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総合シンポジウム
講演要旨集
主催： フラーレン・ナノチューブ・グラフェン学会
共催・後援： 日本化学会
名古屋大学 未来材料・システム研究所
未来エレクトロニクス集積研究センター
協賛： 日本物理学会、応用物理学会、高分子学会、電気化学会
日時： ',''年3月'日(水) 〜 3月1日(金)場所： オンラインバーチャルシンポジウム
発表時間： 特別講演（発表 '( 分 + 質疑応答 ( 分）
招待講演（発表 +, 分 + 質疑応答 ( 分）
一般講演（発表 +, 分 + 質疑応答 ( 分）
ポスタープレビュー （発表 + 分・質疑応答

なし）

展示団体御芳名
（五十音順

敬称略）

テレダイン・ジャパン(株)(株)日本レーザー

広告掲載団体御芳名
（五十音順

敬称略）

アイクストロン(株)エクセルソフト(株)(株)コロナ社
セントラル科学貿易(株)(株)東京インスツルメンツ
テレダイン・ジャパン(株)日本電子(株)(株)日本レーザー
フィルジェン(株)    
       







 

     !

目次
早見表
座長一覧 
プログラム 
講演予稿
特別講演
招待講演



一般講演



ポスター発表

発表索引      " 

  



  

         
       





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    

    !

 



 



#!



  

 

$% &  # 
  
   # 
    
 "       



 



       "  &'  $   & 

 





 

   #

    
(        
     !

  



!

 !
       "# 
 "      # 

 "
 "

        "# 
 "      " )

$ %

 



   
    !      
    ! 
 "  

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

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

 & ' 
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  # 
    !   

   
 (    
        !      !

座長一覧    
3月2日(水)
セッション

（敬称略）

時間

座長

特別講演（中山 勝文）

6 ,, 7 6 3,

湯田坂 雅子招待講演（速水 真也）

6 3, 7 6 (,湯田坂 雅子

一般講演

6 (, 7 +, 3(

稲葉 優文

特別講演（吾郷 浩樹）+, (, 7 ++ ',岡田 晋

招待講演（桐谷 乃輔）++ ', 7 ++ 1,

長汐 晃輔

一般講演

++ 1, 7 +' +,大町 遼

チュートリアル（荒川 公平）+3 ,, 7 +1 3,

山本 貴博

ポスタープレビュー+( 3, 7 +8 +(

福島 知宏
鈴木 弘朗

3月3日(木)セッション
ポスタープレビュー時間

座長

9 1( 7 6 3,

大塚 慶吾
岡田 光博

特別講演（石川 洋二）+3 3, 7 +1 ,,小久保 研

招待講演（ : ;）+1 ,, 7 +1 ',

大野 雄高

一般講演

+1 ', 7 +( ,(宮田 耕充

特別講演（五十嵐 康彦）+( ', 7 +( (,

大淵 真理

一般講演

+( (, 7 +8 3(

: ;

一般講演+8 (, 7 +9 ',

若林 知成

セッション

時間

座長

特別講演（2< %）

6 ,, 7 6 3,

北浦 良

一般講演

6 3, 7 +, 3,

吾郷 浩樹

一般講演

+, 1( 7 +' ,,柳 和宏

特別講演（=  > ）

+3 ,, 7 +3 3,

齋藤 理一郎招待講演（菅原 克明）+3 3, 7 +3 (,齋藤 理一郎一般講演+3 (, 7 +1 3(

蒲江

招待講演（舟山 啓太）+1 (, 7 +( +,

平原 佳織

一般講演

+( +, 7 +8 '(白木 智丈

3月4日(金)  
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!(&&'$ 

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Exciton recombination dynamics in 2D semiconductors
Der-Hsien Lien
Institute of Electronic, College of Electrical and Computer Engineering, National Yang
Ming Chiao Tung University, Hsinchu 30010, Taiwan.
As semiconductors’ thickness approaches the monolayer limit, excitonic quasiparticles
could be observed at room temperature due to the strong Coulomb interaction between
space-confined charge carriers. 2D layered semiconductors in monolayer form (e.g., transition
metal dichalcogenide monolayers) provide an ideal platform to investigate the transport
properties of excitons and their complexes because surface issues in 2D monolayers are not as
severe as in bulk semiconductors. I will show that such thickness-determined excitonic
systems are promising for optoelectronic applications due to their near-unity
photoluminescence (PL) quantum yields (QYs) [1], a key figure of merit dictating the
maximum efficiency achievable in light-emitting diodes, lasers, and solar cells. I will discuss
the comprehensive recombination mechanisms of excitons in monolayers and show that the
non-radiative recombination pathways can be fully suppressed by electrostatic gating, despite
the presence of native defects [2,3]. This research reveals that room-temperature excitons arerobust and bright regardless of monolayer quality, indicating the potential of achieving highly
efficient excitonic devices. To deal with the injection inefficiency caused by Schottky
contacts, I will show an AC carrier injection architecture, a device concept that is capable ofefficiently injecting carriers in various excitonic systems [4], including monolayer
semiconductors, with demonstrations of bright light-emitting devices from infrared toultraviolet regimes [5].
[1] D. H. Lien et al., Science 350, 1065 (2015).
[2] D. H. Lien et al., Science 364, 468 (2019).
[3] H. Kim et al., Science, 373, 448, 2021.
[3] D. H. Lien et al., Nature Communications, 9, 1129, 2018[4] D. H. Lien et al., Nature Electronics, 3, 612–621 2020.

5

3S-2

Electronic property of low-dimensional black phosphorus

Yuanbo Zhang
Department of Physics, Fudan University, China

We investigate the electric property of black phosphors thin flakes with thickness down toa few atomic layers. Two-dimensional black phosphorus exhibits excellent semiconducting
properties. High conductance modulations up to 105 and field effect mobility up to 1000
cm2/Vs at room temperature are achieved in black phosphorus field effect transistors.
Further improving the sample quality leads to observation of quantum Hall effect in thismaterial. In this talk, I will discuss the physics in black phosphorus two-dimensional
electron system, as well as our recent effort in growing low-dimensional structures of black
phosphorus.


6

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1-1Superhydrophobic Carbon Nanotubes with Different Orientations as Mask
Filters realizing Excellent Anti-viral Effect against SARS-CoV-2○Sangsu Lee1, Chae Young Woo2, Han-Jun Kim3, Ali Khademhosseini3, Hyung Woo Lee2, Il
Jeon1
1

Department of Nano Engineering, SKKU Advanced Institute of Nanotechnology (SAINT),
Sungkyunkwan University (SKKU), Suwon 16419, Republic of Korea
2
Department of Nano Fusion Technology, Pusan National University, Busan 46241, Republic of
Korea
3
Terasaki Institute for Biomedical Innovation, Los Angeles, CA, 90024 USA

The COVID-19 outbreak was declared as a pandemic by the World Health Organization(WHO) in December 2019 and is still a highly contagious disease with the number of infections
increasing dramatically every day. The difficulty of stabilizing the pandemic lies in theunceasing mutation of SARS-CoV-2, rendering vaccination inadequate via breakthroughinfections. Wearing face masks is the ultimate solution for now and will not be optional even
until the booster jabs are available to everyone because this disease infection spreads via
airborne saliva droplets. Targeting protection against SARS-CoV-2, our investigation anddiscussion focus on five key aspects: 1) superhydrophobicity, 2) industrial viability, 3)breathability, 4) anti-viral effect and 5) non-toxicity.
In this study, commercially available spunbonded/melt-blown/spunbonded polypropylene(SMS) filter-based face masks are used as the control sample. To find an optimal condition forvertically aligned carbon nanotubes (VACNTs) having the greatest superhydrophobicity, theCNTs were synthesized by changing the amount of catalysts, synthesis time, and substrate types.
In order to obtain VACNTs effectively blocking viruses, it is important to synthesize them on
SiO2 substrates for 20 min using a Fe:Al2O3=4:2 catalyst to grow high-density and short-length
VACNTs. The average water contact angle of the VACNT filter (175.53°) was approximately
51°, which is greater than that of the SMS filters (124.6°). Even the minimum water contact
angle of the VACNT filter was 165.1 °, which is still much larger than the SMS filter. There isa problem of using VACNT as a mask filter, which is that it is nearly impossible to maintain its
vertical alignment. VACNT can be transferred onto a mask substrate using the dry-spinning
process. However, its vertical alignment is not retained. However, post-transferred VACNTs
still possess sufficient hydrophobicity (142.7°) despite the alignment being not perfectly
vertical. In addition, since the dry-spinning method can be applied to the roll-to-roll process,the CNT filter could be added on top of the SMS filter or replace one of the existing layers withease to lower the production cost. It is possible to transfer by adjusting the VACNT thickness.
Through this, we can control the breathability. The high thermal conductivity of the CNT filter
induced a hyperthermal anti-viral effect as evidenced by the swift temperature rise to 56 °C inless than 5 min when the situation of the mask being worn outside was simulated. Inactivationof the viruses on the heated CNTs was confirmed by TEM imaging of denatured viruses. It
transpires hyperthermic antiviral effects which offers stronger protection against the virus aswell as reusability. The toxicity test was conducted in vivo test using rats. It was confirmed that
CNTs attached on a mask substrate are not toxic. In conclusion, we are positive that VACNTs
can be viable on an industrial level within a short time. The VACNT filter warrants its viability,
reinforcing the fight against the COVID-19 pandemic.
Corresponding Author: I. Jeon, Hyung Woo Lee, Ali
E-mail: il.jeon@spc.oxon.org (I.J.), LHW2010@pusan.ac.kr (H.L.), parastoo@hms.harvard.edu (A.K.)

12

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1:ED91> -=1 >1/=1?10 .D 9-:D
.-/?1=5-5:?411:A5=;:91:?
53 13=-0-?5;:;2!&.D .-/?1=5-841911:ED91>+ ,881: "/(9419%;/    
+ ,(-3-: "/( !-?!-:;?1/4:;8   + ,&:0;: "/(%9-88     
+ , *4-:3"/( :A5=;:%/5&1/4:;8    
+ ,4-:0=->17-=-: "/ ( :0:3419   +,&@33"/( @=="<5:5;?1/4:;8    
;==1><;:05:3@?4;=;=5&18    9-5874;=5/419.5;:-3;D-@-/6<

13

1-3
          

○!(%'&()(!#!!#'##%( #"""#'#'#&#(&


'$#!#&''('$)##(&'%!###$!$* &( (  #&(#)%&'* '&("$'$ apan3
Meijo University, Nagoya 468-8502, Japanapan

Carbon nanohorns (CNHs) have great potential for carriers of drug delivery systems.
Bisphosphonates (BPs) inhibit osteoclasts to resorb bones, and, in addition, they reduce theosteoclasts proliferation and promote their apoptosis. Therefore, BPs have been used for thetreatment of bone metastasis. However, BPs have drawbacks of causing adverse side effects
during the systemic circulation. We considered that the BP-loaded CNHs might be applicableto the local treatment of bone metastasis. But ibandronate (IBN), a type of BP, did not adsorb
onto CNHs, because the interaction between relatively hydrophilic IBN and hydrophobic CNHs
was weak. Therefore, we tried to use calcium phosphates (CaPs), a main mineral component ofbones, as mediators between IBN and CNH. An in vitro evaluation of the resulting BP-loaded
CNHs was also performed.
We prepared a supersaturated CaP solution containing oxidized CNHs (OxCNH) and IBN(final concentrations; Ca: 6.6 mM, P: 3.3 mM, OxCNH: 50 μg/mL, IBN: 0.078 mM). The
solution was kept at 25 °C for 30 min to induce coprecipitation. The product was washed withwater. The structure and composition of the resulting product were investigated by transmission
electron microscopy (TEM), energy dispersive X-ray spectroscopy (EDX), and inductively
coupled plasma optical emission spectrometry (ICP). For an in vitro evaluation, murine
macrophages (RAW264.7 cells) and osteoclasts (differentiated from RAW264.7 cells) wereincubated with the product, and cell viability assays and microscopic observations of the cells
were performed.
TEM observation and EDX and ICP analyses indicated that the product consisted of manysmall-sized deposits of IBN-containing CaPs (< 10 nm) on the surfaceof OxCNHs (ca. 100 nm) (Fig. 1). That is, the IBN-loaded CNHs weresuccessfully fabricated by using CaPs as mediators between IBN and
CNHs. The resulting IBN-CaP-CNH composites were engulfed bymacrophages and osteoclasts, and strongly suppressed the cell viability.
Since IBN-CaP-CNH composites were accumulated in lysosomes, it
was presumed that CaPs were dissociated under weakly acidic
conditions in lysosomes and IBN was released to suppress the cell
viability. These results suggested that the IBN-loaded CNHs have a Fig. 1 TEM image of the
product.
great potential for the local treatment of bone metastasis [1].
!(%'!

 $$ '% "'%&

Corresponding Author: M. Nakamura
Tel: +81-29-861-4604, Fax: +81-29-861-3005,
E-mail: ma-ki-nakamura@aist.go.jp

14

–



1-4Electronic structure of bilayer MoS2/WS2 with checkerboard interlayer
metal arrangement○Mina Maruyama1, Nanami Ichinose2, Ryo Kitaura2, Yanlin Gao1, and Susumu Okada1
1Department of Physics, University of Tsukuba, Tsukuba 305-8571, Japan
2Department of Chemistry, Nagoya University, Nagoya 464-8602, Japan

Boundaries of condensed matters with vacuum or other materials cause localized
electron state at or around the boundaries because of the absence of the translational symmetry
across there. Unsaturated covalent bonds at boundaries of semiconductors and insulators
usually induce the localized states near the surfaces and in the gap between valence andconduction bands. Two dimensional materials,
such as graphene, h-BN, and transition metal
dichalcogenides, possesses two different classesof boundaries which also cause unusual electronic
structures depending on the constituent elements
and their mutual arrangements. Both within andbetween their atomic planes, the electronic
structure is modulated at the borders andinterfaces, even though the covalent bonds ofconstituents are fully saturated.
Fig. 1: A geometric structure of bilayer
In this work, using the density functional MoS2/WS2 with checkerboard structure.
theory with effective screening medium method, Purple, gray, and yellow balls indicate Mo,
W, and S atoms, respectively.
we investigate the electronic structure of the inplane and out-of-plane heterostructure of MoS2
and WS2 where MoS2 and WS2 strips arealternately arranged and stacked (Fig. 1).
According to the arrangement of the strips, bilayer
MoS2/WS2 has a checkerboard pattern in terms ofinterlayer metal arrangement. The band edgealignment of the bilayer MoS2/WS2 strongly
depends on the interlayer metal arrangement (Fig.
2): The valence band edge of the Mo above Mo isthe shallowest among four metal arrangements,
while the conduction band edge of W above W is Fig. 2: Projected density of states ofbilayer MoS2/WS2 with checkerboard
the deepest. Therefore, the dimensionality of structure. P1, P2, P3, and P4 indicate theaccumulated carrier in this system is tunable from Mo above Mo, Mo above W, W above Mo,
and W above W, respectively.
0D to 2D by controlling the carrier concentration.
Corresponding Author: M. Maruyama
TEL: +81-29-853-5921, FAX: +81-29-853-5924
E-mail: mmaruyama@comas-tsukuba.jp

15

1-5
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θ'.'%5310+%4536%563'+4'45+/#5'&$:%#.%6.#5+0)

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16

2-1






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4C<1B7=<=4B63>@3AAC@3A=41/@0=<A=C@13A/<23B167<5/53<BA

17

2-2
Experimental Synthesis of NbS2 based 1D van der Waals Heterostructures○Wanyu Dai1, Yongjia Zheng1, Akihito Kumamoto2, Rong Xiang1, Yuichi Ikuhara2, Shigeo
Maruyama1
1Department of Mechanical Engineering, The University of Tokyo, Tokyo 113-8656, Japan
2
Institute of Engineering Innovation, The University of Tokyo, Tokyo 113-8656, Japan

We recently presented the experimental synthesis of one-dimensional (1D) van der Waals(vdW) heterostructures which includes single-walled carbon nanotubes (SWCNTs), boron
nitride nanotubes (BNNTs) and molybdenum disulfide nanotubes (MoS2NTs) [1]. Further, thenucleation and crystal growth behaviors over these highly curved nanotube surfaces were
investigated [2]. It is believed that all materials in the 2D library could be rolled into their 1D
counterparts. [1] Hence, the controlled synthesis of 1D vdW heterostructures based on different
transition metal dichalcogenides (TMDCs) are of great research interest. [3]In this work, we demonstrate the experimental synthesis of 1D vdW heterostructures
combine SWCNTs, BNNTs, and niobium disulfide nanotubes (NbS2NTs) in the radial direction.
By chemical vapor deposition (CVD) method, the BNNTs and NbS2NTs were synthesized over
the SWCNTs templates layer by layer. Scanning transmission electron microscopy (STEM) wasapplied to characterize the structure of as acquired 1D vdW heterostructures. Energy dispersive
spectroscopy (EDS) mapping results shown that the as acquired structures are SWCTN-BNNTNbS2 1D vdW heterostructures along with several 2D NbS2 flakes. (Fig. 1) The out layer
NbS2NTs are highly crystalized. (Fig. 2) The experimental synthesis of SWCTN-BNNT-NbS2
1D vdW heterostructure suggests that it is highly possible to acquire 1D vdW heterostructures
based on more TMDCs in the 2D material library.

Fig. 1 EDS mapping of as synthesized SWCNT-BNNT- NbS2
vdW heterostructures. Scale bar, 100 nm.
[1] R. Xiang, et al., Science, 367, 537 (2020).
[2] Y. Zheng, et al., PNAS, 118, e2107295118 (2021).
[3] S. Cambre, et al., Small, 17, 2102585 (2021)
Corresponding Author: S. Maruyama
Tel: +81-3-5841-6421, Fax: +81-3-5800-6983
E-mail: maruyama@photon.t.u-tokyo.ac.jp

18

Fig. 2 STEM image of SWCNT-BNNT-NbS2
1D vdW heterostructure. Scale bar, 5 nm.

2-3Experimental realization of the WS2-based 1D vdW heterostructure○Yongjia Zheng1, Wanyu Dai1, Akihito Kumamoto2, Jenichi Clairvaux Felizco3, Yuta Sato4, Kazu
Suenaga3, Keigo Otsuka1, Qiang Zhang5, Anton Anisimov6, Esko I. Kauppinen5, Rong Xiang1, Shigeo
Maruyama1
1 Department of Mechanical Engineering, The University of Tokyo, Tokyo 113-8656, Japan
2 Institute of Engineering Innovation, The University of Tokyo, Tokyo 113-8656, Japan
3 The Institute of Scientific and Industrial Research (ISIR), Osaka University, Osaka 567-0047, Japan
4 Nanomaterials Research Institute, AIST, Tsukuba 305-8565, Japan
5 Department of Applied Physics, Aalto University School of Science, Tiilenlyöjänkuja 9A SF-01720 Vantaa, Finland
6 Canatu Ltd., Helsinki FIϋ00390, Finland

We recently presented one-dimensional (1D) van der Waals (vdW) heterostructure that coaxiallyformed by single-walled carbon nanotubes (SWCNTs), boron nitride nanotubes (BNNTs) andmolybdenum disulfide (MoS2) [1]. Also, the nucleation behaviors of these highly curved outer layers
over SWCNT surfaces were investigated [2]. It suggests the family of 2D materials can be possiblyrolled into their 1D counterparts, among which 2D transition metal dichalcogenides (TMDC) have been
already widely investigated. On the other hand, despite the great variety in 2D TMDC materials, theresearch on their corresponding 1D structure is still limited and challenging [3].
In this work, we demonstrate the experimental synthesis of another 1D TMDC materials: WS2based 1D vdW heterostructure which coaxially includes SWCNTs, BNNTs and WS2 nanotubes. Not
only the 1D WS2 is highly crystalline, but also its coverage over nanotube networks is very high. In
Fig1b, the EELS mapping clearly proves that SWCNT is sequentially wrapped by BNNT and WS2
nanotube. This can be a big step forward a wider variety of 1D vdW heterostructures, which opens
opportunities for further studying their new properties and potential applications.

