aresult of the inhomogeneous structure. In our previous study, it has been revealed that UV andvisible PL from GO originate from the quasi-molecular-like small sp2 fragments embedded inGO[2]. However, the physical mechanism of NIR PL in GO has been still controversial. In
this study, we have investigated mechanisms of NIR PL from GO produced by modified
Hummer's method using steady-state and time-resolved spectroscopy.
Figure 1 shows PL spectra of GO in aqueous solution with excitation at various photon
energies from 1.8 to 2.5 eV, where the arrows indicate the excitation photon energies. The PL
spectrum of GO shows a broad emission peak in NIR region (1.7 eV), and the gradual
blueshift and broadening of emission peaks are observed with increasing the excitation energy,
which is also observed in the PLE map as shown in the inset of Figure 1. We attribute the NIR
PL to the electron-hole pair recombination in various size and shape of graphene nanodisc(sp2 carbon cluster) states embedded in GO, in which the nanodisc states have various band
gap corresponding to their structures.
To further verify the mechanisms of the
NIR PL, we conducted time-resolved PL
12measurements. The longer PL decay time andbuild-up are observed at lower emission
10
energy. This result suggests that the energy
transfer from small to adjacent larger carbon
8cluster states embedded in a GO. These
6
provide us further insights into tunable opticalproperties toward GO-based optoelectronic4
devices.
2
References
0[1] Eda, G.; Fanchini, G.; Chhowalla, M., Nat.
1.6 1.8 2.0 2.2 2.4
Nanotechnol. 2008, 3, 270-274.
Emission Photon Energy (eV)[2] Kozawa, D.; Miyauchi, Y.; Mouri, S.; Matsuda, K.,
J. Phys. Chem. Lett. 2013, 4, 2035-2040.

Corresponding Author: D. Kozawa
Tel: +81-774-38-3465, Fax: +81-774-38-3467,
E-mail: d-kozawa@iae.kyoto-u.ac.jp- 139 -

Fig. 1 PL spectra with various excitationenergies of GO in aqueous solution. The arrow
indicate the excitation energy for each PL
spectrum. The inset shows PLE map.

2P-48
Molecular dynamics simulation for water molecules
between two graphene layers○Riichiro Saito1, Masashi Mizuno1
1

Department of Physics, Tohoku University, 980-8578, Japan

Water molecules in nano carbon materials show an interesting behavior which is notobserved in conventional ice. A famous example is the water molecules confined in single
wall carbon nanotubes (SWNTs) which is called ice nanotube in which melting temperatureand lattice structure of ice depend on the diameter or chirality of SWNTs [1,2,3]. The changeof physical properties in the ice nanotube is understood by (1) the confinement of moleculesin nano-meter size and (2) interaction between carbon and water molecules. Here we would
like to discuss water molecules confined in two graphene layers. Compared with ice
nanotubes, the confinement of water molecules in the direction of graphene plane can berelaxing by increasing the inter-layer spacing, while we expect some pressure in the direction
perpendicular to graphene plane by van der Waals interaction between the two graphene
layers. However, a qualitative understanding for water molecules between two graphene
layers is not easily obtained by some analytical discussion or phenomenological theory. In
order to get a realistic picture of motion of water molecules and carbon atoms at a givetemperature, we performed molecular dynamics simulation using a package so called
LAMMPS. LAMMPS is open and free software working on Linux machine and LAMMPS is
widely used not only in physics but also polymer science or even biology. Here we will show
some preliminary results by animation and show what is happening in the system. It should be
noted that we just start this project and that we would like to discuss with many people forpossible direction of the research.
The authors acknowledges Prof. R. Kitaura, Nagoya University for important discussion ofthis subjects and MEXT grant (SATL, No. 25107005).
References:[1] K. Koga et al., Nature 412, 802 (2001).
[2] Y. Maniwa et al. JPSJ 71, 2863 (2002).
[3] D. Takigawa et al. PNAS 105, 39 (2008).

Corresponding Author: R. Saito
Tel: +81-22-795-7754, Fax: +81-22-795-6447,
E-mail: rsaito@flex.phys.tohoku.ac.jp

Water molecules between two graphene layers at
100K by LAMMPS simulation. Because of theperiodic boundary condition, the bottom layer
does not deform.

- 140 -

2P-49Formation of fullerenes and polyynes
by graphite laser ablation in ambient gases○Yurika Abe, Hitomi Endo, Yohji Achiba, Haruo Shiromaru
Department of Chemistry, Tokyo Metropolitan University, Hachioji, 192-0397, Japan
Carbon clusters formed by laser ablation of graphite are sorted into three main
structural categories, namely linear chains, monocyclic rings, and fullerenes. In thepresent study, we examined macroscopic production of linear chains and fullerenes bylaser ablation of a graphite disk in argon gas flow at room temperature, in which theformers were in fact obtained as the polyynes. Laser ablation was performed in a glass
tube with a cone-shaped exit for argon gas, which carried the ablation products to a coldorganic solvent in a glass bottle. Then, soluble products were analyzed by UV
absorption.
A typical UV spectrum of the hexane solution
prepared by ablation at the graphite surface parallelto the gas flow is shown in Fig.1, together with thatof pure C60 solution. As can be seen in the figure, acharacteristic band of C60 appears around 330nm,
indicating formation of considerable amount ofsoluble C60. Among strong unassigned absorption
bands, characteristic peaks of polyynes are also
identified. It shows coexistence of linear-form
carbons and fullerenes in the cluster source. When theablation surface was set so as to let the clusters to beejected toward the exit, polyynes were preferentiallyFig. 1 (a) Absorption spectrum of
hexane solution prepared by 30 min.
irradiation of 300mJ/pulse ns laser.
Assignment is indicated in the figure.
(b) Absorption spectrum of hexane
solution of pure C60.

produced, as demonstrated by the spectrum A in
Fig.2.
It should be noted that the addition of ahydrocarbon (propane) to the ambient argon gas
drastically enhances the polyyne yield as shown in
the figure. It offers clear evidence that thesepolyynes are produced by gas-phase reactions.
Fig. 2 Absorption spectra of hexane

solution prepared by 10 min.
irradiation of 150mJ/pulse ns laser.
The ambient gases are (A) pure argon,(B) with propane, (C) with higher
flow rate of propane.

Corresponding Author: H. Shiromaru
Tel: +81-42-677-1111, Fax: +81-42-677-2525,
E-mail: shiromaru-haruo@tmu.ac.jp- 141 -

2P-50Vibronic interaction in the forbidden transition of polyyne molecules○Tomonari Wakabayashi
Department of Chemistry, Kinki University, Higashi-Osaka 577-8502, JapanThe π-π* excitation in a conjugate linear polyyne molecule gives rise to three excited states. The
electric-dipole transition from the ground state is fully allowed for the one, but symmetry
forbidden for the other two. However, vibronic coupling allows the latter two some transitions
weakly. In order to understand spectral features appearing in the vibronic transition, symmetry
considerations are useful. Using Herzberg-Teller expansion, matrix elements in the vibronic
coupling scheme were examined for the symmetry-forbidden transition. As an example, we chosethe HOMO-LUMO excitation for hydrogen-end-capped polyyne molecules, H(C≡C)nH (n≥2),
and compared the results to the observed absorption and emission spectra [1].
Pronounced features in the absorption and emission spectra were those comprising avibrational progression for a totally symmetric vibrational mode of σg, while the inducing mode
was πg. Depending on the direction for the transition dipole, or the symmetry of the intermediate
state for the intensity borrowing, the number of vibrational quanta necessary for inducing thevibraonic transitions is different. This is crucial for locating the missing origin for the forbidden
transition. Symmetry considerations are made to discuss the assignment of the missing origin in
the forbidden transition for the centrosymmetric linear polyyne molecule [2].
(a)

Πu 0

8

molecules C2nH2 (n=5-8), Chem. Phys. Lett. 446, 65-70

Πg(2007).
[2] T. Wakabayashi, Y. Wada, N. Iwahara, T. Sato: Vibronic

ic (

∆g

)
2

πg
πg
0 ∆u

for

bid

den

+2)
ron
ic (
vib

2

2

πg

+2

(+1)

4

allowed (z)ronallowed (z)Transition Energy / eV

)

vib

+1)

0

nic (

+

Σu

ed (x,yCorresponding Author: T. Wakabayashi
Tel: +81-6-4307-3408, Fax: +81-6-6723-2721,
E-mail: wakaba@chem.kindai.ac.jp

allow

molecules, J. Phys. Conf. Ser. 428, 012004 (2013).

6
vibro

bands in the HOMO-LUMO excitation of linear polyyne

πgallowed (x,y)

K. Hashimoto: Laser induced emission spectra of polyyne

vibronic[1] T. Wakabayashi, H. Nagayama, K. Daigoku, Y. Kiyooka,

+

0

+

Σg

0

∆u ← Σgabsorption

Fig. 1. Schematic diagram for vibronic transitionsin polyyne molecules, showing intermediate states.

- 142 -

3P-1
Thermal Bis-silylation, Carbosilylation, and Bis-germylation of Fullerenes○Daiki Inaba1, Kazuya Minami1, Kyosuke Miyabe1, Ryosuke Iida1, Masahiro Kako1,
Yutaka Maeda2, Michio Yamada2, Tadashi Hasegawa2, Takeshi Akasaka3
1

Department of Engineering Science, The University of Electro-Communications, Chofu,
Tokyo 182-8585, Japan2
Department of Chemistry, Tokyo Gakugei University, Koganei, Tokyo 184-8501, Japan
3
Life Science Center of Tsukuba Advanced Research Alliance, University of Tsukuba,
Tsukuba, Ibaraki, 305-8577, Japan

Chemical functionalization of fullerenes has been attracting much attention from bothmechanistic and synthetic viewpoints. Introduction of heteroatoms such as electropositive
silicon has been known to an effective method to modify the electronic characteristics ofhollow fullerenes and endohedral metallofullerenes. The facile silylation reactions offullerenes have been described using reactive silicon compounds such as silylenes, disiliranes,
and silyl radicals. Electrochemical analyses and theoretical calculations have disclosed thatthe silylated fullerene derivatives have more negative charge on the cage than the parent
fullerenes. Such derivatization of fullerenes would contribute to the application of fullerenes
as functional materials. For example, a silirane derivative of C60 with a higher LUMO isexpected to be a promising compound to increase the open-circuit voltage of organic solar
cells. However, silylation of C60 and C70 have been limited to photolytic reactions using
ultraviolet irradiation and nucleophilic addition of anionic silicon reagents, in which
degradations of silylated products take place disadvantageously under those conditions.
Therefore, alternative procedures for silylation of fullerenes are desirable for developmentof various silylated fullerene-based materials. Recently, thermal addition of endohedral
metallofullerenes with disiliranes, siliranes, and silylenes have been demonstrated to afford
the corresponding silylated derivatives.[1-3] In addition, thermal reactions of C60 withsiliranes have been reported by employing thermally generated silylenes as the silylating
reagent. As our continuing research of functionalization of fullerenes, we have conducted thebis-silylation and bis-germylation of C60 and C70 under non-photolytic conditions. Although
the silylene addition and bis-silylation of C70 under photolytic conditions have been described
previously, such examples are rather sparse. Herein we report the thermal reactions of C60 and
C70 with disilirane, digermirane, and siliranes, indicating that bis-silylation, bis-germylation,
silylene addition, and carbosilylation of C60 and C70 proceed at higher temperatures without
photoirradiation.(Schemes 1, 2)         
Scheme 1.

Scheme 2.
R
R

C60, C70

+

R
M

M

!

R
R
M = Si, R = mesityl
M = Ge, R = 2, 6-diethylphenyl

R
Dip

M
C70

C60, C70

Si

R

Dip

!
C70

Dip

M
R

+

Si
Dip

Dip = 2, 6-diisopropylphenyl[1] Y.Iiduka et al. J. Am. Chem. Soc. 127, 9956–9957(2005). [2] M. Yamada et al. J. Am. Chem. Soc. 127,
14570–114571(2005). [3] M. Yamada et al. J. Am. Chem. Soc. 132, 17953–17960(2011). [4] K. Sato et al. J. Am.
Chem. Soc. 134, 16033–16039(2012).
Corresponding Author: Masahiro Kako Tel: +81-42-442-5570  E-mail: kako@e-one.uec.ac.jp- 143 -

3P-2
Synthesis of [60]Fullerene Derivative with 1,3-Dipolar Cycloaddition as a
Novel Structure for Bulk-Heterojunction Photovoltaic Cells○Hisashi Tokutomi1, Masaru Sekido2

1

Division of Production System and Design Engineering, Advanced Engineering Course,
Sendai National College of Technology, Natori, 981-1239, Japan.
2
Department of Materials and Environmental Engineering, Sendai National College ofTechnology, Natori, 981-1239, Japan.

Bulk-Heterojunction (BHJ) solar cell is expected to be the lightweight, flexible, andpotential low cost solar cell. To overcome low power conversion efficiency of BHJ solar cellcaused by lower crystal orientation, [1] novel structure of BHJ solar cell model for highcrystal orientation using Linked C60 (L-C60) is designed (Figure 1).

Linked-C60 dyad (L-C60)

Figure 1. Novel structure of BHJ solar cell model (Wide arrow is electron transfer way).

L-C60 is the C60 dyads containing sebacoyl carbon chain and AS (aniline and sebacoyl
carbon chain) as a spacer. L-C60 is expected to interact with the crystal part of P3HT
(poly(3-hexylthiophene-2,5-diyl)) to help its crystal orientation to give high power conversion
efficiency. AS spacer was synthesized by using aniline and sebacoyl chloride (29% isolated
yield). Functionalized-C60 (F-C60) was synthesized by Prato reaction [2.3] (24% isolated
yield) and F-C60 was then reacted with AS spacer to form L-C60 (64% reacted yield). Figure 2
is 1H NMR shift of AS spacer and reacted compound. According to 1H NMR spectrum, thepeak of AS spacer was observed at reacted compound. Since non-reacted AS spacer waswashed by acetone, AS Spacer and F-C60 was stacked by π-π stacking. By using thedeveloped methods is also applicable to synthesize other C60 dyads containing various
spacers.
b)a)

Figure 2. 1H NMR shift of AS spacer (a) and reacted compound (b)[1] Chem. Mater. 2010, 22, 5371-5376.
[2] J. Am. Chem. Soc. 1993, 115, 9798-9799.
[3] J. Am. Chem. Soc. 2008, 130, 8733-8740.

Corresponding Author: H. Tokutomi
Tel: +81-22-381-0329, Fax: +81-22-381-0329
E-mail: a1301019@sendai-nct.jp- 144 -

3P-3
Electrochemical synthesis of Li@C60 supraatom○Hiroshi Ueno 1, Naohiko Ikuma 1, Kei Ohkubo 2, Hiroshi Moriyama 3, Shunichi Fukuzumi 2,4,
Ken Kokubo 1
1

Division of Applied Chemistry, Graduate School of Engineering, Osaka University,
2-1 Yamadaoka, Suita, Osaka 565-0871, Japan.
2
Department of Material and Life Science, Graduate School of Engineering, Osaka
University, and ALCA, Japan Science and Technology (JST), Suita, Osaka 565-0871, Japan3
Department of Chemistry, Faculty of Science, Toho University, 2-2-1 Miyama, Funabashi,
Chiba 274-8510, Japan
4
Department of Bioinspired Science, Ewha Womans University, Seoul 120-750, Korea
The ionic nature of Li+@C60 is one of the remarkable characteristics among allreported endohedral metallofullerenes [1,2]. The ionic property makes it an open possibility toapply as electrolyte in suitable organic solvents such as o-dichlorobenzene (o-DCB) andbenzonitrile, and we have succeeded in the electrochemical synthesis of Li+-encapsulated C60
radical anion without any supporting electrolytes [3]. However, the isolation andcharacterization of the obtained Li+@C60•– were still insufficient for its further application due
to its lower concentration and difficulty in isolation process. On the other hand, counter
anion-exchanging is one of the chemical modifications of Li+@C60 salts to give higher
solubility in several organic solvents [4]. Such improved solubility can lead Li+@C60 to more
applicable solution processes including our electrochemical application. As a continuinginterest of our studies on the ionic properties of Li+@C60 salts, we herein report the ionic
conductivity of several Li+@C60 salts, electrochemical synthesis, and complete isolation of
Li+@C60•– based on the large solubility difference between Li+@C60 salts and Li+@C60•–.
All measured samples showed enough high ionic conductivity for electrochemical
CathodeAnodereduction of Li+@C60 cation. On thesynthesis of Li+@C60•– using CH2Cl2
Pt
electrode
0.3 mA
solution of [Li+@C60](NTf2–)*, only the(Constant)≡product was deposited on the surface of
253 K
2 dayscathode due to the lower solubility ofthe product for the solvent used (Figure1). Through NIR, EPR, NMR, and•–ElectrochemicallyRaman spectroscopy, the deposited
reduced around cathodesample was fully characterized as
NTf2 counter anion,
CH2Cl2
Li-encapsulated
fullerene
Li@C60•–++@C (cation)
Li
Li+@C60•– (neutral)
60(Li @C60 ) supraatom which is far
different from the starting Li+ @C60 salt Figure 1. Pattern diagram of the electrochemical
reduction of [Li+@C60] cation in CH 2Cl2.
having an external counter anion.
* NTf2–; bis(trifluoromethylsulfonyl)imide anion (N(SO2CF3)2–)[1] Sawa, H. and Tobita, H. et al. Nat. Chem. 2010, 2, 678. [2] Aoyagi, S. et al. Angew. Chem. Int. Ed. 2012, 51,
3377. [3] Kokubo, K. et al. Chem. Commun. 2013, 49, 7376. [4] Matsuo, Y. et al. The 45th
Fullerenes-Nanotubes-Graphene general Symposium (2013) 2P-36.
Corresponding Author: K. Kokubo
Tel: +81-6-6879-4592, Fax: +81-6-6879-4593, E-mail: kokubo@chem.eng.osaka-u.ac.jp- 145 -

3P-4
Separation of a missing small-bandgaped metallofullerene
Gd@C60 by in situ trifluoromethylation○Hiroyuki Niwa, Yusuke Nakanishi, Zhiyong Wang, Ryo Kitaura,
Haruka Omachi and Hisanori Shinohara*
Department of Chemistry & Institute for Advanced Research, Nagoya University, Nagoya
464-8602, Japan.
Ever since the first mass spectroscopic observation of La@C60 in 1985[1], many
attempts to solvent-extract, separate and purify M@C60 (M = Ca, Er, Eu etc.) have beenreported [e.g., Ogawa et al. JACS on Er@C60[2]]. However, even today, the final
purification and isolation (i.e., more than 99 % purity) of M@C60 have not yet been
done. Because of their high reactivity due to their small-bandgap or the radical property,
M@C60 is entirely insoluble in common organic solvents. Recently, our group havereported a brand-new stabilization method of small-bandgap metallofullerenes such as
M@C2n (2n = 70–74) by in situ trifluoromethylation[3].
Herein, we report the first synthesis and separation of pertrifluoromethylated Gd@C60
derivatives. DC arc-discharge was carried out with a Gd/graphite composite rod as
positive electrodes and polytetrafluoroethylene (PTFE) situated below the arc-discharge
region[3]. The LD-TOF mass spectra of the crude extract shows that the generation of
Gd@C60 and/or its derivatives (Fig 1a). After the separation of the crude extract by the
TiCl4 treatment[4,5] and recycle HPLC, enhanced peaks of Gd@C60(CF3)4 andGd@C60(CF3)5 were observed by MALDI-TOF-MS mass spectral analysis (Fig. 1b).
DFT calculations on the causes of the electronic stability of trifluoromethylated
Gd@C60 will also be presented.