Fig.1 (a) Annular dark-field (ADF) image of 1D SWCNT-BNNT-WS2 heteronanotubes. (b) ADF image
and electron energy-loss spectroscopic (EELS) mapping of a SWCNT partially wrapped with BNNT
and WS2 nanotube.
Corresponding Author: S. Maruyama[1] R. Xiang et al., Science, 367(6477), 537 (2020).
[2] Y. Zheng, et al., PNAS, 118(37), e2107295118 (2021).
[3] R. Xiang and S. Maruyama, Small Sci., 1(2), 2000039, (2021),

19

Tel: +81-3-5841-6421,
Fax: +81-3-5841-6983,
E-mail: maruyama@photon.t.u -tokyo.ac.jp

2-4






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*(;9,+)?.52+(:5330.8(:054-853:56,2,*:85+,:5;4+,82?04.2(?,89& '(4+*59:099;,5-:/09
68,*05;93,:(209;8.,4::5),952<,+4,,--,*:0<,3,:/5+09,2,*:85+,9;)9:0:;:05445;8.85;6=,/(<,6;)209/,+(6(6,85-8,62(*04..52+,2,*:85+,=0:/!,2,*:85+,(4+(*/0,<04. ( *536(8()2, 65=,8 *54<,89054 ,--0*0,4*?  =0:/ .52+ ,2,*:85+, 8,-,8,4*,
+,<0*,9 & ' 6085,! 09 30>,+ =0:/ 9654.,201, ! ,2,*:85+, :5 -583 :/, /52,
:8(49658:2(?,8!5,4/(4*,:/,*54+;*:0<0:?5-/52,:8(49658:2(?,8(4+952(8*,220:/0;3
)09:80-2;5853,:/(4,9;2-54?2030+,0! 09/,(<02?(++,+04:5 6085,!68,*;8958
952;:054=/02,0! 09/?.859*560*2,(+04.:59;)9,7;,4:9:()020:?099;,95-+,<0*,9,4*,
/5=:5)(2(4*,(4+9:()020:?+,*8,(904.:/,;9(.,5-0! +56(4:=0:/3(04:(0404.
/0./(::/,9(3,:03,),*53,9(4,3,8.04.685)2,3
!5 952<, :/09 685)2,3 =, ;6.8(+, 5;8 /52, :8(49658: 2(?,8 -853 6085,! :5
52?&)09 6/,4?2  :803,:/?26/,4?2(304,! (4+ =, -04+ :/(: *536(8,+ =0:/
6085,!!8,7;08,92,99(35;4:5-0! +5604.:58,(*/:/,),9:04.52+
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*(4),,<,42,99=/,4.52+,2,*:85+,8,62(*,+)?!,2,*:85+,",56:030@,:/,8,2(:0549/06
),:=,,4+5604.8(:05(4+65=,8*54<,89054,--0*0,4*?04!,2,*:85+,+,<0*,9(99/5=404
-0.;8, !/,56:030@,++5604.8(:05-58!04!,2,*:85+,+,<0*,909 =/0*/09:/,25=,9:8,7;08,++5604.8(:05-586,85<910:,952(8*,22:58,(*/ (2359::/,
3(>03;3 ,--0*0,4*? -58 ) (*:0<, 2(?,8 +,<0*,9 !/, 8,7;08,3,4: 5- ,>:8,3,2? 25=+5604.8(:05-58!(9/52,:8(49658:2(?,804!,2,*:85+,+,<0*,99;**,99-;22?04*8,(9,9:/,9:()020:?5-5;8+,<0*,9=/,8,(9/0./*(4),(*/0,<,+(::/,9(3,:03,",(::80);:,
:/0904.,405;9)(2(4*,:5:/,8,3(81()2,*53)04(:0545-!(4+!=/,8,!9-(*020:(:,
*(880,8:8(49658:04:/,30>,+!!2(?,8:/;9+,*8,(904.:/,8,7;08,3,4:-580! +5604.=/02,!09+09:80);:,+049654.,201,!30>,+9:8;*:;8,)8,(104.:/,9/(*12,9
5-:8(+0:054(22(?,8,+9:8;*:;8,(4+3(104.:/0*1,8/52,:8(49658:2(?,8:5),65990)2,;8=581
+0962(?9(/;.,(+<(4:(.,5-!9:5-;4*:054(9,2,*:85+,9046,85<910:,952(8*,229  *('(0..)(,!,'$,."    6  
 $.-&(,$.!230$   6     .-0!#.,!-1*(!-.     6   +$.-!2$0'$,   (&30$/2(,(5!2(.-.%(#./(-&".-"$-20!2(.-(-+!4$0.%$+$"20.#$

20

2-5
Utilization of Multifunctional Environment-Friendly Organic Dopants
Inspired from Nature for Carbon Nanotube-Based Planar Heterojunction
Silicon Solar Cells○Jeong-Seok Nam1, Jiye Han1, Seungju Seo2, Qiang Zhang3, Esko I. Kauppinen3, Shigeo
Maruyama2, Il Jeon1
1

Department of Nano Engineering, SKKU Advanced Institute of Nanotechnology (SAINT),
Sungkyunkwan University (SKKU), Suwon, 16419 Republic of Korea
2
Department of Mechanical Engineering, The University of Tokyo, Tokyo, 113-8656 Japan3
Department of Applied Physics, Aalto University School of Science, Espoo, FI-00076 Finland

Carbon nanotubes (CNTs) have to be chemically doped for their conductivity to match up
with the conventional transparent conductors. Nitric acid and trifluoromethanesulfonic acid
(TFMS) have been the common choice of p-dopant.[1] However, nitric acid produces toxic NO2
and explodes when mixed with organic compounds. In addition, TFMS is a superacid with apKa value of –14.7 and therefore extremely corrosive beyond measure.[2] Natural acids, which
consist of hydrocarbons with carboxyl, sulfonic, or phosphoric groups, are biodegradable, easy
to synthesize, and easily obtained from nature.[3] It also has the potential to qualify for
replacing inorganic acids. In this work, we tested naturally available acids, specifically, acetic
acid, formic acid, lactic acid, and citric acid as the p-dopant for the CNT transparent electrode.
From the result, lactic acid shows the multifunctional effect of p-doping with excellent doping
stability as well as antireflection. The doping effect and its stability are investigated by diverse
methods, such as van der Pauw four-probe measurement as well as Raman, photoelectron yield,
and absorption spectroscopy. The sheet resistance decreases by 22.1% when carbon nanotube
films are doped by lactic acid and the doped films are stable for more than 20 days. The power
conversion efficiency of carbon nanotube-laminated silicon solar cells improves from 8.2% to10.3% by using nature-inspired lactic acid. Such a great improvement is ascribed to not only
the p-doping and antireflection effects but also the passivation effect of lactic acid on the Si
surface defect sites as evidenced by both the Fourier-transform infrared and the Quasi-steadystate photoconductance lifetime measurements.

[1] I. Jeon, et al. J. Mater. Chem. A, 8, 11141 (2020)[2] J. W. Lee, et al. Nano Lett, 19, 2223 (2019)[3] J. Han, et al. Adv. Energy Mater, 2101221, 1 (2021)
Corresponding Author: I. Jeon
E-mail: il.jeon@spc.oxon.org

21

2-6
Homogeneously Miscible Fullerene inducing Vertical Gradient in
Perovskite Thin-Film towards Highly Efficient Solar Cells○Kyusun Kim1, Ziang Wu2, Yue Ma3,4, Han Young Woo2, Il Jeon1,4
1

Department of Nano Engineering, SKKU Advanced Institute of Nanotechnology (SAINT),
Sungkyunkwan University (SKKU), Suwon 16419, Republic of Korea
2
Department of Chemistry, KU-KIST Graduate School of Converging Science and Technology, Korea
University, Seoul 02841, Republic of Korea
3
Laboratorium für Organische Chemie, ETH Zürich, CH-8093, Zürich, Switzerland
4
Department of Mechanical Engineering, The University of Tokyo, Tokyo 113-8656, Japan

Fullerene-based n-type charge-collecting materials have emerged as a solution to highperformance perovskite solar cells. However, their application to perovskite solar cells waslimited in the device architecture and only a small amount of fullerene additives could be
introduced to the device system, because of the immiscibility of the fullerene species with polar
solvents. To overcome this, triethylene glycol monomethyl ether chain-attached fullerene
derivatives are synthesized and applied to normal-type perovskite solar cells. The newly
synthesized fullerenes exhibit excellent solubility in polar solvents. A novel approach to
introducing miscible fullerenes into perovskite devices and inducing a favorable verticalgradient is proposed. Forming an overcoat on an electron-transporting layer and waiting for a
few minutes, the fullerene derivatives progressively permeate into the fullerene-doped
perovskite active film. In this talk, we attached, triethylene glycol monomethyl ether (TEG)
chains to PC61BM to greatly enhance its miscibility with the perovskite precursor. The
synthesized
TEG-attached
PC61BM,[6,6]-phenyl-C61-butyricacid
2-[2-(2methoxyethoxy)ethoxy]ethyl ester (PC61B-TEG), and a branched substituent with two TEGsattached PC61BM, [6,6]-phenyl-C61-butyric acid 1-methyl 3-[2-(2,5,8,11-tetraoxadodec-1-yl)4,7,10,13-tetraoxatetradec-1-yl] ester (PC61B-BiTEG) were highly polar and miscible with theperovskite precursor. Here, we explored three ways to introduce novel fullerene derivatives into
PSCs: direct mixing with the precursor prior to film fabrication, overcoating the electrontransporting layer, and overcoating + waiting between drop-casting and spin-coating of theperovskite precursor solution on the overcoated layer of PC61B-TEG to induce gradientdispersion into the perovskite precursor. By fabricating perovskite solar cells combining direct
mixing, overcoating and waiting techniques, a remarkably high device efficiency of 23.34% isachieved. The high performance is attributed to the fullerene additives with a vertical gradientpassivating the perovskite defectsites effectively and the overcoat
enhancing the charge transfer.
The device performance iscertifiedbyanationallaboratory, which is the highest
efficiency among the fullerene
additives-used perovskite solar
cells.
Corresponding Author: I. Jeon
Tel: +82-31-299-4187
E-mail: Il.Jeon@spc.oxon.org

Fig. 1 Configuration of PC61B-TEG-added device.

22

2-7
20 years of NanoAmando@ towards Elementary Diamond Nanoparticles:
their experimental evidence
○ Toshihiko Tanaka1, Tetusya Aoyama2, Yasuhiro F. Miura3, Eiji Osawa4
1

Department of Chemistry and Biochemistry, National Institute of Technology,
Fukushima College, 30 Aza-nagao, Tairakamiarakawa, Iwaki, Fukushima, 970-8034, Japan2
Ultrahigh Precision Optics Tech. Team, RIKEN RAP, 2-1 Hirosawa, Wako, Saitama, Japan
3
Hamamatsu University School of Medicine, 1-20-1 Handayama,
Higashi-ku, Hamamatsu City, Shizuoka, Japan
4
Nano Carbon Research Institute Ltd., Asama Research Extension Center,
Shinshu University, 3-15-1 Tokida, Ueda, Nagano, JapanThe last author founded NanoCarbon Research Institute Ltd. in 2002 and has kept it over
20 years, thus to all over the world supplying the standard product of the aqueous colloidal
solutions of nanodiamonds (NDs), NanoAmando@ (NA). It provided the success of drugdelivery system1 for cancer therapy and most researchers of NDs perhaps know this productthrough this impact publication. Furthermore, it has often showed unique properties, having
both positive ze-ta potentials and a tiny graphitic layer on the surface of NDs. However, thedifference between NA and other commercial solutions is an open question. It is to say thatthe intrinsic properties of NDs have not been clarified enough in spite of huge amount ofpublications on NDs. One problem should be homogeneity of NDs. I think that he has
struggled with this so hard and has reached a certain level. Hence, we will present herein the
progress of NA in these years together with recent results on its intrinsic properties: assemblyor electric conduction.
We consider that the main NDs
component of recent NA are appreciably
homogeneous because of the following 3
reasons: 1) DLS measurements often reacha low size value down to 2.6 nm; 2) theyalso show hierarchic aggregation2; and 3)
the NA often gives rectangular precipitatessuch as whiskers or nanosheets. The low
value itself indicates a high purity Figure 1. An example of schmatic model of hierarchic
aggregation
because of its Rayleigh scattering, which
is proportional to r6 (r: diameter of a particle); the contamination of larger particles below 10
nm should shift primary particles peak appreciably larger. In hierarchic aggregation, primaryparticles first assemble to 1st aggregates (15-25 nm) which aggregates further forms 2nd
aggregates (50-70 nm)[Fig.1] and there are two blank areas (10-15 nm, 25-50 nm) where
aggregates could be unstable. The precipitates perhaps indicate the instant growth of hydrate
colloidal crystals through drying. Hence, these three facts strongly suggest that the primaryparticles are rather elementary diamond nanoparticles (EDIANs) that are similar both in sizeand shape. Furthermore, recently the high electric conductivity of the soft gel from NA wasfound and we also presume that it is also due to the progress.
[1]E.K.Chow, X.-Q. Zhang, M. Chen, R. Lam, E. Robinson, H. Huang, D. Schaffer, E. Osawa, A. Goga, D. Ho,
Sci. Trans. Med., 3, 73 (2011)[2] Technical Report No.2, NanoCarbon Research Institute Ltd.2007
Corresponding Author:Eiji Osawa / Tel: +81-0268-75-8381 / E-mail: osawa@nano-carbon.jp

23

2-8

Isolation of C70-Based Endohedral Fulleride Li@C70○Daiki Kitabatake,1 Hiroshi Ueno,1,2 Fuminori Misaizu1
1
2

Department of Chemistry, Tohoku University, Sendai 980-8577, JapanThe Frontier Research Institute for Interdisciplinary Sciences, Tohoku University

Endohedral metallofullerenes (EMFs) are one of the well-studied nanocarbon
materials during the past 3 decades. Among EMFs, C60 and C70-based EMFs haveattracted special interest owing to their predicted electronic properties arising from thesuperatomic electronic structure. However, these materials are generally known to bedifficult to obtain in macroscopic yield, and therefore almost the reported studies havefocused on the isolatable higher fullerene-based EMFs. Although Shinohara and coworkers had successfully isolated the La@C60 and La@C70 as highly extractable
trifluoromethylated forms,[1, 2] isolation and unambiguous characterization of C60 and C70
based-EMFs with no chemical addends have been never accomplished except for Li@C60
reported previously.[3]In this talk, we report the first isolation ofneutral Li@C70 by selective one-electron
reduction of recently isolated cationic
Li+@C70.[4]UV-vis-NIR
absorption
spectrum of the product in o-DCB showedbroad absorption at around 700-1000 nm atroom temperature (see Fig.), whichindicated the formation of singly bonded
Li@C70-Li@C70 dimer through the couplingof spin centre on Li@C70s.[5] Notably, theFig. Temperature dependance of UV-vis-NIR

absorption of the dimer decreased as absorption spectra of the product in o-DCB.
temperature increased, and new absorption assignable to Li@C70 monomer appeared at
1280 nm.[6] These results revealed the equilibrium behavior between Li@C70 and(Li@C70)2 in the solvent, which was consistent with the results of theoretical calculation.
[1] A. Nakagawa et al., Nat. Commun. 2018, 9, 3073. [2] Z. Wang et al., ACIE. 2016, 55, 199.
[3] H. Ueno et al., Chem. Sci. 2016, 7, 5770. [4] D. Kitabatake et al., The 60th FNTG 2021, 1P-11.
[5] D. V. Konarev et al., New J. Chem. 2019, 43, 2726.
[6] D. R. Lawson et al., J. Phys. Chem. 1992, 96, 7175.
Corresponding Author: H. Ueno, Tel: +81-22-795-7645, E-mail: hiroshi.ueno.d5@tohoku.ac.jp

24

2-9
Kinetic study of photopolymerization and thermal-depolymerizationin C60 films○Tatsuma Izumi1, Masato Nakaya1, Jun Onoe1
1

Department of Energy Science and Engineering, Nagoya University, Aichi 464-8603, Japan

C60 film is attracted as a novel thermoelectric material because of its giant Seebeck coefficient(S = −120 mV/K). For practical use, it is necessary to increase a very low electrical conductivity(σ = 10−6 Ω−1cm−1) of the C60 film to raise a power factor (PF = S2σ). In general, although the σof solid materials can be controlled by chemical carrier doping, this method reduces the |S| owing
to the trade-off relationship between |S| and carrier density. Polymerization is a possible way torealize C60-based high-PF materials, because the C60 polymer film exhibits a large σ due to anincrease in the carrier mobility [1]. In the present study, we evaluated the proportion distributionof C60 monomer, dimer, trimer, and oligomers, which is an important factor for the σ and thermal
stability, by examining the kinetics of photopolymerization and depolymerization in C60 films.
All experiments were carried out in an ultrahigh vacuum (UHV) chamber (base pressure: 10−6
Pa). A C60 film (300 nm thick) was formed on a cesium iodide (CsI) substrate by thermal
evaporation of C60 powder (99.98%) in a quartz crucible. Thereafter, C60 polymerization was
induced by irradiation of ultraviolet (UV) light (wavelength range: 300–410 nm, fluence: 0.2
W/cm2). Photopolymerized products in the C60 film were evaluated using in situ Fourier-transform
infrared (FT-IR) spectroscopy (resolution: 2cm−1).
Figure 1 (a) shows the FT-IR spectra before and after 40h photoirradiation of pristine C60 film.
The intensity of the four intense IR peaks (1429, 1183, 576, 526 cm−1) attributed to C60 molecule
decreased and new IR peaks appeared in the range of 700–800 cm−1 after photoirradiation. These
new peaks were assigned to C60 dimer, trimer, and oligomers via [2 + 2] cycloaddition reaction[2]. We examined the time evolution of the IR peaks corresponding to monomer [AM(t)] and dimer[AD(t)] based on equations (1) and (2). Here, the rate constant k of AM0 was assumed to be equal
to that of ADf in a short irradiation time region.
AM(t) = AM0 exp(−kt) (1), AD(t) = ADf {1−exp(−kt)} (2)By fitting the time-variation of the experimental absorbance of the monomer (1183 cm−1) anddimer (peak at 796 cm−1) using Eqs. (1) and (2), we evaluated the proportion of C60 monomer,
dimer, and oligomers in the photo-irradiated C60 film [Fig. 1 (b)], and found that the proportionof the oligomers was saturated to be 25% even after 40 h photoirradiation. In other words, C 60
oligomers are hard to be produced only by varying photoirradiation time. To estimate theactivation energy (Ea) of the dissociation of the dimer and oligomers, we examined the kinetics ofthermal-depolymerization of the dimerand oligomers, and obtained Ea to be
1.26 eV for the dimer, which is in an
excellent agreement with that reported
previously [3], whereas 1.78 eV for theoligomers. We will discuss a way tocontrol the proportion distributions of
the dimer and oligomers using thedifference in Ea between them.
[1] J. Onoe et al., J. Appl. Phys., 96, 443 (2004).
[2] J. Onoe et al., AIP Adv., 10, 085212 (2020).
[3] P. Zhou et al., Chem. Phys. Lett. 211, 337 (1993).
Corresponding Author: Jun Onoe
Tel: +81-52-789-3784
E-mail: j-onoe@energy.nagoya-u.ac.jp

Fig. 1 (a) FT-IR spectra of the C60 film before and after 40 h
photo-irradiation, and (b) the time evolution of the proportionof C60 monomer (circle), dimer (square), and oligomers(triangle) in the photoirradiation C60 film.

25

2-10
Development of Mobility and Charge Measurement System for Nanomaterials
Tomoya Ono, Kanata Oguri, and ○Toshiki Sugai
Department of Chemistry, Toho University, Miyama 2-2-1 Funabashi, 274-8510, Japan
Ion mobility spectrometry (IMS) combined with mass spectrometry has revealed novel
information on nanomaterials such as fullerenes[1]. However, the sizes of nanomaterials havebeen growing wider and wider to carbon nanotubes or graphene for example. These materials
cannot be detected by mass spectrometry so other measurement systems should be combinedwith IMS to study them. We have been working on nanocarbon materials such as graphene
quantum dots with our newly developed IMS combined with ion trap and opticalmeasurement system. Even with the new system it is still difficult to clarify their structures
because mobility depends on both of structures and charges of samples. To overcome thisdifficulty, here we present simultaneous
mobility and charge measurement system.
The system consists of an electrospray ion
source (ESI) for production of positively
charged nanoparticles from polystyrene
particles (D=205 nm) dispersed in water, a
trap type IMS, and a charge detector.
Aggregated polystyrene particles withseveral tens of charges were produced by
Fig. 1 Charge and size correlation of
ESI and trapped in the IMS system undercharged polystyrene particle aggregates.
ambient condition. Then the particles were
drifted around several centimeters, and thenwere detected by the charge detector. Figure 1 shows the correlation between detected charge
and diameter calculated from the drift time and the amount of charge with the assumption of
spherical structure. The observed distribution is well described by Rayleigh limit model
deduced with water surface tension, which is believed as a standard ionization model ofESI[2]. This well fit result shows the whole measurements were performed without
contradiction. The left end of the distribution is around 200 nm coming from single particles.
This system can be applied any nanomaterials with wide size distribution.
[1] G. von Helden et al., J. Chem. Phys., 95, 3835 (1991).
[2] L.Rayleigh, Philos. Mag., 14, 184 (1882).

TEL: +81-47-472-4406, E-mail: sugai@chem.sci.toho-u.ac.jp

26

2-11
New energy cycle “HI cycle” to repeat solar hydrogen generation andbattery power generation○Shinji Kawasaki, Kenta Kobayashi, Yosuke Ishii
Department of Life Science and Applied Chemistry, Nagoya Institute of Technology,
Nagoya 466-8555, Japan

We propose a new energy cycle “HI cycle” to repeat solar hydrogen generation and battery
power generation (Fig. 1). Solar hydrogen generation from HI solution enables the use ofnarrower band gap photocatalyst than that from water does. We demonstrated that the solarhydrogen generation from HI solution with methylammonium lead iodide (MAPbI3) is
effectively improved by the addition of single-walled carbon nanotubes (SWCNTs). SEM andTEM observations along with EDS analysis and Raman measurements revealed that SWCNTs
improved the hydrogen generation by absorbing the by-product iodine molecules. It was also
shown that we can fabricate zinc-iodine battery with the paper form zinc metal and the
I@SWCNT sample recovered from the photocatalysis cell. The battery worked very efficiently
with initial cell voltage of about 1.2 V. The capacity of the battery, corresponding to the amountof the encapsulated iodine molecules, revealed that SWCNTs had the ability to absorb the byproduct iodine molecules very effectively in the photocatalysis cell. We also confirmed that theelectrolyte solution after the discharge experiment should include not only iodide ions but alsoa considerable amount of hydrogen ions. It means that the solution returns to the starting pointof the “HI cycle” after the battery discharge. Raman measurements revealed that iodine-filled
SWCNTs formed by the solar hydrogen generation experiment were transformed back to empty
tubes by the discharge experiment. This confirms that SWCNTs can be used repeatedly forhydrogen generation and energy storage using the proposed “HI cycle”.

Fig.1 New energy cycle “HI Cycle” for repeated solar hydrogen generation and battery power
generation.

Corresponding Author: S. Kawasaki
Tel: +81-52-735-5221, Fax: +81-52-735-5221
E-mail: kawasaki.shinji@nitech.ac.jp.

27

2-12
Synthesis of Pt nanoparticles supported on Single-Walled Carbon
Nanotubes and its performance for fuel cell application○Miftakhul Huda1, Tomoya Kawahara1, Satoru Hashimoto2, Masaya Kawasumi3, Yutaka
Matsuo1,3
1Department of Chemical System Engineering, Graduate School of Engineering, Nagoya University,
Nagoya 464-8603, Japan
2
Meijo Nano Carbon Co., Ltd., Nagoya 463-0003, Japan
3
Institute of Materials Innovation, Institutes of Innovation for Future Society, Graduate School ofEngineering, Nagoya University, Nagoya 464-8603, Japan

Single-walled carbon nanotubes (SWCNT) is a versatile material for future application inelectrochemical fields such as fuel cell electrodes by utilizing its high conductivity, highporosity, and high oxidation resistance. However, it is difficult to utilize SWCNT bysynthesizing metallic nanoparticles supported on SWCNT due to its inert surface. Here, we
demonstrated a simple solvo-thermal method to synthesize Pt metallic nanoparticles with auniform size and high metal loading supported on e-DIPS-based SWCNT (diameter of 2 nm)
without using any chemical template, harmful acid or oxidant. Similar method has been used
to synthesize ultrathin Platinum nanowire without a support [1]. CV/LSV measurements wereconducted to measure its performance as a catalyst of oxygen reduction reaction for fuel cellapplication using rotating disk electrode (RDE) test.
DMF 6 mL, Etylene glycol 4 mL, and H2PtCl6.6H2O 8wt% 100 mg were mixed and stirred
before added with SWCNT. Then, the solution was reacted in autoclave at 170℃ to promote
the synthesis of Pt nanoparticles. Pt nanoparticles supported on SWCNT with an average sizeof 3.5 nm and Pt loading of 18.6 wt% were obtained. CV/LSV measurements revealed that the
Pt@SWCNT mass activity of 577 A/g-Pt and the specific activity of 800ȣA/cm2-Pt were two
fold higher than those of commercial Pt/C. This result demonstrated that metallic nanocatalysts
supported on SWCNT are promising as a cathode electrode for future fuel cell with high current
density and high voltage durability. This work is supported by NEDO (20001303-0).

Fig. 1 a) TEM image of Pt@SWCNT. b) The size distribution of Pt nanoparticles. c) CV measurement resultof Pt@SWCNT using RDE test.
[1] B.Y. Xia et al. J. Am. Chem. Soc., 135, 9480 (2013).
Corresponding Author: M. Huda
Tel: +81-52-789-3231,
E-mail: huda.miftakhul@material.nagoya-u.ac.jp

28

3-1
Optical Properties of Multi-Layer Graphene○Masahiro Kamada1, Takamoto Yokosawa1, Taisuke Ochi1, Ken-ichi Sasaki2,
and Tomohiro Matsui1
1

Advanced Research Laboratory, Anritsu Corporation,
5-1-1 Onna, Atsugi, Kanagawa 243-8555, Japan
2
NTT Research Center for Theoretical Quantum Physics, NTT Basic Research Laboratories,
NTT Corporation, 3-1 Morinosato Wakamiya, Atsugi, Kanagawa 243-0198, Japan

Not only monolayer graphene but also multi-layer ones are important to study especially inapplication point of view. For example, multi-layer graphene has a band gap, and the lightabsorption is expected to become the maximum at the layer number of 87 [1]. However, anefficient method to identify the number of layers has not been established, although it canestimate rather easily by optical contrast up to 6 layers [2,3]. Here, the contrast of graphene
exfoliated on SiO2/Si substrate is a resultant of the interference of light reflected at interfaces
between Si, SiO2 and graphene. In this context, the contrast is expected to change periodicallyby increasing the number of graphene layers.
In this paper, optical contrast of multi-layer graphene up to 100 nm thick (300 layers) on
SiO2 with 285 nm thick is studied. The contrast Ci (i = R, G, B) is analyzed from the RGB
components of optical images and defined as Ci = 1Igr,i / I0,i , where Igr and I0 are the RGB
intensity of graphene and SiO2 surface, respectively. The thickness dependence of Ci is shownin Fig.1. The contrast of G (green) component (CG) takes its maximum at t ~ 8 nm, and thensaturates at t ~ 50 nm. Such reentrant and saturation behavior is also observed for CR and CB
but with different maximum values atdifferent thickness. In addition, these are well
reproduced by the contrast measured atcertain wavelength rather than the RGB
values.
This reentrant behavior isconsistent with the expected periodic
behavior and qualitatively reproduced by adetailed calculation, which will be presented
elsewhere [4]. On the other hand, thesaturation and the difference between CR, CG,
and CB was not fully expected. It probably
indicates that the thick graphene graduallyloses its transparency and gets closer to bulk
graphite. By using these RGB contrast, one
Fig.1 Thickness dependence of RGB contrast
can estimate the number of layers up to ~120
between graphene and SiO2 substrate. The thick lines(40 nm) with ~10 layers of certainty.
are guides to the eye.

[1] K. Sasaki and K. Hitachi, Commun. Phys. 3, 90 (2020).
[2] P. Blake       91, 063124 (2007).
[3] B. Ma   Carbon 109, 384 (2016).
[4] K. Sasaki, et al., in this symposium
Corresponding Author: T. Matsui, M. Kamada
Tel: +81-(0)46-296-6594
E-mail: Tomohiro.Matsui@anritsu.com, Masahiro.Kamada@anritsu.com

29

3-2
Complex Raman tensor in Black Phosphorus and 2D materials○Riichiro Saito1, Nguyen Tuan Hung2, Yan Zhao3, Shiyi Han3, Lianming Tong3
1

Department of Physics, Tohoku University, Sendai 980-8578, Japan
Frontier Research Institute for Interdisciplinary Sciences, Tohoku University, Japan
3
College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, P. R. China
2

Raman tensor, ࡾǡ is a tensor for calculating Raman-scattering amplitude combined with given
vectors ࢋ࢏ and ࢋࢌ of incident and scattered lights. Using the Raman tensor, Raman intensity૛is given by หࢋࢌ ࡾࢋ࢏ ห ǤIn the quantum description of Raman tensor, Raman tensor is given by
the product of two electron-photon matrix elements and one electron-phonon matrix element.
These matrix elements are generally complex values and thus Raman tensor is generally given
by a complex tensor. When we represent a complex number  as  ൌ ȁȁ୧஢ , the phase ɐdoes not give any physical meaning since most of physical properties is given by ȁȁଶ Ǥ
However, when the values of ɐ for two matrix elements of the complex Raman tensor isdifferent from each other as shown in Fig. 1, the difference of ɐ’s can be seen in Raman
spectroscopy.
Here we report that the phase difference ofcomplex Raman tensor is observed for black
phosphorus by using circularly polarized light in
the polarized Raman spectroscopy after passing
the quarter wave plate. In this measurement, thepolarized Raman intensity peak is shifted fromthe crystal orientation as shown in the top of Fig.
1, which can not be explained by real Raman
tensor. By comparing with calculated complex
Raman tensor for each phonon mode by firstprinciples calculation as a function of laser
excitation energy, we explain the origin of theshift in the polarized Raman spectroscopy.
Further, we also discuss the calculated Raman
tensor of two-dimensional transition metal
dichalcogenides and their physical origin
Fig. 1 When the phases, ɐୡ and ɐୟare not the same in the Raman tensor,
we can observe the difference of ɐୡ െɐୟ as a shift of angle Ƚ଴ in thepolarized Raman measurement in the
Raman intensity by using circularly
polarized light.

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

30

3-3
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w. FIB
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10
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0

1.30

1.35

1.40

Energy (eV). 1 PL spectra of MoSe2/WSe2 heterobilayerswith and without FIB process. Inset: Optical imageof the MoSe2/WSe2 heterobilayers.

,..#/-,+"&+$10%,. 41+ .&  0/1"
#)     
* &)* 0/1" & #(3,0,1 !'-

31

3-4
Color-Tunable Light-Emitting Devices Based on Compositionally Graded
Monolayer Transition Metal Dichalcogenide Alloys○Hao Ou1, Jiang Pu1,*, Tomoyuki Yamada1, Naoki Wada2, Hibiki Naito2, Zheng Liu3,
Yasumitsu Miyata2, Taishi Takenobu1,*
1

Department of Applied Physics, Nagoya University, Nagoya 464-8603, Japan
Department of Physics, Tokyo Metropolitan University, Tokyo 192-0397, Japan
3
Inorganic Functional Materials Research Institute, AIST, Nagoya, 463-8560, Japan
2

Monolayer transition metal dichalcogenides (TMDCs) show many exotic optical
performances, enabling them potential candidates for future optoelectronics [1]. Conventionally,both mechanically exfoliated and chemically grown monolayer TMDCs have binary atomic
composition, i.e. two types of atoms, and then, their electronic structure are fixed. In contrast,
when producing ternary alloy of TMDC, the physical and chemical properties could drasticallychange as tuning the ratio of hetero-atoms [1]. As a result, the device applicability of thematerial is also expanded, such as transistors and photodiodes. However, the light-emitting
devices using TMDC alloys have not yet been achieved, possibly due to the sample qualities
and/or technical issues of device fabrications. Here we report on the realization of color-tunable
light-emitting device using WS2xSe2-2x alloy with spatially varying ternary atomic composition.
By the dynamic control of growth parameters during chemical vapor deposition (CVD)
process, spatially graded monolayer WS2xSe2-2x alloy was successfully synthesized. From thephotoluminescence (PL) spectra, position-dependent PL energy change owing to gradualvariation of composition could be confirmed, since the PL peak shifts between typical WS2
peak and WSe2 peak. We then utilized the alloy to fabricate light-emitting device, using thetwo-terminal electrolyte-based light-emitting device structure (Fig. 1) [3].
The alloy device shows clear electroluminescence (EL) at relatively low driving voltage (2to 4V), giving the first demonstration of TMDC-based alloy light-emitting device. Furthermore,
we found that with tuning the applied voltage fordevice, the light-emitting position (location of EL)
shifts monotonically between two electrodes (Fig. 1,
up). Because of the spatially graded composition ofalloy, the EL spectrum also changes (Fig. 1, down).
As a result, the color of light emission should present
voltage (location) dependence. By analyzing both
EL images and spectra, it’s noticed that the emission
color was continuously tuned. Our demonstration onlight-emitting device using monolayer TMDC alloy,
along with the observed continuous tunability of EL
color, provide a new approach to the broadband
optoelectronic applications based on monolayer
semiconductors.
[1] J. Mann et al., Adv. Mater. 26, 1304389 (2014).
[2] J. Pu et al., Adv. Mater. 30, 1707627 (2018).
[3] J. Pu et al., Adv. Mater. 29, 1606918 (2017).
Corresponding Author: J. Pu and T. Takenobu
Tel: +81-52-789-5165, Fax: +81-52-789-5165,
E-mail: jiang.pu@nagoya-u.jp, takenobu@nagoya-u.jp

Fig. 1. Light-emitting device structure (up)and EL images with corresponding EL
spectra.

32

3-5
G/D ratio of SWCNT solution○Hiromichi Kataura1, Mayumi Tsuzuki1, Takeshi Tanaka1
1

Nanomaterials Research Institute, AIST, Tsukuba 305-8565, Japan

Defect assessment of single-wall carbon nanotubes (SWCNTs) is very important forelectronic device applications of SWCNTs, because the electronic mobility is highly dependingon their structural defects. Intensity ratio of G-band and D-band (G/D ratio) in Raman spectra
is often used for the defect assessment of sp2 carbon materials including SWCNTs. In case of
SWCNTs, however, it is known that we must consider the resonance effects because G-band
intensity is highly depending on the optical absorption of the incident laser light. Furthermore,in this work, we found that the G/D ratio depends on the sort of surfactants when we measure
the Raman spectra of SWCNT aqueous solutions. Fig.1 shows the G/D ratios of NOPO Hipco
solutions for different concentrations of sodium deoxy cholate (DOC) mixed with sodium
cholate (SC). Since the used SWCNTs were from same solution without any additional
sonication, observed G/D change was simply caused by the difference of wrapping surfactants.
We found that both the G-band and D-band intensities were changed by changing DOC
concentration. Because the change of G/D value is very large, we must consider this surfactant
effects for the defect assessment of SWCNTs.
Since we used mixed chirality sample for this measurement, detailed resonance analysis isvery difficult. We are now preparing single chirality sample for the advanced experiments. We
will show the latest results in the meeting.

G/D ratio @633 nm

120

NOPO HiPco in SC 0.1% + DOC x%
aqueous solution

100

80

60

40

0

0.1

0.2

0.3

0.4

0.5

0.6

Concentration of DOC (%)

Fig. 1 G/D Raman intensity ratios of NOPO Hipco aqueous solutions. Concentration of DOC was changed from0.01 to 0.5% keeping both concentrations of SWCNT and SC (0.1%). All measurements were done without any
additional sonication.
Corresponding Author: H. Kataura
E-mail: h-kataura@aist.go.jp

33




3-6




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37

3-10

Direct synthesis of graphene nanoribbon ballistic Josephson junction○Naofumi Sato, Toshiro Kaneko, Tomohiro Otsuka2, Toshiaki Kato
1

2

Graduate School of Engineering, Tohoku University, Sendai 980-8579, Japan
Research Institute of Electrical Communication, Tohoku University, Sendai 980-8577, Japanraphene nanoribbon (GNR), strips of two-dimensional (2D) graphene into one-dimensional(1D) structure, gather intense attentions because of their superior electrical features. Until now, wedeveloped a novel method based on the advanced plasma CVD with nanoscale metal catalyst (metal
nanobar) for position selective synthesis of GNR in wafer scale [1, 2]. In this study, we attempted to
grow GNR from MoRe (Molybdenum-rhenium) nanobar, known as a superconductor metal, for the
integrated synthesis of GNR-based Josephson junction devices.
Systematic investigation revealed that GNR
can be synthesized from the MoRe nanobar (Fig.1).
Detailed measurements at cryogenic temperatures
revealed that resistance of GNR device rapidly
decrease with temperature and clear two-step
depletions are observed around 15K and 5K.
Furthermore, the zero resistance is realized below Fig. 1. Schematic illustration of suspended GNR
3K (Fig.2). These indicate Josephson junction is grown from MoRe nanobar by our plasma CVD.
successfully formed in our device. The color mappingof the differential resistance dV/dI as a function ofgate voltage ܸ୥ and source-drain current ‫ܫ‬ୱୢ shows
the critical current tends to be modulated by ܸ୥ ,indicating the Josephson junction may be formed
throughtheMoRe-GNR-MoRestructure.
Furthermore, the clear oscillations of critical current
were observed in the specific gate voltage region,
which can be explained by Fabry–Pérot interferencesin the supercurrent through the junction. This meansthat the carriers in the GNR are ballistically   Temperature dependence of resistance intransported in our MoRe-GNR-MoRe Josephson MoRe-GNR-MoRe junction device.
device. These results can contribute to realizing large
scale integration of GNR-based high performance
Josephson junction devices.
[1] T. Kato and R. Hatakeyama, Nature Nanotechnology, 7, 651-656 (2012).
[2] H. Suzuki, T. Kaneko, Y. Shibuta, M. Ohno, Y. Maekawa, T. Kato, Nature Communications, 7, 11797-1-10 (2016).
Corresponding Author: T. Kato -7046"   -9225,
   !

38

3-11

Fabrication and electronic transport properties ofmultilayer NbxMo1-xS2/MoS2 in-plane heterostructures○Hiroto Ogura1, Seiya Kawasaki1, Zheng Liu2, Takahiko Endo1, Yusuke Nakanishi1,
Hong En Lim1, Kazuhiro Yanagi1, Toshifumi Irisawa3, Keiji Ueno4, Kosuke Nagashio5,
Yasumitsu Miyata1
12Department of Physics, Tokyo Metropolitan University, Hachioji, 192-0397, Japan
Innovative Functional Materials Research Institute, AIST, Nagoya, 463-8560, Japan
3
Nanoelectronics Research Institute, AIST, Tsukuba, 305-8562, Japan
4
Department of Chemistry, Saitama University, Saitama 338-8570, Japan
5
Department of Materials Engineering, The University of Tokyo, Tokyo, 113-8656,
Japan

Heterostructures of transition metal dichalcogenides (TMDCs) have attracted muchattention for high-performance tunneling field-effect transistors (TFETs) due to their air
stability and atomically steep interfaces. So far, band-to-band tunneling at theheterojunction has been often studied for various TMDC-based vertical heterostructures[1, 2]. In contrast, in-plane semiconductor heterojunctions of TMDCs have been also
proposed recently to be promising for TFETs [3]. Especially, multilayer TMDCs possess
an advantage in terms of the availability of highly doped TMDCs. Therefore, it isimportant to characterize the in-plane heterostructures based on various multilayer
TMDCs. In this study, we have fabricated and investigated the electronic transport
properties of multilayer NbxMo1-xS2/MoS2 in-plane heterostructures.
Multilayer NbxMo1-xS2 or WSe2 crystals were prepared on the SiO2/Si substrates bymechanical exfoliation, and MoS2 was then grown by chemical vapor deposition [4].
Cross-sectional HAADF-STEM observations reveal the growth of MoS2 from the edgeof the WSe2 crystal and the formation of an atomically steep interface (Fig. 1a). Multilayer
NbxMo1-xS2/MoS2 in-plane heterostructures were also formed in the same manner (Fig.
1b). Interestingly, the NbxMo1-xS2/MoS2 heterostructure shows a negative differential
resistance (NDR) trend below 100 K (Fig. 1c). These results provide important insights
into the application of multilayer TMDC in-plane heterostructures in future device
applications.