Fig. 1 (a) LD-TOF mass spectra of crude extracts (top: without PTFE, bottom: with PTFE) (b)
MALDI-TOF mass spectra after separation.
[1] J. R. Heath et al., J. Am. Chem. Soc., 107, 7779 (1985) [2] T. Ogawa et al., J. Am. Chem. Soc., 122,
3538 (2000). [3] Z.Wang et al., Angew. Chem., Int. Ed., 52, 11770 (2013). [4] K. Akiyama et al., J. Am.
Chem. Soc., 134, 9762 (2012). [5] Z. Wang et al., J. Phys. Chem. C 116, 25563 (2012).
Corresponding Author: Hisanori Shinohara
Tel: +81-52-789-2482, Fax: +81-52-747-6442, E-mail: noris@nagoya-u.jp- 146 -

3P-5
Spontaneous exciton dissociation in carbon nanotubes
Y. Kumamoto, M. Yoshida, A. Ishii, A. Yokoyama, ○T. Shimada, Y. K. Kato
Institute of Engineering Innovation, The University of Tokyo, Tokyo 113-8656, Japan
Simultaneous photoluminescence and photocurrent measurements on individual
single-walled carbon nanotubes reveal spontaneous dissociation of excitons into freeelectron-hole pairs [1]. A simple model is constructed to consistently describe the excitation
power and voltage dependence of the photoluminescence and photocurrent. Using this model,
we find that a significant fraction of excitons are dissociating before recombination.
Furthermore, the combination of optical and electrical signals also allows for extraction of theabsorption cross section and the oscillator strength. Our observations explain the reasons forphotoconductivity measurements in single-walled carbon nanotubes being straightforward
despite the large exciton binding energies.
Work supported by KAKENHI, SCOPE, KDDI Foundation, and the Photon Frontier
Network Program of MEXT, Japan.
[1] Y. Kumamoto, M. Yoshida, A. Ishii, A. Yokoyama, T. Shimada, and Y. K. Kato, arXiv:1307.5159 (2013).
Corresponding Author: Y. K. Kato
Tel: +81-3-5841-7702, Fax: +81-3-5841-7772
E-mail: ykato@sogo.t.u-tokyo.ac.jp- 147 -

3P-6
Quantum interference effect in Raman spectra of metallic nanotubes andgraphene○ Eddwi H. Hasdeo, Ahmad R.T. Nugraha, and Riichiro Saito
Department of Physics, Tohoku University, Sendai 980-8578, Japan
In graphene and metallic single wall carbon nanotubes (m-SWNTs), the existence of gapless linear
energy bands (Dirac cones) modify the G band (in-plane optical phonon modes) Raman spectra. Oneof the well-known phenomena is the Kohn anomaly effect, in which the phonon energy (lifetime)
becomes lower (shorter) due to the interaction between the G phonon and an electron-hole pair in thelinear energy band [1]. The other phenomenon is the asymmetric spectral shape of the G band, also
known as Breit-Wigner-Fano (BWF) line shape, which long been observed in m-SWNTs [2] andrecently observed in graphene as a function of Fermi energy [3]. This BWF lineshape asymmetry is
still not well explained theoretically. In this presentation, we explain the origin of BWF line shape bymeans of quantum interference of phonon G band spectra and electronic Raman spectra (ERS). The
ERS are electronic spectra whose origin comes from an electron-hole pair excitation in the Dirac cone
[4].
In the case of m-SWNTs, the exciton-exciton interaction between a photo-excited exciton and an
exciton in the linear band is relevant to the ERS. We calculated ERS spectra as a function of laser
excitation energy which schematically reproduces the experimental BWF spectral shape. We foundthat the direct Coulomb interaction between the two excitons surprisingly vanishes at q=0 because of
the symmetry of the two sub-lattices of SWNTs unit cell even though the Coulomb interaction at q=0
is generally considered to be a maximum [5]. In the case of graphene, we use the same method to
obtain the electron-electron interaction matrix element and we will present the G band asymmetry as afunction of Fermi energy. We also predict that the radial breathing phonon mode (RBM) spectra in
m-SWNTs exhibit the opposite BWF asymmetry to that of the G band, by showing the laser energy
dependence of RBM spectra.
[1] “Raman spectroscopy in graphene related systems”, A. Jorio et al, Wiley (2011)[2] S. D. M. Brown et al., Phys. Rev. B 63, 155414, (2001)[3] D. Yoon et al., Carbon, 61, 373-378, (2013)[4] H. Farhat et al., Phys. Rev. Lett. 107, 157401 (2011).
[5] E. H. Hasdeo et al.Phys. Rev. B 88, 115107, (2013).
Corresponding Author: E. H. Hasdeo
TEL: +81-22-795-6442, FAX: +81-22-795-6447, E-mail: hasdeo@flex.phys.tohoku.ac.jp- 148 -

3P-7
Observation of Upconversion Photoluminescence from Single-walled
Carbon Nanotubes○Naoto Akizuki 1, Yuhei Miyauchi 1, 2, Shinichiro Mouri 1, and Kazunari Matsuda 1
1

2

Institute of Advanced Energy, Kyoto University, Uji, Kyoto 611-0011, Japan
Japan Science and Technology Agency, PRESTO, 4-1-8 Honcho, Kawaguchi, Saitama
332-0012, Japan

PL Intensity (arb. units)

Photoluminescence (PL) properties of single-walled carbon nanotubes (SWNTs) havebeen intensively studied over the past decade because of their potential applications in
optoelectronics and bioimaging, as well as for exploring fundamental exciton physics in
one-dimensional electronic systems [1]. Here, we report a novel PL property in SWNTs:
ability to emit PL by photoexcitation with lower energy photons than those of the emission,
which is called upconversion PL (UCPL). UCPL has been attracting much interest related to
optical manipulation of phonons in solid, high efficiency solar cells, and bioimaging. Ourfindings will thus provide a new dimension for the optical application of SWNTs.
The SWNTs were dispersed with 0.2 wt% SDBS in D2O. Figure 1 shows PL spectra of
SWNTs around (6,5) E11 exciton peak observed under excitation with higher (2.18 eV, dotted
line, normal PL) and lower (1.13 eV, solid line,
UCPL) energy photons than (6,5) E11 exciton
energy (1.26 eV). There are distinct peaks at thephoton energy close to (6,5) E11 in the both PL
spectra. Excitation density dependence of the
UCPL intensity is shown in the inset of Fig. 1.
The UCPL intensity depends on the excitation
density nearly linearly under weak excitation
0
0
0.5
1.0
Excitation Density (mJ/cm )conditions; this result rules out the possibility
that the observed UCPL originates from a two
photon excitation process that should show aquadratic dependence. On the basis of theobservations of temperature and excitation
photon energy dependence, the UCPL is
attributed to the excitation processes mediatedby large energy optical phonons in SWNTs. We Fig. 1. PL spectra with the excitation
will discuss the detailed mechanism of the photon energy of 2.18 eV (dotted line)
UCPL, and the further enhancement of the and 1.13 eV (solid line) normalized at E11
UCPL intensity by introducing lower energy intensity. Upconversion PL spectrum was
local states in SWNTs.
measured under the pulsed excitation
2[1]Y. Miyauchi, J. Mater. Chem. C 1, 6499 (2013)
Corresponding Author: N. Akizuki

density of 0.13 mJ/cm2. The inset showsthe excitation density dependence of the
UCPL intensity.

Tel: +81-774-38-3465,
E-mail: akizuki.naoto.88x@st.kyoto-u.ac.jp- 149 -

3P-8
Electronic structures of CNT with a defect under carrier accumulations○UIshiyama, Susumu Okada
Graduate School of Pure and Applied Sciences,Universityof Tsukuba, Tennodai, Tsukuba 305-8577, Japan
 Carbon nanotubes (CNTs) are attracting much attention due to its possible application for semiconductor
electronic devices in the post-silicon era. It has been shown experimentally that CNTs work as a conducting channelof field-effect transistors(FETs). However, the operating mechanism of the CNT-FET is not fully understood. In
particular, it is still unclear how the defects introduced into CNT affect on the electronic properties of CNT undercharge accumulation being one of important issues for device applications. In this work, we aim to elucidate thefundamental electronic properties of CNT with an atomic defectunder the charge accumulation by the electrode.
 All calculations are performed by using the density functional theory. To express the exchange correlation
potential among interacting electrons, we apply the local density approximation. We usean ultrasoft pseudopotential
to describe the interaction between valence electrons and ions. The effective screening medium (ESM) method isapplied to investigate electronic properties of CNT with carriers under the electric field in the framework of the firstprinciples calculations. Here, we use the (10,0) CNT with a monatomic defect per triple periodicities of CNT along
its axis. To simulate the CNT-FET device, we consider the model system shown in Fig. 1, in which CNT is locatedabove the planar electrode simulated by the effective screeningmediummimickingthe ideal metalelectrode.
 Figure 2 shows the calculated electrostatic potential of (10,0) CNT with an atomic defect and excess electrons of0.5e. As shown in Fig. 2, substantial potential modulation occurs around the defect: the potential possesses peakaround the defect indicating the electric field concentration around the defect. By evaluating the distribution of theaccumulated electrons, we found that the accumulated electrons are mainly distributed around the atomic defect.
Therefore, the electric field concentration is ascribed to the carrier concentration around the defect.

     Fig. 1 A structural model of nanotubes under the

Fig. 2 Electrostatic potential of CNT with an atomic

electric field.

defect under the electric field. Dotted lines denote awall of CNT.

Corresponding Author:U Ishiyama
Tel: +81-29-853-5600 (ext. 8233), Fax: +81-29-853-5924,
E-mail: sokada@comas.frsc.tsukuba.ac.jp- 150 -

3P-9
Metal Deposition Effects on Photoluminescence and Raman Scattering
Spectra of Suspended Single-walled Carbon Nanotubes○Akihiko Ozao1, Shohei Chiashi2, Genta Yamaguchi1, Yoshikazu Homma112Department of Physics, Tokyo University of Science, Tokyo, 162-8601, Japan
Department of Mechanical Engineering, The University of Tokyo, Tokyo, 113-8656, Japan

0.04
0.03
0.02
0.01
0
−0.01
−0.02
−0.03
−0.04

or
or
or

1

(11, 6)(9, 7)(12, 5)Strain [%]ΔEem [eV]Photoluminescence (PL) of single-walled carbon nanotubes (SWCNTs) are known to besensitive to the environment, such as gas, surfactants and dispersants adsorbed on them [1, 2,
3]. However, the effect of metal deposited on SWCNTs has not been analyzed in detail. In thiswork, we observed the effects of gold and iron deposition on suspended SWCNTs using PL
spectroscopy and Raman scattering spectroscopy.
The suspended SWCNTs were grown on a patterned quartz substrate and metals were
deposited by vacuum deposition. PL spectra and Raman scattering spectra were obtained
before and after the deposition. The deposition and optical measurements were repeatedalternately. With depositing metals, PL emission energy shifted depending on the chirality of
SWCNT (Fig. 1). Also, the G-band of Raman scattering spectrum, which represents in-planevibration mode of graphene, down-shifted after deposition. Those PL emission energy shift
and G-band down-shift are likely to be caused by axial deformation of SWCNTs due to gold
and iron particle formation. And the strain was estimated about 0.1 - 1% (Fig. 2).

0.5

0

0
50
100
15
2
Metal surface density [ x10 atoms/cm ]Fig. 1

Au
Fe

0
100
15
2
Metal surface density [10 atoms/cm ]Metal surface density dependence of PL

emission energy shift (ΔEem). Open circles and filled

Fig. 2Estimated strain in SWCNTs as afunction of metal surface density.

circles are the result of gold deposition and irondeposition, respectively.

[1] J. Lefebvre, et al., Appl. Phys. A, 78, 1107 (2004).
[3] T. Hertel, et al., Nano Lett., 5, 511 (2005).
Corresponding Author: Y. Homma
Tel: +81-3-5228-8244, Fax: +81-3-5261-1023,
E-mail: homma@rs.tus.ac.jp- 151 -

[2] S. Chiashi, et al., Nano Lett., 8, 3097 (2008).

3P-10
NMR study of 13C enriched single-wall carbon nanotubes○Noboru Serita1, Yusuke Nakai1, Yasumitsu Miyata1,2, Yutaka Maniwa1,
and Takeshi Saito3,4
1

Department of Physics, Tokyo Metropolitan University, Hachioji, 192-0397, Japan
JST, PRESTO, Kawaguchi, 332-0012, Japan
3
Nanotube Research Center, National Institute of Advanced Industrial Science and2Technology (AIST),
4Technology Research Association for Single Wall Carbon Nanotubes (TASC)
The bond length between the nearest neighbor carbon atoms (C-C bond length) is an
important parameter for the understanding of the physical properties of carbon materials.
Although the precise C-C bond lengths of single-wall carbon nanotubes (SWCNTs)

have been remained unclear, recent X-ray diffraction measurements revealed the C-C
bond lengths of highly-enriched (6, 5) SWCNTs [1]. NMR also has been a useful probeof structural characterization. For instance, the bond length of C60 was successfully
determined through NMR [2]. The C-C bond length can be estimated from 13C-13C
magnetic dipolar coupling that affects 13C NMR spectra. Since the natural abundance of13

C isotope that has a spin I = 1/2 is only 1.1%, it is necessary to enrich 13C isotopes forthe investigation of the C-C bond length through the dipolar coupling.
We prepared 13C enriched SWCNTs synthesized by the enhanced direct injection
pyrolytic synthesis (e-DIPS) method [3]. By using a density gradient ultracentrifugation
method, we removed magnetic impurities from our sample. The obtained 13C-NMR
spectra cannot be described only by the usual sp2 hybridized orbital [4], but appear torequire 13C-13C dipolar interaction as well. In this presentation, we report ourexperimental data in detail and discuss the origin of the 13C NMR spectra.
[1] R. Mitsuyama et al., submitted.
[2] C. S. Yannoni et al, J. Am. Chem. Soc., 113, 3190 (1991)[3] T. Saito et al., J. Nanosci. Nanotech. 8, 6153 (2009).
[4] K. Matsuda et al., J. Phys. Soc. Jpn. 82, 015001 (2012).
Corresponding Author: Y. Nakai
Tel: +81-42-677-2498, Fax: +81-42-677-2483, E-mail: nakai@tmu.ac.jp- 152 -

3P-11
Numerical study of electronic states in double-walled carbon nanotubes---Formation of metallic bands by covalent bridge between tubes--Yuhei Natsume
Department of Physics, Chiba University, Chiba 263-8522, Japan
Band structure calculation has been made for double-walled carbon nanotubes (DWCNT)by Atomistix ToolKit [1].
Tough the interaction between tubes is attributed to Van der Waals forces, the covalentbridge appears in Bloch states at Fermi surfaces. As a result, we get the metallic bands in DW
CNT, even for cases where DWCNT is composed of inner and outer CNT’s with energy gaps[2]. In short, the Fermi surfaces are induced from bonding-aintibonding splitting between
CNT’s. Such the splitting occurs both for LUMO’s and HOMO’s.
As a typical example of numerical calculation, we show the electron density for covalent
bands in 2s and 2p levels in Fig.1, where semiconducting (8,0) CNT is surrounded bysemiconducting (13,0) CNT. The ratio of radiuses is 1.62. The axis of tubes are the z-direction.
As far as the distribution of total density, the Van der Waals interaction plays an important role.
For overall properties,
the states of inner
CNT are independentof those of outer CNT.
In contrast, Blochstates at Fermi levels
present quite different
features as shown in
Fig.2. In fact, we findthe bridge between
inner CNT and outer
CNT,
which
has
Fig.1(a )Electron density in (x,y) plane.
(b) Electron density in (y,z) plane.
covalent characters.
We would like to emphasize that multiwalled CNT’s have a strong tendency to acquire
metallic properties.
[1]Atomistix ToolKit & Virtual

NanoLab, Quantum Wise Japan,
Shinjyuku,
Tokyo,
Japan
http://www.quantumwise.co.jp/[2] H.-S.Philip Wong and Deji
Akinwande,”Carbon Nanotube
and Graphene Devise Physics”,(Cambridge University Press,2011).
Corresponding Author:
Y. Natsume
Tel: +81-43-204-6260,
Fax:+81-43-204-6261
natsume@faculty.chiba-u.jp

Fig.2(a)Bloch states in (x,y) plane.

- 153 -(b)Bloch states in (y,z) plane.

3P-12
Electronic Structure of Carbon and BN Nanotubes:
A Comparative First Principles Study◦Yuya Uchida, Takashi Koretsune, and Susumu Saito
Department of Physics, Tokyo Institute of Technology,
2-12-1 Oh-Okayama, Meguro-ku, Tokyo 152-8551, Japan

Carbon nanotubes have been intensively studied both theoretically and experimentallyfor last two decades due to its characteristic electronic properties. Because of the large unit
cell sizes of general chiral nanotubes, the detailed electronic and geometric structures were
not understood well. In our previous research, we have studied the electronic and geometricstructures of carbon nanotubes with various chiralities systematically for the ﬁrst time using
the helical symmetry[1].
In this study, we report the electronic structures of BN nanotubes with various chiralities
obtained by the local density approximation in real-space density functional theory(DFT).
By extending the helical-symmetry DFT program for carbon nanotubes to BN nanotubes,
we now can investigate BN nanotubes of all chiralities with small unit cell including only
two atoms. We study the carbon and BN nanotubes comparatively(Fig.1), and discuss thechirality dependence of the electronic properties of BN nanotubes.
(b)

5

5

0

0

-5

-5
energy[eV]energy[eV]

(a)

-10

-10

-15

-15

-20

-20

-25

0

k

-25

π

π

0
k

Figure 1: Band structures of (a)(9,0)Carbon nanotube and (b)(9,0)BN nanotube[1]K. Kato, T. Koretsune, and S. Saito, Physical Review B 85 115448 (2012).
Corresponding Author: S. Saito
E-mail: y-uchida@stat.phys.titech.ac.jp- 154 -

3P-13
Photoconductivity spectroscopy of individual suspended carbon nanotubes
T. Uda, Y. Kumamoto, M. Yoshida, A. Ishii, Y. K. Kato
Institute of Engineering Innovation, The University of Tokyo, Tokyo 113-8656, Japan
To investigate photoconductivity of chirality-identified carbon nanotubes, we havefabricated field-effect transistors with individual air-suspended nanotubes [1]. Trenches are
etched into SiO2/Si substrates, and Pt/Ti are deposited on both sides of the trenches. By
ethanol chemical vapor deposition, carbon nanotubes are grown over the trenches. We havealso constructed a system which can simultaneously measure photocurrent andphotoluminescence excitation spectra [2]. Nanotubes are excited with a wavelength-tunable
continuous wave Ti:sapphire laser, and photoluminescence is detected by an InGaAs
photodiode array attached to a spectrometer. Photoluminescence imaging and excitation
spectroscopy allows us to locate the nanotubes and identify their chirality. For photocurrent
microscopy, excitation laser is modulated by an optical chopper and a lock-in amplifier isused for detection.
Work supported by KAKENHI, KDDI Foundation, and the Photon Frontier Network
Program of MEXT, Japan.
[1] S. Yasukochi, T. Murai, S. Moritsubo, T. Shimada, S. Chiashi, S.Maruyama, and Y. K. Kato, Phys. Rev. B
84, 121409 (2011).
[2] Y. Kumamoto, M. Yoshida, A. Ishii, A. Yokoyama, T. Shimada, and Y. K. Kato, arXiv:1307.5159 (2013).

Corresponding Author: Y. K. Kato
Tel: +81-3-5841-7702, Fax: +81-3-5841-7772
E-mail: ykato@sogo.t.u-tokyo.ac.jp- 155 -

3P-14
Environment-Friendly Functionalization Method to Obtain
Water-Dispersible Carbon Nanotubes
Mohammad Jellur Rahman1, !Tetsu Mieno1,2
1

Graduate School of Science and Technology, Shizuoka University, Shizuoka 422-8529, Japan2
Department of Physics, Shizuoka University, Shizuoka 422-8529, Japan

Carbon nanotubes (CNTs) are promising candidates for microelectronics, polymer composites,
biochemistry, pharmaceuticals, and medical engineering, due to their unique mechanical andelectrical properties [1,2]. To realize the applications strategic approaches toward their stabledispersion in liquids are necessary. For this, usually harsh chemical processes are followed,
which degrade their properties and are not environmentally safe [3]. Therefore, enhancementof dispersibility preserving their properties is a crucial issue. We have developed an easy andenvironment-friendly method to functionalize both single-walled and multiwalled CNTs
(SWNTs and MWNTs) using citric-acid-assisted RF oxygen plasma treatment, which is lessdestructive to their structure. Pristine SWNTs and MWNTs are pretreated in pure ethanol anddried under reduced pressure. Then, they are wetted by citric acid solution and placed in a RF
(13.56 MHz) plasma chamber. Finally, oxygen plasma reaction is operated on the wet CNTs
under optimum condition. The resultant CNTs can be easily dispersed in pure water owing to
the attachment of a large number of carboxyl groups onto their surfaces. Dispersibility isobserved by the UV-visible spectroscopy, precipitation tests, and transmission electron
microscopy. Successful attachment of the carboxyl groups is confirmed by the Fouriertransform infrared spectroscopy and thermogravimetric analysis. Preservation of the structuralquality is verified by Raman spectroscopy, which suggests the preservation of their basic
properties. These water-dispersible CNTs are good candidates for electronic coating industries,
composite technology and biomedical engineering.
(

SWNTs
MWNTs

(a)

(c)

".@ 3 4 5 6(

86(# ()7 >=A(;:BC,

6dn/dt ( -10 x ABS/hr)

10

4
2
0

p-CNTss-CNTsf-CNTs(b)!.@ 3 4 5 6".23 4 5 6!.23 4 5 6& $ % ' ()* + * ,& 1 % $ ()* + - ,# & ' " ()- ./ 0.- / ,!""" #$"" #""" %$"" %""" &$"" &""".&

3 7 89 :;< =9 >()? < ,Fig.1 (a) Settling speed, dn/dt, calculated from the Abs (250 nm) versus time graphs for the pristine CNTs
(p-CNTs), sonicated CNTs (s-CNTs), and functionalized CNTs (f-CNTs). (c) Schematic of the production of
stable suspension. (a) FT-IR spectra of the pristine and functionalized SWNTs and MWNTs.
[1] M. F. L. De Volder, et al. Science 339, 535 (2013). [2] M. Endo, et al. in Carbon nanotubes-Topics in Applied
Physics, (Springer, Heidelberg, 2008). [3] A. Hirsch, O. Vostrowsky, Top. Curr. Chem. 245, 193 (2005).
Corresponding Author: T. Mieno, Tel. and Fax: + 81-54-238-4750, E-mail: sptmien@ipc.shizuoka.ac.jp- 156 -

3P-15
A Test for the growth of single-wall carbon nanotubes
on the porous glass (PG) sheet by ACCVD technique
Kyohei Nagao1, żShinzo Suzuki1, Shinji Ogami1, Yosuke Ito1,
Hiroshi Nagasawa2, Yohji Achiba3
1