Figure 1 (a) Schematic and cross-sectional HAADF-STEM images of multilayer WSe2/MoS2 in-plane
heterostructure. (b) Schematic and cross-sectional TEM images of multilayer NbxMo1-xS2/MoS2 in-plane
heterostructure. (c) Output curves of the Nb xMo1-xS2/MoS2 device at different temperatures at the back-gate
voltage of 80 V.
[1] T. Roy et al., ACS Nano, 9, 2, 2071–2079 (2015). [2] K. Nakamura et al., ACS Appl. Mater. Interfaces.,12, 51598-51606 (2020). [3] T. Fukui et al., The 82nd JSAP Autumn Meeting, 13a-N307-11 (2021). [4] K.
Kojima et al., Nanoscale, 11 12798 (2019).
Corresponding Author: Y. Miyata, Tel: +81-042-677-2508, E-mail: miyata-yasumitsu@tmu.ac.jp

39

3-12
Edges of Layered MoS2 Observed by Field Electron Emission and
Field Ion Microscopy○Yahachi Saito
Toyota Physical and Chemical Research Institute, Nagakute 480-1192, Japan

Monolayer MoS2 possesses a variety of polymorphs such as 1H, 1T and 1T’. Among them,the 2-dimentional 1T’ structure is predicted to be in a topological insulator (TI) phase [1], andthe presence of gapless helical edge states is suggested [2]. Knowledge of atomic andelectronic structures of layered MoS2 would deepen the understanding the fascinating 2dimentional (2D) TI phase.
Field electron emission and field ion microscopies (FEM and FIM) are powerful techniques
to study atomic structures and dynamics of solid surfaces and edges. For graphene, FEM andFIM show characteristic images representing electronic orbitals at its edges [3]. In the present
report, experimental results of FEM and FIM study on layered MoS2 are presented.
MoS2 field emitters were prepared by mechanicalexfoliation of a bulk MoS2 single crystal.
Measurement procedures of FEM/FIM are describedin Ref. [4].
A scanning electron microscopy (SEM) image ofan edge of the exfoliated MoS2 single crystal isshown in Fig. 1. Clear-cut edges with polygonal
shapes are revealed. The thickness of the MoS2
flake is estimated to be around 100nm, and thus theemitter is multilayered. Figure 2 (a) is an FEM
image of the exfoliated MoS2, showing an array ofelongated broad spots. The elongation of spots is Fig. 1 SEM image of an edge of exfoliated
MoS2. Acceleration voltage of SEM, 5kV.
caused by the 2D nature of MoS2,
like graphene emitters [3].
Figure 2 (b) shows thecorresponding FIM image, forwhich Ne gas was used as an
imaging gas, exhibiting arrays of
streaks and dipole spots (indicatedby arrows) running transverse to
the layered plane of MoS2. These
FIM patterns, possessing atomic
resolutions, originate from atomic
positions and empty electronic
Fig. 2 (a) FEM and (b) FIM images of the exfoliated MoS2.
orbitals at the edges of MoS2.
[1] X. Qian et al., Science 346, 1344 (2014).
[2] H. Mine et al., Phys. Rev. Lett. 123, 146803 (2019).
[3] Y. Saito, J. Vac. Sci. Technol. B 40, 012803 (2022). [4] Y. Saito ed., Nanostructured Carbon
Electron Emitters and its Applications (Jenny Stanford Publishing, Singapore, 2022).
Corresponding Author: Y. Saito
Tel: +81- 561-57-9616, Fax: +81- 561-63-6302, E-mail: ysaito@toyotariken.jp

40

3-13
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41

Figure 1. (a) Scanningelectron microscope imageofthehigh-density
CNT/HfO2/CNT memristor
device.
(b) Memristor’s responseto the input voltage training
at different stages of
Pavlov’s dog training
regime.

3-14Multi-element photo-thermo-electric devices
by a micro-scale CNT film array○Daichi Suzuki1, Yuma Takida2, Yukio Kawano3–5, Hiroaki Minamide2, Nao Terasaki1
1

Sensing System Research Center, AIST, Saga 841-0052, JapanRIKEN Center for Advanced Photonics, RIKEN, Miyagi 980-0845, Japan
3
Faculty of Science and Engineering, Chuo University, Tokyo 112-8551, Japan
4
FIRST, Tokyo Institute of Technology, Tokyo 152-8552, Japan
5
National Institute of Informatics, Tokyo 101-8430, Japan2

One of the unique advantages of a carbon nanotube (CNT) film is a high photo-thermoelectric (PTE) efficiency due to the low-dimensional structure of CNTs. The PTE effect, whichconverts photons and heat to electricity, can be utilized for variety of applications such asbroadband sensors and energy harvesters. Meanwhile, we previously have developed a terahertz(THz) soft camera patch sheet through a laser ablation process [1]. In this presentation, we
report the high sensitivity THz detector and spectroscopy, achieved by arraying multi-element
micro-scale THz detectors in series.
The critical method for enhancing PTE voltage 'V is to increase the number of detectors inseries connection, which is well-known as a structure of thermopile. Especially in photo sensing
applications, it is important to reduce the interval spacing between detector elements to increase
the aperture ratio of the CNT film (photo absorbing material) to reduce energy loss (Fig. 1a).
Figure 1b shows a multi-element THz detector. Each detector element that involves a p-njunction was arrayed in 5 Pm intervals by using the laser ablation process and was connected
in series on the rear side of the polyimide film via the contact holes on both ends. As a result of
the series connection, the THz response increased 4-fold compared to the single-element THz
detector (Fig. 1c). We expect that the presented technique of CNT film arrays can be applied
not only to sensing applications as shown in Fig. 1d but also to thermoelectric generators.

Fig. 1. (a) Schematics of the photo-thermo-electric effect for single/multi-element THz detector. (b) Photographic
image of a multi-element THz detector. (c) THz response comparison. (d) THz spectroscopy by the multi-element
THz detector. The arrows indicate the resonant peaks (fingerprint spectrum) of the medicine.
[1] D. Suzuki et al., Adv. Funct. Mater., 31, 2008931 (2021).
Corresponding Author: D. Suzuki, Tel:+81-942-81-3620, Fax:+81-942-81-4018, E-mail: daichi.suzuki@aist.go.jp

42

3-15
Optimization of Fabrication and Post-Treatment Conditions of
CNT/Polymer Composite Ribbons for Higher Thermal Conductivity○Nikita Kumari, Ryo Abe, Naofumi Okamoto, Manish Pandey, Masakazu Nakamura
Nara Institute of Science and Technology, 8916-5 Takayama-cho, Ikoma, Nara 630-0192, JapanThe ongoing development of high-efficiency integrated circuits led to significant heatgeneration due to increased power density. The undesired heating of the electrical circuits is amajor threat to their performance and durability. Therefore, flexible interconnecting materials
possessing high thermal conductivity (TC) are highly desirable for the thermal management ofequipments. Taking the theoretically calculated TC (> 6000 W/mK) of individual c arbon
nanotubes (CNT) into consideration, they are getting significant research interest [1]. Moreover,
CNTs are also lightweight, corrosion-resistant, and flexible materials. Although the theoretical
calculation of isolated CNTs exhibits exceptional TC, the difficulty in handling them as
aggregates limits the application of CNTs. In aggregates, CNTs are quite entangled due to thehigh aspect ratio and strong van der Waals interaction. Therefore, orientation techniques aredesirable to utilize the individual-CNT’s thermal properties at a macroscopic scale.
We have recently established a new orientation technique to fabricate scalable films of
CNT/polymer composite through a programmable robotic dispenser, as schematically shown in
Fig. 1(a) [2]. In this work, CNT/polymer composite films were fabricated using this technique.
Further, for the quantitative and qualitative analysis of CNT-orientation, the films were
subjected to mapping of G-band intensity ratio obtained through polarized Raman spectroscopy(I00°/I90°) and scanning electron microscopy (SEM), Fig. 1(b). For the oriented films,
improvement in the corresponding thermal diffusivity and TC was also obtained. Moreover, it
was found that the post-treatment, i.e., washing the film with a good solvent for organic
component, also had a noticeable effect on the TC, which can be attributed to variation in theresidual organic components in the film. Further, via optimization of post-treatment of theoriented-CNT films, the state-of-art in-plane TC of more than 200 W/mK was obtained [3].
In this presentation, optimizations of film fabrication and the post-treatment conditions will
be discussed in detail.
Acknowledgement: This work was
supported
by
JST
CREST
(JPMJCR18I3).
[1] B. Kumanek, D. Janas, J. Mater. Sci., 54,
7397 (2019).
[2] M. Pandey et al. Appl. Phys. Express,
13, 065503 (2020).
[3] H. Ma et al. J. Mater. Sci., 56, 1064
(2021).
Corresponding Author: M. Nakamura
Tel: +81-743-72-6031, Fax: +81-743-726047,
E-mail: mnakamura@ms.naist.jp

Fig. 1 (a) Schematic representation of film fabrication via
robotic dispenser and a digital image of the coated CNT/polymer
composite films. (b) The SEM image of a representative film.
The two-sided arrow represents the coating direction.

43

3-16
Reduced Graphene Oxide Films with High Structural Quality Fabricatedby a Two-Step Reduction of Graphene Oxide○K. Kanishka H. De Silva, Kazuma Shibata, Pamarti Viswanath, Masamichi Yoshimura
Graduate School of Engineering, Toyota Technological Institute, Nagoya, 468-5811, Japan.

Graphene oxide (GO) has emerged as a precursor to fabricate graphene-like materials due
the ability of mass scale production at a low cost. However, the structural quality of graphene
obtained by the reduction of GO (known as reduced graphene oxide -RGO) is inferior to pristinegraphene. Attempts have been made to obtain RGO with high structural quality by optimizing
reduction strategies, such as using catalysts [1], microwave reduction [2], and oxidation ofgraphite to get less defected graphene oxide [3]. Yet, these methods are energy and time
consuming and also result in low yield. Hence, the challenge is still open to fabricate highquality RGO in an easier and productive way. We present a two-step reduction of GO using a
mixture of hydroiodic acid and trifluoroacetic acid (HI/TFA) within a few minutes followed bythermal annealing in the presence of ethanol at 800 oC. Ethanol acts as a lattice defects repairing
agent during annealing step [4]. Raman spectrum of the obtained RGO sheets show very sharp
peaks with a low intense D-band and a high intense G’-band (Fig. 1(a)). Using the peak widths,
ID/IG ratio and the following equations, the distance between defects (LD) in the graphene lattice
was determined [5]. According to equation 1, the LD values for GO, chemically reduced GO,
and thermally annealed GO were all less than 2 nm, while according to equation 2, for GO
reduced via two-step reduction LD is about 21 nm (Fig. 1(b)). Following this reduction strategy,
we succeeded in fabricating highly conductive and transparent monolayer RGO films, whichfurther confirms the quality of the fabricated RGO films is of high quality.
ூ‫ܮ‬ଶ஽ ሺ݊݉ሻଶ ൌ ͷǤͶ ൈ ͳͲିଶ ‫ܧ‬௅ସ ሺܸ݁ ସ ሻ ூವ(1)ಸ‫ܮ‬ଶ஽ ሺ݊݉ሻଶ ൌସǤଷ ൈ ଵ଴య ூವ ିଵቂ ቃாಽర ሺ௘௏ ర ሻ ூಸ

a
D
1000

b

G’

G
1500

(2)

2000
2500
Raman shift (cm-1)

3000

Fig. 1 (a) Raman spectrum of the high quality RGO sheets and (b) Schematic showing the RGO with low defectdensity after two-step reduction.
[1] J-C. Yoon et al. ACS Nano, 15, 11655 (2021).
[2] D. Voiry et al. Science, 353, 1413 (2016).
[3] Wang et al. J. Phys. Chem. Lett., 12, 10009 (2021).
[4] K.K.H. De Silva et al. Jap. J. Appl. Phys. 58, SIIB07 (2019).
[5] Cançado et al., Nano Lett., 11, 3190 (2011).
Corresponding Author: K. Kanishka H. De Silva
Tel: +81-52-809-1852,
E-mail: sd16501@toyota-ti.ac.jp

44

ポスター発表$ 

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48

1P-5
Synthesis of Boron Nitride Nanotubes with the Chirality-Sorted Carbon
Nanotubes as the Template○Ruixi Zhang1, Ya Feng1, Yongjia Zheng1, Ming Liu1, Shuhui Wang1, Keigo Otsuka1,
Takeshi Tanaka2, Hiromichi Kataura2, Rong Xiang1, Shigeo Maruyama1
1

Department of Mechanical Engineering, The University of Tokyo, Tokyo 113-8656, Japan
Nanomaterials Research Institute, National Institute of Advanced Industrial Science andTechnology (AIST), Tsukuba 305-8565, Japan

2

Since the one-dimensional van der Waals heterostructures [1] were first synthesized in 2020,
many kinds of electronic devices based on this type of heterostructure, such as transistor [1] anddiode [2], have been developed and their electrical properties were evaluated. It is well known
that the chiral carbon nanotubes are either semi-conducting or metallic. Plenty of research havebeen conducted to prepare single chirality carbon nanotubes for realizing the controllable
electrical properties of carbon nanotubes. Based on this idea, in this research, single chirality
carbon nanotubes were used as the template to be wrapped by boron nitride nanotubes(BNNT),
which is believed to protect or even improve the intrinsic electrical properties of carbon
nanotubes, and to further fabricate electronic devices with better performance.
Currently, the sorted single chirality carbon nanotubes were prepared in water withassistance of surfactants. The wrapping of surfactants on carbon nanotubes prevented thecoating of boron nitride outside to form the heterostructure [3]. Therefore, in this research, anannealing method was proposed to remove the surfactant on the surface of single chirality
carbon nanotubes. The removal of surfactant from the surface of individual carbon nanotube
can be realized in a relatively low temperature (500oC) and low vacuum (30 Pa) condition.
Before annealing, the original solution sample was measured by optical absorption to define
the optical density of single-wall carbon nanotubes (SWCNT). The optical density shown in
Fig.1. The dispersed SWCNT solution was dropped onto Mo/SiO2 TEM grid; after drying out,
two of such grids were put into the chamber and annealed for 7 hours. After annealing, one of
the two grids was put into BN furnace to synthesize BN nanotubes. The BN growth was
conducted at 1075oC for 1 hour. Thereafter, the two grids were examined by TEM tocharacterize the atomic structures. As shown in Fig. 2, the BNNT well-crystalized structure canbe found, which proved that the annealing condition worked well for the removal of thesurfactant. In addition, the successful synthesis of SWCNT-BNNT structure indicated that thesorted single chirality carbon nanotubes in water can be processed to synthesize boron nitride
nanotubes outside.
Reference[1] R. Xiang, et.al,
Science, Vol 367, 2020.
[2] Y. Feng, et.al, ACS
Nano, Vol 15, 2021.
[3] Y. Zheng, et.al,
PNAS, Vol 118, 2021.

Fig. 1 Absorption spectra of SWCNT samples.

Fig. 2 TEM images of BNNT grownon the chirality-sorted SWCNT

49

Corresponding Author:
S. Maruyama
Tel: +81-3-5841-6421,
Fax: +81-3-5841-6408,
E-mail:maruyama@photon.t.utokyo.ac.jp

1P-6
CO2-driven tuning of growth rate, lifetime, and incubation ofhorizontal arrays of carbon nanotubes○Ryoya Ishimaru1, Keigo Otsuka1, Taiki Inoue2, Shohei Chiashi1, Shigeo Maruyama1
1

Department of Mechanical Engineering, The University of Tokyo, Tokyo 113-8656, Japan2
Department of Applied Physics, Osaka University, Osaka 565-0871, Japan

Single-walled carbon nanotubes (SWCNTs) are an ideal channel material in highperformance transistors provided that their chirality and density are well controlled. Direct
growth of long and dense nanotube arrays suitable for the applications requires further
understanding of the mechanisms that determine the speed, lifetime, and incubation of SWCNT
growth. Thick CNT forests have been synthesized by adding oxidant gases (e.g., CO2 [1] orH2O [2]) to carbon source gases, which suggests that oxidants maintain catalyst activity bysuppressing catalyst encapsulation with carbon. Here we traced the growth process of individual
SWCNTs under the supply of oxidant gases during ethanol chemical vapor deposition (CVD)towards the tuning of the length and density of horizontally aligned SWCNTs.
We employ the isotope decoding technique [3,4], which decouples the growth rate, lifetime,and incubation time of nanotubes. With the total flow rate of ethanol fixed at 5 sccm, three
discrete ratios of 13C ethanol were introduced every 1 min, serving as labels embedded in
SWCNTs. We conducted two experiments with different flow rates of CO2, where CO2 addition
started from the middle (6 min) of 24 min CVD process. After the CVD, Raman mapping
measurements were performed to locate the isotope labels and thereby obtain the growth rate
profiles (Fig. 1) of nanotubes synthesized with additive CO2 (CO2/EtOH=3/1). The growth rate
decreased for most nanotubes at 6 min upon the introduction of CO2, and their average change
was −17%. Interestingly, the sensitivity to CO2 significantly differs from tube to tube. We also
compare the growth lifetime (Fig. 2) and incubation time (Fig. 3) with/without additive CO2(CO2/EtOH=1/1), indicating that CO2 has positive influences on lifetime and nucleation incontrast to the suppressed growth rate, likely due to the removal of excessive carbon from
catalysts. Our results indicate that long and dense SWCNT arrays could be synthesized throughthe optimized amount and sequence of additive CO2.

Fig. 1 Growth rate change ofindividual nanotubes that kept
growing after CO2 addition.

Fig. 2 Lifetime distributions of
SWCNTs grown (a) without and(b) with CO2.

[1] T. Sato et al., Carbon, 136, 143 (2018).
[3] K. Otsuka et al., ACS Nano, 12, 3994 (2018).
Corresponding Author: S. Maruyama

Fig. 3 Incubation time distributionsof SWCNTs grown (a) without and(b) with CO2.

[2] T. Yamada et al., Nano Lett., 8, 4288 (2008).
[4] B. Koyano et al., Carbon, 155, 635 (2019).

E-mail: maruyama@photon.t.u-tokyo.ac.jp

50

1P-7
Two Sedimentation methods for Nanotube Aggregates: Size and Porosity
Ranges where Inner Fluid Buoyancy Occurs○Yuichi Kato1, Takahiro Morimoto2, Kazufumi Kobashi2, Tetsuji Yamaguchi3, Tetsuya Mori3,
Takushi Sugino1, Toshiya Okazaki2
1 Nanomaterials Research Institute, National Institute of Advanced Industrial Science andTechnology (AIST), Osaka 563-8577, Japan
2 CNT-Application Research Center, AIST, Tsukuba 305-8565, Japan
3 HORIBA, Ltd., Kyoto 601-8510, Japan
Fine tuning of the structure for disentangled carbon nanotube (CNT) agglomerates isimportant to enhance the CNT composite material’s performance. Quantitative analysis ofporosity (߶) in liquid of the CNT agglomerates (when we disentangle CNTs, ߶ of CNT
agglomerates may increase) has been limited despite its importance. Recently, we proposed ananalysis of ߶ and sedimentation particle size (D) of the agglomerates by centrifugal
sedimentation.[1] We consider “inner fluid buoyancy (IFB)”, that is the buoyancy caused by
the smaller fluid density inside the agglomerate that sediments in a density gradient than thefluid outside.
Here, we introduce two sedimentation methods to estimate ߶ and D based on the range of ߶and D where IFB is significant. You will estimate ߶ and D with linear analysis of sedimentations
in density gradients (Fig.1b, left) if the particles located in region A (Fig 1a). The other is
combination of homogeneous sedimentation and image analysis (Fig.1b, right). This approach
can be applicable the particles located in both region A and B because theoretically IFB can beignored.