Department of Physics, Kyoto Sangyo University, Kyoto 603-8555, Japan
2
Nano-support Co., Ltd., Kanagawa 251-0024, Japan3
Department of Chemistry, Tokyo Metropolitan University, Tokyo 192-0397, Japan
Abstract:
ACCVD technique has been widely used in the field of single-wall carbon nanotube(SWNT) growth, partly because that the ambient temperature suitable for the formation of
SWNTs is relatively lower (typically, less than 800°C), and the purity of SWNTs in as-grownmaterial is better than those obtained by other technique, e.g. arc-burning procedure.
In 2005, Aoki et al., reported about the formation of SWNTs in the porous glass (PG)
material by using ACCVD technique [1], where a kind of metal particles (e.g. Co particles)
were deposited on the PG material before ethanol was introduced as carbon source for making
SWNTs in the PG material. The advantage of using PG material is that, it is very easy to makeany kind of shape (rod, sheet.., etc.) made of PG, which implies that the as-grown PG-SWNT
complex itself is expected to be used as an optical or other kind of device.
In this presentation, in order to investigate thegrowth of SWNTs on the porous glass sheet by
PG-ACCVD technique, four different kinds of
PG-sheet were prepared (shown in Figure 1), where
each average pore size (diameter) is controlled to
10nm, 30nm, 50nm, and 100nm, respectively. After
optimizing the condition for the PG-ACCVD process
in our apparatus, a test for the growth of SWNTs isplanned.
Figure 1. Four different kinds of PG-sheet (8mm width, 1mm thickness), where the averagepore-size is 10nm, 30nm, 50nm, and 100nm (from the left to the right).
References:[1] Y. Aoki, S. Suzuki. S. Okubo. H. Kataura, H. Nagasawa, and Y. Achiba, Chem. Lett., 34, 562(2005).
Corresponding Author: Shinzo Suzuki
Tel: +81-75-705-1631, Fax: +81-75-705-1631,
E-mail: suzukish@cc.kyoto-su.ac.jp- 157 -

3P-16
Molecular recognition on external grooves of bundled surfaces ofsingle-walled carbon nanotubes○Tsuyohiko Fujigaya1,2, JongTae Yoo1, and Naotoshi Nakashima1,2,3
1Department of Applied Chemistry, Graduate School of Engineering, Kyushu University,

744 Motooka, Fukuoka 819-0395, Japan

2World Premier International (WPI), International Institute for Carbon-Neutral Energy

Research, Kyushu University 744 Motooka, Nishi-ku, Fukuoka 819-0395, Japan

3Japan Science and Technology Agency, CREST, 5 Sanbancho, Chiyoda-ku, Tokyo,

102-0075, Japan

Recently, one-dimensional nano-spaces in the(A)(B)
bundle of single-walled carbon nanotubes (SWNTs)such as interstitial channel and external groove
attract attentions in experimentally and theoretically
due to their intense van der Waals interaction withmolecules. Here, we investigated an effect of SWNT Fig. 1 SEM images of silica gel coated byisolated and (B) bundled SWNTs. Scalebundle for SWNT-molecular interaction using the (A)bars: 1 m.
affinity
chromatography [1] incorporating SWNT bundles
as a stationary phase.
(A)
In a preparation of the stationary phase, different
concentrations of SWNT dispersions in
1-methyl-2- pyrrolidinone (NMP) were mixed withsilica sphere and the precipitates were collected [2].
As shown in SEM images, bundled structures of
SWNTs were observed on the silica surface
prepared from higher concentration (Fig. 1B),
(B)
while such a structure was hardly seen on that fromlower one (Fig. 1A).
Quite interestingly, we noticed the changes ofthe order of retentions between isolated andbundled SWNTs caused by the unusual behavior of
p-terphenyl in the chromatograms (Fig. 2) and theresult suggests the specific recognition of bundled
Fig. 2 Chromatograms of PAHs using (A)isolated and (B) bundled SWNTs as SWNTs for p-terphenyl. We consider thatstationary phase at flow rates of (A) 0.1 andp-terphenyl
stronglyinteracts
withthe(B) 0.7 mL/min.
one-dimensional external groove in the SWNT
bundle due to its structure. Also diameter dependency of the degree of groove recognition wasobserved [3].We believe that this unique aspect will provide a promising feature for new
applications of SWNTs.
[1] J. Yoo et al., Nanoscale 2011, 3, 2517.
[2] T. Fujigaya et al., Carbon 2011, 49, 468.
[3] J. Yoo et al., Nanoscale 2013, 5, 7419.
Corresponding Author: Naotoshi Nakashima
E-mail: nakashima-tcm@mail.cstm.kyushu-u.ac.jp
Tel & Fax: +81-92-802-2842- 158 -

3P-17Fabrication and Properties of Functionalized Multiwall Carbon Nanotube/
PA-6 Composite○Yoshimi Muraoka, Hiroki Sato, Masaru Sekido
Department of Material Science and Engineering, Sendai National College of Technology,
Natori 981-1239, JapanDue to their combination of outstanding mechanical characteristics, extremely large inter-facial contact area, high aspect ratio, and low mass density, CNTs are considered as the ideal
reinforcement fillers for the nanocomposite materials. The challenges for the development ofhigh-performance CNTs/polymer nanocomposites are homogeneous dispersion of CNTs inpolymeric matrix. For this purpose we have developed simple solution-evaporation method
using functionalized Multiwall Carabon Natotubes(MWCNTs) followed by mechanically
melt-compounding for the fabrication of composites.
MWCNTs were functionalized by using 1,3-dipolar cycloaddition reaction to obtainwater-soluble functionalized MWCNTs. MWCNTs (200 mg) were mixed with
N-methylglycine (2.0 g) and 3,4-dihydroxybenzaldehyde (2.0 g) in DMF (500 mL) and thereaction mixture was stirred at 120 oC for 5 days. After removing DMF under reducedpressure remaining precipitate was washed with water and acetone to give functionalized
MWCNTs. The obtained functionalized MWCNTs were used as filler for the nanocomposites
without further purification.
MWCNTs/nylon-6 (PA6) nanocomposites have been prepared by simple melt-compounding
and tensile strength was compared with various loading of MWCNTs. In the present study wereport the effect of MWCNTs and functionalized MWCNTs loading for the improvement of
mechanical properties of nanocomposites.
Corresponding Author: M. Sekido
Tel: +81-22-381-0329, Fax: +81-22-381-0329
E-mail: sekido@sendai-nct.ac.jp- 159 -

3P-18Printed SWCNT thin film CMOS inverters
based on chemically doped ion gels
○Yoshifumi Wada 1, Ryota Inukai 1, Taiyo Fujimoto 1, Hiroki Hamahata1, Satoki Matsuzaki 1,
Kazuhiro Yanagi 2 and Taishi Takenobu 1,3
1

2

Department of Applied physics, Waseda University, Tokyo 169-8555, Japan
Department of Physics, Tokyo Metropolitan University, Tokyo 192-0397, Japan
3
Kgami Memorial Laboratry, Waseda University, Tokyo 169-0051, Japan

Single-walled carbon nanotubes (SWCNTs) have been of high interest due to their
excellent performance such as high mobility, flexibility and printability. Recently, SWCNT
thin films, the random networks of SWCNT, open the route for the application as printablesemiconductors.[1] Though there was problem of trade-off with on/off ratio and current
density, electrolyte-gated transistors (EGTs) of SWCNT thin film realized ambipolarswitching with high on/off ratio (>105) in low voltage (<2V).[2] Importantly, SWCNT thinfilm EGTs are achievable using ion gels, which is one of the printable solid electrolytes. Thus,
it is expectable to fabricate low-voltage logic circuit with printing method. The first step tologic circuit is the fabrication of CMOS inverters. To fabricate a CMOS inverter, both p- andn-type transistors are needed. Because SWCNT thin film EGTs are ambipolar characteristics,
the point to control polarity is turn-on voltage, which is controllable by the chemical doping
using donative organic molecules.[3] However, the combinations of donative organic
molecules and ion gels for EGTs have not been reported.
Here, we fabricated CMOS inverters based on n-type and ambipolar SWCNT thin film
EGTs (Fig.1). First, SWCNT thin films were fabricated by ink-jet printing method. Then,
Au/Ni electrodes were fabricated by vacuum evaporation as source and drain electrode. Iongels were fabricated on a SWCNT thin film by drop-cast method. After dropping ion gels, Au
foil was placed on ion gel as gateelectrode. To change turn-on voltage of
EGTs, we added
polyethylenimine(PEI) as donative polymer of ion gel.
By adding PEI to ion gels, we couldchange turn-on voltage of EGTs.
Finally we fabricated CMOS inverters
and obtained low-voltage (1.5V)
operation with maximum gain of 28(Fig.2). This method has potential toachieve vacuum-process-free logic
circuits with applying metallic SWCNT
Fig.1 SWCNT thin film CMOS Fig.2 Transfer characteristics
thin-film electrodes.
inverter based on EGTs

[1] H. Okimoto et al. J.J.Appl. Phys. 48, 06FF03 (2009).
[2] M. Ha et al. Nano Lett. 13, 954 (2013)[3] R. Shimizu et al. Appl. Phys. Express 5, 125102 (2012)
Corresponding Author: T. Takenobu
Tel: +81-3-5286-2981, Fax: +81-3-5286-2981,
E-mail: takenobu@waseda.jp- 160 -of SWCNT thin film inverter

3P-19Surface modification of multi-walled carbon nanotubes
with benzyl radical derivatives generated by photo-irradiation○Tomoya Takada1, Batbuyan Munkh-od 1, Shigeaki Abe 2
1

Department of Materials Chemistry, Asahikawa national College of Technology, Asahikawa
071-8142, Japan
2
Graduate School of Dental Medicine, Hokkaido University, Sapporo 060-8586, Japan

Surface modification of carbon nanotubes (CNTs) is an essential subject for their industrial
application, since homogeneous dispersion of CNTs in solvents are effectively enhanced byappropriate surface modification. In addition, functional groups introduced by surface
modification of CNTs act as reaction sites for subsequent bond formation with, for example,
other organic molecules and polymers. Many methods for the surface modification have beenreported previously. However, modification methods
employing photochemical reactions have been
scarcely studied. In this work, a simple method for thesurface modification of CNTs with radicals formed byphoto-irradiation was developed. Benzyl radical
derivatives were employed in this study; these radical
derivatives can be smoothly generated by bondcleavage of benzyl halide derivatives. In general,
CNTs are capable of capturing radicals throughcovalent bonds (Fig. 1). Therefore, applying thephotochemical radical generation, development of a Fig. 1 Scheme of the surface modificationnovel one-pot surface modification method of CNTs in this work
is expected.
As a radical source, 4-(chloromethyl)benzoic acid (CMBA, Wako Chemicals, Co. Ltd.)was used in this work. CMBA and multi-walled carbon nanotubes (MWCNTs, diameter
10-30 nm, Wako Chemicals, Co. Ltd.) were added into dimethylformamide (DMF) and thendispersed by sonication. Light from an Xe lamp (wavelength 300-600nm) was irradiated tothe mixture at room temperature for 24 hours. During the irradiation, oxygen in the mixture
solution was purged with Ar gas. MWCNTs after the irradiation were filtered, washed anddried in the air. Amount of the 4-carboxyl benzyl radicals introduced on the MWCNTs
surface was determined by conventional acid-base back titration; carboxyl groups attached on
MWCNTs were neutralized with sodium hydroxide (NaOH) aqueous solution, and theamount of residual NaOH was then measured by titration with hydrochloric acid (HCl).
On the basis of the back titration results, partial neutralization of NaOH aqueous solution
caused by carboxybenzyl groups introduced on MWCNTs was confirmed. In addition,
dispersibility of the modified MWCNTs in water was drastically improved compared to thatof pristine MWCNTs. These results indicate that carboxybenzyl groups generated byphoto-induced C-Cl bond cleavages are successfully attached to the MWCNTs surface. Other
results (for example, effect of the addition of triphenylamine as an electron generator) will
also be shown in the symposium. This work has been supported by JSPS KAKENHI(Grant-in-Aid for Scientific Research (C)) No. 25420814.
Corresponding Author: T. Takada
Tel/Fax: +81-166-55-8036 , E-mail: takada@asahikawa-nct.ac.jp- 161 -

3P-20“Laminated” ion-gel film as high capacitance insulator
for carbon-nanotube transistor○Taiyo Fujimoto 1, Ryo Shimizu 1, Yuki Takagi 1, Yoshifumi Wada 1, Kazuhiro Yanagi 2,
Taishi Takenobu 1,3
1

Department of Applied Physics, Waseda University, Shinjuku 169-8555, Japan
2 Department of Physics, Tokyo Metropolitan University, Hachioji 192-0397, Japan
3
Kagami Memorial Laboratory, Waseda University, Tokyo 169-0051, JapanIon gel, which is a mixture of ionic liquid and organic polymer is promising candidates forgate dielectrics of field effect transistor due to exceptionally large specific capacitances [1].
Recently, low voltage operation of carbon-nanotube transistors based on the ion gel has been
already performed [2] and proved the usefulness of ion gel in reduction in consumed electric
power. Realization of three-dimensional integrated circuits has strongly been desired in orderto improve both functionality and energy efficiency. However, still, ion gel is not suitable forinsulator of three-dimensional integrated circuits, because specially controlled deposition ofion-gel films with arbitrary film thickness has not been established. Therefore, in this study,
we focus on the "laminating" method, in which ion gel is deposited on plastic substrate and,then, whole films are laminated on semiconducting carbon nanotube films for fabricatingtransistors.
Figure 1 shows a schematic illustration of fabrication process by the laminate method.
Semiconducting single-walled carbon nanotube (S-SWCNT) thin film was formed on Si/SiO2
substrate by inkjet printing and Au was evaporated as source, drain and side-gate electrodes.
On the other hand, ion gel was spin coated on polyimide substrate and cut into enough size tobe used as insulator of transistors. Finally, ion gel was laminated to Si/SiO2 substrates. As
shown in transfer characteristics of Fig. 2, the fabricated nanotube transistor showed
ambipolar transport with low-operation voltage, suggesting the effectiveness of laminating
method.
In summary, we succeeded in both specially controlled deposition of ion-gel films with
arbitrary film thickness and the fabrication of ambipolar nanotube transistors, which isimportant first step for the three-dimensional ion-gel devices.

Fig.1 Schematics of side-gated EDLT fabricated by the laminate method

Fig.2 Transfer characteristic[1] J. Lee et al, J. Am. Chem. Soc. 2007 , 129 , 4532 ., [2] M. Ha et al, Nano Lett. 2013, 13, 954.,
Corresponding Author: Taishi Takenobu, Tel&Fax: +81-3-5286-2981, E-mail: takenobu@waseda.jp- 162 -

3P-21
Polyglycerol-functionalized single-walled carbon nanotubes
for drug loading and delivery○Hongmei Qin, Li Zhao, Keisuke Nakamura, Takahide Kimura and Naoki Komatsu
Department of Chemistry, Shiga University of Medical Science, Seta, Otsu 520-2192, Japan
A variety of nanoparticles have been investigated as a nonviral vector in drug and genedelivery systems. Among these nanoparticles, single-walled carbon nanotubes (SWNTs) haveattracted a great deal of attention because of their large specific surface area and hydrophibic
nature. In addition, various functions can be added to SWNTs through organic reactions on
the SWNT surface and edges. Recently, we have found that polyglycerol (PG) can graft onto
nanoparticles (nanodiamond [1], ZnO [2] and Fe3O4 [3]) and afford very good hydrophilicity
and biocompatibility. In this study, we apply this methodology to the synthesis of
PG-functionalized SWNTs (SWNT-PG).
After mixed acid treatment, the resulting SWNTs containing carboxyl groups at theedges were allowed to react with glycidol to give SWNT-PG through ring opening
polymerization. The SWNT-PG exhibited good solubility and stability not only in water(>15.9 mg/mL), but also phosphate buffer saline (PBS) (>10.5 mg/mL), making the in vivo
use of SWNT more promising in biomedical applications. In addition, a large hydrophobic
sidewall surface area is expected to provide high loading capacity of aromatic molecules
including a cancer drug, doxorubicin (DOX), through π-π stacking and hydrophobic
interaction. After simple mixing of the SWNT-PG solution with DOX at pH 8 overnight,
SWNT-PG-DOX complexes was formed and free, unbound DOX in solution was removed bywashing. DOX-loading on SWNTs were confirmed by the red-shift of the absorption around
480nm (Fig 1a) and the quenching of fluorescence (Fig 1b).

3.0

4000

(a)
Fluorescence Intensity

3.5

DOX
SWNT-PG-DOX

2.5
Abs.

2.0
1.5
480nm

1.0
0.5
0.0
200

400

600

(b)

2000

1000

0
500

800

Wavelength/nm

DOX
SWNT-PG-DOX

3000

550

600

650

700

Wavelength/nm

Fig. 1. Absorption (a) and fluorescence (b) spectra of free DOX and SWNT-PG-DOX with the same DOX
concentration (excitation at 480 nm).
[1] L.Zhao, N. Komatsu, et al. Angrew. Chem. Int, Ed., 50, 1388-1392 (2011)[2] L.Zhao, N. Komatsu, et al. J. Indian Chem. Soc., 88, 1787-1790 (2011)[3] L.Zhao, N. Komatsu, et al. Adv. Funct. Mater., 22, 5107-5117 (2012)
Corresponding Author: Naoki Komatsu
Tel: +81-77-548-2102, Fax: +81-77-548-2405, E-mail: nkomatsu@belle.shiga-med.ac.jp- 163 -

3P-22
Simple and loss-free printing of carbon nanotubes for flexible electronics○Hiroyuki Shirae, Dong Yong Kim, Kei Hasegawa, and Suguru Noda*
Department of Applied Chemistry, Waseda University, Tokyo 169-8555, Japan
Carbon nanotubes (CNTs) are an attractive candidate material for electrodes and wirings inflexible electronic devices owing to their fair electric conductivity, excellent stability inambient, flexibility, and compatibility with printing processes. Their uniform films withexcellent conductivities have been realized through mild dispersion followed bycentrifugation and printing, however a significant fraction of expensive CNTs are wasted
during centrifugation. Moreover, in the fabrication of patterned electrodes/wirings, photo- orelectron-beam lithography is often applied to the uniform films, which causes additional lossof CNTs. Toward the practical application of CNTs to flexible electronics, simple andloss-free printing of conductive CNT films is highly demanded.
In this work, we propose and examine a repetitive dispersion-centrifugation process, which
minimize the damage to CNTs via mild dispersion and the material loss of CNTs via reuse ofundispersed CNTs. We also propose and examine a filtration process using a metal mask witha membrane filter, which yields patterned CNT films with minimal material loss.
We used the sub-millimeter-long few-wall carbon nanotubes (FWCNTs) synthesized by
our fluidized-bed chemical vapor deposition process at a high carbon yield ~ 70% [1].
FWCNTs were added at 0.01 wt% to the 0.5 wt% aqueous solution of sodium
dodecylbenzenesulfonate (SDBS). Ultrasonication (40 W, 40 kHz) was applied for 3 min to
the solution in iced water bath and then centrifugation was applied to the solution at 3500 rpm
for 10 min. Supernatant (1/4 of the solution) was taken out and the same amount of the SDBS
aqueous solution was added to the solution. A CNT film was made from the sampled
supernatant via vacuum filtration over a polytetrafluoroethylene (PTFE) membrane filter andwashed with hot water. These processes are repeated for ~ 10 cycles and the weight andconductivity of the film were evaluated for each cycle.
By using a metal mask during vacuum filtration, CNT line patterns were easily formed on
the filter, which were then transferred to polyethylene terephthalate (PET) films (Fig. 1).
Without using the metal mask, uniform CNT films were easily formed on the filter, which canbe self-supporting (Fig. 2). Uniform CNT films with steady weight and conductivity wereformed from the 3rd to 11th cycles via repetitive dispersion-centrifugation process (Fig. 3).

Fig. 1 Photo (a) andSEM images (b,c)
of CNT lines on
PET.

Fig. 2 A photo of aself-supporting
CNT film.

Fig. 3 Weight (left) and normalized conductance (right) ofuniform CNT films prepared at different cycles.

[1] D.Y. Kim, et al., Carbon 49, 1972 (2011).
Corresponding Author: S. Noda, Tel&Fax: +81-3-5286-2769, E-mail: noda@waseda.jp- 164 -

3P-23Chemical Vapor Deposition of MoS2 on Carbon Nanotube
for Organic Thin Film Solar Cells○Il Jeon,1 Dai Kutsuzawa,2 Yu Hashimoto,2 Takashi Yanase,2 Taro Nagahama,2Toshihiro Shimada,2 and Yutaka Matsuo1
1

Department of Chemistry, School of Science, The University of Tokyo, 7-3-1 Hongo,
Bunkyo-ku, Tokyo 113-0033, Japan
2
Division of Materials Chemistry, Faculty of Engineering, Hokkaido University, Kita-ku,
Sapporo 060-8628, Japan
Making bulk heterojunction using high mobility n-type semiconductors is one of thechallenges in fabricating high performance organic thin film solar cells. One strategy is to use
inorganic nanowires as n-type semiconductors because they will show high charge mobility
with morphology suitable for the bulk heterojunction. However, this approach has not beensuccessful so far because of the transport barriers and charge traps present on the surface ofthe nanowires[1]. In this work, we attempted growing nanowires of layered semiconductor
MoS2, which can be used as an n-type semiconductor. Since the layered materials do not havedangling bonds on the surface, the charge traps will not be present on the surface in principle.
Since there are layered materials with a variety of constituent elements, we can tune their
LUMO levels by choosing suitable materials[2]. In order to control the morphology of MoS2,
we have used atmospheric chemical vapor deposition using MoO3 and S as sources onbundles of single wall carbon nanotubes (SWCNT).
Figure 1 shows the TEM image, local Auger electron spectrum (AES) and Raman spectraof MoS2 grown on SWCNT. Hexagonal plates are surrounding SWCNTs, which wereidentified as MoS2 by AES and Raman. The MoS2-covered SWCNT was dispersed in ethanol
and was scattered on TiO2 nanocrystal layer / ITO. P-type semiconductor P3HT was
spin-coated on it and its power conversion efficiency ( ) was measured. A sample withpristine SWCNT without MoS2 was prepared for comparison. As a result, we obtained=0.46% for a cell containing MoS2-SWCNT and =0% for SWCNT.

[1] K. Takanezawa, K. Tajima, K. Hashimoto, Appl. Phys. Lett. 93, 063308 (2008).
[2] T. Shimada, F. S. Ohuchi, B. A. Parkinson, Jpn. J. Appl. Phys. 33, 2696 (1994).
Corresponding Author: Y. Matsuo & T. Shimada
TEL/FAX: +81-3-5841-1476; TEL/FAX: +81-11-706-6576
E-mail: matsuo@chem.s.u-tokyo.ac.jp, shimadat@eng.hokudai.ac.jp- 165 -

3P-24
Dispersion of SWCNTs in Wrapping of Belt-Type -Conjugated Polymer
Wataru Sagawa1, ○Masahiro Takahashi1, Keiki Kishikawa11, Shigeo Kohmoto1
1

Faculty of Engineering, Chiba University, Chiba, 263-8522, Japan

Scheme 1 Wrappings of CNT and fullerene with belt-type -conjugated polymer.

By making multiple  conjugated systems
connect with controlling the joint direction by an
ethynyl group, we aimed at construction of the"belt type  conjugated polymer" which cantransform the mainl chain into a two-dimensional
plan. The following advantages are acquired,when a complex is formed so that thismacromolecule may wrap in CNT, fullerene, etc. Fig. 1 Structure of polymer 1.
(i) Since the flexible region of the macromolecule
Table 1. Properties of Polymer 1.
is restricted, the rise of delta S is suppressed. (ii)
a)
PDIa)
n
Since multiple - interactions (large delta H) are
1.6
5.8
2.6×10３created by cylindrical  conjugation face,efficiently inclusion (big delta G) is expected a) Measured by GPC with polystyrene
standards.
(Scheme 1).
Alternating
copolymerizationofthediethynylbenzene
wascarriedout
todiiodoxanthene by the Sonogashira coupling
reaction, and Polymer 1 was obtained as yellow
powder of the weight average molecular weight
2,600 (Fig.1, Table 1). Ultrasonic churning of
CoMoCAT(1 mg), and Polymer 1(10 mg) was
carried out in THF(10mL), and dark black
dispersion was obtained. Even if it centrifuged
this SWNTs dispersed solution (10,000G, 10 min),the supernatant liquid solution has held the
distributed state of dark black. From the UV/vis Fig. 2 UV/vis spectrum of Dispersed CNT
spectrum, characteristics absorption of SWNTs with polymer 1 and monomeric unit.
without chiral selectivity was observed (Fig.2).
With the model compound corresponding to the monomer of this Polymer 1, althoughdispersion of SWNTs was tried under the same conditions, it was hardly able to disperse. By
repeating  conjugated polymer to a belt type, it has attained distributing powerful CNT.
Corresponding Author: M. Takahashi
Tel:+81-43-290-3397, Fax:+81-43-290-3401, E-mail: masahiro@faculty.chiba-u.jp- 166 -

3P-25Chirality purification of DNA-wrapped single-walled carbon nanotubes
toward thin film transistors○Yuki Kuwahara1,2, Fumiyuki Nihey2,3, Shigekazu Ohmori2, Takeshi Saito1,2
1

National Institute of Advances Industrial Science and Technology (AIST),
Tsukuba 305-8565, Japan
3
Technology Research Association for Single Wall Carbon Nanotubes (TASC),
Tsukuba 305-8565, Japan
2
NEC Corporation, Tsukuba 305-8501, Japan
It is well known that single-walled carbon nanotubes wrapped with DNA (DNA-SWCNTs)
based on the non-covalent interaction can be sorted by single-chiralities of SWCNTs by using
specific DNA sequence and ion exchange chromatography (IEX) technique [1]. In ourprevious works, we had reported the effective way to fabricate SWCNT thin film transistors(SWCNT-TFTs) by preparing homogeneous network of DNA-SWCNTs without the process
of extracting semiconducting SWCNTs [2]. This method needs optimally adjusting the
SWCNT density to be around the percolation threshold, because of the existing metallic
SWCNTs. Because the increase in the ratio of semiconducting SWCNTs results in theincrease in the SWCNT density of the percolation threshold, the development of
DNA-SWCNTs with a semiconducting single-chirality is important for the upgrade of
SWCNT-TFT performances.
In this study, we purified CoMoCAT and eDIPS [3] SWCNTs by IEX for the fabrication of
SWCNT-TFTs using purified DNA-SWCNTs.
Acknowledgment: This work was supported by Iketani Science and Technology Foundation.
A part of this work was conducted at the Nano-Processing Facility, supported by IBEC
Innovation Platform, AIST and "Nanotechnology Network Japan" of the Ministry of
Education, Culture, Sports, Science and Technology (MEXT), Japan.
(a)

(b)

Fig.1 Absorption spectra of DNA-SWCNTs before and after IEX.
(a) eDIPS, (b)CoMoCAT[1] X. Tu et al., Nature. 460, 250 (2009).
[2] Y. Asada et al., Adv. Mater. 23, 4631 (2011).
[3] T. Saito et al., Nanosci. Nanotechnol. 8, 6153 (2008).
Corresponding Author: Takeshi Saito
Tel: +81-29-861-4863, Fax: +81-29-861-4413,
E-mail: takeshi-saito@aist.go.jp- 167 -

3P-26
Effects of pulse conditions on growth of (6,5) enriched single-walled carbon
nanotubes under pulse plasma CVD○Bin Xu, Toshiaki Kato, Koshi Murakoshi, and Toshiro Kaneko
Department of Electronic Engineering, Tohoku University, Sendai, 980-8579 Japan
Single-walled carbon nanotubes (SWNTs) have very unique one dimension structure whichleads to many novel characteristics like high mechanical strength, enhanced optical absorption,high current density, and so on. Since the electronic and optical properties of SWNTs aremostly decided by their chirality, chirality-controlled SWNTs synthesis is one of the major
challenges in nanotube science and applications. Plasma CVD that has a relative low reaction
temperature and can precisely control the synthesis time are often used to synthesize nanocarbon materials [1-3]. By using plasma CVD, we have realized synthesis of SWNTs withnarrow-chirality distribution [4,5].
In our previous study, the correlation between the incubation time and SWNTs chirality
distribution was investigated. We found that SWNTs with only small diameter andnarrow-chirality distribution can be grown by using
short time plasma CVD [4]. To increase the SWNTs
quantity, we improved the previous method andintroduced a novel method, which is pulse plasma
CVD. SWNTs synthesized by pulse plasma CVD
can be with large quantity as well as
narrow-chirality distribution.
For the synthesis of SWNTs with higher purity,
we also tried to elucidate the effects of pulse
parameters such as on and off times on the growthof narrow chirality-distributed SWNTs. The
chirality distribution of SWNTs becomes narrower
with an increase in off time (Fig.1), which can be
explained by the combination of the incubation
time difference between small and large diameter Fig.1: Diameter distribution of SWNTs with
SWNTs and changes of catalyst particle size due to the variation of off time
Ostwald ripening.
[1] T. Kato, L. Jiao, X. Wang, H. Wang, X. Li, L. Zhang, R. Hatakeyama, and H. Dai : Small 7, 574 (2011).
[2] T. Kato and R. Hatakeyama: ASC Nano 6, 8508 (2012).
[3] T. Kato and R. Hatakeyama: Nature Nanotechnology 7, 651 (2012).
[4] T. Kato and R. Hatakeyama: ACS Nano 4, 7395 (2010).
[5] Z. Ghorannevis, T. Kato, T. Kaneko, and R. Hatakeyama: J. Am. Chem. Soc. 132, 9570 (2010).
Corresponding Author: B. Xu
Tel: 022-795-7046, Fax: 022-263-9225,
E-mail: xu12@ecei.tohoku.ac.jp- 168 -

3P-27
Selective recognition of semiconducting single-walled carbon nanotubes
with large diameters by using polyfluorenes carrying mono-alkyl chain
Takahiro Fukumaru1, Fumiyuki Toshimitsu1, Tsuyohiko Fujigaya1,2, Naotoshi
Nakashima1,2,3
1

Department of Applied Chemistry, Graduate School of Engineering, Kyushu University,
744 Motooka, Fukuoka 819-0395, Japan
2 WPI-I2CNER, Kyushu University, 744 Motooka, Fukuoka 819-0395, Japan
3
Japan Science and Technology Agency, CREST, 5 Sanbancho, Chiyoda-ku, Tokyo,
102-0075, JapanFor the fundamental nanotubes science aswell as fabrication of high-performance
single-walled carbon nanotubes (SWNTs)
devices, sorted SWNTs with a specific chirality
are strongly demanded. One of the mostpromising approaches is to design and synthesize Fig.
1
Chemicalstructuresofa molecule that enables to selectively poly(9,9-dioctyl-fluorene-2,7-diyl) (2C8-PFO)
recognize/extract
SWNTs. (left) and poly(9-octyl-9H-fuluorene-2,7-diyl)
Poly(9,9-dioctyl-fluorene-2,7-diyl) (2C8-PFO, (C8H-PFO) (right).
in Fig. 1, left)[1] are attractive molecules
because they recognize and extract only semiconducting SWNTs, while the mechanism is still
unclear. Here we focused on the alkyl chain number on the PFOs to understand themechanism.
Wesynthesized
polyfluorene
carrying
mono-octyl
moiety(poly(9-octyl-9H-fuluorene-2,7-diyl (C8H-PFO in Fig. 1, right), and characterized its
selective recognition/extraction ability toward SWNTs.
C8H-PFOwassynthesizedbyYamamoto coupling of fluorene monomer
carrying Br-terminated mono-octyl moiety.
Fig. 2 shows the 2D-PL mapping of the
SWNT solution in toluene with C8H-PFO(C8H-PFO-SWNTs, left) and 2C8-PFO(2C8-PFO-SWNTs, right) for comparison.
Fig. 2 2D-PL maps of C8H-PFO-SWNTs (left) andIn the case of C8H-PFO-SWNTs, little bit
2C8-PFO-SWNTs (right) for comparison.
larger diameter SWNTs (0.9 – 1.1 nm) wereextracted and many (n,m)SWNTs such as(9,5)SWNT (chiral angle: 20.66 º) and (10,5)SWNT (chiral angle: 19.16 º) were observed,
which indicated that C8H-PFO recognized larger diameter semiconducting SWNTs withbroad chiral angle (>20 º). In other words, the second alkyl chain in fluorene unit enabledboth the chiral angle selection and diameter selection for semiconducting SWNTs. Molecularmechanics simulation was revealed that C8H-PFO showed superior diameter selective
recognition to 2C8-PFO.
[1] A. Nish et al. Nat. Nanotechnol. 2, 640 (2007).
Corresponding Author: N. Nakashima
Tel: +81-92-802-2840, Fax: +81-92-802-2840,
E-mail: nakashima-tcm@mail.cstm.kyushu-u.ac.jp- 169 -

3P-28
Cloning Growth of Single-Walled Carbon Nanotubes
from Activated Nanotube Edges‫ۑ‬Takanori Umino, Taiki Inoue, Shohei Chiashi and Shigeo Maruyama
Department of Mechanical Engineering, The University of Tokyo, Tokyo 113-8656,
Japan
The chirality controlled synthesis is one of the most important topics in the researchof single-walled carbon nanotubes (SWNTs). Recently, metal-catalyst free chemical
vapor deposition (CVD) growth of SWNTs from nanotube edges (also referred to as“cloning”) has been reported [1, 2]. Although this technique is promising for chirality
controlled synthesis [2], further improvement of the yield is required.
Here, we performed CVD growth of SWNTs from nanotube edges to understand themechanism and improve the growth yield. Firstly, horizontally aligned SWNTs weregrown from patterned Fe catalysts on quartz substrates and partially removed byphotolithography and O2 plasma treatment. Figure 1 (a) shows a scanning electron
microscopy (SEM) image of patterned SWNTs. The samples were then placed in a
CVD chamber and annealed in air at 200 qC, followed by water vapor exposure at 800
or 900 qC. In these processes, nanotube edges were activated as the template for thegrowth of SWNTs. Finally, CVD growth was performed at 800, 850, or 900 qC using
ethanol gas as the carbon feedstock. As shown in Fig. 1 (b), SWNTs were grown fromsome of the nanotube edges. Although the occurrence ratio of SWNT growth to original
nanotube edges was less than 1 % in the case of one cycle of activation and growth, theyield of SWNTs gradually increased by repeating the cycles. In Raman scattering
spectra, G-band and D-band were obtained from SWNTs grown from nanotube edges.
Atomic force microscopy observation revealed the SWNT diameters of the grown parts
and the original parts(a)(b)
were almost same.

[1] Y. Yao, et al., Nano Lett.,
9 (2009) 1673.
[2] J. Liu, et al., Nat.
Commun., 3 (2012) 1199.

10 Pm

10 Pm

Fig. 1 SEM images of (a) partially etched SWNTs for the growth
template and (b) the sample after the growth process.
Corresponding Author: Shigeo Maruyama
TEL: +81-3-5841-6421
FAX: +81-3-5800-6983
E-mail:maruyama@photon.t.u-tokyo.ac.jp- 170 -

3P-29Growth of high-density carbon nanotube arrays
toward thermal interface materials○Nuri Na1,2, Kei Hasegawa2, Suguru Noda2,*
1
2

Department of Chemical System Engineering, The University of Tokyo, Japan
Department of Applied Chemistry, Waseda University, Tokyo 169-8555, Japan

Carbon nanotubes (CNTs) are a candidate for future thermal interface materials (TIMs)
owing to their high thermal conductivity (3000 W/m K) and mechanical flexibility. However,typical CNT arrays grown by conventional chemical vapor deposition (CVD) method havethermal conductivity far below the expected values because of their porous structure (> 90%
porosity) and high thermal resistances at the contact with opposing substrates. Therefore, inthis work, we target at high-density CNT arrays with uniform height for TIM applications.
Two approaches are possible in preparing CNT arrays on metal foils; one is transfer of
CNT arrays grown on oxide substrates to the foils and the other is direct growth of CNT
arrays on the foils. We deposited Ni, Co, or Fe catalyst on TiN or Al2O3 underlayer by
sputtering, annealed them with pure H2 at 500-700 C, and then carried out CVD by feeding
C2H2 at a pressure of 3-300 mTorr. We evaluated the height and density of CNTs by scanningelectron microscopy (SEM) with by energy dispersive X-ray spectroscopy.
The height and density of CNT arrays changed largely with a trade-off relationship,depending on the catalyst and underlayer used. Fig. 1 shows the typical CNT arrays grown by
Ni particles on TiN/SiO2/Si, which had a density as high as 2.6×1012 cm-2 prior to CVD. At ahigh C2H2 pressure of 30 mTorr,
CNT arrays initially had a highdensity (0.7 g cm–3 for 0.5 μm-tall
arrays) but abruptly lost the density
due to the rapid catalyst
deactivation. Whereas at a low
C2H2 pressure of 3 mTorr, CNT
arrays had a moderate and constantdensity (0.4 g cm–3). We thenexamined the two step growth
where the CNT nucleation wasenhanced by feeding C2H2 at 30
mTorr for the initial 20 s and thenthe CNT growth was sustained byfeeding C2H2 at 3 mTorr for 1-60
min. This method yielded CNT
arrays with a steady density as high as
0.5 g cm–3 with a uniform height(Fig 1e). Careful control over Fig 1. (a) CNT height vs. growth time, (b) mass density vs. CNT
nucleation and growth of CNT height. Cross-sectional (c-e) and top-view (f-h) SEM images ofarray are keys to tailor CNT CNT arrays grown at constant C2H2 partial pressures (3, 30 mTorr)and by the two-step growth method.
structure for application to TIMs.
*Corresponding Author: Suguru Noda, Tel&Fax: +81-3-5286-2769, E-mail: noda@waseda.jp- 171 -

3P-30
Selective Growth of Single-Walled Carbon Nanotubes with Specific
Diameter and Chirality by Irradiating Free Electron Laser during Growth○Keisuke Yoshida1, Takumi Sagara1, Yusaku Tsuda1, Koji Ishii2, Kenichi Yamakawa1,
Hirofumi Yajima2, Nobuyuki Iwata1 and Hiroshi Yamamoto1
1

Department of Electronics & Computer Science,College of Science & Technology, Nihon
University, 7-24-1 Narashinodai, Funabashi, Chiba 274-8501 Japan2
Department of Applied Chemistry, Faculty of Science, Tokyo University of Science, 1-3
Kagurazaka, Shinjyuku-ku, Tokyo 162-0826, Japan

Single-Walled carbon nanotubes (SWNTs) have been regarded as one of the best
candidates for future applications in nanoelectronic devices due to its high mobility, highcurrent-carrying capacities, and so on. The drawback for nanoelectronics using SWNTs isthat almost all of the current available technologies for the SWNTs growth can only produce a
mixture of metallic and semiconducting one. We demonstrate the novel technique tosynthesize as-grow semiconducting SWNTs with approximately 1.1 nm in diameter including(14,0), (13,2), (10,6), (9,7) chiralities using free electron laser (FEL) irradiation with thewavelength of 800 nm during growth[1]. However, the mechanism to control the chirality
and the diameter by the FEL has not been clear yet. The aim of this study is to elucidate therole of the FEL irradiation for the selective SWNTs growth.
Figure1 shows the Raman spectra of the SWNTs grown with the 765 nm FEL irradiation
for RBM. The appearance of a lot of peaks indicates that the selective growth is notachieved by the 765nm-FEL. From the Kataura plot and the RBM peaks of the SWNTs
grown with the 765nm-FEL, grown SWNTs had both of semiconducting and metallic
properties. Same results were obtained using 835nm-FEL. Considering the CVD conditionis suitable to grow SWNTs with 1.1 nm, the 800nm-FEL is effective for selective growth withspecific chirality. The origin is expected to be the catalyst diameter just before CVD. We
will clarify the relationship between the catalyst diameter and suitable FEL wavelength forselective growth, which must be connected to the role of the FEL irradiation for the selective
growth.

Fig.1 Raman spectra of the SWNTs grownwith the 765 nm FEL. Used excitation laser
was 441 nm, 532 nm, 632 nm and 785 nm.

Fig.2 Diameter of the SWNTs grown with the
765 nm FEL on Kataura plot[2].

[1] K.Sakai, et al., IEICE TRANS. Electron, E94-C (2011) 1861.
[2] R. Saito, PHYSICAL REVIEW B, VOLUME 61, 2981 (2000)- 172 -

3P-31Tuning the Seebeck coefficient of single-wall carbon nanotubes
by encapsulation of guest materials

1○Tomohiro Ueda1, Yusuke Nakai1, Yasumitsu Miyata1,2 and Yutaka Maniwa1
Department of Physics, Faculy of Science, Tokyo Metropolitan University, 1-1
Minami-Osawa Hachioji, Tokyo 192-0397, Japan
2
JST, PRESTO, Kawaguchi, 332-0012, Japan

Modification of the electronic state of single-wall carbon nanotubes (SWCNTs) is amethod of generating novel physical properties. One simple method of modifying theelectronic structure of SWCNTs is encapsulating molecules or atoms into channels of
SWCNTs. Our recent study has shown that highly-enriched semiconducting SWCNTs films
exhibit a large Seebeck coefficient [1]. Since the Seebeck coefficient is sensitive to theelectronic state, it is expected that the Seebeck coefficient varies with introducing guest
materials into the channels of SWCNTs. In order to achieve a better thermoelectricperformance in SWCNT films, we investigate the effects of various materials encapsulated
inside SWCNTs on the Seebeck coefficient.
In order to examine encapsulation of guest materials in the inner channels, we performed
powder X-ray diffraction (XRD) measurements of SWCNT films which we conductedencapsulation treatment through a vapor phase method. We found that the intensity of (1 0)peak from SWCNT bundles is weaker than that of empty SWCNTs, and that new
characteristic XRD peaks appear after the encapsulation treatment. These results suggest thatguest materials are encapsulated in the channels of SWCNTs. We then measured Seebeckcoefficient of the SWCNTs samples encapsulating various materials, and found that theirSeebeck coefficient is significantly different from empty SWCNTs. These results suggest that
introducing guest materials into the channels of SWCNTs is an effective way to tune thethermoelectric performance.
[1] Y. Nakai et al., to appear in Appl. Phys. Express.
Corresponding Author: Y. Nakai
Tel: +81-42-677-2498-, Fax: +81-42-677-2483,
E-mail: nakai@tmu.ac.jp- 173 -

3P-32
Molecular structure of the thiophene oligomers encapsulated insingle-walled carbon nanotubes by molecular dynamics simulations○Hiromu Tabata1, Akinori Sekine 1, Kazumi Inoue2, Yousuke Kataoka 2
and Hironori Ogata1,2,3
1

Graduate School of Engineering, Hosei University, Koganei, 184-8584, Japan
Department of Faculty of Bioscience and Applied Chemistry, Hosei University, Koganei,
184-8584, Japan
3
Research Center for Micro-Nano Technology, Hosei University, Koganei, 184-0003, Japan
2

Single-walled carbon nanotubes (SWNTs) have a hollow space in the nanometer size thatcan be encapsulated various functional molecules. Recently, thiophene oligomer encapsulated
SWNTs are synthesized and their optical properties were reported[1,2]. Their optical properties
depend on the orientation of thiophene oligomers encapsulated. π -stacking type or
herringbone type has been reported to the molecular arrangement of thiophene oligomers.
However the systematic studies of thiophene oligomers encapsulated in SWNTs with various
diameters and chirality’s have not been reported. In this study, we report the effects ofchirality and tube diameter of SWNTs on the molecular orientations of the thiopheneoligomers by using molecular dynamics(MD) simulations.
In our MD simulations, we used the Dreiding intramolecular potential and the OPLS
intermolecular potential. By placing the SWNT and quaterthiophene in a rectangular cell, toobtain a stable structure at 298K after the relaxation in the 1 K with the NVT ensemble.
Figure 1 shows the structure of the molecular orientation of quaterthiophenes(4T)
encapsulated in (10,10) tube. 4T molecules are oriented in units of three molecules inparallel along the longitudinal axis of the tube. The detailed systematic results that effects ofchirality and tube diameter has on the thiophene oligomers in SWNTs will be presented.