Fig. 1a) Size and porosity ranges where IFB significantly occurs. b) Two sedimentation methods for estimation.
[1] Y. Kato et al. The Journal of Physical Chemistry C 123, 21252-21256 (2019).
Corresponding Author: Y. Kato
Tel: +81-29-861-9275
E-mail: yuichi.katou@aist.go.jp

51

1P-8






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52

1P-9
Unconventional Temperature Dependence of Thermoelectric Properties
on Semiconducting SWCNT Films○Yota Ichinose1, Manaho Matsubara2, Akari Yoshida1, Shigeki Saito1, Kan Ueji1,
Yohei Yomogida1, Takahiro Yamamoto2, and Kazuhiro Yanagi1
12Department of Physics, Tokyo Metropolitan University, Tokyo, Japan
Department of Physics, Tokyo University of Science, Shinjuku, Tokyo, Japan-1|S| (PVK )Single-walled carbon nanotubes (SWCNTs) are ideal one-dimensional nanomaterials withthe potential to exhibit significant thermoelectric (TE) performance [1]. To understand the TE
properties in SWCNT thin films, we need to clarify the relationship between the TE properties
and the carrier conduction mechanism. Previously we have experimentally investigated the TE
properties of SWCNT thin films by changing the chemical potential (μ) position and measuring
the temperature (T) dependence. It is known that the carrier conduction of SWCNT thin-film
systems generally follows Mott’s variable-range-hopping (VRH) model in the T-dependence[2]. On the other hand, we found that the Seebeck coefficient (S) shows an abnormal increaseat low temperatures under certain conditions and reported the phenomenon in the previous
FNTG conference. However, the mechanism has
not been understood using conventional models.
Therefore, we investigated the background of the120
phenomenon by analyzing the T dependence of S,
electrical conductivity (σ), and thermoelectric
80
conductivity (L12).
Here we discuss the T-dependence of the TE
40
properties of semiconducting (6,5) SWCNTs with
In bandpurity over 99% and with controlled μ position.
Mott-VRH
0
Figure 1 indicates the T-dependence of S value
when μ is located within the conduction (or600
In gapvalence) band or in the bandgap. As shown inCal.
figure 1, when μ is located within the conduction
400(or valence) band, S follows the general Mott-VRH
model. However, with μ in the bandgap, S shows200
an abnormal increase at the low T region. The
Mott-VRH model cannot reproduce thisunconventional behavior. Therefore, we modified0
the conventional Mott-VRH model and analyzed
050 100 150 200
the data. As a result, we succeeded in reproducing
Temperature(K)the experimental results, as shown by the solid lineFig.
1.
Temperaturedependence of the Seebeckin the figure. Here, the analysis suggested thecoefficient.
The
chemicalpotential in band (top)necessity of the μ shifts with temperature changes
and in bandgap (bottom). The points indicate theand adding an energy-dependent term in the Mottexperimental data.
VRH. In the presentation, we discuss thisbackground in detail.
[1] Hicks & Dresselhaus, PRB 47, 16631 (1993). [2] K. Yanagi et al., ACS Nano 4, 4027 (2010).
Corresponding Author: K. Yanagi, +81-42-677-2494, yanagi-kazuhiro@tmu.ac.jp53

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54




1P-11




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1P-13Rayleigh scattering spectra from SWCNTs with water adsorption andencapsulation○Koki Kozaki, Ryotaro Kaneda, Shu Sato, Keigo Otsuka, Shigeo Maruyama, Shohei Chiashi
Department of Mechanical Engineering, The University of Tokyo, Tokyo 113-8656, JapanThe synthesis of one-dimensional hetero structures such as single-walled carbon nanotubes
wrapped with boron-nitride nanotube (SWCNT@BNNT) was recently reported[1], and theirproperties have attracted much attention. Technology in encapsulating molecules inside
nanotube is also expected to be applicated in fields such as drug delivery system. In this study,
Rayleigh scattering spectra from SWCNT@BNNT and SWCNT encapsulating water molecules
were measured in various conditions and their optical properties were investigated. Rayleighspectra measured in water vapor were analyzed based on the temperature dependence, theadsorption of water molecules on the outside, and the water encapsulation.
SWCNTs were synthesized with ACCVD method across a slit substrate. Then boron-nitride
layer was synthesized on the outer surface of some SWCNTs using CVD method as shown in
Fig. 1(a), and other SWCNTs were opened with a pulse laser irradiation. To control theenvironment around samples, an environmental chamber suited for measuring Rayleighscattering light was used. As the chamber was evacuated, heat transfer from SWCNTs issuppressed, and the incident laser irradiation easily heated up SWCNTs. As the result, the peaksin Rayleigh scattering spectra shifted to lower energy. Next, water vapor or air was introduced
into the chamber, and Rayleigh spectra were measured with different pressure. With increasingwater vapor pressure, the peak shifted to higher energy. In addition, Rayleigh spectra from
opened SWCNTs were also measured. The pressure dependance of the peak energy on water
vapor and air was shown in Fig. 1(b). In the low pressure range, there was no difference between
water and air cases. On the other hand, in the case of water vapor, the optical transition energy
was almost the constant above a pressure, indicating that water molecules adsorbed on the mostouter surface of SWCNT@BNNT.
(a)
(b)
20 μm

 Fig.1 (a)SEM image of a suspended SWCNT@BNNT. (b)Water vapor and air pressure dependance of the opticaltransition energy of SWCNT@BNNT. The solid circles and the open circles represent air atmosphere and water
vapor atmosphere, respectively.
[1] R. Xiang et al. Science, 542, 537 (2020).
Corresponding Author: S. Chiashi
Tel: +81-03-5841-6407, Fax: +81-03-5841-6407,
E-mail: chiashi@photon.t.u-tokyo.ac.jp57

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58

1P-15
Potential for improving efficiency and durability of perovskite-silicontandem solar cells with single-walled CNT electrodes○Hiroki Nagaya1, Bowen Zhang1, Mohamad Almesfer1, Xiyang Qiu1, Haosheng Lin2,
Esko I. Kauppinen3, Shohei Chiashi1, Yutaka Matsuo2, Keigo Otsuka1, Shigeo Maruyama1
1

2

Department of Mechanical Engineering, The University of Tokyo, Tokyo 113-8656, Japan
Department of Chemical Systems Engineering, Nagoya University, Nagoya 464-8603, Japan3
Department of Applied Physics, Aalto University, Espoo 02150, Finland

Tandem solar cell is a photovoltaic device of using the transmitted light of a solar cell (topcell) to generate power in a different type of solar cell (bottom cell), which can overcome thetheoretical limit of a solar cell alone. Lee et al. fabricated tandem solar cells using single-walled
CNT film as the transparent electrode [1], and further optimization of the transmitted spectrum
for the tandem solar cell is required. Figure 1 shows a schematic of a perovskite solar cell as
the top cell, with CNT film as a transparent electrode. To improve transmittance, we first
calculated the relationship between the thickness of the hole transport layer (spiro-MeOTAD)
of the perovskite solar cell and the transmitted spectrum by using the e-ARC software [2]. As
shown in Fig. 2, the transmittance of the perovskite solar cell changes with the film thickness
by the interference of light, and the power conversion efficiency (PCE) of the bottom cell canbe accordingly optimized. However, if the film thickness of spiro-MeOTAD is made thinnerthan 150 nm, the PCE of the perovskite solar cell itself is expected to decrease, so we ran thecalculation for the thicker spiro-MeOTAD. In metal electrodes, the PCE decreases if spiroMeOTAD is thick [3]. In contrast, since the CNT electrode is in contact with the perovskite
layer as shown in Fig. 1, we expect the PCE to remain nearly the same even the spiro-MeOTAD
is thicker. In addition to the thickness of the spiro-MeOTAD, the transmitted spectrum can be
optimized by depositing the appropriate thickness of PMMA layer on the surface. This will not
only improve the PCE of the bottom cell, but also improve the durability [4]. The PCE of thebottom cell [5] was calculated as a function of spiro-MeOTAD and PMMA thickness (Fig. 3).
Simulated PCE using the model of the bottom cell was 22.6% under AM 1.5G. The calculationshows that the PCE of the bottom cell can be improved by the appropriate thickness
combination of spiro-MeOTAD and PMMA. The calculation indicates the possibility of
improving the efficiency and durability of tandem solar cells at the same time.

Fig. 1 Schematic of CNT electrode
perovskite solar cell (Top cell).

Fig. 3 Simulated PCE of bottom cell as afunction of spiro-MeOTAD and PMMA
thickness.
[1] C. Lee et al. Solar RRL 4.12 (2020). [2] A. Nakane et al. Journal of Applied Physics 120.6 (2016).
[3] I. Grill et al. ACS applied materials & interfaces 9.43 (2017).
[4] T. Sakaguchi et al. MRS Communications 8.3 (2018).
[5] H. Sai et al. Progress in Photovoltaics: Research and Applications 27.12 (2019).
Corresponding Author: S. Maruyama

Fig. 2 Simulated perovskite
solar cell transmitted spectra.

E-mail: maruyama@photon.t.u-tokyo.ac.jp59

1P-16Fabrication of Single-Walled Carbon Nanotubes Devices by Stacking
Nanomaterials○Shu Sato1, Satoru Matsushita1, Ryotaro Kaneda1, Keigo Otsuka1, Shigeo Maruyama1,
Shohei Chiashi1
1Department of Mechanical Engineering, The University of Tokyo, Tokyo 113-8656, Japan

Single-walled carbon nanotubes (SWCNTs) are nanomaterials that have highmechanical strength, flexibility, and high electrical conductivity, but their electrical and opticalproperties are known to vary greatly depending on the surrounding environment. Twodimensional materials such as hexagonal boron nitride (h-BN) and graphite are atomically thinand tough against bending, so applications to high-performance flexible devices are studied [1].
Heterostructures composed of these nanomaterials are expected to exhibit properties which are
not found in individual nanomaterials. For example, SWCNTs on h-BN have a higher current
carrying capacity than that on Si/SiO2 substrates [2]. In this study, we developed methods oftransferring and stacking nanomaterials with polymers and investigated the heterostructuredevices.
A flake of h-BN was transferred onto a back-gate made of platinum with polypropylene
carbonate (PPC) stamps [3], and then horizontally aligned SWCNTs synthesized on quartz
substrate were transferred onto the h-BN with polystyrene (PS) stamps. The fabricated device
was shown as Fig. 1(a). The G-band Raman mapping in Fig. 1(b) showed that SWCNTs weretransferred onto h-BN and their alignment was retained. The G-band intensity above the metal
back-gate were weaker than that on h-BN. The output and transfer characteristics of this device
were analyzed.
Graphite was transferred with polyvinyl chloride (PVC) film stamps and cut with apulsed laser to form two back-gates without using photoresist. Then, h-BN and SWCNTs weretransferred on the cut graphite with PS (shown as Fig. 1(c)), and the heterostructure ofgraphite/h-BN/SWCNT was successfully fabricated (Fig. 1(d)). In addition, the similar
heterostructures were also fabricated on plastic substrates. The transfer, cutting, and stacking
techniques were effective in fabricating heterostructures even on flexible substrates.
(a)

(b)

Drain SWCNTs Source
h-BN
Si/SiO2
Gate(Metal)Vg1 Vg2

Vg

Vg1

SWCNTs(c)Vg2electrode

Si/SiO2h-BN
Si/SiO2(d)

Drain SWCNTs Source
h-BN

20 μm

Gate
(Graphite)
Vg1 Vg2

Vg

h-BN

Graphite

SWCNTs10 μm

Fig. 1 (a) Schematic image and (b) optical microscope and G-band Raman mapping image of a heterostructuredevice of h-BN and SWCNTs transferred on a metal back-gate. (c) Schematic image and (b) optical microscopeand G-band Raman mapping image of a heterostructure device of h-BN and SWCNTs transferred on graphite cut
with a pulsed laser.
[1] Li Xiang, et al., Carbon, 161, 656 (2020).
[2] J. W. Huang, et al., Nano Lett., 15, 10, 6836 (2015).
[3] K. Kinoshita, et al., npj 2D Mater Appl, 3, 22 (2019).
Corresponding author : S. Chiashi
Tel/Fax: +81-3-5841-6408, E-mail: chiashi@photon.t.u-tokyo.ac.jp60

1P-17
Electrochemical stability of single-walled carbon
nanotube electrodes in aqueous electrolyte.
○Namuun Uuganbayar, Shinya Jindo, Yosuke Ishii, Shinji Kawasaki
Department of Life Science and Applied chemistry, Nagoya Institute of Technology,
Nagoya 466-8555, Japan㸦 b㸧m-SWCNT

㸦 c㸧
㸧 s-SWCNT

1.4 V

1.4 V

1.4 V

0.9 V

0.6 V

0V
1200100
1

1400 200

Intensity / arb. units㸦 a㸧RBM

Intensity / arb.
Intb. units

Intensity / arb. units

Since single-walled carbon nanotubes (SWCNTs) have excellent electrical conductivity andchemical stability, they are expected as good battery electrode materials. However, theirelectrochemical stability has not yet been fully understood. It is well known that SWCNTs havevarious tube diameters and exhibit diverse electronic states depending on their chirality.
Therefore, it is necessary to clarify the relationship between these properties and theelectrochemical stability of SWCNTs. In this study, we investigate the electrochemical stabilityof several SWCNTs with different tube diameters (SWCNT1.0, SWCNT1.5, and SWCNT2.5,
with average tube diameters of 1.0 nm, 1.5 nm, and 2.5 nm, respectively) under applied
potential in an aqueous electrolyte.
We found that ‫ ܫ‬ୋశ Ȁ‫ܫ‬ୈ decreased with the increase in applied potential for all the three
SWCNT samples. XPS measurements revealed that the fraction of O 1s increases withincreasing applied potential, suggesting that electrochemical oxidation is the cause of thedecrease of ‫ ܫ‬ୋశ Ȁ‫ܫ‬ୈ in the Raman spectra with increasing applied voltage.
Fig. 1 (a) shows the change in Radial Breathing Mode (RBM) of SWCNT1.0. As can be seenfrom Figure 1 (a), the peak on the high wavenumber side decreases. This indicates that
SWCNTs with smaller diameters are more reactive. On the other hand, Fig.1 (b) and (c) show
the change in G-band peak profile. Judging from Fig.1 (b) and (c), it is plausible that metallic
tubes are more reactive than semiconductive tubes.

0.9 V

0.6 V

1600

300 1800

−1

1200
1

0.6 V

0V

0V

Raman shift / cm 1

0.9 V

1400

1600

1800
−1

Raman shift / cm

1200

1400

1600

1800
−1

Raman shift / cm

Fig. 1 Raman spectra of SWCNT1.0. Hg/HgO reference electrode was used. (a) and (b) 532 nm laser, (c)633 nm laser were used as excitation source.
Corresponding Author: S. Kawasaki
E-mail: kawasaki.shinji@nitech.ac.jp61

1P-18Fabrication and characterization of horizontal arrays of
SWCNT-BNNT heteronanotubes○Satoru Matsushita1, Taiki Sugihara1, Guangyao Zhu1, Keigo Otsuka1, Taiki Inoue2,
Shohei Chiashi1, Shigeo Maruyama1
1

Department of Mechanical Engineering, The University of Tokyo, Tokyo 113-8656, Japan2
Department of Applied Physics, Osaka University, Osaka 565-0871, Japan

Carbon nanotube (CNT) arrays have been a promising candidate for transistor channels
that could outperform silicon counterparts. In practice, non-ideal CNT-insulator interfaces
lead to large subthreshold swing (SS), hysteresis, and threshold voltage variation. In twodimensional semiconductors, the encapsulation of channel materials between hexagonalboron nitride (BN) layers has reduced SS and hysteresis [1]. We expect CNTs to similarly
benefit from the co-axial coating with BN nanotubes (BNNTs) [2]. However, horizontal
arrays of such heteronanotubes, which are essential for practical devices, are difficult toprepare because elaborate air-suspended CNTs are required for the co-axial BNNT
growth. Here, we develop a procedure tosynthesize CNT@BNNT heteronanotube
arrays by utilizing two types of transfer
techniques towards the transistor applications.
As shown in Fig. 1(a), CNT arrays are grownon single-crystalline quartz substrates andtransferred over trenches via anthracene
crystals [3]. After synthesizing outer BNNTs bychemical vapor deposition [2], the heteronanotube arrays are transferred by apolystyrene-based stamping method onto
another substrate for device fabrication. The
Raman mapping image in Fig. 1(b) verifies thepresence of nanotubes in an array form. The
downshift of G-band suggests the coating of BN
layers on a CNT (Fig. 1(c)). The heteronanotubes are ~30-nm-thick with some inhomogeneity along their axes (Fig. 1(d)). We
will also discuss the selective etching of BNNTs[4] for the direct contact of inner CNTs andsource/drain metal while the remaining BNNTs
serve as gate dielectric layers in transistors.
[1] Q. A. Vu et al., 2D Mater. 5, 031001 (2018). [2] R. Xiang
et al., Science 367, 537 (2020). [3] K. Otsuka et al., Nat.
Commun. 12, 3138 (2020). [4] J. Son et al., Nat. Commun.
9, 3988 (2018).
Corresponding Author: S. Maruyama
Tel: +81-3-5841-6421, Fax: 03-5800-6983
E-mail: maruyama@photon.t.u-tokyo.ac.jp

62(a) Schematic for fabrication procedure ofheteronanotube arrays. (b) G-band
mapping image of a nanotube array. (c)Typical Raman spectra of SWCNT-BNNT
and SWCNT. (d) AFM image of a nanotube
array.

1P-19High-frequency characterization of carbon nanotube thin-film transistors
based on immersion deposition method○Shugo Kogure1, Saya Ishimaru1, Hiromichi Kataura2, and Yutaka Ohno1,3
1

2

Department of Electronics, Nagoya University, Nagoya 464-8603, Japan
Nanomaterials Research Institute, National Institute of Advanced Industrial Science andTechnology, Ibaraki 305-8565, Japan
3
Institute of Material and Systems for Sustainability, Nagoya University, Nagoya 464-8601,
Japan

A high-density film of isolated semiconducting carbon nanotubes (CNTs) is the key torealize high-performance device applications. Previously, we have developed a method to
obtain a high-density CNT thin film based on the immersion deposition technique to realize
CNT TFTs with a high on-current and on/off ratio. [1] In this study, we have investigated thehigh-frequency characteristics of the CNT TFTs by measuring S-parameters.
We fabricated bottom-gate CNT TFTs by the self-align process based on the back-side
exposure process on a polyethylene-naphthalate substrate (PEN) as shown in Fig. 1. [2] The
semiconducting CNT thin film was deposited by the immersion deposition method. First, thesurface of the Al2O3 gate insulator was modified by poly-L-lysine, and then a CNT thin film
was deposited by immersing the sample in a dispersion of semiconducting CNTs. Here, thesemiconducting CNTs separated by gel chromatography were dispersed in a phosphate buffer
solution (0.1 mol/l, pH 7.4) containing sodium dodecyl sulfate (0.1 wt%). The highfrequency S-parameters were measured by a vector network analyzer (Keysight, E5061B).
Figure 2 shows the current-gain cutoff frequencies (fT) and maximum oscillation
frequencies (fmax) evaluated from the S-parameters for various channel length (Lch) at VDS of-5 V and VGS of -3 V. fT and fmax of 60.1 and 42.3 MHz were respectively achieved for thedevice with Lch of 3 Pm. Since the channel length can be reached by precision printing
techniques, the results imply a possibility of realizing printed radio-frequency devices suchas RFIDs.
[1] S. Kogure et al., The 61st FNTG General Symposium, 1P-41 (2021).
[2] T. Kashima et al., DOI: 10.21203/rs.3.rs-68702/v1.

fmax (Hz)

100M

10M

Lch (Pm)
3
5
10
20
30
50

1M
1M

Fig. 1 Schematic device structure.

10M

fT (Hz)Fig. 2 fmax versus fT.

Corresponding Author: Yutaka Ohno, Phone: +81-52-789-5387, E-mail: yohno@nagoya-u.jp

63

100M

1P-20Design and fabrication of low-power flexible sensing circuits
based on carbon nanotube○Naohiro Mitsuzawa1, Taiga Kashima1, Hiromichi Kataura2, and Yutaka Ohno1,3
1

Department of Electronics, Nagoya University, Nagoya 464-8603, Japan

2Nanomaterials Research Institute, National Institute of Advanced Industrial Science andTechnology, Tsukuba 305-8565, Japan
3Institute of Material and Systems for Sustainability, Nagoya University, Nagoya 464-8601, Japan

Recent developments of CNT-based flexible electron devices [1] and energy harvesters [2]have shown great promise of a realization of self-powered wearable sensors. However, thepower generated by energy harvesters is generally small and unstable, and ultra-low power
sensing system with a robustness against the instability of power source is needed. In this study,
we aim to develop low-power flexible sensing circuits consisting of a small number of CNT
TFTs. We propose novel sensing circuits based on ring oscillators that are tolerant to thefluctuation of supply voltage.
Figure 1 shows schematic diagrams of the sensing circuits we proposed in this study. The
circuits consist of the ring oscillator in which a resistive sensor is inserted, and the oscillation
frequency can vary according to the resistance of the sensor. To compensate the variation in theoscillation frequency due to fluctuations of the supply voltage, the sensing circuits also have areference ring oscillator. Circuit #1 outputs the logical conjunction of two oscillation signals.
Circuit #2 outputs signals of the reference and sensing alternately by switching the signal passaccording to the clock signal. In the circuit design, we used the device model based on our
fabricated CNT TFTs. [1]Figure 2 shows the simulation results. In the case of Circuit #1, the reference (Vref) and sensor
signals (Vsen) oscillated at 150 and 1144 Hz, respectively. The output signal (Vout) was Vsen
modulated by Vref, showing the circuit operation as designed. The power consumption of thiscircuit was 0.31 PW. Similar operation was obtained for Circuit #2 with a power consumptionof 0.68 PW.
(b)
The designed circuits were (a)fabricated on a polyethylene
naphthalte (PEN) substrate,using semiconducting CNTs as
the channel of TFTs. The
inverters were configured with Fig. 1 Schematic circuit diagram of proposed sensor circuits.
a zero-VGS load. The fabricated (a) Circuit #1, (b) circuit #2.
(b)circuits were able to be (a)operated at a low supply
voltage of 3 V, and theirfundamental operations wereconfirmed.
[1] T. Kashima et al., DOI:
10.21203/rs.3.rs-68702/v1[2] M. Matsunaga et al., Nano
Energy 67, 104297 (2020).

Fig. 2 Simulated voltage waveforms of sensor circuits at VDD = 3 V.
(a) Circuit #1, (b) circuit #2.

Corresponding Author: Yutaka Ohno, Phone: +81-52-789-5387E-mail: yohno@nagoya-u.jp64

1P-21
Suppression of minority current in carbon nanotube thin-film transistors
by drain bias stress○Tomoki Hori1, Hiromichi Kataura2, Yutaka Ohno1,3
1

Department of Electronics, Nagoya University, Nagoya 464-8603, Japan
Nanomaterials Research Institute, National Institute of Advanced Industrial Science andTechnology, Tsukuba, Tsukuba 305-8565, Japan
3
Institute of Materials and Systems for Sustainability, Nagoya University, Nagoya 464-8601,
Japan
2

Complementary carbon nanotube thin-film transistors (CNT TFTs) are the key device torealize low-power flexible electronics. However, CNT TFTs often exhibit the minority current
at off state and so-called ambipolar characteristics, causing excess power consumption at staticstate in CMOS circuits. In this study, we report the suppression of the minority current byapplying drain bias stress. The fundamental idea is to form the positive trap charges in the gateinsulator and passivation layer in the vicinity of drain contact, so that, the electric field causing
minority carrier injection from the drain is relaxed.
The schematic structure of the flexible CNT-TFT is shown in Figure 1. The gate insulator
and passivation layer of Al2O3 were formed by atomic layer deposition. Due to fixed charges in
the passivation layer, the carrier type was converted from positive to negative as shown by
dotted curve in Fig. 2. [1,2] However, the large minority (hole) current was observed at thenegative VGS region. The hole conduction was suppressed by applying a large drain-gate voltageof 6 V for 9 min as shown by solid curve. This can be explained by an accumulation of positive
charges jumped in the gate insulator by the high field at the drain end. The positive charges
built up at the drain end may increase the potential and prevent the hole injection from the drain
at off state. The threshold voltage was also shifted in the negative direction, implying a
possibility of tuning the threshold voltage by independently applying gate bias stress.

Fig. 1 Schematic structure of CNT-TFT.

Fig. 2 Transfer characteristics before and after drain
bias stress at VDS = 0.2 V.

[1] N. Moriyama et al. Nanotechnol. 21, 165201 (2010).
[2] T. Hori et al. Int. Conf. on Materials and Systems for Sustainability 2021, 1181 (2021).
Corresponding Author: Y. Ohno, Phone: +81-52-789-5387, E-mail: yohno@nagoya-u.jp65

1P-22           
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1P-24
Boron-assisted CVD growth of multilayer h-BN
and application to heterostructures with MoS2
Toru Otake1, Satoru Fukamachi2, Kenji Kawahara2, and Hiroki Ago1,2,*
1Interdisciplinary Graduate School of Engineering Sciences, Kyushu University, Fukuoka,
816-8680, Japan, 2 Global Innovation Center (GIC), Kyushu University, Fukuoka, 816-8680,
Japan
Multilayer hexagonal boron nitride (h-BN) is a key material to unveil the intrinsic andunique physical properties of various 2D materials by protecting their surfaces fromenvironmental disturbance. Although monolayer h-BN can be widely synthesized by catalytic
CVD, there is no reliable methods to synthesize high-quality multilayer h-BN due to difficultyof growing uniform multilayers. We previously reported the CVD growth of multilayer h-BNusing Fe-Ni alloy thin films [1,2], but the h-BN thickness (2-3 nm) was not enough to screen
the influences from the environment. Here, we demonstrate that the addition of elemental
boron (B) in the catalytic CVD increases the h-BN thickness up to 4-5 nm while keeping the
thickness uniformity. Moreover, these h-BN multilayers were stacked with CVD-grownmonolayer MoS2, dramatically increasing the PL intensity of the MoS2.
Figure 1a shows an optical microscope image of multilayer h-BN grown on a Fe-Ni foil
under our standard growth condition. The h-BN was inhomogeneous and contained several
very thick flakes with thickness over 100 nm. We have previously reported that decreasing
the cooling rate improves the h-BN film uniformity [1]. However, for very slow cooling rates,
almost no h-BN was found on the Fe-Ni foil (Figure 1b), probably because both B and N atoms
remain inside the foil and the slow segregation induces the etching of growing h-BN. Here,
we found that pre-deposition of a B film on the Fe-Ni foil increases the h-BN thickness evenafter the slow cooling process, as shown in Figure 1c. Such effect was not observed when
flowing N2 gas, so that we speculate that there is a deficiency of B atoms in the Fe-Ni foil during
the CVD growth. The TEM (Figure 1d) and AFM measurements indicated that the h-BN hasa thickness of 4-5 nm. In the Symposium, we also present the significant enhancement of the
PL emission from MoS2 monolayers integrated with our CVD-grown h-BN multilayers.

Figure 1. Optical images of transferred h-BN grown under the normal condition (a), the slow coolingcondition (b), and the  cooling condition with a pre-deposited B layer (c). (d) Cross-sectional TEM
image of the sample shown in (c).
References: [1] Y. Uchida et al., ACS Nano, 12, 6236 (2018). [2] Y. Uchida et al., ACS Appl. Electron.
Mater., 2, 3270 (2020).

68

1P-25Layer by layer sulfurization of WSe2 toward formation of Janus WSeS
○X. He, S. Aoki, Y. Iwamoto, T. Kaneko, and T. Kato
Graduate School of Engineering, Tohoku University, Sendai 980-8579, Japan
Since the discovery of graphene, 2D materials with various properties have received
increasing attention in the fields of novel electronic, optical, spintronic and valleytronic devices.
As important derivatives of 2D materials, Janus 2D materials, such as Janus transition metal
dichalcogenides (TMDs), were first discovered in 2017 and have attracted much attention due
to their unique structural electrical properties [1]. Janus TMD with mirror asymmetry can obtaincarrier confinement and window effects by connecting different TMDs in-plane and out-ofplane, and also Rashba effect and normal piezoelectric polarization, which is expected to be
applied in quantum devices, optical devices, sensors, actuators, and other electromechanicaldevices (Fig. 1(a)) [2]. In spite of the potential abilities of Janus TMD, the number of papers
reported about the Janus TMD formation is very limited, denoting synthesis of Janus TMD isstill within the early stage. Further understanding of reaction mechanism is important to realize
controllable formation of high-quality Janus TMD.
In this study, detailed mechanisms of sulfurization were investigated through the thermal
reaction of mechanically exfoliated WSe2 toward Janus WSeS formation (Fig. 1(b)). It is foundthat by controlling substrate temperature, reaction time, and sulfur heater temperature, drasticchanges of WSe2 to WS2 are found, which happened within 15 sec. When the flux of sulfur isreduced by decreasing the sulfur heater temperature, the reactions are slow down andcontrollable sulfurization are realized. Initially only the outermost layer is replaced by S. After
that, sulfur invades the second and subsequent layers, and finally all Se is replaced by S.
These are important information for the controllable formation of high-quality Janus TMD.

Figure 1: (a) Structure diagram of TMD and Janus TMD. (b) Optical microscope image of few
layer WSe2 used in this study.

[1] A. Y. Luet al., Nature Nanotechnol., 12, 744–749 (2017).
[2] R. Li, Y. Cheng, and W. Huang, Small, 14, 1802091-1–11 (2018).
Corresponding Author: Toshiaki Kato
Tel: +81-22-795-7046, Fax: +81-22-263-9225, E-mail: kato12@ tohoku.ac.jp69

1P-26
       
    
○Kenta Kusakabe1, Yuta Fujisaki1, Taiki Inoue2, Shigeo Maruyama1, Shohei Chiashi1
1Department of Mechanical Engineering, the University of Tokyo, Tokyo 113-8654, Japan2
Department of Applied Physics, Osaka University, Osaka 565-0871, Japan

Graphene is a nanomaterial with excellent
thermal and electrical properties, and there aresome ways to produce it. Among them, CVD
synthesis is one of the methods to produce highquality and large-area graphene at an acceptable
cost [1]. The synthesis of graphene on metal
catalysts has been widely studied, but there are few
studies on catalyst-free synthesis [2], which is lessprone to impurities and have application
advantages such as no need for cleaning or otherprocessing. In this study, we report the CVD
synthesis of graphene on non-catalytic substrates
such as graphite, h-BN, and sapphire.
Mechanically-exfoliated graphite, exfoliated hBN, and a sapphire substrate (A-face) were placedin an electric furnace and CVD synthesis was
conducted with controlling the pressure,temperature, and flow rates of acetylene, argon,
and hydrogen (Figs. 1-3). In Fig. 1 and 2,
hexagonal-shaped graphene pads were observed,
suggesting that graphene on graphite and h-BN
was of high quality. Figure 3 shows the SEM
image and Fig. 4 shows the Raman spectrum ofgraphene directly-synthesized on sapphire. The
2D/G intensity ratio is 2.6, suggesting that thematerial is monolayer graphene [3]. The
reticulated patterns in the SEM image were
wrinkles of graphene, which may be caused by thedifference in thermal expansion between grapheneand sapphire during the temperature reduction
process after synthesis [4,5].
[1]
[2]
[3]
[4]
[5]

Fig. 1 SEM image of graphene on h-BN.

Fig. 2 AFM image of graphene on graphite.

Fig. 3 SEM image of graphene on sapphire.

K.S. Novoselov et al. Nature, 490, 192 (2012).
S. Tang et al. Carbon, 50, 321 (2012)
Y. Hao et al. Small, 6, 195 (2010).
D. Yoom et al. Nano Lett., 11, 3227 (2011).
N. Mishra et al. Small, 15, 1904906 (2019).

Corresponding Author: S. Chiashi
Tel: +81-3-5841-6407, Fax: +81-3-5841-6408,
E-mail: chiashi@photon.t.u-tokyo.ac.jp

Fig. 4 Raman spectra at one
point of graphene on sapphire.

70

1P-27
Electronic structure and transport properties of multilayer Nb-doped MoS2
○ Shota Yamaguchi1, Ryosuke Mizuno2, Hiroyuki Mogi2, Hong En Lim1,
Takahiko Endo1, Yusuke Nakanishi1, Kazuhiro Yanagi1, Kosuke Nagashio3,
Shoji Yoshida2, Hidemi Shigekawa2, Yasumitsu Miyata1
1

Department of Physics, Tokyo Metropolitan University, Hachioji 192-0397, Japan
Faculty of Pure and Applied Sciences, University of Tsukuba, Tsukuba 305-8573, Japan3
Department of Materials Engineering, The University of Tokyo, Tokyo 113-8656, Japan
2

In recent years, transition metal dichalcogenides (TMDCs) have drawn significant attention
because of their atomically-thin layered structures and superior electronic properties. In somedevice applications, it is frequently required to use degenerate semiconductors with high carrier
density. For such application, previously reported studies have employed multilayer Nb-doped
MoS2, which has a high hole density of approximately 1019 cm-3 [1,2]. However, their electronic
structure has not been investigated in detail. In this study, we have characterized the multilayer
Nb-doped MoS2 by using scanning tunneling spectroscopy (STS) and transport measurements.
The results are compared to those of chemical vapor deposition (CVD) grown monolayer MoS2
for reference.
The multilayer Nb-doped MoS2 flakes were prepared on SiO2/Si substrates by mechanicalexfoliation, and In/Au electrodes were deposited to fabricate field-effect transistors (FETs). As
shown in Fig. 1a, it shows a p-type behavior with weak gate voltage dependence. The CVDgrown monolayer MoS2, on the other hand, is an n-type semiconductor that exhibits strong gate
dependence. Using this combination, a PN junction was fabricated. The vertical heterostructureof these p- and n-type MoS2 shows a rectification property as expected (Fig. 1b). Meanwhile,
the STS measurements reveal that dI/dV curves of the Nb-doped and CVD-grown MoS2 arealmost identical with the Fermi levels located within each respective bandgap (Fig.1c). These
results suggest that the carrier density of the surface Nb-doped MoS2 is much different fromthat of bulk ones.

Figure 1 (a) ID–VG curves of the FETs fabricated using the Nb-doped multilayer MoS2 and the CVD-grownmonolayer MoS2. (b) ID–VG curves of Nb-doped MoS2/CVD-MoS2 vertical heterostructure at different gate
voltages. (c) dI/dV curves of the Nb-doped multilayer MoS2 and the CVD-grown monolayer MoS2.
[1] J. Suh et al. Nano Lett. 14, 6976-6982 (2014).
[2] K. Nakamura et al. ACS Appl. Mater. Interfaces, 12, 51598–51606 (2020).
Corresponding Author: Y. Miyata, Tel: +81-042-677-2508, E-mail: miyata-yasumitsu@tmu.ac.jp

71




1P-28




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72

1P-29Introducing lattice vacancies as adsorption sites in monolayer MoS2
○Yangzhou Zhao1, Hiroki Yokota2, Haruna Ichikawa2, Yasushi Ishiguro2, Kazuyuki Takai1,2
1Graduate School of Science and Engineering, Hosei University, Tokyo 184-8584, Japan
Dept. of Chemical Science and Technology, Hosei University, Tokyo 184-8584, Japan2

In view of verifying the influence by lattice vacancies on the structure and electronic
properties, the monolayer MoS2 sample is irradiated with low energy Ar+ ion beam in order tointroduce vacancies under a well-controlled condition, and evaluated by Raman spectroscopy,
photoluminescence (PL) and electrical conductivity measurement.
After Ar+ beam irradiation, both of the line widths of E2g and A1g peaks in the Raman spectra
become broad as increasing of irradiation dose which is experimentally controlled by theirradiation time of the beam. The observed increase of the line width is attributed mainly to theincrease of the satellite peaks’ contribution caused by the introduction of lattice vacancies [1].
Interestingly, the effect of the irradiation is more significant for E2g in spite of less influence of
charge transfer by molecular adsorption, where A1g peak is much more sensitive due to its large
electron-phonon coupling [2][3].
As for electrical conductivity澿 the FET measurements indicate that only the Ar gas
introduction does not affect the electrical transport properties of MoS2-FET. However, thethreshold voltage for MoS2-FET shifts to the negative side after Ar+ beam irradiation, withminor mobility decrease. However, positive shift appears upon the irradiation time, suggesting
the hole doping during the Ar+ ion irradiation. This might be explained by charge transfer fromterminating oxygen atoms of introduced defects originating from the residue oxygen gas in themeasurement vacuum chamber.



Fig.2 FET-conductivity for monolayer MoS2
irradiated with Ar+ ion beam at dosage
from 0 to 3.7×1013 cm-2.

Fig.1 Dosage dependence of Raman peak position
for E2g and A1g of monolayer MoS2 irradiatedwith Ar+ ion beam.

[1] Soungmin Bae et al., Phys. Rev. App., 7, 024001(2017).
[2] B. Chakraborty et al., Phys. Rev. B, 85, 161403(2012).
[3] N. Kodama et al. FNTG(2018).
Corresponding Author: Kazuyuki Takai
E-mail: takai@hosei.ac.jp73

1P-30
Polarized Raman spectroscopy in layered WTe2
○Hirofumi Nema, Yasuhiro Fujii, Shogo Saito, Eiichi Oishi, Akitoshi Koreeda
Department of Physical Sciences, Ritsumeikan University, Shiga 525-8577, Japan

Layered materials such as graphite and transition metal dichalcogenides (TMDCs) are
expected for use in valleytronics and optoelectronics [1,2]. WTe2 belongs to TMDCs andattracts much attention due to its huge positive magnetic resistance [3] and pressure-induced
superconductivity [4,5]. However, the unconventional behavior of a Raman peak in WTe2 is not
fully understood in a previous study [6]. Therefore, additional measurements are necessary to
improve our understanding of the behavior.
In this study, we report polarized Raman spectroscopy of bulk WTe2. Figure 1 (a) shows theobtained spectra for the HH configuration. In the spectra, 7 peaks (P1-P7) were observed, asreported in the previous study [6]. In addition, an unreported peak (P0) was observed at around
9 cm-1 (Fig. 1 (b)). Judging from the results of the first-principles calculations [6], the peakcorresponds to A1 mode. We will discuss the detailed results of polarization dependence during
the poster presentation.

Fig. 1 Raman spectra of WTe2 at around (a) P1-P7, and (b) P0. R(L) represents
the right(left)-handed polarized light.
[1] H. Schomerus, Phys. Rev. B 82, 165409 (2010).
[2] Q. Wang et al., Nat. Nanotechnol. 7, 699 (2012).
[3] M. N. Ali et al., Nature 514, 205 (2014).
[4] D. Kan et al., Nat. Commun. 6, 7804 (2015).
[5] X. Pan et al., Nat. Commun. 6, 7805 (2015).
[6] W.-D. Kong et al., Appl. Phys. Lett. 106, 081906 (2015).
Corresponding Author: H. Nema
Tel: +81-77-561-5752, Fax: +81-77-561-5752,
E-mail: h-nema@fc.ritsumei.ac.jp74

1P-31
Negative circularly polarization of moiré exciton luminescencein WSe2/MoSe2 heterobilayers
8 $.0& #$)*&$/0)+ $ $)* )%$/) &.#$)$"0#$ )50)-$/.0

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PL intensity (a. u.)/*($''4 /#$) /-).$/$*) ( /' $#'*" )$ .  . $. ) $ ' /2*$( ).$*)'.4./ ( ) +*.. .. . $)/-$"0$)" *+/$' +-*+ -/$ . - '/  /* 1'' 4  "- . *! !- *( ) -'.# / -*./-0/0- .*(+*. *! .- !.$)/$)"+'/!*-(/* )"$) -/# *+/$''4 " ) -/  3$/*)$ +-*+ -/$ . /#-*0"# (*$-6 +// -). /*2-. )*1 ' ,0)/0(+# )*( )# (*$-6+// -).+ -$*$/-++*/ )/$')"$1 -$. /*.+/$''4*- - ). (' . *! /#  5 -*$( ).$*)' 3$/*) (*$-6 3$/*) 2#$# *!! -. /#  +*..$$'$/4 !*- ). *# - )/,0)/0( ($// -.),0)/0(.$(0'/$*)*!()4*4+#4.$.    - 2 ./0$ /# )*1 '(*$-6 3$/*)+-*+ -/$ .$)/2$./  * # / -*$'4 -.  *) $-0'-'4 +*'-$5  +#*/*'0($) . )   .+ /-*.*+4 $"0-   .#*2. /# $-0'-'4+*'-$5 .+ /-0) -, 3$//$*)2$/#$!! - )/ 3$//$*)+*2 -*)$/$*).
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1 kW/cm[1] K. Shinokita et al., Adv. Funct. Mater. 29, 190260(2019).
[2] K. Seyler et al, Nature 66, 567 (2019).
[3] K. Shinokita et al., Nano Lett. 21, 5938 (2021).
"$$%#"!!'&"$ !"&     (        %!"&%'$)"&"'#

0
1.28

1.30

1.32 1.34
Energy (eV)

1.36



Fig.                       75

1P-32
Battery electrode properties of HB sheets○Marina Ukai, Shinya Jindo, Yosuke Ishii, Shinji Kawasaki
Department of Life Science and Applied Chemistry, Nagoya Institute of Technology,
Nagoya 466-8555, Japan

Currently, lithium-ion batteries (LIBs) are used in a variety of products such as smartphones
and electric vehicles, and the global demand for LIBs is increasing. In LIBs, graphite, whose
theoretical capacity is 372 mAh/g, is used as anode electrode materials. Commercially available
LIBs charge the graphite anode up to almost the theoretical limit. Therefore, in order to increase
the energy density of LIBs, we have to explore new anode materials. Recently, it was predictedby a theoretical study that hydrogen boride (HB) can work as a high capacity (862 mAh/g)
anode of LIBs. However, experimental measurements of its electrochemical behavior have notbeen made yet. Therefore, we conducted an experimental study to verify the theoretically
predicted properties by actually synthesizing HB sheets and using them as LIB electrodes.
HB sheets were produced by exfoliation and ion exchange of MgB2 at room temperature andatmospheric pressure. The successful synthesis of HB sheets was confirmed by X-ray
photoelectron spectroscopy (XPS), X-ray diffraction (XRD), and soft X-ray emission
spectroscopy (SXES). Mg signal was not detected from the HB sheets by XPS. This result
indicates that ion exchange from MgB2 to HB was carried out completely. We confirmed bytransmission electron microscopy (TEM) that the obtained HB sheets were well dispersed andexists as a thin film.
Fig. 1 shows the observed charge-discharge curves of the HB sheet. As shown in Fig. 1, thereversible capacity of the HB sheet is about 75 mAh/g, which is much less than the predictedvalue 862 mAh/g. We’ll discuss Li ion storage property of the HB sheet in more detail in the
symposium.

+

Potential / V (vs. Li/Li )

3

2

1

0
0

Capacity / mAh g

−1

100

Fig. 1 Charge-discharge curves of HB sheet electrode measured with constant current of 25 mA/g.
Corresponding Author: S. Kawasaki
E-mail: Kawasaki.shinji@nitech.ac.jp76

1P-33
Photovoltaic Effect in MoS2/hBN HeterostructureżShaochun Zhang1, Mengsong Xue1, Ryo Kitaura1
1

Department of Chemistry, Nagoya University, Nagoya 464-8602, Japan

The photovoltaic effect is an essential process to convert light to electricity. In addition
to the pn junction-based photovoltaic effect, which has been utilized in solar cells, anotherphotovoltaic effect (BPVE), the bulk photovoltaic effect [1], has recently attracted attention.
BPVE arises not from band bending but from the shift of electron could in real space uponlight excitation. Recently, low-dimensional materials, including WS2 nanotubes [2] andvdW heterostructures [3], have proven to show BPVE.
In this work, we have exploredvarious two-dimensional-based vdW
heterostructures,
MoS2/hBN

includingheterostructures,

andobserved non-zero photocurrent atzero bias voltage. Figure1 shows theroomtemperature

photo-current

mapping image by scanning the laser
spot across the device. A typical shortcircuit current under zero bias wasdozensnanoamperes,

and

the

current-voltage (I-V) curves show

Fig.1 Photo-current mapping for hBN-MoS2 device

linear relationship. Laser-power dependence of the photocurrent were also measured,
which show the characteristic crossover from linear to square-root dependence. In thepresentation, we will discuss more details about the photovoltaic effect in our devices.