Figure 1. The structure of 4T@SWNT[1] Loi, M. A. et al. Adv. Mater. 2010, 22, 1635.
[2] Gao,J et al. Small 2011, 7, 1807.
[3] Yamashita, H.; Yumura, T. et al., J. Phys. Chem. C 2012, 116, 9681
Corresponding Author: Hironori Ogata,Tel: +81-42-387-6229, Fax: +81-42-387-6229, E-mail: hogata@hosei.ac.jp- 174 -

3P-33
Influence of growth substrates on chemical reactivity of CVD graphene○Ryosuke Inoue1, Yasumitsu Miyata1,2, and Yutaka Maniwa1
1

Department of Physics, Tokyo Metropolitan University, Hachioji, 192-0397, Japan
2
JST, PRESTO, Kawaguchi, 332-0012, JapanThe control of chemical reactivity of graphene is one of the important issues for its chemicalfunctionalization and etching. In many cases, graphene is grown on metal substrates such as copper
foil by chemical vapor deposition (CVD). It remains an unsettled question how the growth substrates
affect the chemical reactivity of graphene. Especially, it is reported that generally-used cupper foil ispolycrystalline and its surface shape strongly depends on crystal faces [1]. Such surface shape could
relate to the reactivity through the change in crystallinity and internal stress of graphene. To test thishypothesis, we have investigated that the effect of crystal faces on chemical reactivity of CVD
graphene.
Graphene was grown on commercially-available copper foil (Nilaco) by methane CVD. The
graphene grown was then etched by annealing under hydrogen or oxygen atmospheres. The surfaceof the used copper foil mainly consists of (111) face with large roughness and of relatively-flat (100)face. After the hydrogen etching, we found that there is a large difference in etching rates between
the (111) and (100) faces (Fig.1a). This difference means that the (100) face can produces morestable graphene than on the (111) face. Raman imaging reveals that there is non crystal-facedependence in the intensity of D-band and 2D-band of graphene (Fig.1b-d). This result suggests thatthe reactivity of CVD grapene on cupper foil is infuluenced by not its crystallinity but the roughnessof substrates. The present finding gives a useful guide for the control of graphene etching andfunctionalization .

Fig.1 (a) Optical microscope image of graphene on Cu foil after hydrogen etching. (b) Dark-field
image, (c) D-band intensity, and (d) 2D-band intensity maps of the same graphene grains.
[1] X. H. Kong, et al., Appl. Phys. Lett. 103, 043119 (2013)
Corresponding Author: Yasumitsu Miyata
TEL:+81-42- 677-2508, FAX:+81- 42-677-2483, E-mail: ymiyata@tmu.ac.jp- 175 -

3P-34
Synthesis and Characterization of Metal Intercalated bilayers Graphene○Imai Kentaro, Shogo Sato, Kuniharu Matsuki, Nobuyuki Iwata, Hiroshi Yamamoto
College of Science &Technology, Nihon University, 7-24-1 Narashinodai, Funabashi-shi, Chiba
2748501
Graphite intercalation compounds (GIC) is prepared on various substances.

Superconducting[1]

transition temperature Tc of GIC with Ca are reported at 11.5K . In this study we aim at realizing
a room temperature superconductivity (RTS) in a metal intercalated bilayer graphene due to anelectron-exciton coupling rather than electron-phonon coupling. The Tc is expected to be higher
than room temperature as long as a disorder and a roughness of the graphene layers are much
reduced.

aqueous solution. The PMMA/graphene layer wastransferred on the SiO2/Si substrate, and evaluated by amicro Raman spectroscopy and a four probes electricmeasurement system.
Figure1 shows the Raman spectrum of graphene. The
peaks of G, D, and G’, respectively, were observed at
1593, 1347 and 2699.4 cm-1, indicating the presence ofa graphene sheet.

Figure2 shows the temperaturedependence of the sheet resistance of the graphene. The
sheet resistivity increased as decreasing temperature.
It is expected that the defect and/or roughness are present.
The result of synthesis and characterization intercalated
bilayers graphen will be discussed.
[1] N. Emery et al.: Phys. Rev. Lett. 95 (2005) 087003[2] A Reina et al.: Nano letters. 9 (2009) 30.

- 176 -

Intensity (arb. units)hydrogen. After the graphene growth on copper foil,
the specimen was coated by a poly methyl methacrylate(PMMA) layer[2]. The copper foil was etchedcompletely as soaking the specimen in an iron(III) nitrate

1000
800
600
400
200
0
1000

1500

2000

2500

3000

Wavenumber (cm-1)

Figure1:Raman spectra of graphene between
1500 and 3000 cm-1.
4000

Sheet resistance [ / sq.]

Graphene was prepared by chemical vapor deposition(CVD) method. We grew graphene on copper foil witha 20 μm thickness at temperatures up to 1000°C for 30
min by CVD of carbon using a mixture of methane and

3500
3000
2500
2000
1500
1000
75 100 125 150 175 200 225 250 275 300 325

Temperature [K]Figure2:Tenperature
characterization at 300~90k

Resistivity

3P-35
CVD Growth of Graphene Nanoribbons on Cu (100) Film
○ Rozan Mohamad Yunus1, Masahiro Miyashita1, Masaharu Tsuji1,2, Hiroki Hibino3, andHiroki Ago*,1,2
12Graduate School of Engineering Sciences, Kyushu University, Fukuoka 816-8580, Japan
Institute for Materials Chemistry and Engineering, Kyushu University, Fukuoka 816-8580,
Japan
3
NTT Basic Research Laboratories, NTT Corporation, Kanagawa 243-0198, Japan

Graphene is a one-atom thick lattice of honeycomb arranged carbon atoms, which exhibits
excellent electronic, optical, thermal, and mechanical properties [1]. Unlike thesemiconductor silicon, graphene has no band gap which is crucial for electronics applications
such as field-effect transistors with a high on/off ratio. Theoretical and experimental works
have demonstrated that quantum confinement into a one dimensional structure, so calledgraphene nanoribbons (GNRs), can potentially open the band gap [2]. Recently, several
approaches have been developed to produce GNRs such as lithographic methods andunzipping of carbon nanotubes. The reliable production of narrow GNRs by a bottom up
approach has still not been well established and is a significant challenge.
Previously, we studied the domain structures of single-layer graphene grown on
heteroepitaxial metal films in terms of crystalline plane dependence [3-5]. Based on theseresults, we have developed a novel method to synthesize GNRs using CVD. Ambient pressure
CVD growth on a flat epitaxial Cu (100) metal film was performed at 900-1000 ºC under aflow of CH4/H2/Ar mixed gas. We observed the growth of nanoribbons on the entire metal
surface where the nanoribbons alignment reflects̴ 43 nmthe crystallographic orientation of the underlying̴ 50 nmCu film. From SEM measurements, narrow GNRs
with the width about 40-50 nm were obtained as
̴ 45 nmshown in Figure 1. The Raman spectrum oftransferred GNRs on SiO2/Si revealed that thesenanoribbons are single-layer graphene with low
defects. Moreover, the dark-field low energy
500 nmelectron microscope (LEEM) measurements
Figure 1: SEM image of GNRs on SiO2/Si
suggested that these GNRs have zigzag edges
regardless of the nanoribbons width. Our bottom-up approach offers a new method to growsingle-layer GNRs which are oriented in a specific direction of the metal film for futurecarbon-based electronics and spintronics applications.
[1] A. K. Geim, Science, 324, 1530 (2009)., [2] X. Li. et al., Science, 319, 1229 (2008)., [3] H. Ago et al., ACS
Nano, 4 (2010) 7407., [4] Y. Ogawa et al., J. Phys. Chem. Lett., 3 (2012) 219., [5] H. Ago et al., J. Phys. Chem.
Lett., 3 (2012) 2228.
Corresponding Author: Hiroki Ago (Tel & Fax: +892-583-7817, E-mail: ago@cm.kyushu-u.ac.jp)- 177 -

3P-36
Liquid-phase exfoliation of graphene from graphite withtriphenylene derivatives○Ryusuke Funahashi1,2, Gang Liu 1, Shuji Aonuma2, Takahide Kimura1,
Naoki Komatsu1
1

Department of Chemistry, Shiga University of Medical Science, Otsu 520-2192, Japan2
Department of applied chemistry, Osaka Electro-Communication University,
Osaka 572-8530, Japan

Liquid phase exfoliation has been frequently
used for production of graphene from graphite in
the presence or absence of an exfoliant. A flat-conjugated molecule such as pyrene or
porphyrin derivatives is reported to be efficient
exfoliant [1-2], because π-π and hydrophobic
interactions between the flat molecule andgraphene can accelerate the exfoliation of graphite
Fig. 1 Structures of triphenylene derivatives 1 and 2
and stabilize the resulting graphene insolution. In this paper, we appliedb)triphenylene derivatives (Fig. 1) as a)novel exfoliants for liquid phase
exfoliation of graphene from graphite.
After a mixture of graphite and thetriphenylene 1 or 2 was bath-sonicatedin THF, the resulting suspension wascentrifuged at 114 g or 1028 g to give
black supernatant. The supernatants
were analyzed with absorption and Fig. 2 STEM images of exfoliated graphene with 1 (a) and 2 (b)Raman spectroscopies, and STEM.
The existence of graphene wasconfirmed by the STEM shown in
Fig. 2. The Raman spectra shown in
Fig. 3 indicate that a few-layer
graphene is considered to exist
judging from the ratio of G’ / G andthe symmetrical shape of G’ band. It
is concluded that triphenylene
derivatives have the ability to
exfoliate graphite to produce Fig. 3 Raman spectra of commercial graphite, and exfoliated graphenewith triphenylenes 1 and 2graphene in solution phase.
[1] C. Casiraghi et al. Carbon, 53, 357 (2013). [2] Hee-Tae Jung et al. Chem. Commun., 46, 5091 (2010).

Corresponding Author: Naoki Komatsu Tel: +81-77-548-2102, Fax: +81-77-548-2405,
E-mail: nkomatsu@shiga-med.ac.jp- 178 -

3P-37
Plasma effects on growth of graphene nanoribbon
from nickel nanobar under rapid heating plasma CVD○Hiroo Suzuki, Toshiaki Kato, Toshiro Kaneko
Department of Electronic Engineering, Tohoku University, Sendai 980-8579, Japan
Graphene nanoribbons combine the unique electronic and spin properties of graphene witha transport gap that arises from quantum confinement and edge effects. This makes them anattractive candidate material for the channels of next-generation transistors. Althoughnanoribbons can be made in a variety of ways, the reliable site and alignment control ofnanoribbons with high on/off current ratios remains a challenge. Plasma chemical vapor
deposition (CVD) is known as fruitful method for the structural-controlled growth anddamage-free functionalization of nano carbon materials such as carbon nanotubes [1-3] andgraphene [4,5].
We have developed a new, simple, scalable method based on the advanced plasma CVD
method for directly fabricating narrow (~23 nm) graphene nanoribbon devices with a clear
transport gap (58.5 meV) and a high on/off ratio (>104) [6]. Since the establishment of our novel
graphene nanoribbon fabrication method, direct conversion of a Ni nanobar to a graphene nanoribbon is
now possible. The growth mechanism of graphene nanoribbon, however, is not wellunderstood, which is important for the stable fabrication of graphene nanoribbon devices.
We investigate the growth mechanism ofgraphene nanoribbon by comparing
evaporation rate of nickel between plasma
and thermal CVD (Fig. 1). It is found thatthe evaporation rate of nickel is low inplasma CVD compared with that ofthermal CVD. This should relate with thedifference of carbon concentration innickel. In plasma CVD, large amount ofhydrocarbons can be supplied to nickel
due to high rate dissociation of carbon
source gas. The balance of evaporation
rate of nickel and amount of supplying
carbon closely relates with growth of Fig.1: Nickel evaporation rate as a function of CVD time.
graphene nanoribbon.
[1] T. Kato and R. Hatakeyama, J. Am. Chem. Soc. 130, 8101 (2008).
[2] T. Kato and R. Hatakeyama, ACS Nano 4, 7395 (2010).
[3] Z. Ghorannevis, T. Kato, T. Kaneko, and R. Hatakeyama, J. Am. Chem. Soc. 132, 9570 (2010).
[4] T. Kato, L. Jiao, X. Wang, H. Wang, X. Li, L. Zhang, R. Hatakeyama, and H. Dai, Small 7, 574 (2011).
[5] T. Kato and R. Hatakeyama, ACS Nano 6, 8508 (2012).
[6] T. Kato and R. Hatakeyama, Nature Nanotechnology 7, 651 (2012)
Corresponding Author: H. Suzuki
Tel: +81-22-795-7046, Fax: +81-22-263-9225,
E-mail: suzuki12@ecei.tohoku.ac.jp- 179 -

3P-38
Influence of electrolyte concentration for electrochemical exfoliation ofgraphene○Haruya Okimoto, Hiroki Kuronuma, and Masahito Sano
Department of Polymer Science and Engineering, Yamagata University, Yonezawa, 992-8510,
Japan

Corresponding Author: H. Okimoto Tel/FAX: +81-238-26-3074
E-mail: haruya@yz.yamagata-u.ac.jp[1]D.C. Alsmeyer and R.L. McCreery, Anal. Chem., 64, 1528(1992).

- 180 -

(a)(b)

CountsFig. 1 AFM image of exfoliatedgraphene at (a) 10 mmol/L and (b)100 mmol/L.

CountsRecent developments in liquid phase exfoliation of graphite
to give graphene mean it is now possible to prepare dispersed
grapehene cheaply and easily. For example, theelectrochemical exfoliation using electrolyte is one of low-cost
synthesis of graphene. However the mechanism of theelectrochemical exfoliation are usually more complicated ascompared to those of the chemical intercalation since theformer relates to several components of the system(solvent,voltage etc.) which can interfere with the major process.
Understanding the influence of several components leads tothe control of the properties of exfoliated graphene. In thisstudy, we demonstrate how electrolyte concentration forelectrochemical exfoliation of graphite affects the shape andthickness of exfoliated graphene.
Electrochemical exfoliation was done in an electrolysis cell.
This cell has graphite foil(Grafoil, Grafguard) as anode and Pt
plate as cathode in electrolyte solution. Na2SO4 was used aselectrolyte for exfoliation. The electrolyte concentration was 1
mmol/L to 1 mol/L.
Fig. 1 shows the AFM image of exfoliated graphene using 10
mmol/L and 100 mmol/L electrolyte solutions. The edge of the
exfoliated graphene at 10 mmol/L was usually etched structure
than that at high electrolyte concentration. At low electrolyte
concentration, the exfoliation process become very slow
compared with exfoliation at high electrolyte solution. In theelectrochemical reaction between graphite and acid, graphite
intercalation was accompanied with graphite oxidation at
positive potential.[1] Therefore, the long-time applied voltage
for exfoliation of thin graphene at low concentration leads tooxidize graphene surface. As a result, the exfoliated graphene
at 10 mmol/L was damaged than that at 100 mmol/L.
Fig. 2 shows the thickness diagram of exfoliated graphene by
1 mmol/L and 1 mol/L concentration. The low concentrationof electrolyte led to thicken the thickness of graphene. If
grafoil was exfoliated by sonication, the thickness of
exfoliated graphene was 10 to 100 nm. Therefore, we suggestthat the changing of the electrochemical exfoliated graphene
thickness depends on the electrolyte concentration.
As a result, we suggest that the electrolyte concentration
affects the shape and thickness of exfoliated graphene byelectrochemical exfoliation.

30 (a)
15

040 (b)
20
1M
0
0
2
4
6
Thickness (nm)Fig 2 Histograms of graphene
thickness at (a) 100 mmol/L and(b) 1 mmol/L.

3P-39High gain CMOS inverters based on transition metal dichalcogenides○Jiang Pu 1, Jing-Kai Huang 2, Yoshihiro Iwasa 3,4, Lain-Jong Li 2, Taishi Takenobu 1,5
12

Department of Applied Physics, Waseda University, Tokyo 169-8555, Japan
Institute of Atomic and Molecular Sciences, Academia Sinica, Taipei 11529, Taiwan
3
Department of Applied Physics, The University of Tokyo, Tokyo 113-8656, Japan
4
RIKEN Center for Emergent Matter Science (CEMS), Wako 351-0198, Japan
5
Kagami Memorial Laboratory, Waseda University, Tokyo 169-0051, Japan

Two dimensional (2D) materials such as monolayer transition metal dichalcogenides(TMDCs) are attracting potential electronic applications as a transistor fabricated for logic
electronics because of its large bandgap and high mobility. Owing to their atomic scale
thickness, 2D TMDCs offer a high degree of electrostatic control than those of bulk forms,
which provide significant advantage for constructing low-power electronic devices. Recently,
integrated circuits based on bilayer MoS2, including inverters and ring oscillators, havedemonstrated [1]. Although the MoS2 transistors typically show n-type behavior, further
advances require CMOS circuits composed of n-type and p-type transistors. Moreover,current researches have been performed on mechanically exfoliated TMDCs, which hamper
the practical utility of TMDCs for application to large-area integration. In this paper, wedemonstrate CMOS inverters fabricated with large-area MoS2 and WSe2 electric double layertransistors (EDLTs). The huge capacitance of ion gels enables the strong depletion of donor
carriers and efficient carrier doping, resulting in realizing high gain CMOS inverters.
The large-area trilayer MoS2 and monolayer WSe2 films were synthesized on sapphire
substrates through chemical vapor deposition [2-4]. The gold electrodes, ion gels and top-gate
Pt foil were stacked on film surface to build EDLTs. The fabricated WSe2 EDLTs exhibitedhigh hole mobility of 55cm2/Vs and excellent current on/off ratio of 107, whereas the MoS2
EDLTs showed high electron mobility of 60 cm2/Vs. Because of large specific capacitance ofion gels, the CMOS inverters constructed from p-type WSe2 and n-type MoS2 operated atsignificantly low voltage of 0.5V, which consequently yielded extremely high gain of 110 thatis the highest value in atomically thin 2D materials (Fig. 1). Our results provide thesubstantial possibility of 2D materials for large-area low-power CMOS logic devices.

Fig. 1 Output (left) and gain (right) characteristics of a WSe2 and MoS2 based CMOS inverter[1] H. Wang et al. Nano. Lett. 12, 4674 (2012).
Corresponding Author: T. Takenobu[2] J. Pu, T. Takenobu et al. Nano. Lett. 12, 4013 (2012)..
Tel/Fax: +81-3-5286-2981[3] J. Pu, T. Takenobu et al. Appl. Phys. Lett. 103, 023505 (2013)..
E-mail: takenobu@waseda.jp[4] J. K. Huang, J. Pu, T. Takenobu et al. ACS. Nano. DOI: 10.1021/nn405719x (2013).