[1] Ashley M. Cook et al. Nat. Commun. 8, 14176 (2017).
[2] Y.J.Zhang et al. Nature 579, 349 (2019)[3] Akamatsu et al. Science 372, 68 (2021)

Corresponding Author: Ryo Kitaura
Tel: +8152-789-2477, Fax: +81-52-747-6442
E-mail: r.kitaura@nagoya-u.jp77

1P-34
Machine learning determination of the twist angle of bilayer graphene byRaman spectroscopy○Pablo Solís-Fernández1, Hiroki Ago1,2
1

2

Global Innovation Center (GIC), Kyushu University, Fukuoka 816-8580, Japan
Graduate School of Engineering Science, Kyushu University, Fukuoka 816-8580, Japan

Recent findings on the properties of twisted bilayer graphene (tBLG), specially thediscovering of superconductive states at low twist angles [1], have sparked an increased interestin twisted 2D materials. The ability to synthesize BLG by CVD with some control of the twist
angle has also improved in recent years [2]. It is thus necessary to find fast, reliable, and nondestructive methods to precisely determine the twist angle of tBLG. Given the large amount of
information encoded in the Raman spectrum of tBLG, Raman spectroscopy can provide suchmethod. However, changes in the Raman spectra induced by the twist angle can be very subtle,
thus making the angle identification tedious. Here, we propose the use of machine learning(ML) analysis techniques for the automated classification of the Raman spectrum of tBLG into
a selected range of twist angles [3]. Distinctive features of the Raman spectrum of a tBLG
sample are extracted and provided to a pretrained ML model that can then predict the twist
angle of the sample (Figure 1). The proposed ML classification is low computationallydemanding, providing fast and accurate results with ~99 % of agreement with the manual
labelling of the spectra. Given the ubiquitous nature of the Raman signal in 2D materials, thismethod can be expanded to determine the twist angle of other 2D heterostructures, or to evaluate
different properties, such as the levels of doping and strain. The flexibility and non-invasivenature of the Raman measurements, paired with the predictive accuracy of the ML, is expected
to facilitate the exploration of the emerging research field of twisted van der Waals
heterostructures.

Fig. 1 Schematic of the ML process to determine the twist angle of BLG.
[1] Y. Cao et al., Nature, 556, 43 (2018).
[2] P. Solís-Fernández et al., ACS Nano, 14, 6834 (2020).
[3] P. Solís-Fernández et al., ACS Appl. Nano Mat., accepted, doi:10.1021/acsanm.1c03928 (2022).
Corresponding Author: P. Solís-Fernández
Tel: +81-92-583-8975, Fax: +81-92-583-8975
E-mail: ps-fernandez@gic.kyushu-u.ac.jp78

1P-35
Hierarchic Aggregation of Elementary Diamond Nanoparticles:
Its Tolerance under Various Conditions○ Tomoya Yoshihara1, Masaya Nemoto1, Toshihiko Tanaka1, Tetsuya Aoyama2,
Yasuhiro F. Miura3, Eiji Osawa4
1

Department of Chemistry and Biochemistry, National Institute of Technology,
Fukushima College, 30 Aza-nagao, Tairakamiarakawa, Iwaki, Fukushima, 970-8034, Japan2
Ultrahigh Precision Optics Tech. Team, RIKEN RAP, 2-1 Hirosawa, Wako, Saitama, Japan
3
Hamamatsu University School of Medicine, 1-20-1 Handayama,
Higashi-ku, Hamamatsu City, Shizuoka, Japan
4
Nano Carbon Research Institute Ltd., Asama Research Extension Center,
Shinshu University, 3-15-1 Tokida, Ueda, Nagano, Japan

Scattering Intensity/d 3

Elementary diamond nanoparticles (EDIANs) are aggregated by trace ions in their aqueous
colloidal solutions and salt out at only ~10-3 M of salt.1 We consider that such sensitivity
demonstrates a unique physical insight of them. Protein molecules also have similar sizes inwater and never salt out at such a low concentration. We believe that not only their surfacefunctional groups (-NH-, COOH, etc.) but also their intrinsic strong electric polarization2
should be considered.
We have presented herein their hierarchic aggregation in aqueous solutions. We diluted
nanodiamond (ND) solutions  NanoAmando@, NanoCarbon Research Institute Ltd.,
containing EDIANsfrom 2.5 with ultrapure water and measured their size distribution
spectra by using the novel analysis method where Rayleigh scattering are concerned in DLS.
Usually, commercial DLS spectrometers calculate the spectra according to Mie scattering;and under 100 nm, we have to calculate them rather according to Rayleigh scattering. Diluting
aggregation4 took place and in the mid region from 0.1 to 1 % of ND, EDIANs and theiraggregates are mixed as shown in Fig.1 .
EDIANS
Their aggregation is hierarchic: they
aggregate discontinuously from EDIANs
to 1st aggregates and then further jump to
2nd aggregates except small aggregatessuch as dimers which sometimes
contaminate EDIANs. These aggregates
1st Aggregateswere scarcely observed in two blank zones
2nd Aggregates[(1) 10-15 nm, (2) 30-50 nm, on various
conditions (temperature, salt, etc.). Why
are the two blanks there? Perhaps theird:diameter (nm)aggregates would not be stable if theyshould be formed. We will discuss a few Figure 1. A size3 distribution spectrum [scattering
calculated
from
a
DLS
models of the hierarchic aggregation with intensity/(diameter)
measurement] of a 0.25% NanoAmando aquaous
respect to the similarity of EDIANs both solution.
in size and shape.
[1] Nemoto, et al., FNTG 60th Abstract Book (2021); [2] A. S. Barnard, E. Osawa; Nanoscale 6, 1188 (2014); [3]Technical Report No.2, NanoCarbon Research Institute Ltd.2007; [4] N.O. Mchedlov-Petrossyan, N. N.
Kamneva, A. I. Marynin, A. P. Kryshtal, E. Osawa, Phys. Chem. Chem. Phys., 17, 16186 (2015).
Corresponding Author:Toshihiko Tanaka / Tel: +81-246-46-0810 / E-mail: ttanaka@fukushima-nct.ac.jp791P-36
Synthesis of Hetero Transition Metal Dichalcogenide Nanotubes○Mai Nagano1, Yohei Yomogida1, Md. Ashiqur Rahman1,2, Yusuke Nakanishi1,
Yasumitu Miyata1, Kazuhiro Yanagi1
1Department of Physics, Tokyo Metropolitan University, Hachioji, Tokyo 192-0372, Japan
2 Department of Physics, Comilla University, Cumilla-3506, Bangladesh

One-dimensional van der Waals heterostructure, especially coaxially stacked heteronanotubes, have attracted much attention because of their unique physical properties [1]. Novelsynthesis schemes of hetero structured nanotubes like hexagonal boron nitride (BN)/carbon
nanotubes and transition metal dichalcogenide (TMDC) /carbon nanotubes have beendeveloped through the formation of BN or TMDC layers on the surface of carbon or BN
nanotubes [1, 2]. These results suggest that the nanotubes can work as templates for formationof another nanotubes. Semiconducting TMDC nanotubes, which are discovered by Tenne et al[3], are one of the inorganic nanotubes. They exhibit semiconducting characteristics regardless
how they are rolled. Therefore, for the formation of 1D hetero
semiconductor interfaces in hetero-structured nanotubes, hetero
structured TMDC nanotubes is the most appropriate. In thisstudy, we tried to synthesize semiconducting hetero-nanotubes
consisting only of semiconducting TMDCs nanotubes.
We used WS2-nanotubes as a template for formation of MoS2
nanotubes. First, we prepared WS2 nanotubes through thesulfurization of the tungsten oxide nanowires, which wereobtained by solvothermal synthesis [4]. We employed formationof outer-layer nanotubes through the deposition of transition
metals and their sulfurization approach, which was reported in Fig.1 Raman spectra of before
the study on two-dimensional TMDCs [5]. In this study, the and after 2nd sulfurization. ‫ۃ‬molybdenum was deposited on the surfaces of the synthesized and ▼ show the Raman peaks
WS2 nanotubes and reacted with sulfur for 10 min in Ar flow to of
and
MoS2,
WS2
synthesize WS2/MoS2 hetero-nanotubes.
respectively.
a)b)Fig. 1 shows the Raman spectra of samples
before and after 2nd sulfurization. After 2nd
sulfurization, we observed two Raman peaksof MoS2 and WS2. Fig. 2 shows transmission
electron microscopy (TEM) image ofsamples. Comparing the two pictures, weobserved the formation of multilayered MoS2
around WS2 nanotubes (Fig. 2b). These
Fig.2 TEM image of samples. (a) Before 2nd
results indicate the successful synthesis ofsulfurization. (b) After 2nd sulfurization.
hetero-nanotubes consisting only ofsemiconductor TMDCs.
References: [1] R. Xiang et al. Science, 367, 537 (2020). [2] M. Liu et al., ACS Nano 15, 8418 (2021), [3] R.
Tenne et al., Nature 360 444 (1992), [4] Y. Yomgida et al., Appl. Phys. Exp. 12, 085001 (2019), [5] C-R. Wu et al.
Nano Lett., 16, 7093 (2016).
Corresponding to Yohei Yomogida (yomogida@tmu.ac.jp) & Kazuhiro Yanagi (yanagi-kazuhiro@tmu.ac.jp)80

1P-37
Low temperature chemical modification of Nanodiamondand its effects on structure and magnetism○Takuma Tsuji 1, and Kazuyuki Takai1,2

1Graduate School of Science and Engineering, Hosei University, Tokyo 184-8584, Japan

2

Research Center for Micro-Nano Technology, Hosei University, Tokyo 184-0003, Japan

Surface chemical modification of Nanodiamond (ND) covered with graphene layers is an
important strategy to tune its electronic / chemical properties owing to its large specific surface
area. Especially, oxidation and hydrogenation introduce the large electric polarization on thesurface of ND, which could change electric screening of excitons in the photo absorption,
carrier density, hydrophilicity and so on. The surface modifications of ND has been generally
carried out by chemical reactions at high temperature in the gas phase. However, effects on the
core-diamond structure are suggested in the high temperature reactions [1]. In this study, theoxidation and hydrogenation of ND were carried out at low temperature in the liquid phase andtheir effects are evaluated in terms of structure and magnetism.
NDs repeatedly oxidized three times using the Brodie method [2] and hydrogenated by
Lithium Aluminum Hydride (LAH) in anhydrous THF solvent [3], are labeled as BND3, HNDL, respectively. The core-diamond structure and magnetism of ND were investigated measured
by XRD (smartLab, Rigaku), and SQUID magnetometer (MPMS-XL, Quantum Design),
respectively.
As shown in Fig. 1, the peak position, intensity, and full width at half maximum do not change
from those in pristine ND in the oxidized and hydrogenated NDs, confirmed that the
crystallinity of the core-diamond structure is maintained in the surface chemical treatments
under low temperature liquid phase conditions. In addition, no crystalline impurities were foundto be introduced by the synthesis processes. The magnetization curves at 2 K shown in Fig. 2
exhibit increasing in the magnetization with the surface modifications. The observed
enhancement in the magnetization upon the oxidation is attributed to the increase in theparamagnetic components due to the modification of the topology in the graphene layer on thesurface of ND [4]. Although the contributions of amorphous impurities undetectable by XRD
in the synthesized process should be examined, the increase in magnetization duringhydrogenation would be also attributed to the same reason as that for the oxidation.
The surface chemical modifications under low temperature liquid phase conditions which did
not affect the core-diamond structure of ND are promising methods to control the electronic
properties of NDs such as the magnetism.
[1] X. Xu, Z. Yu, Particuology, 10, 339-344, (2012). [2] M. R. Karim, et. al, J.Phys.Chem. C 120, 21976, (2016).
[3] A. Ambrosi, et al., Chem mater, 24, 2292-2298, (2016). [4] K. Tajima, et al., Polyhedron, 136, 155, (2017).

Magnetization(emu/g)Intensity (arb unit)

0.4
HND-L
BND3
ND
10

55

ND
BND3
HND-L

0.2

0

100

0

2θ ()
Fig. 1 XRD profiles of NDs

5000
10000
Magnetic field (Oe)Fig. 2 Magnetization curves to NDs at 2K

81

1P-38Synthesis and Extraction of Carbon-Encapsulated Iron Carbide
Nanoparticles for Perovskite Solar Cell Application
Jiye Han1,2, Kyusun Kim1, Il Jeon1,2
1

Department of Nano Engineering, SKKU Advanced Institute of Nanotechnology (SAINT),
Sungkyunkwan University (SKKU), Suwon 16419, Republic of Korea
2
Department of Nano Fusion Technology, Pusan National University, Busan 46241, Republicof KoreaIn this study, an effective method for obtaining large amounts of metal nanoparticles
encapsulated by carbon layers using aerosol-assisted chemical vapour deposition was
introduced [1-3]. By optimizing the conditions, iron carbide nanoparticles with sizes ranging
from 5 nm to 100 nm were produced along with carbon nanotubes. Smaller nanoparticles withdiameters of less than 20 μm were then extracted from the carbon assortments throughsonication, centrifugation, and filtration. The nanoparticles exhibit a tendency to aggregate overtime owing to the π–π interaction between the graphitic carbon shells surrounding the ironcarbides. The aggregation of the metal ion nanoparticles was controlled to maximise the lightabsorption by the gap-surface plasmon effect in PSCs. Application of the metal nanoparticles
to the devices increased the PCE from 19.71% to 21.15%. The improvement is attributed to theincreases in all three major photovoltaic parameters, namely, JSC, VOC, and the fill factor (FF).
Both the JSC trend over the nanoparticle aggregation time and the computational study showthat the plasmonic effect accounts for the high JSC [4,5]. Meanwhile, high VOC and FF are
ascribed to the improved charge transport due to the presence of the nanoparticles, which we
postulate the high electron affinity and host–guest interaction within the nanoparticles to haveinduced favourable effects. The carbon-encapsulated metal nanoparticle-added solar cells
exhibited a high device stability analogue to the control devices, confirming that metal ion
migration does not occur owing to the protection by the carbon shell.
[1] A.G. Nasibuli et al. ACS Nano, 5 (2011).
[2] C.T. Wirth, et al.    ,  (20).
[3] B. McLean, et al. J. Appl. Phys., 129 (2021).
[4] V.L. Dalal, et al.  , 50(1979).
[5] T. Liu, et al. Energy Environ. Sci., 50 (2020).
Corresponding Author: I. Jeon
Tel: +82-31-299-4187
E-mail: il.jeon@spc.oxon.org

821P-39Three-dimensional quantum Hall effect in Weyl semimetal○F. R. Pratama1,2, Nguyen T. Hung1,2, Riichiro Saito1
1 Department of Physics, Tohoku University, Sendai 980-8578, Japan
2 Frontier Research Institute for Interdisciplinary Sciences, Tohoku University, Sendai 980-8578, JapanThe quantum Hall effect (QHE) is the quantization of the Hall conductivity in strong
magnetic field at low temperature [1]. The QHE provides a useful tool to determine the finestructure constant and to study the Landau levels in condensed-matter systems. Generally, the
QHE is observed in two-dimensional (2D) materials such as 2D electron gas [1] and graphene[2, 3]. Recently, three-dimensional (3D) QHE is discovered in topological materials Cd3As2 [4]and ZrTe5 [5], which show some characteristic features distinguishable from that of the 2D QHE,
for example, the less-obvious quantization of the Hall conductivity in 3D systems. However, atheoretical study is required to explain the origins of the features of 3D Hall conductivity. In
this study, by using a simple model of the Weyl semimetal, we show that the quantization of theHall conductivity in 3D system arises from a logarithmic singularity of the density of states(DOS), as opposed to that of the delta function singularity in 2D DOS. Further, we discusstemperature and in-plane electric field effects in the quantization of the Hall conductivity.

[1] K. v. Klitzing, Phys. Rev. Lett. 45, 494 (1980).
[2] Y. Zhang et al., Nature 438, 201 (2005).
[3] K. S. Novoselov et. al., Science 315, 1379 (2007).
[4] C. Zhang et. al., Nature 565, 331 (2019).
[5] F. Tang et. al., Nature 569, 537 (2019).

Corresponding Author: F. R. Pratama
E-mail: pratama@flex.phys.tohoku.ac.jp

83

2P-1
Facile synthesis of icosapropyl [60]fullerene○Kazuhira Miwa1, Shinobu Aoyagi1, Takahiro Sasamori1,2, Shogo Morisako1,2, Hiroshi Ueno3,
Yutaka Matsuo4,5, Hideki Yorimitsu61
2

Graduate School of Science, Nagoya City University, Nagoya 467-8501, Japan

Faculty of Pure and Applied Sciences, University of Tsukuba, Tsukuba 305-8571, Japan
3

Frontier Research Institute for Interdisciplinary Sciences and Graduate School of Science, Tohoku
University, Sendai 980-8578, Japan
4

Graduate School of Engineering, Nagoya University, Nagoya 464-8603, Japan
5

School of Engineering, The University of Tokyo, Tokyo 113-8656, Japan
6

Graduate School of Science, Kyoto University, Kyoto 606-8502, Japan

A variety of functionalized C have been obtained by the introduction of functional groups to the C60
surface until now. The reactions of metastable polyanions of C60 with electrophiles could be an accessible
methodology for the introduction of functional groups. For example, when the corresponding polyanionic
C60 generated by reduction with Li was trapped by an excess amount of CH3I, multiply methylated C60 was
obtained [1]. However, the predominant components were C60(CH3)6 and C60(CH3)8, and a variety of
methylated C60, i.e., a series of C60(CH3)n (0 ≤ n ≤ 24), were formed due to the lability of the polyanionic C60.
We present an efficient multiple alkylation reaction of C60 using an in situ reduction/substitution reaction
system using sodium dispersion (SD) and dialkyl sulfate (Scheme 1). SD is a well-known and effective
reductant, and dialkyl sulfate is an electrophile that is inert to SD. Thus, the coexistence of SD and dialkyl
sulfate allows the reactant to undergo repetitive tandem reduction/substitution reactions in situ [2]. The direct
analysis in real time mass spectrum (DART-MS) of multiply propylated C60 (C60(nC3H7)n) obtained by themethod (Scheme 1) shows that the distribution of the substitution number (n) was remarkably narrower (18≤ n ≤ 24) and the predominant component was icosapropyl C60 with n = 20 (Figure 1).

[1] J. W. Bausch et al., JACS. 1991, 113, 3205.

[2] K. Miwa et al., Molecules 2022, 27, 450.

Corresponding Author: S. Aoyagi, E-mail: aoyagi@nsc.nagoya-cu.ac.jp

84

2P-2
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85

  /<2 1=<2B1A32 /A A632P-3
Efficient and safe purification of carbon nanotubes using FeCl3 vapor
Takuma Goto1, Hideaki Tanaka1, Toshio Osawa1, Mochen Li2, Hisashi Sugime2,
Suguru Noda1,2,*
1

Department of Applied Chemistry and 2Waseda Research Institute for Science and Engineering,
Waseda University, 3-4-1 Okubo, Shinjuku-ku, Tokyo 169-8555, Japan

Removal of catalyst metals and purification of carbon nanotubes (CNTs) are highly
demanded for various applications of CNTs. Methods including the oxidation and successive
acid treatment and the chlorine gas treatment have been developed, however, they suffer fromdamages to CNTs, poor re-dispersibility of purified CNTs [1], and/or toxic reagents [2].
In this study, an efficient and safe dry purification method was developed that exposes CNTs
to FeCl3 vapor at 1000 ιC. Fig. 1 shows the transmission electron microscope (TEM) imagesof three different CNTs before and after purification. Not only Fe (a,c) but also Ni and Y (b)were removed via the reaction of M(s) + xFeCl3(g)ЍMClx(g) + xFeCl2(g), leaving the hollow
graphitic spheres. In this initial trial, a small amount of CNTs (5-10 mg) were treated using an
excess amount of FeCl3 (100 mg) using a horizontal reactor.
Then Tuball CNTs were purified at a larger amount (50 mg) using a comparable amount of
FeCl3 (100 mg) and a vertical reactor. The purification reaction was proceeded by heating CNTs
and FeCl3 simultaneously. The purified CNTs were characterized by scanning electron
microscope-energy dispersive X-ray spectroscopy (SEM-EDS) and Raman scattering
spectroscopy. The purified CNTs had a significantly reduced Fe content from 20.9 to 5.0 wt%(Fig. 2a) with an increased intensity ratio of G-band to D-band peaks (IG/ID) of 106 (Fig. 2b),
showing the efficient removal of Fe without damaging CNTs.