- 181 -

3P-40High efficiency graphene doping
Kai-Wen Cheng1, Po-shin Lin1 ,Ya-Ping Hsieh1
1
Graduate of Institute of Opto-Mechatronics, National Chung Cheng University, ROC

Figure of meritsdcsop

Graphene, a monoatomic layer of carbon, has inspired work in many fields from fundamental
science to application oriented research. Due to its unique combination of metallic characterand its limited absorption due to its atomic thickness, graphene is well suited as a transparent
optical conductor (TOC). To compete with mature TOC technologies, such as Indium tin oxide,
graphene’s performance as an electrical conductor has to be improved.
Increase of carrier concentration has been identified as the most feasible route to improving
graphene film conductance. As an alternative, chemical doping has been widely used .While
impressive results have been shown, the produced samples are still falling short of therequirements on conductance and transmittance to replace ITO.
We here present a novel approach to increasing the conductance of graphene. For theseexperiments we utilize single layer polycrystalline graphene synthesized by chemical vapor
deposition on Cu substrate to produce high quality samples of centimeter scale. Our approachrelies on considering the effect of doping on carrier mobility instead of focusing on maximizing
the doping density, as has been the most common route for chemical doping. By carefully tuning
the concentration of dopant we are able to identify a transport region in which the positive effectof charge addition is outweighing the detrimental consequences of charged impurity scattering.
We accomplish this fine doping control by in-situ measurement of carrier concentration andmobility throughout the doping process and find that we can increase the film conductivity by
up to 300%.
We furthermore demonstrate that a second doping step can further increase the charge carrier
density without significantly deteriorating the carrier mobility as identified by electrical and
Raman measurements. Consequently an additional increase of conductivity by up to 300% canbe seen. The reason of this additional increase was found to be interactions of the first andsecond dopant.
The presented results not only improve our understanding of the doping process and its
relation to the graphene morphology but have significant impact on the commercial potentialof graphene. The doping process increases graphene conductivity by almost one order ofmagnitude and thus produced samples exhibit some of the highest conductivity reported in theliterature and can rival ITO. Our findings therefore open the field of graphene-based transparent
circuits and electrodes for novel applications
120
100
80
60
40
20
0

Our method
Layer by layer@AuCl3

Minimum industry standard
Graphite

1

2

AuCl3
doped

3 Ranking 4

Figure 1 Comparison of Figure of Merit for different graphene samples
Corresponding Author: Ya-Ping Hsieh
E-mail: yphsieh@ccu.edu.tw- 182 -CVD
Graphenesolutiongraphene56

3P-41
Drastic Change in Photoluminescence Properties ofSize-separated Graphene Quantum Dots
1

1

, Shinichiro Mouri1, Ryo Kitaura3,
Hisanori Shinohara3, Toku Yasuda4, Naoki Komatsu4, and Kazunari Matsuda1○Naoto Fuyuno , Daichi Kozawa , Yuhei Miyauchi

1, 2

1

Institute of Advanced Energy, Kyoto University, Uji, Kyoto 611-0011, Japan
Japan Science and Technology Agency, PRESTO, 4-1-8 Honcho Kawaguchi, Saitama
332-0012, Japan3
Department of Chemistry and Institute for Advanced Research, Nagoya University,
Nagoya 464-8602, Japan
4
Department of Chemistry, Shiga University of Medical Science, Otsu 520-2192, Japan
2

Normalized PL Intensity (arb. units)

Frequency

Graphene quantum dots (GQDs), which are nanometer-size graphene flakes, haveattracted a great deal of interest from the viewpoints of fundamental physics andoptoelectronics. It has been reported that GQDs show photoluminescence (PL) in
visible light region, however, the mechanism of PL in GQDs has not been wellunderstood. Considering quantum size effect, the optical properties of GQDs should be
affected by their overall size, although the size-dependent PL in GQDs is controversial.
In the present study, we conducted size separation of GQDs by high performanceliquid chromatography (HPLC) and observed drastic change in PL depending on theoverall size of GQDs. The GQDs were fabricated by acid treatment of pitch-basedcarbon fibers [1] and size of GQDs was confirmed by transmission electron microscope
50(TEM) images. Figure 1a shows size distribution (a)Large GQDs
histograms of large and small GQDs sample
40
Small GQDs
separated by HPLC. Average sizes of large and30
small GQDs are 10.8 and 6.8 nm, respectively.
Figure 1b shows PL spectra of large and small
20
GQDs obtained from excitation wavelength of 280
10
nm. The large and small GQDs show emission
0
peak at 530 nm and 330 nm, respectively. By01020
detail measurements, PL of GQDs is found to be
Lateral Size (nm)composed of four discrete features and drastic PL (b)Large GQDs
change by size separation is understood by the
Small GQDs
1.0change in relative intensity of those PL features.
lex=280 nm
These results indicate that PL originates fromsmall sp2 fragments embedded in GQDs and0.5
drastic PL shift is explained by the change in the
population of sp2 fragments in the GQDs with
0
300 400 500 600 700 800
different overall sizes.
[1] J. Peng et al., Nano lett. 12, 844 (2012).
Corresponding Author: N. Fuyuno
Tel: +81-774-38-3465, Fax: +81-774-38-3467
E-mail: fuyuno.naoto.67n@st.kyoto-u.ac.jp

Emission Wavelength (nm)Fig. 1 (a) Size distribution histogramsand (b) normalized PL spectraof GQDs separated by HPLC.

- 183 -

3P-42
Energetics and Electronic Structure of Graphene Edges○Ayaka Yamanaka, Susumu Okada
Graduate School of Pure and Applied Sciences, University of Tsukuba, Tennodai, Tsukuba
305-8577, Japan
Graphene is attracting much attention due to its possible application for semiconductor
electronic devices. In particular, graphene is regarded as the one of promising emerging
materials in the next generation. Therefore, it is urging us to unravel fundamental propertiesof graphene for designing and fabricating graphene-based electronic devices. In this work, we
study the energetics and electronic structure of graphene with various edge structures toprovide a theoretical insight for fabricating the graphene devices with nano-scale.
All calculations are performed by using the density functional theory. To express theexchange correlation potential among interacting electrons, we apply the local density
approximation. We use an ultrasoft pseudopotential to describe the interaction between
valence electrons and ions. The effective screening medium (ESM) method is applied toinvestigate behaviors of graphene nanoribbon under the electric field in the framework of thefirst-principles calculations.
In this study, we consider graphene nanoribbons with various edge shape of which edge
angles are θ = 0° (armchair), 8°, 16°, 23°, and 30° (zigzag) shown in Figs. 1 (a), 1 (b), 1 (c), 1(d), and 1 (e), respectively. As shown in Fig. 1 (f), the edge formation energy depends on theedge angle: edge formation energy keep(a) 0°(b) 8°(c) 16° (d) 23°(e) 30°constant value of 0.35 eV up to the angle θ =15°, while the energy monotonically increase
with increasing the edge angle. Therefore, theedge with near armchair shapes areenergetically favorable for the H-terminatedgraphene ribbon. Small edge formation energy
is ascribed to the semiconducting electronic
properties of graphene nanoribbons with neararmchair edges. On the other hand, increase ofdensity of state at EF arising from edge states(f) Edge Formation Energy
leads to the monotonical increase of edge
formation energy for large θ. We also study
the electronic structures of these graphene
nanoribbons under a parallel electric field. We
find that the π and π* states repulse each other
under the electric field leading to the decreaseof edge formation energy.
Corresponding Author: A. Yamanaka
Tel: +81-29-853-5600 (ext. 8233),
Fax: +81-29-853-5924,
E-mail: ayamanaka@comas.frsc.tsukuba.ac.jp

Fig.1 (a)-(e) Geometric structures and (f) edge
formation energy of hydrogenated graphene
nanoribbons.

- 184 -

3P-43
Fine Control of Oxidation of Graphitic Carbons by Oxidation of Graphite
or Reduction of Highly Oxidized Graphene Oxide○Yuta Nishina1,2, Naoki Morimoto1
1

Research Core for Interdisciplinary Sciences, Okayama University,
Okayama 700-8530, Japan2
Precursory Research for Embryonic Science and Technology, Japan Science andTechnology Agency, 4-1-8 Honcho, Kawaguchi, Saitama 332-0012, Japan
Control of oxidation level in the graphite- and graphene-like materials is important to tailor
the functionality to suit the relevant areas of applications that include optoelectronics,
physical-, biological-, and energy-related materials. For example, carboxyl group-freegraphene oxide (GO) would be desirable for the production of defect free graphene by
reduction. In contrast, oxygen functional groups are necessary for the synthesis of GO
composites with nanoparticles, organic molecules, and heteroatoms. Application for
conductive films, electrodes for lithium ion battery, super capacitor, and catalyst for fuel cellwould often require the functionalization processes to improve GO’s performance.
We have achieved the fine tuning of the oxygen content by oxidation and reduction
processes. The oxidation content was analyzed by elemental analysis, and properties of eachGOs were measured by XPS, XRD, electron conductivity, oxidation ability, and cyclic
voltammetry.

Corresponding Author: Y. Nishina
Tel: +81-86-251-8483
E-mail: nisina-y@cc.okayama-u.ac.jp- 185 -

3P-44Structural and magnetic changes of nanodiamond-copper
composites during HPHT Sintering Process
Fedor Shakhov 1, Vladimir Osipov 1, Sergei Kidalov 1, Kazuyuki Takai 2, Toshiaki Enoki 3,
Alexander Vul’ 1
1
Ioffe Physical-Technical Institute, St. Petersburg 194021, Russia
2
Department of Chemical Science and Technology, Hosei University, Tokyo 184-8584, Japan3
Department of Chemistry, Tokyo Institute of Technology, Tokyo 152-8551, JapanThe surface modification of nanodiamond is important in view of the investigation of theorigin of the spin magnetism of nanodiamond. Especially, building a nano-composite isinteresting method which enables to introduce the interface between nanodiamond surface andtransition metal chemically inert for carbon. In this study, a series of copper composites with
detonation nanodiamonds (DND) [1] was prepared at high pressure-high temperature (HPHT)
conditions, and evaluated in terms of the spin magnetism.
The composite synthesis was performed by sintering a mixture of DND and Cu-particles
under the temperature varied from 1100 oC to 1900 oC and the pressure of ~7 GPa for ~ 60 sec.
The weight contents of DND phase were about 20 wt.% in all synthesized Cu / DND
composites. The magnetic susceptibilities of prepared composites were studied by using
SQUID magnetometer in the temperature range 2 - 300 K.
The magnetic susceptibilities of all the samples well follow the Curie-Weiss law in thetemperature range below 100 K. The Curie-Weiss term in the magnetic susceptibility isrelated with the presence of paramagnetic spins (S = 1/2) of unpaired free radicals locating in
the DND particles and not in the host copper matrix which is well conductive. Recently, we
found that these paramagnetic spins (S = 1/2) are originated from the own vacancy-based
defects of diamond lattice located within thin (~ 1.5 nm) undersurface layer of DND particles
with mean size ~5 nm [2]. The concentrations of localized spins in a DND phase ofsynthesized composites is about 5.4 - 6.0×1019 g-1, which are a little bit lower than those inpristine DND in the powder form (~ 6.3×1019 g-1). The increasing in the temperature of HPHT
synthesis from 1100 oС to 1900 oC does not practically affect on the concentration of unpaired
radicals in DND phase, although the subtle reducing with raising the synthesis temperature isobserved. These results mean that vacancy-based defects of DND are not so movable at shorttime of HPHT synthesis. Moreover, during rapid HPHT synthesis of Cu / DND composites,
DND particles inside the matrix do not subjected to the intensive graphitization process
causing additional spin magnetism and their crystalline cores are well conserved and stable inmelted copper even at temperatures up to 1900 oC. The observed structural stability isunderstood taking the fact into account that copper does not create covalent bonds andinterfacial compounds with external carbon atoms of DND. Further development andoptimization the synthesis technique of DND / Cu composites will be also discussed in thispaper. This work was supported by the Japan-Russia Research Cooperative Program within
the grants: RFBR 12-02-92107 ЯФ_а and JSPS.
[1] А. Aleksenskiy, M. Baidakova, V. Osipov, A. Vul. The Fundamental Properties and Characteristics ofNanodiamonds. In: “Nanodiamonds: Applications in Biology and Nanoscale Medicine” Ed. Dean Ho. Spinger
New York, Dordrecht, Heidelberg. London. 2009. p.55-78.
[2] A.I. Shames, V.Yu. Osipov, A.E. Aleksenskiy, E. Ōsawa, A.Ya. Vul'. Diamond Relat Mater., 20, 318 (2011).
Corresponding Author: Fedor Shakhov (fedor.shakhov@mail.ioffe.ru).

- 186 -

3P-45Synthesis and characterization of Pt , Pt-Ru nanoparticles on carbon
nanomaterials by one-step electrodeposition○1Shohei Hayase, 1Haruhiko Yoshitake, 2Wang Zhipeng 1,3Hironori Ogata
1

Department of Chemical Science and Technology,Hosei University Koganei 184-8584
Japan
2
Institution for Sustainability Research and Education, Shinshu University Nagano
380-8553 ,Japan
3
Research Center for Micro-Nano Technology,Hosei University,Koganei 184-0003,Japan
Direct methanol fuel cells (DMFCs) are one of the most promising transportable powersources which can be used in mobiles, laptops, and small power generation. The basic
operation principle of DMFCs involves methanol oxidation and oxygen reduction on the
precious metal catalysts, which are loaded on the support surfaces. As is well-known, thedispersion of Pt-based alloys on carbon supports as well as catalyst particle size and shapeplays a dominant role in the electrochemical performance for fuel cells. In this study, we
explore the carbon materials as a catalyst support for Pt-based nanoparticles by one-step
electrodeposition. The morphology, microstructure, chemical compositon, andelectrochemical properties of the carbon nanosheets (CNS) -, Single walled Carbon
Nanotubes(SWNTs) or highly ordered pyrolytic graphite(HOPG) supported Pt-based
nanoparticles were systematically investigated.
Figure.1 shows the one example of the CV responses of Pt-Ru/HOPG and table.1 shows theelectrochemical characteristic of methanol oxidation. The detailed results on the relationshipbetween the condition of electrodeposition, the chemical compositon of nanoparticles andtheir electrocatalytic performance for methanol oxidation will be presented.
2
5

-2

3

Current density[mA/cm2]

Current density[mA/cm2]

4

2
1
0

-1
-2

-4
-6
-8
-10
-12
-14
-16

-3
-4
-0.4

HOPG

0

HOPG

-18
-0.2

0.0

0.2

0.4

0.6

0.8

0.0

1.0

Potential [V, vs Ag/AgCl]

0.2

0.4

0.6

0.8

Potential [V, vs Ag/AgCl]

Figure 1. CV responses of Pt-Ru/HOPG

Table.1 Electrochemical characteristic of methanol oxidation

1) Zhipeng Wang, Mao Shoji and Hironori Ogata, Appl. Surf. Sci.259(2012)219-224.
Corresponding Author: Hironori Ogata,Tel: +81-42-387-6229, Fax: +81-42-387-6229, E-mail: hogata@hosei.ac.jp- 187 -

1.0

3P-46
Hydration of Nanodiamond Surface Revisited: Intercalation Hypothesis
Ryoko Yamanoi1, Amanda Barnard2, Shuichi Sasaki1, and Eiji sawa1*
1

NanoCarbon Research Institute, AREC, Shinshu University, Ueda, 386-8567, Japan
2
CSIRO, Material Science and Engineering, Clayton, Victoria 3052, Australia

Self-polarization across diamond core and graphitic shell in the detonation nanodiamond (DND)
led to novel facet-dependent multi-pole charge-distribution for particles with diameters smaller than
3nm [1,2]. Early observation by Korobov et al. on water layers freezing at -8°C on the surface of
DND hydrogel by means of DSC§ was interpreted as strong H-bonding of water molecules to thehighly negative-charged {111} facets [3]. However, it was recently realized that the DND particles
they used contained substantial fractions of the smallest oligomers of primary particles. Our recent
success in isolating true primary particles of detonation nanodiamond (PPDND) with a record low
average diameter of 2.8±0.5 nm [4] prompted us to repeat the DSC experiments on the hydrogel. In
addition to the H-bond peak, now appearing at -11°C, a broader peak centered at -16°C was detectedduring melting (Fig. 1). The purpose of this presentation is to assign the origin of the latter peak.
SCC-DFTB# calculations of 3nm diamond models revealed substantial space below the surface
shell (Fig. 2). Furthermore, the central region of every {111} facet has negative curvature whichmust be accompanied with large strain. If these regions were etched off the surface during drastic
oxidation process to remove soot in the purification of crude DND, the holes thus formed will serveas passages for solvent molecules, which will eventually be intercalated tight in the narrow spacesurrounded by deformed graphene patches. We suggest these trapped water molecules constitute thepeak at -16°C in Fig. 1.

)LJ'6&§WUDFHRIPHOWLQJ33'1'             )LJ2SWLPL]HGJHRPHWU\RID33'1'PRGHOThe possibility of intercalation pockets accessible from the open surface, although still
hypothetical, explains superb suppression of side effects in our DDS that uses DND as drug carrier
and being developed for cancer thermotherapy [5]. When an anti-cancer drug molecules(doxorubicin ammonium salt) are loaded on DND by salting-in technique, they will go deep into
the pockets below the particle surface inactivated, and won’t come out until pulled out by changing
pH of blood or salting-out.
[1] Barnard, A. S.; Sternberg, M. J. Mater. Chem., 17, 4811 (2007). [2] Barnard, A. S.; Osawa, E. Nanoscale 6, 1188
(2014). [3] M. V. Korobov et al., J. Phys. Chem. C. 111, 7330 (2007). [4] S. Sasaki et al., Presented in this General§
Symposium. [5] Moore, L. K. et al., Disruptive Sci. Technol. 1, 54 (2012). Differential scanning calorimetry.
#Self-consistent charge density function tight binding theory. *Corresponding Author: osawa@nano-carbon.jp, Tel:
+81-268-75-8381, Fax: +81-268-75-8551.

- 188 -

3P-47
Doping of zinc to the iron oxide nanotubes by using a poly-condensation of
metal nitrate hydrates on the surface of surfactant
ż Yuta Kosugi1, Shunji Bandow2
Department of Materials Science & Engineering1 and of Applied Chemistry2,
Meijo University, Nagoya 468-8502, Japan
The iron oxide nanotubes (Fe-ox-NTs) are formed by the sol-gel technic using a
poly-condensation of iron nitrate hydrate on the surface of self-assembled block-copolymer of a
Pluronic F-127 [1-3], and the structural properties of the product were studied [4].

From thesestudies, we found that the structure of crude Fe-ox-NTs was classified into amorphous likedisordered J-Fe2O3 or Fe3O4.

By annealing the

2.8

sample in open air at 320 ȚC, such disordered phase waswithout destructing the tube structure. An annealing
temperature dependence of the band gap estimated byusing the Kubelka-Munk analysis [5,6] of the opticalabsorption indicated a minimum of ca. 2.3 eV whenannealing at ~300 ȚC as shown in Fig. 1.

Although themagnitude of this minimum is just located in the green
light region where the radiant flux ofBand gap (eV)relaxed and the structure was changed to D-Fe2O3

2.7
2.6
2.5
2.4
2.3
2.2
150

200

250

300

Annealing temperature (°C)

350

Fig. 1. Annealing temperature dependenceof the band gap of Fe-ox-NTs determinedby the Kubelka-Munk analysis.

the sun light shows maximum, a
LUMO level of the iron oxide isslightly deeper than the reduction
potential of hydrogen. In the present
study, we tried to dope Zn element toFe-ox-NTs in order to approach a
LUMO level to the reduction potentialof hydrogen.

A doping of Zn toFe-ox-NT was carried out by mixing a

Fig. 2. TEM of Zn-Fe-ox-NTs prepared from (a) 2 wt % of Zn
nitrate hydrate mixture and (b) 10 wt %. Black-contrasted
materials in (b) are the particles agglomerated.

zinc nitrate hydrate to an iron nitrate hydrate up to a few tens wt %. As a result, we found from
TEM observation that the tubule structure was dominantly formed in the low concentration of zinc
nitrate hydrate by ~10 wt %, but increasing the particle contents (Fig. 2). Although XRD
profiles of all the products are also assignable to amorphous like disordered J-Fe2O3 or Fe3O4
even adding Zn, XPS clearly indicated the existence of Zn element. These features, including
the band gap determined from the optical absorption, will be presented in the poster.
[1-3] Y. Shiraki et al., 42nd FNT, March 6-8 (2012), Tokyo, 3P-49, 43rd FNT, Sep. 5-7 (2012), Sendai, 3P-38,
44th FNTG (March, 2013), 2P-45. [4] S. Bandow et al., 45th FNTG, Aug.5-7 (2013), Osaka, 3P-14. [5] V.
Džimbeg-Malþiü et al., Technical Gazette 18, 117 (2011). [6] S.S. Kumar et al., Inter. Nano Lett. 3, 30 (2013).
Corresponding Author: S. Bandow, Tel: +81-52-838-2404, E-mail: bandow@meijo-u.ac.jp- 189 -

3P-48Synthesis of high purity carbon nanocoils on the sheet-like carbon deposits
and reduction of byproducts using Fe fine particles○Yoshiaki Shimizu1, Koji Maruyama1, Tetsuo Iida1, Yoshiyuki Suda1, Hideto Tanoue1,
Hirofumi Takikawa1, Hitoshi Ue 2, Kazuki Shimizu 3, Yoshito Umeda4
1

Department of Electrical and Electronic Information Engineering, Toyohashi University ofTechnology, Toyohashi, Aichi 441-8580, Japan
2
Fuji Research Laboratory, Tokai Carbon Co., Ltd., Oyama, Shizuoka 410-1431, Japan
3
Development Department, Shonan Plastic Mfg. Co., Ltd., Hiratsuka, Kanagawa 254-0807, Japan
4
Toho Gas Co., Ltd., Nagoya, Aichi 456-8511, Japan
1. Introduction
Carbon nanocoil (CNC) is a nano-carbon material with “coiled” structure composed offibers with diameters of 100－500 nm. It is very important to take into account the purityof CNCs during application, such as in electromagnetic wave absorbers. Generally, CNCs
are synthesized from composite catalysts including Fe-Sn. In our laboratory, we havesynthesized high purity CNCs grown from the surfaces of the sheet-like carbon deposits
using Fe particles of 3－5 μm diameters. The sheet-like carbon deposits consist of fibrouscarbon materials containing CNCs and other carbon materials (byproducts). The CNCs
mainly exist on the surfaces of the sheet-like carbon deposits. In our previous study, we
have improved the purity of CNCs more than 90 % (1). In this study, we used Fe fineparticles with 0.02 μm diameters and focused on reducing of byproducts.
2. Experimental
Fe catalyst particles of 0.02 μm (The Nilaco Corporation, 224050) or 3－5 μm(Kojundo Chemical Laboratory Co., Ltd, 085523) diameters and SnO2 solutions (Kojundo
Chemical Laboratory Co., Ltd, 235061) were dissolved in ethanol. The surfaces of Si
substrates were spin-coated or drop-coated with the solution and sintered at 350◦C in air for
5 min. The substrates supporting catalytic particle layer were placed into an automatic
CVD apparatus (1). Nitrogen (N2) and acetylene (C2H2) gases were supplied to theapparatus for 10 min to grow CNCs while temperature at 780◦C. The N2 and C2H2 flow
rates were 1400 and 350 ml/min, respectively. Products were observed using a scanningelectron microscope (SEM).
3. Results
Cross sectional SEM images of synthesized sheet-like carbon deposits with Fe catalyst
particles of 0.02 μm and 3－5 μm diameters are shown in Fig. 1. We can see that numerous
CNCs grew. However, a byproduct layer also formedat the base of the CNCs (2). Fig. 1(a) shows that the
byproduct layer thickness is 20 μm. It is less thanthat with Fe catalyst particles 3－5 μm (120 μm).
The purity of CNCs is more than 90 % and became
the highest in this study when the mole ratio of
Fe:Sn=1:2.6.
[1] M. Yokota, et al: J. Nanosci. Nanotechnol, 10 (2011) 3910
[2] K. Hirahara, et al: Carbon, 56 (2013) 264
Corresponding Author: Y. Shimizu
E-mail: shimizu.yoshiaki@pes.ee.tut.ac.jp- 190 -

Fig. 1 Cross sectional SEM images ofsynthesized carbon nanomaterials with Fe
catalyst particles of (a) 0.02 μm and(b) 3－5 μm diameters.

3P-49Synthesis and characterization of two-dimensional semiconductor
heterojunction based on transition metal dichalcogenides○Shohei Mori1, Yasumitsu Miyata1,2, Yutaka Maniwa1
1

Department of Physics, Tokyo Metropolitan University, Hachioji, 192-0397, Japan
2
JST, PRESTO, Kawaguchi, 332-0012, JapanThe heterojunctions in two-dimensional materials have attracted much attention because of
their interface-related properties and electronics applications. To date, several groups havereported the synthesis of metal-insulator junction consisted of graphene and hexagonal boron
nitride [1-3]. In contrast, realizing the two dimensional semiconductor heterojunctions is still
highly desired as components of various electronic devices. To solve this issue, we focus ourattention on the heterostructure of two different kinds of transition metal dichalcogenides(TMDs) as shown in Fig.1a.
In this presentation, we report the formation of the heterojunction consisting of single-layer
WS2 and MoS2. As precursors of these TMDs, thin films of WO3 and MoO3 were preparedon Si wafers by vacuum deposition. These oxide thin films were sulfurized by annealing
under sulfur/argon atmosphere. The heterostructure of WS 2/MoS2 was prepared by two-step
growth processes of WS2 and MoS2 on the same substrate. Optical microscope observations
reveal that two-dimensional crystals grown consist of two kinds of films with different
contrast and sharp interface (Fig.1b). Furthermore, the existence both of single-layer MoS2
and WS2 is confirmed from their photoluminescence spectra (Fig.1c). These results show that
the TMD-based semiconductor heterojunction can be formed by the two-step sulfurization
process. The present semiconductor heterostructure would provide a promising system
for the realization of one-dimensional electron gas and electronic devices such as p-njunctions.

Fig.1 (a) Schematic illustration of WS2/MoS2 heterojunction. (b) Optical microscope image and fluorescentimage in the box (inset) of typical WS2/MoS2 heterostructure. (c) Photoluminescence spectra of WS2/MoS2
sample at different points (MoS2, WS2, and WS2/MoS2) and single-layer W1-xMoxS2. The spectrum of W1-xMoxS2
is shown for comparison.
[1] Y. Miyata, et al. Appl. Phys. Express 5 (2012) 085102.,[2] M. Levendorf et al. Nature, 488 (2012) 627., [3] P. Sutter et al. Nano Lett., 12 (2012) 4869.
Corresponding Author: Yasumitsu Miyata
TEL:+81-42- 677-2508, FAX:+81- 42-677-2483,
E-mail: ymiyata@tmu.ac.jp- 191 -

3P-50Electro-Chemical Doping Properties of
MoS2-Single Wall Carbon Nanotube Hybrid Film
Hideaki Endo, ○Hideki Kawai, Kai Hasegawa, Seiya Kaji, Kazuhiro Yanagi
Department of Physics, Tokyo Metropolitan University, Tokyo 192-0397, JapanThe transition-metal dichalcogenide MoS2 has attracted great interest due to its distinctive
electronic and optical properties. The layered materials can be shaped into mono-layer whichshows distinct physical properties from their bulk counterpart. The materials are typically
prepared by mechanical exfoliation techniques or chemical synthesis. Extraction of
mono-layers by dispersion of bulk materials (liquid exfoliation) is also possible,1 but
formation of uniform film of monolayer is technically difficult by just aggregating thedispersed MoS2. In this study, we tried to control the aggregation processes of the dispersed
MoS2 by inserting single-wall carbon nanotubes (SWCNT) in order to demonstrate theproperties of monolayer MoS2 in the film. Here we produced the MoS2- SWCNT hybrid films,
and we investigated their optical and electronic properties by the carrier injection using
electro-chemical doping techniques. First we dispersed MoS2 to sodium cholate 2% solutions
by tip-type ultra-sonicators, and the solutions were purified by several centrifugation
processes, and mixed with electronic type selected SWCNT solutions. Then the thin films
were formed. Figure 1 shows the change of optical absorption spectra of the MoS2-metallic
SWCNT hybrid films by the electro-chemical doping techniques. The A and B opticalabsorption peaks of MoS2 were clearly disappeared as the shift of the potential to - 2.0 V (vsAg/Ag+), suggesting the success of the electron
injection to MoS2. Figure 2 shows the Raman
spectra of MoS2-metallic SWCNT hybrid films.
The two peaks around 385 cm-1 and 400 cm-1
were attributed to E2g and A1g modes of MoS2,
respectively. As the shift of potential to -2.8 V,
the A1g mode was clearly disappeared. This isconsistent to the results of electrochemical
doping upon the monolayer of MoS2 reported by
Chakraborty et al.2 In the transport properties of
MoS2-metallic SWCNTs hybrid films and Figure 1 optical absorption spectra of
MoS2-metallic SWCNT hybrid films as ametallic SWCNT films, we observed the distinct functionof potential voltages
enhancement of current in the hybrid films
around the positive gate voltage, 3.5V, reflecting
the carrier injection to MoS2. The results
indicate that the optical and electricalcharacteristics of MoS2-SWCNT hybrid films
were controlled by electro-chemical doping
techniques.
Ref: [1] J. Coleman et al., Science 331, 568 (2011) [2]
Chakraborty et al., PRB 85, 161403(R) (2012)
Corresponding Author: Kazuhiro Yanagi
Tel: +81-42-677-2494
E-mail: yanagi-kazuhiro@tmu.ac.jp- 192 -

Figure 2 Raman spectra of MoS2-metallc
SWCNT hybrid film as a function of potential
voltagesⓎ⾲⣴ᘬAuthor Index

Author Index<A>
Abe, Shigeaki
Abe, Yurika
Abiko, Yoshihiro
Achiba, Yohji
Ago, Hiroki
Akama, Toshiki
Akasaka, Takeshi
Akiyama, Wataru
Akizuki, Naoto
Akutagawa, Tomoyuki
Alberti, Mariza N.
Ando, Yoshinori
Aoki, Nobuyuki
Aonuma, Shuji
Aoyagi, Shinobu
Arai, Shigeo
Araki, Takuma
Asaka, Kinji
Asaka, Koji
Asano, SatoshiAta, Seisuke

3P-19
2P-49
2P-24
1P-6, 2-4, 2P-49,
3P-15
1P-44, 2P-45, 3P-35
2P-24
1P-12, 3P-1
1P-4, 2P-5
1P-13, 3P-7
2-11
1P-2
1P-33, 2P-28
1P-4, 2P-5
3P-36,
2P-7, 2-11
2P-33
1P-9
3-1
2P-40
1P-26
3-3

<B>
Baba, Keisuke
Bandow, Shunji
Barnard, Amanda
Bayer, Thomas
Berber, Mohamed
Bird, Jonathan P
Bishop, Sean
Bissett, Mark

2P-1
3P-47
3P-46
3-6
1P-24
1P-4, 2P-5
3-6
2P-45

<C>
Carvalho, Alexandra
Castro Neto, Antonio H.
Cha, JinHyeok
Chen, Zhongming
Cheng, Kai-Wen
Chenxing, Wang
Chiang, Bo-Suei
Chiashi, Shohei

1-8
1-8
2P-18
1P-10
3P-40
2P-40
3-11
1P-34, 2-1, 2S-5,
2-8, 2P-15, 2P-18,
2P-32, 2P-41, 3P-9,
3P-28- 193 -

<D>
Diederich, François
Ding, Wuxiao

1P-2
2P-36

<E>
Eda, Goki
Endo, Hideaki
Endo, Hitomi
Endo, Tomoaki
Endoh, Hiroyuki
Enoki, Toshiaki

1-8, 1P-48, 1P-49
3P-50
2P-49
2P-7
1P-20
3P-44

<F>
Fujigaya, Tsuyohiko

Funahashi, Kazuma
Funahashi, Ryusuke
Futaba, Don
Fuyuno, Naoto

1P-22, 1P-24, 1P-29,
2P-25, 3P-16, 3P-27
1P-47
2P-28
1P-26, 1P-28, 2P-31
3P-18, 3P-20
1-7
1P-35
1P-6
3P-27
2P-43
2P-29
1P-5, 1P-18, 3P-3,
2-12
2P-44
3P-36
2-2, 3-3
3P-41<G>Goto, Takumi
Guldi, Dirk M.

1P-21
1P-2

Fujii, Hiromu
Fujii, Keisuke
Fujii, Shunjiro
Fujimoto, Taiyo
Fujimoto, Yoshitaka
Fujita, Hayato
Fujita, Wataru
Fukumaru, Takahiro
Fukumori, Minoru
Fukuzawa, Masashi
Fukuzumi, Shunichi<H>
Hamahata, Hiroki
Harima, Hiroshi
Hasdeo, Eddwi H.
Hasegawa, Kai
Hasegawa, Kei
Hasegawa, Tadashi
Hasegawa, Yuri
Hashikawa, Yoshifumi

3P-18
2P-10
1P-11, 3P-6
2P-30, 3P-50
1P-10, 1P-41, 2P-18,
3-2, 3P-22, 3P-29
1P-12, 3P-1
2P-7
2P-2

Huang, Jing-Kai
Huang, Wenxin

2-4
3P-23
2-12
2P-10
1P-12
1P-19
2-2, 3-3
2P-13
2P-24
3P-45
3-5
1-3
3P-35
1P-19
1-2
3-3
2P-19, 2P-21
1P-28
1P-15
1P-28, 2-7, 2P-31
1-5
2-1
3-10
1P-43, 3-11, 3-12
2P-15
1P-30, 2S-5, 2-6,
2P-15, 2P-16, 2P-41,
3P-9
1P-16
3P-21
2P-39
2-11
1P-43, 3-7, 3-11,
3-12, 3P-40
3P-39
2P-25

<I>
I, Akiko
Ichida, Masao
Ichihashi, Toshinari
Iida, Ryosuke
Iida, Tetsuo
Iijima, Sumio
Ikenaga, Eiji
Ikuma, Naohiko
Im, Inseob
Imai, Kentaro

3-5
2P-47
1P-39
3P-1
3P-48
1P-38, 1P-39, 2P-36
2-3
2-9, 2-10, 3P-3
1-3
3P-34

Hashimoto, Kenro
Hashimoto, Yu
Hasobe, Taku
Hasuike, Noriyuki
Hasuike, Yuhei
Hata, KatsuhikoHata, KenjiHata, Tomoyuki
Hatakeyama, Rikizo
Hayase, Shohei
Hayashi, Kenjiro
Hayashi, Tatsuya
Hibino, Hiroki
Higuchi, Kentaro
Hino, Shojun
Hirabayashi, Tatsuya
Hiraiwa, Atsushi
Hirakawa, Takuya
Hirana, Yasuhiko
Hirano, Atsushi
Hiroshiba, Yasuhiro
Hisama, Kaoru
Hiura, Hidefumi
Hofmann, Mario
Homma, Naoki
Homma, Yoshikazu
Hong, Liu
Hongmei, Qin
Honma, Itaru
Hoshino, Norihisa
Hsieh, Ya-Ping- 194 -

Inaba, Daiki
Inaba, Masafumi
Inoue, Chozo
Inoue, Kazumi
Inoue, Ryosuke
Inoue, Sakae
Inoue, Taiki
Inoue, Yoshihisa
Inukai, Ryota
Irie, Michiko
Ishii, Akihiro
Ishii, Koji
Ishiyama, U
Ito, MasahiroIto, Yasuhiro
Ito, Yoshiaki
Ito, Yosuke
Ito, Yusuke
Itoh, Chihiro
Iwaizako, T
Iwasa, Yoshihiro
Iwata, Nobuyuki
Izumi, Yudai

3P-1
2P-19, 2P-21
1P-40
1P-1, 3P-32
3P-33
1P-33
2-8, 3P-28
1-6
3P-18
1P-39
2P-17, 3P-5, 3P-13
1P-17, 3P-30
3P-8
2-6, 2P-16
1P-28
1P-4
3P-15
2-6, 2P-16
1P-9, 2P-10, 3-1
1P-44
2P-44, 3P-39
1P-17, 3P-30, 3P-34
2-3<J>Jang, Jin
Jeon, IL
Jinnouchi, Ryota
Jippo, Hideyuki
Juhasz, Gergely

1-3
2P-3, 3P-23
1-5
3-4
1P-15

<K>
Kaji, Seiya
Kako, Masahiro
Kanazawa, Naoki
Kaneko, Toshiro
Kasama, Yasuhiko
Kaskela, Antti
Kataoka, Yosuke
Kataoka, Yousuke
Kataura, Hiromichi
Kato, Hiroki
Kato, Toshiaki
Kato, Yuichi
Kato, Yuichiro K.
Kauppinen, Esko I.
Kawabata, Akio

2P-22, 3P-50
3P-1
1P-27
2P-24, 3P-26, 3P-37
2P-7
2P-23
1P-1
3P-32
1P-26, 1P-28, 2-7,
2P-31
1P-30, 2-6, 2P-16
2P-24, 3P-26, 3P-37
2P-29,
2P-17, 3P-5, 3P-13
2P-23, 3S-7
2-3

Kawachi, Kazuhiko
Kawahara, Kenji
Kawai, Hideki
Kawai, Hiroki
Kawai, Tsuyoshi
Kawarada, Hiroshi
Kawasaki, Shinji
Kawashima, Yuki
Kawasuzuki, Tomoya
Kidalov, Sergei
Kigure, Shota
Kihara, Hideyuki
Kikuchi, Hayato
Kikuchi, Koichi
Kim, Dong Young
Kim, Junpil
Kimura, Takahide
Kishikawa, Keiki
Kishimoto, Shigeru
Kisoda, Kenji
Kitakawa, Haruki
Kitaura, Ryo
Kiyomiya, Masaharu
Kobashi, Kazufumi
Kobayashi, Keita
Kobayashi, Tatsuki
Kobayashi, Toshiyuki
Kobayashi, Yoshihiro
Kodama, Takeshi
Kohmoto, Shigeo
Kohno, Naoki
Koinuma, Michio
Kokubo, Ken
Komatsu, Ken-ichirou
Komatsu, Naoki
Konabe, Satoru
Kondo, Daiyu
Konno, Toshio
Koretsune, Takashi
Kosaka, Masaki
Kosugi, Yuta
Kotsugi, Masato
Kozawa, Daichi
Kudo, Hikaru
Kumamoto, Yusuke

2P-7
1P-44
2P-22, 2P-30, 3P-50
2P-13
1P-25, 2P-20
2P-19, 2P-21
2P-14
1P-5, 2-12
2-1
3P-44
2P-35
2P-27
1P-32
1P-6
1P-10, 3-2, 3P-22
3-9
3P-21, 3P-36
3P-24
1P-19, 1P-23, 2P-23
1P-9, 2P-10
2P-43
1P-31, 1P-42, 2P-6,
2P-33, 2P-38, 3P-4,
3P-41
1P-26, 1P-37
3-3
1P-37
1P-6
3S-8
2P-43
1P-6, 2-4
3P-24
1P-18
2P-46
2-9, 2-10, 3P-3
2P-7
3P-21, 3P-36, 3P-41
1P-46, 1P-49
3-5
1P-3
1-7, 3P-12
1P-41
3P-47
2-3
1-8, 1P-50, 2P-26,
2P-47, 3P-41
2P-22
3P-5, 3P-13- 195 -

Kutsuzawa, Dai
Kuwahara, Yuki
Kwon, Eunsang

1-8
1-8
1P-38
3P-38
1P-36
1P-35, 2P-19, 2P-21,
2P-42
3P-23
3P-25
2P-7

<L>
Laiho, Patrik
Lee, Chih-Yu
Lee, Heaseong
Lee, Jeonyoon
Lee, Seungjoo
Li, Lain-Jong
Li, YanLin, Po-shin
Liu, Gang
Liu, Jianfeng
Lyth, Stephen

2P-23
2P-19, 2P-21
1-3
2P-18
1-3
2P-44, 3P-39
2S-4
3P-40
3P-36
3-6
3-6

Kumar, Amara Kiran
Kumar, Rajeev Sharma
Kunioka, Masao
Kuronuma, Hiroki
Kurumi, Satoshi
Kusunoki, Michiko<M>
Ma, Shao-Wei
Machida, Tomoki
Maeda, Michihiko
Maeda, Yutaka
Manako, Takashi
Maniwa, Yutaka
Maruyama, Koji
Maruyama, Mina
Maruyama, Shigeo
Masubuchi, Satoru
Masuda, Hideki
Masuda, Hiroyuki
Masuda, Yoshiho
Matsuda, Kazunari

Matsuda, Ken-ichi
Matsuda, Mitsuaki
Matsuki, Kuniharu

3-7
1-6, 1P-45
1P-19
1P-12, 3P-1
1P-20, 2P-37
3P-10, 3P-31, 3P-33,
3P-49
3P-48
2P-9
1P-34, 2-1, 2-8,
2P-18, 2P-32, 2P-41,
3P-28
1-6, 1P-45
1P-8
2-9, 2-10
2P-19, 2P-21, 2P-42
1-8, 1P-13, 1P-16,
1P-28, 1P-31, 1P-48,
1P-49, 1P-50, 2P-26,
2P-47, 3P-7, 3P-41
1P-36
2P-10
3P-34

Matsumoto, Morihiro
Matsumoto, Yasumichi
Matsuo, Shintaro
Matsuo, Yutaka
Matsushita, Tomohiro
Matsuura, Tomohiro
Matsuzaki, Satoki
Matsuzawa, Yoko
Mieno, Tetsu
Mikami, Ninako
Mikie, Tsubasa
Minami, Kazuya
Mitoma, Nobuhiko
Miura, Asuka
Miyabe, Kyosuke
Miyamoto, KatsuhikoMiyashita, Masahiro
Miyata, Yasumitsu
Miyauchi, Yuhei

Miyazaki, Daiki
Miyazaki, Takafumi
Miyazawa, Kun'ichi
Mizuno, Masashi
Mohamed, Berber
Momiyama, Daiki
Mori, Shohei
Morikawa, Sei
Morimoto, Naoki
Morimoto, Takahiro
Moriya, Rai
Moriyama, Hiroshi
Mouri, Shinichiro
Mukai, Ken
Munkh-od, Batbuyan
Murakami, Tomo
Murakami, Toshiya
Murakoshi, Koshi
Muraoka, Yoshimi
Murata, Michihisa
Murata, Yasujiro
Muro, Takayuki

1-9
2P-46
3-9
1P-5, 2P-3, 2P-4,
3P-23
2-3
2P-14
3P-18
2P-27
3P-14
1-5
2-10
3P-1
1-9
2P-18
3P-1
2P-5
3P-35
1P-31, 3P-10, 3P-31,
3P-33, 3P-49
1P-13, 1P-16, 1P-28,
1P-31, 1P-48, 1P-49,
1P-50, 2P-26, 2P-47,
3P-7, 3P-41
1P-27
1-2
1-1, 1P-3
2P-11, 2P-48
1P-22
1P-4, 2P-5
3P-49
1-6, 1P-45
3P-43
1P-14
1-6, 1P-45
1-3, 3P-3
1P-16, 1P-48, 1P-49,
1P-50, 2P-26, 2P-47,
3P-7, 3P-41
3-1
3P-19
2-3
1P-9, 2P-10, 3-1
3P-26
3P-17
2P-2
2P-2
2-3

- 196 -

Myodo, Miho<N>
Na, NuriNagahama, Taro
Nagao, Kyohei
Nagasawa, Hiroshi
Naitoh, Yasuhisa
Nakagawa, Takafumi
Nakahara, Hitoshi
Nakahara, Kentaro
Nakai, Yusuke
Nakajima, Yuta
Nakamura, Hiroko
Nakamura, Keisuke
Nakamura, Maki
Nakamura, Naoto
Nakanishi, Yusuke
Nakano, Haruhisa
Nakano, Kaichiro
Nakano, Motohiro
Nakashima, Naotoshi

Nakashima, Takuya
Nakazaki, Tafu
Narita, Kouhei
Naruse, Shihono
Nasibulin, Albert
Natsume, Yuhei
Negishi, Ryota
Negishi, Yuichi
Nihei, Mizuhisa
Nihey, Fumiyuki
Nii, Daisuke
Nishigaki, Hiroshi
Nishina, Yuta
Niwa, Hiroyuki
Noda, Shoko
Noda, Suguru
Noguchi, TakuyaNoji, Naoki
Nomura, Kazuya
Nonoguchi, Yoshiyuki

2P-21

3P-29
3P-23
3P-15
3P-15
2P-30
2P-4
2P-40
2P-37
3P-10, 3P-31
1P-19
2-2
3P-21
1P-39
1P-4, 2P-5
2P-6, 3P-4
3-5
2P-37
1P-25
1P-13, 1P-15, 1P-16,
1P-22, 1P-24, 1P-29,
2-5, 2P-12, 2P-25,
2P-29, 3P-16, 3P-27
1P-25
2P-3
2P-8
2P-38
2P-23
3P-11
2P-43
2P-3
2-3
1P-20, 3P-25
2-6, 2P-16
2P-10
3P-43
2P-6, 3P-4
1-2, 2P-6
1P-10, 1P-41, 2P-18,
2P-38, 3-2, 3P-22,
3P-29
2-1
1P-1
1P-7
1P-25, 2P-20

Norimatsu, Wataru
Nouchi, Ryo
Nugraha, Ahmad R. T.
Numata, Hideaki<O>
Ochiai, Yuichi
Ogami, Shinji
Ogasawara, Kazuki
Ogata, Hironori

1P-35, 2P-19, 2P-21,
2P-42
1-9
1P-11, 3P-6
1P-20

Okazaki, Toshiya
Okimoto, Haruya
Omachi, Haruka
Omatsu, Takashige
Ono, Akira
Ono, Shoichi
Onoe, Jun
Osawa, Eiji
Osawa, Toshio
Osipov, Vladimir
Otsuka, Keigo
Ozaki, Taisuke
Ozao, Akihiko

1P-4, 2P-5
3P-15
1P-34, 2P-32
1P-1, 2P-1, 3P-32,
3P-45
2P-43
2P-7
2P-4
2P-20
3-4
2-3
2P-28
1P-5, 1P-18, 2-12,
3P-3
3P-25
1P-19, 1P-23, 2P-23,
2P-26
2P-13
2P-39
1P-5, 2-11
1P-7, 1P-46, 1P-49,
2P-8, 2P-9, 2P-35,
3P-8, 3P-42
1P-14
3P-38
1P-31, 1P-42, 3P-4
2P-5
1P-27
2P-7
1P-8
1-4, 3P-46
1P-10
3P-44
2-8
3-4
3P-9

<P>
Pac, ChyongjinPeng, Fei
Pu, Jiang

1-3
2S-4
2P-44, 3P-39

Ogawa, Takuji
Ogawa, Tomoyuki
Ogumi, Keisuke
Ohashi, Kenji
Ohfuchi, Mari
Ohkochi, Takuo
Ohkohchi, Masato
Ohkubo, Kei
Ohmori, Shigekazu
Ohno, Yutaka
Ohto, TatsuhikoOka, Nobuto
Okada, Hiroshi
Okada, Susumu- 197 -

<Q>
Qin, Xiaojun
Quintero, Ricardo

2S-4
3-2

<R>
Rahman, Mohammad Jellur
Ribeiro, Ricardo Mendes
Ryan, James

3P-14
1-8
2P-3

<S>
Sada, Takao
Saeki, Akinori
Sagara, Takumi
Sagara, Takuya
Sagawa, Wataru
Saito, Riichiro
Saito, Susumu
Saito, Takeshi
Saito, Yahachi
Sakai, Hayato
Sakai, Keijiro
Sakai, Seiji
Sakurai, Shunsuke
Sano, Masahito
Sano, Yoshiaki
Sano, Yosiaki
Sanzen, Toshitada
Sasaki, Kazunari
Sasaki, Mikio
Sasaki, Shuichi
Sastre-Santos, Angela
Sato, Hiroki
Sato, Kentaro
Sato, SatoshiSato, Shintaro
Sato, Sho
Sato, Shogo
Schweizer, W. Bernd
Seino, Yuuma
Seki, Shu
Sekido, Masaru
Sekine, Akinori
Sekita, Michael
Sekitani, Tsuyoshi
Serita, Noboru

1P-29
2-10
1P-17, 3P-30
1P-36
3P-24
1P-11, 2P-11, 2P-48,
3P-6, 3-8
1-7, 3P-12
1P-26, 1P-37, 3-1,
3P-10, 3P-25
2P-40
2-12
1P-14
2P-7
2-2
3P-38
2P-1
1P-1
2P-23
3-6
1S-1
1-4, 3P-46
2-12
3P-17
3-8
3-9
3-5
2P-7
3P-34
1P-2
1-2
2-10
1P-21, 3P-2, 3P-17
3P-32
1P-2
1P-20
3P-10

Shakhov, Fedor
Shibuya, Megumi
Shimada, Takashi
Shimada, Toshihiro
Shimizu, Kazuki
Shimizu, Ryo
Shimizu, Yoshiaki
Shimomura, Shuichi
Shinohara, Hisanori
Shiomi, Junichiro
Shirae, Hiroyuki
Shiraishi, Tomonari
Shiromaru, Haruo
Solís-Fernández, Pablo
Someya, Takao
Song, Hayong
Suda, Yoshiyuki
Sugai, Toshiki
Sugimoto, Kunihisa
Sugisaki, Yuma
Sugita, Tomoko
Sun, Bo
Suzuki, Hiroo
Suzuki, Kaoru
Suzuki, Kazuma
Suzuki, Shinzo
Suzuki, Tomoko<T>
Tabata, Hiromu
Tachibana, Masaru
Tada, Tomofumi
Tajima, Yusuke
Takada, Tomoya
Takada, Yuko
Takagi, Yuki
Takahashi, Makoto
Takahashi, Masahiro
Takahashi, Migaku
Takai, Kazuyuki
Takashima, Akito
Takashima, Kengo
Takenobu, Taishi

3P-44
2P-19, 2P-21
3P-5
3P-23
3P-48
3P-20
3P-48
1-1
1-2, 1P-31, 1P-42,
2P-6, 2P-33, 2P-38,
3P-4, 3P-41
2P-18
3P-22
1P-13
2-4, 2P-49
2P-45
1P-20
2P-14
3P-48
1-5, 1P-32, 1P-34,
2P-32
2-11
1P-42
1P-26
1P-33
3P-37
1P-36
2P-19, 2P-21
1P-27, 3P-15
1P-33

3P-32
1-1
2-1
2S-6
3P-19
2P-27
2P-30, 3P-20
3-5
3P-24
2P-7
3P-44
2-3
1P-47
1P-4, 2P-22, 2P-30,
2P-44, 3P-18, 3P-20,
3P-39- 198 -

Tanaka, Yu
Tancini, Francesca
Taniguchi, Takaaki
Taniguchi, Takashi
Tanoue, Hideto
Tashiro, Kosuke
Terada, Katsuhide
Terashima, Yoshiki
Thendie, Boanerges
Tobari, Yuta
Toh, Minglin
Tokutomi, Hisashi
Tomai, Takaaki
Tomura, Takuya
Tonouchi, Noriyuki
Toriumi, Naoto
Toshimitsu, Fumiyuki
Toyokuni, ShinyaTsai, Shang-Lin
Tsuboi, Yuka
Tsuda, Yusaku
Tsuji, Masaharu
Tsuzuki, Akiko
Tsuzuki, Mayumi

1P-19
3P-48
2P-37
2P-43
1P-26, 1P-28, 2-7,
2P-31
1P-27
1P-2
2P-46
1-6, 1P-45
3P-48
2P-14
1P-32
1P-21
1P-31
1P-34, 2P-32
1-8, 1P-48, 1P-49
3P-2
2P-39
1P-19
1P-20
1P-4, 2P-5
2-5, 2P-29, 3P-27
1S-2
1P-43
1P-49, 1P-50
1P-17, 3P-30
1P-44, 2P-45, 3P-35
2P-12
2P-31

<U>
Uchida, Yuya
Uda, Takushi
Ue, Hitoshi
Ueda, Tomohiro
Ueda, Yuto
Ueno, Hiroshi
Ueno, Keiji
Umeda, Yoshito
Umemura, Kazuo
Umino, Takanori

3P-12
2P-17, 3P-13
3P-48
3P-31
2P-17
3P-3
1S-3
3P-48
2-6, 2P-16
3P-28

<V>
Vul’, Alexander

3P-44

<W>
Wada, Yoshifumi

2P-30, 3P-18, 3P-20

Takesue, Masafumi
Takikawa, Hirofumi
Tamura, Noriyuki
Tanaka, Hirofumi
Tanaka, Takeshi

Wakabayashi, Tomonari
Wakahara, Takatsugu
Wakamiya, Atsushi
Wang, Feijiu
Wang, Huafeng
Wang, Qing
Wang, Yi-Wen
Wang, Zhiyong
Wardle, Brian L
Watanabe, KenjiWei, Xiaojun

2P-50
1-1, 1P-3
2P-2
2P-26
1P-30, 2P-41
2P-33
3-12
2P-6, 3P-4
2P-18
1-6, 1P-45
1P-28

<X>
Xu, Bin

3P-26<Y>
Yagi, Hajime
Yajima, Hirofumi
Yamada, Atsuo
Yamada, Chisato
Yamada, Maho
Yamada, Michio
Yamada, Takeo
Yamada, Tatsuya
Yamada, Yasuhiro
Yamada, Yoichi
Yamada, Yuki
Yamaguchi, Genta
Yamaguchi, Junichi
Yamaguchi, Takehiro
Yamakawa, Kenichi
Yamamoto, Hiroshi
Yamamoto, Takahiro
Yamamoto, Takayuki
Yamamoto, Yuki
Yamamoto, Yuta
Yamanaka, Ayaka
Yamanoi, Ryoko
Yamasaki, Akira
Yamashita, Hiroki
Yamashita, Koichi
Yamazaki, Yu
Yanagi, Chihiro
Yanagi, Kazuhiro
Yanase, Takashi
Yang, FengYang, Juan

1-2
1P-17, 3P-30
3-2
1P-30
2-2
1P-2, 1P-12, 3P-1
3-3
1P-23
3-9
2P-7
3-2
3P-9
3-5
1-6
1P-17, 3P-30
1P-17, 3P-30, 3P-34
1P-47, 2P-15, 2S-5
1P-33
2P-10
2P-33
3P-42
1-4, 3P-46
1P-27
2P-34
2P-13
2-9
1P-33
2P-22, 2P-30, 3P-18,
3P-20, 3P-50
3P-23
2S-4
2S-4

- 199 -

Yang, Mei
Yang, Zehui
Yasuda, Hidehiro
Yasuda, Toku
Yeo, Kee Sheng
Yokoi, Hiroyuki
Yokoo, Kuniyoshi
Yokota, Tomoyuki
Yokoyama, Akio
Yokoyama, Naoki
Yomogida, Yohei
Yoo, JongTae
Yoshida, Keisuke
Yoshida, Masahiro
Yoshida, Masaru
Yoshitake, Haruhiko
Yudasaka, Masako
Yuge, Ryota
Yumura, Motoo
Yumura, Takashi
Yunus, Rozan Mohamad

1P-38, 2P-36
1P-22
1P-8, 1P-37
3P-41
2P-3
2P-46
2P-7
1P-20
3P-5
2-3, 3-5
2P-31
3P-16
1P-17, 3P-30
2P-17, 3P-5, 3P-13
2P-27
3P-45
1P-38, 1P-39, 2P-36
1P-39, 2P-37
3-1
2P-34
3P-35

<Z>
Zhang, Jinying
Zhang, Minfang
Zhao, LiZhao, PeiZhao, Weijie
Zhipeng, Wang
Zhou, Bo
Zhou, Lizhong

2P-6
1P-38, 2P-36
3P-21
2P-41
1-8
3P-45
3-5
1P-48, 1P-49

」෗ࢆࡈᕼᮃࡢ᪉࡬
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JEOLの最新表面分析装置

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原子分解能分析電子顕微鏡

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誘導体化フラーレン用HPLCカラム

COSMOSIL Buckyprep-D
R● 誘導体化フラーレン用HPLCカラム● トルエン移動相中で誘導体化フラーレンが分離可能■C60インデン付加体の分析例
C60インデンは誘導体化フラーレンの一種であり、有機薄膜太陽電池のn型半導体材料として注目されている化合物です。
コスモシール Buckyprep-Dを用いることにより高い分離性能が得られます。

COSMOSIL Application Data
Buckyprep

Buckyprep-D

Column:Column size: 4.6mmI.D.-250mm
Mobile phase: Toluene
Flow rate:
1.0 ml/min
Temperature: 30qC
Detection:
UV 325nm
Sample:Inj.Vol.:

C60 [Indene]2 (1.0mg/ml)
1.0Pl

NACALAI TESQUE, INC

Data courtesy of Yusuke Tajima, Dr. Sci.
Organic Optoelectronics Laboratory, RIKEN (Institute of Physics and Chemistry)■Buckyprepシリーズの用途

フラーレン分離のスタンダードカラム

COSMOSIL Buckyprep

誘導体化フラーレンの分離

COSMOSIL Buckyprep-D

金属内包フラーレンの分離

COSMOSIL Buckyprep-M・誘導体化フラーレン (Buckyprep-D)

・金属内包フラーレン (Buckyprep-M)

COSMOSIL Application DataCOSMOSIL Application Data

Column:Buckyprep-D
Column size: 4.6mmI.D.-50mm
Mobile phase: Toluene
Flow rate:
1.0 ml/min
Temperature: 30qC
Detection:
UV325nmColumn:Buckyprep-M
Column size: 4.6mmI.D.-250mm
Mobile phase: Toluene
Flow rate:
1.0 ml/min
Temperature: 30qC
Detection:
UV312nmSample:Inj.Vol.

(0.125mg/ml)
1; C602; C70(0.250mg/ml)
3; [6,6]-Phenyl-C61 Butyric Acid Methyl Ester[PCBM](0.125mg/ml)
4; [6,6]-Phenyl-C71 Butyric Acid Methyl Ester[ [70]PCBM ](0.375mg/ml)
1.0Pl
NACALAI TESQUE, INC

Sample:Sc2@C76(I)Sc2@C78
Sc2@C80(I)C86

Sample courtesy of Prof. H.Shinohara,
Department of chemistry, Nagoya University

C86

Sc
Sc2@C76(I)C84
C84

Sc2@C78
Sc2@C80(I)NACALAI TESQUE, INC

詳しい情報はWeb siteをご覧ください。

ナカライテスク株式会社〒604-0855

京都市中京区二条通烏丸西入東玉屋町498

価格 ・ 納期のご照会 フリーダイヤル 0120-489-552
製品に関するご照会 TEL : 075-211-2746 FAX : 075-211-2710

Web site :http://www.nacalai.co. jp

Cover moreground, easily
ナノサイエンスや地質学、バイオなど、ラマン分光の技術をもっと活用できる分野は多岐にわたります。Thermo Scientific TM DXR TMxi イメージング顕微ラマンは、高度な性能を視覚的に操作することにより、初心者から熟練者まで分析業務をとてもシンプルにすることができるケミカルイメージング装置です。これであなたもラマンのエキスパート。広大なエリ
アを秒単位で探索し、確実にターゲットを捉えます。

革新的ラマンイメージング• www.thermoscientific.jp/DXRxi/

DXRxi イメージング顕微ラマン
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ラマンイメージングソフトウェア
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Analyze.jp@thermofisher.com www.thermoscientific.jp

1401【第46回FNTG広告】1C/A4（180×260）/高解像度（PDF/X-4）納品

溶液中の粒子のナノレベル微細化・分散に

ホーン先端部の振幅の安定性を、より高めた Advance タイプ になりました。
近年のナノテクノロジーの発展及び粉体関連技術の向上により、より微細な粒子に対する乳化分散処理の要望が増えてまいりました。
超音波ホモジナイザーを使用し、均質な乳化分散処理を行い、安定させることにより製品の機能は向上します。
ブランソン社では 20kHz 機と、40kHz 機の 2 タイプを用意しております。
1 次粒子の凝集力にも拠りますが、20kHz 機では 100nm 程度までの分散
力があります。40kHz 機は、さらに細かいレベルで分散ができる可能性があります。

20KHz 超音波ホモジナイザー
BRANSON SONIFIER シリーズ

高周波 40KHz 超音波ホモジナイザー
BRANSON SLPe シリーズ

ブランソン社の製品は、ホーン先端部の振幅の安定性が高く、強力なキャビテーションが得られ、効率良く、再現性の高い分散処理が行えます。

主なアプリケーション
分散
カーボンナノチューブ
磁性粉
ポリマー

粉末冶金

有機顔料

酸化鉄

ラテックス

研磨剤

電池

半導体

電子基盤

金属酸化物

製紙

フィラー
液晶

無機顔料

セラミック

シリカ

アルミナ

セメント

感光体

記録材料

カーボンブラック

ファンデーション

光触媒

触媒

ワクチン

貴金属

金属

宝石

体外診断薬

タイヤ

発酵菌類

歯磨き粉

シャンプー

その他

乳化
エマルジョン製剤 農薬 トナー ラテックス 界面活性剤 クリーム 乳液 クリーム 等------------------------------------------------------

1C×1P（180×260mm）

アイクストロン社のカーボンナノチューブ＆グラフェン成長用CVD装置

BM Series

Dense CNT

Horizontal SWCNT

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モノレイヤーグラフェン用、マルチレイヤーグラフェン用etc.）■ プラズマエッチングによる簡単クリーニング

アイクストロン株式会社

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E-mail: JAPANINFO@aixtron.com〒140-0001 東京都品川区北品川 1-8-11 Daiwa 品川 North ビル 9F TEL: 03-5781-0931 FAX: 03-5781-0940

䝣䝻䞁䝔䜱䜰䜹䞊䝪䞁䛾䝣䝷䞊䝺䞁〇ရ⣧ᗘ㻔㻴㻼㻸㻯㠃✚䠂䚸௦⾲್䠅
ෆᐜ௚

᭱పᩘ㔞
䠄䡃䠅
10
2
2
1
1

ST

99
99.5
99.5/ ᪼⳹⢭〇ရ
99.9/ ᪼⳹⢭〇ရ
99.9/ ᪼⳹⢭〇/ ༢⤖ᬗရ97䝣䝷䞊䝺䞁 C70

SU

98/ ᪼⳹⢭〇ရ

0.5

nanom mix

ST

ศᏊᵓ㐀

㖭䚷䚷᯶
ST
TL
SU
SUH
SC

nanom purple䝣䝷䞊䝺䞁 C60

nanom orangeΰྜ䝣䝷䞊䝺䞁

nanom spectra[60]PCBM(phenyl C61-butyric acid methyl
ester)

E100

䚷䚷䚷 C60,C70, 䛭䛾௚㧗ḟ䚷䚷䚷䝣䝷䞊䝺䞁䛾ΰྜ≀䚷䚷䚷 䈜ᚤ⢏໬ရ䠄 ST-F䠅䜒䛒䜚䜎䛩
99

O
O

50
1

E100H

99.5

1

E102

99.9

0.5

98/ ␗ᛶయ䝖䞊䝍䝹1

nanom spectra䚷E400
bis[60]PCBM䈜఩⨨␗ᛶయ䛾ΰྜ≀(bis-phenyl C61-butyric acid methyl ester)

nanom spectra䚷E124

O

O
O

O

[60,70]PCBM

nanom spectra

E110(phenyl C71-butyric acid methyl
ester)

E112[70]PCBM

1㼇㻢㻜㼉㻼㻯㻮㻹䚸㼇㻣㻜㼉㻼㻯㻮㻹䛾ΰྜ≀

199/ ␗ᛶయ䝖䞊䝍䝹

0.5

O
O

䈜఩⨨␗ᛶయ䛾ΰྜ≀99.5/␗ᛶయ䝖䞊䝍䝹୺ᡂศ䈜఩⨨␗ᛶయ䛾ΰྜ≀

0.5

nanom spectra䚷Q100

99

0.5

nanom spectra䚷㻽㻠㻜 㻜

99/ ␗ᛶయ䝖䞊䝍䝹

1[60]䜲䞁䝕䞁௜ຍయ[60]䜲䞁䝕䞁䠎௜ຍయ䈜఩⨨␗ᛶయ䛾ΰྜ≀nanom spectra䚷D100Ỉ㓟໬䝣䝷䞊䝺䞁

2+
2+ n/2≀(n = ca.10)

2+nanom spectra䚷A100Ỉ⣲໬䝣䝷䞊䝺䞁

C60OHn䚷n=10䜢୺ᡂศ䛸䛩䜛ΰྜ+n/2

C60Hn䚷 n=30䜢୺ᡂศ䛸䛩䜛ΰྜ≀(n = ca. 30)

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