Fig. 1. TEM images of three different CNTs before/after purification. Fig. 2. Fe content (a) and IG/ID (b).
[1] P. Hou, et al., Carbon 46, 2003 (2008). [2] G. Merder, et al., New J. Chem. 37, 790 (2013).
Corresponding Author: S. Noda, Tel: +81-03-5286-2769, Fax: +81-03-5286-2769, E-mail: noda@waseda.jp

86

2P-4
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87

2P-5
Influence of Laser-intensity on the Fermi-level dependence of highharmonic generation in nanocarbon materials○Hiroyuki Nishidome1, Kohei Nagai2, Kento Uchida2, Yuta Murakami3, Kenji Kawahara4,
Takahiko Endo1, Junko Eda1, Hitomi Okubo1, Yohei Yomogida1, Yasumitsu Miyata1,
Hiroki Ago4, 5, Koichiro Tanaka2, 6, Kazuhiro Yanagi1
1 Department of Physics, Tokyo Metropolitan University, Tokyo 192-0397, Japan
2 Department of Physics, Kyoto University, Kyoto 606-8502, Japan3

Department of Physics, Tokyo Institute of Technology, Tokyo 152-8551, Japan

4 Global Innovation Center (GIC), Kyushu University, Fukuoka 816-8580, Japan
5 IGSES, Kyushu University, Fukuoka 816-8580, Japan
6 Institute for Integrated Cell-Material Sciences, Kyoto University, Kyoto 606-8501, JapanThe recent advancement in intense mid-infrared laser sources has enabled us to investigate
high-harmonic generation (HHG) in solids [1]. Since this phenomenon demonstrates
unconventional behaviors beyond the perturbation regime, a lot of studies have investigated thegeneration mechanisms. Previously, we have revealed the Fermi-level dependence of HHG in
semiconducting single-walled carbon nanotubes (SWCNTs) [2]. We observed significant
enhancement and reduction of high harmonics as the sift of Fermi-level [2]. However, recently,
we found that HHG in graphene was almost constant as the shift of the Fermi-level. To
understand its background, we performed the theoretical calculation by changing various
parameters. We found that when the laser power is so strong, such as that the number of laserdriven carriers is larger than the injected carriers, the change in HHG becomes very small. The
calculation suggests that the laser intensity significantly influences the Fermi-level dependenceof HHG. However, we could not use graphene to confirm this suggestion experimentally,
because of the degradation of the graphene at high-intensity laser and the negligibly small signal
intensity at the low-intensity laser. Thus, in this study, we investigated the influence of laserintensity (IL) on the Fermi-level dependence of HHG in metallic SWCNTs.
We prepared aligned-metallic-SWCNT film and employed a side-gating device with ionicgel to tune Fermi level through the gate (a) IL = 0.01 TW/cm2(b) IL = 0.07 TW/cm2
voltage VG. The sample was irradiated by
a 0.26 eV mid-infrared pulse laser, and weinvestigated the relations between HHG
and carrier injection. Figure 1 shows HHG
intensity under (a) low- and (b) highpower laser and source-drain current as afunction of VG in metallic SWCNTs. Bothgraphs show the same tendency. However,the HHG with lower laser intensitychanges more drastically, indicating thatthe laser intensity also influences on
Fermi-level dependence of HHG.
[1] S. Ghimire et al. Nat. Phys., 15, 10 (2019). [2]Nishidome et al., Nano Lett 20, 6215 (2020)           

Fig.1 HHG intensity (top) and source-draincurrent(bottom) in metallic SWCNTs as a function of gate
voltage.

88

2P-6
Circular dichroism of metallic and semiconducting
doped carbon nanotubes○Taisei Maeda1, Riichiro Saito1
1

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

Chiral carbon nanotubes have a symmetric structure with respect to the mirror symmetry. In
the case of circularly polarized light, the left circular polarization and the right circularpolarization are mirror-image to each other. Therefore, chiral carbon nanotubes exhibit circulardichroism. The origin of the circular dichroism in undoped carbon nanotubes was shown by
Sato et al [1]. When carbon nanotube in doped, a new peak of circular dichroism spectra appears
by the new plasma absorption. It has been reported that the plasmon-related peak is much larger
than that of undoped nanotubes [2,3].
In this study, we calculated the optical conductivity to obtain of metallic and doped
semiconducting nanotubes for a wide range of chiral nanotubes.We calculated the circulardichroism for a variety of chiral nanotubes, including all chiral (n,m) metallic andsemiconducting nanotubes with n less than 20. In Fig. 1,we plot so-called CD Kataura-plot asfunction of 1/d୲ for undoped nanotubes. In Fig2, we show CD Kataura-plot for doped(E୊ =2.0eV) carbon nanotubes.For the plasmon peaks in Fig. 2(shaded area) is expanded in Fig.
3.The results show that undoped nanotubes and doped nanotubes share a strong circulardichroism for light in the UV region. In the case of undoped nanotubes, we can see a family
pattern for E୧୨ transition. Therefore, for nanotubes with larger diameters due to doping, there
is a correlation between the diameter and energy of CD peak position. In Fig. 3 the fitting
function as shown in Eq. (1) which in concerned with the result by Dairia et al.[2].
Energy஼஽௣௘௔௞ [eV] = 0.9667/݀௧ [nm] + 1.228 (1)[1] N. Sato et al.    9, 034018 (2018).
[2] S. Daria et al. Phys. Rev.B. 99, 075403 (2019).
[3] R. Saito et al. J. Appl. Phys. 128, 164301 (2020)
Corresponding Author: T. Maeda
E-mail: maeda@flex.phys.tohoku.ac.jp

Fig.1 Diameter dependence of theFig.2 Diameter dependence of theFig.3 Expanded view of the grayCD peak position of undoped

CD peak position of doped( E୊ =area in Fig. 2 andnanotubes appears

2.0eV) nanotubes appears

89

fitting function

2P-7
Appropriate properties of carbon nanotube for
3D current collector of lithium-ion battery○Kentaro Kaneko1, Suguru Noda1,2
1

2

Department of Applied Chemistry, Waseda University, Tokyo, Japan.
Waseda Research Institute for Science & Engineering, Waseda University, Tokyo, Japan

High-energy-density secondary battery is necessary to satisfy the increasing demand forenergy storage. Conventional electrodes of lithium-ion battery have heavy foils of metals as
current collectors. To achieve high energy density by eliminating non-capacitive components,
we developed electrodes based on 1 mass% 3D current collector of submillimeter-long fewwall carbon nanotube (CNT) that held 99 mass% active materials [1]. The metal-foil free CNTbased electrodes were demonstrated, however, only one type of CNT was used. We here report
the effects of the structural properties of CNT on the battery performance.
The graphite-CNT negative electrode and the lithium cobalt oxide (LCO)-CNT positiveelectrodes (97:3 mass ratio) were prepared by ultrasonication in 2-propanol and filtration. 10
types of CNT prepared by fluidized bed CVD method [2] were used. 2032-coin cells wereassembled using polypropylene separator and electrolyte (1M LiPF6, EC:DEC=1:1, v:v).
At the first charge, solid electrolyte interphase (SEI) formed on negative electrode, causing
irreversible capacity (difference between charge and discharge capacities). The irreversible
capacity increased with increasing SSA, causing depletion of active lithium and decreasing
reversible capacity (Fig. 1a). Then the rate and cycle performances were evaluated (Fig. 1b).
The capacity was higher with CNTs of smaller SSA (187, 240 m2 g–1) at current densities d 2
mA cm–2 while the capacity was higher with CNTs of moderate SSA (287, 501 m2 g–1) at a highcurrent density of 10 mA cm–2. CNTs of lower SSA is beneficial to suppress the side reaction
while those of moderate SSA is beneficial to achieve high rate-performance.

Fig. 1. (a) Reversible and irreversible capacities vs SSA of CNT. (b) Rate and cycle performance.
[1] K. Hasegawa, S. Noda, J. Power Sources 321 (2016) 155.
[2] M. Li, M. Risa, T. Osawa, H. Sugime, and S. Noda, Carbon 167 (2020) 256.
Corresponding Author: S. Noda,

Tel: +81352862769, Fax: +81352862769

90

E-mail: noda@waseda.jp

2P-8
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2P-9
Size enhancement of monolayer WS2 with sandwiched growth substrates○Ryoki Hashimoto1, Yasuhiko Hayashi1, Yasumitsu Miyata2, Hiroo Suzuki1
1

Graduate School of Natural Science and Technology, Okayama University, Okayama
700-8530, Japan2
Department of Physics, Tokyo Metropolitan University, Hachioji 192-0397, Japan

Transition metal dichalcogenides (TMDCs), one of the semiconducting
two-dimensional materials, has been attracting attention for optoelectronic device applications
such as solar cells, photodetectors, and light-emitting diodes due to their high flexibility, lightabsorption, and emission coefficient with direct band-gap. The most common issue on the
crystal growth of TMDCs for practical applications is grain size control to achieve the smaller
number of the grain boundaries in a continuous sheet of TMDCs, which can reduce the negative
influence from defects and impurities at the grain boundaries. This research investigated thechemical vapor deposition (CVD) growth of monolayer WS2 and their size control based on thevaper-liquid-solid (VLS) method with metal salt employing the modified configuration of
growth substrates.
The cold-wall CVD system conducted the CVD
growth with the infrared gold image furnace. Na2WO4 was
employed as W sources, and its solution was spin-coated on a
Si/SiO2 substrate. The vapor of (t-C4H9)2S2 was introduced intoa CVD chamber as an S source. We employed the modified
configuration of the growth substrates; the spin-coatedsubstrate (B) was covered by another clean substrate (A). The
maximum crystal size obtained on the B side was more than
400 µm for WS2 (Fig. 1(a)). These sizes were tens of times
larger than the conventional case using a single substrate (~10μm). We investigated the effect of growth temperature on the
crystal size (Fig. 1(b)) and photoluminescence (PL)characteristics such as PL intensity distribution, PL peakenergy, and full width at half maximum. These results
suggested the increase in the growth temperature causes thesize enhancement of WS2 single crystal; however, it could
decrease the crystallinity and its spatial uniformity.
Corresponding Author: H. Suzuki
Tel: +81-86-251-8133
E-mail: hiroo.suzuki@okayama-u.ac.jp

92

Fig.1: (a)Optical microscope imageof the large-size monolayer WS2.
(b) Growth temperaturedependence of the crystal size ofmonolayer WS2.

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93

2P-11One-dimensional spatially-separated excitons in an ultrathin onedimensional lateral heterostructure○Nanami Ichinose1, Liu Zheng2, Susumu Okada 3, Mina Maruyama 3, and Ryo Kitaura1
1

2

Department of Chemistry, Nagoya University, Nagoya 464-8602, Japan
Innovative Functional Materials Research Institute, AIST Nagoya 463-8560, Japan3
Department of Physics, University of Tsukuba, Tsukuba 305-8571, Japan

Two-dimensional (2D) heterostructers have attracted considerable attention. [1] [2] Althoughvan-der-Waals-stackings-based heterostructers have been intensively studied so far [3] [4], theresearch on lateral heterostructers is still limited due to the difficulty in fabrication. In this work,
we have focused on the growth and optical properties of lateral heterostructers with a periodicity
of down to nanometer scale. These are atomically thin 2D layers with one-dimensional (1D)
stripes, namely 1D quantum wells (QWs), that align periodically, providing a novel 1-2D
mixed-dimensional platform for exploring properties arising from the one-dimensionality.
In this study, we fabricated 2D lateral heterostructers of WS2/MoS2 on hexagonal boron nitride
by sequential growth of WS2 and MoS2 through rapid switching of supply of W and Mo source.
Figure 1 shows high angle annular dark-field scanning transmission electron microscopy(HAADF-STEM) image of lateral heterostructers, WS2/MoS2. In the HAADF-STEM images,
W atoms are imaged as bright spots, whereas Mo and S
atoms are images as much darker spots. As seen in theimage, the MOCVD-grown lateral structure possesses
atomically steep interfaces with a width down to 0.8 nm; wehave also confirmed that an one-atom-thick junction canalso be grown by our MOCVD setup. Figure 2 shows a PL
spectrum of hetero structer WS2/MoS2 with a periodicity of
about 5 nm measured at 5 K. The PL spectrum shows PL
peaks at 1.55 eV, which are absent in the PL spectra of WS2
or MoS2 monolayers alone. Judging from peak position, Fig. 1 A HAADF-STEM image of asignificant saturation, and long lifetime of 120 ps, we think WS2/MoS2 heterostructure.
this peak arises from 1D spatially-separated exciton at a
1D stripe. In the presentation, I will provide details of thegrowth process and detailed analyses of optical properties.
[1] A. K. Geim et al. Nature, 499, 419 (2013).
[2] Y. Kong et al. Nature materials, 13, 1135 (2014).
[3] C. Zhu et al. Nature communication, 11, 772 (2020).
[4] Y. Kobayashi et al. ACS Nano,13, 7527 (2019).
Corresponding Author: R. Kitaura
Tel: +81-52-789-2482, Fax: +81-52-747-6442
Web: http://nano.chem.nagoya-u.ac.jp/
E-mail: r.kitaura@nagoya-u.jp
Fig. 2 A PL spectrum of a
WS2/MoS2 heterostructure at 5K.

94

2P-12
Electronic transport properties of multilayer MoS2-based PN diodes○Seiya Kawasaki1, Hiroto Ogura1, Takahiko Endo1, Yusuke Nakanishi1, Hong En Lim1,
Kazuhiro Yanagi1, Toshifumi Irisawa2, Kosuke Nagashio3, Yasumitsu Miyata1
1

Department of Physics, Tokyo Metropolitan University, Tokyo 192-0397, Japan
2
Nanoelectronics Research Institute, AIST, Tsukuba, 305-8562, Japan3
Department of Materials Engineering, The University of Tokyo, Tokyo 113-8656, JapanThe quantum tunneling effect in PN junctions, reported by Esaki et al. in 1958 [1], has attracted
much attention in recent years for the realization of low power consumption devices. For example, thecontrol of tunnel current has been demonstrated for the in-plane PN junctions based on twodimensional semiconductors such as transition metal dichalcogenides (TMDCs)(Fig.1a) and black
phosphorus [2,3]. In particular, multilayer TMDCs are promising for performance improvement
because of their high air stability and highly-tunable carrier densities. In this study, we report thegrowth and characterization of in-plane heterojunctions based on multilayer MoS2.
Nb-doped multilayer p+-MoS2 was exfoliated onto SiO2/Si substrates. Multilayer n-MoS2 was thengrown from the edge of the p+-MoS2 flakes using chemical vapor deposition (CVD). Field-effecttransistors (FETs) were fabricated by plasma etching and deposition of In/Au electrodes (Fig.1 b, c).
As shown in Fig. 1d, the I-V curve shows the rectification characteristics at Vg = 0 V. In contrast, anegative differential resistance trend (NDR trend) was observed for Vg = 30~50 V. This suggests the
band-to-band tunneling (BTBT) current flows for the forward bias due to the formation of broken gap
semiconductor heterojunction as shown in Fig. 1e. The present results provide a basis to optimize thedevice structure and carrier control for the high performance of tunnel FETs.

Fig.1: (a) Structure model of MoS2. (b) Optical microscope image, (c) structure model, (d) I-V curves at different gate
voltages, and (e) the expected band alignment of p+-MoS2/n-MoS2 device at Vg = 30 V and Vd = 0.5 V.

[1] L. Esaki., Phys. Rev. 109, 603 (1958). [2] S. Kim et al., Nat. Nanotechnol. 15, 203-206 (2020). [3] T. Fukui et al., The
82nd JSAP Autumn Meeting, 13a-N307-11 (2021).
Corresponding Author: Y. Miyata, Tel: +81-042-677-2508, E-mail: miyata-yasumitsu@tmu.ac.jp95

2P-13
Electrically tunable moiré trions in twisted WSe2/MoSe2 heterobilayers○Duanfei Dong1, Wenjin Zhang1, Kenji Watanabe2 , Takashi Taniguchi2,
Keisuke Shinokita1, and Kazunari Matsuda1
1Institute of Advanced Energy, Kyoto University, Uji, Kyoto 611-0011, Japan

2

National Institute for Materials Science, Tsukuba, Ibaraki 305-0044, Japan

Voltage (V)The formation of moiré patterns provides a new platform for the exploration of optoelectronic
properties of two-dimensional materials, which has attracted extensive attention in various
research fields [1]. A moiré pattern can be formed by vertically stacking two monolayer
semiconducting transition metal dichalcogenides with a twist angle or a mismatch in lattice
constant. These periodic moiré patterns can generate spatially distributed potentials to trap theelectron-hole pairs (excitons), which has been proved to have notable effects on opticalemissions [2,3]. Besides excitons, their charging counterparts (charged excitons or trions) will
add an aspect of moiré excitonic states, however, the impact of charging effects is still unclear.
In this study, we have studied the interlayer moiré excitonic states in superlattices, andexplored the influences of electric doping. We fabricated the R-type heterostructure devices bystacking MoSe2 to WSe2 (MoSe2/WSe2 heterobilayer) with a very small twist angle of a few
degrees, using mechanical exfoliation and dry-transfer techniques (inset of Fig. 1). The
heterobilayer was encapsulated by hexagonal boron nitride (h-BN) with semi-transparent thingraphite gates. Figure 1 shows the counter map of gate-dependent photoluminescence (PL)spectra of heterostructure device at 5 K. The several discrete PL lines are clearly observed
around 1.345 eV from gate-voltage of -10 to -20 V, which represents the PL peaks from moiré
excitons in the neutral region. The new lines at the lower energy side around 1.335 eV appear
from 0 to 20 V, which might come from the PL peaks of trions trapped in moiré potential due
Intensity (count)to the electron doping (moiré trion). The
30
5600
Laser: 1.959 eVmoiré trion peaks become weak and broaden
P = 0.32 W/cm2
M-T
MoSe2/WSe2)
T=5K
above 20 V due to high carrier density. The
20 MoSe2/WSe2
4667
binding energy of the moiré trion was଴‫ܯ‬௑
10  
evaluated as 10 meV. Moreover, we will

3733
‫ܯ‬௑଴
M0x
discuss the detailed moiré trion structures   
0 
M-Tfrom the temperature dependence of PL
2800
spectra of the device.






-10

[1] P. Rivera et al., Nat. Nano. 13, 1004 (2018).
[2] K. L. Seyler et al., Nature 567, 66 (2019).

M0x

-20

[3] K. Shinokita et al., Nano Lett. 21, 5938 (2021).

1.30

1.32

1.34

1867

1.36

Energy (eV)Corresponding Author: Kazunari Matsuda
Tel: +81-774-38-3460, Fax: +81-774-38-3460
E-mail: matsuda@iae.kyoto-u.ac.jp

Figure 1. PL spectra of MoSe2/WSe2 heterobilayer at
5 K. M୘ି and Mଡ଼଴ are denoted as interlayer moiré
trion and exciton PL signals, respectively.

96

2P-14         

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(b)

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2.0 eV

Odd-number-layer

Odd-number-layer
1.0 eV

spin
σxyy
e/ℏ

spin
σxyy
e/ℏ

4
0
-4

0.8 eV

0.6 eV
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0.0 eV-12

Even-number-layer

2.0 eV

1.0 eV

0.8 eV

chargeσyxx

charge
σyxx

0

-40

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-80
1
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1.5

2

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0.0 eV

0

1

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982P-16
Vapor-phase synthesis of single-walled MX2 nanotubes templated on
surfactant-dispersed boron-nitride nanotubes
ࠐShinpei Furusawa1, Yohei Yomogida1, Yuta Sato2, Kazuhiro Yanagi1, Kazu Suenaga3,
Yusuke Nakanishi1*, and Yasumitsu Miyata1*
12

Department of Physics, Tokyo Metropolitan University, Hachioji, 192-0397, Japan

National Institute of Advanced Industrial Science and Technology (AIST), Tsukuba 305-8565, Japan.
3

The Institute of Scientific and Industrial Research, Osaka University, Osaka 567-0047, Japan.

Transition metal dichalcogenide nanotubes (MX2NTs) are one-dimensional (1D) materials
that exhibit some intriguing phenomena such as exciton-polaritons and bulk photovoltaic effect[1]. Understanding the origin of these phenomena necessitates the characterization of singlewalled (SW) MX2NTs isolated from typical multi-walled ones. Recently, Xiang et al haverealized SW-MoS2NTs in 1D coaxial heterostructures based on carbon nanotubes [2, 3], yetdetailed electronic properties of individual MoS2NTs remains elusive. Electrically and opticallyinactive boron-nitride nanotubes (BNNTs) can serve as an ideal template for precisely studying
the electronic properties of MX2NTs; however, BNNT-templated syntheses of MX2NTs is still
limited due to the difficulties in the preparation of well-dispersed BNNT templates.
Here we present the facile synthesis of MX2NTs
using surfactant-dispersed BNNTs as templates. We
have developed an efficient dispersion of aspurchased BNNTs by using Triton X-100, thesurfactant that can be easily removed to provide clean
BNNTs by simple thermal treatment. Comprehensive
microscopic and spectroscopic analyses suggests that
this approach can afford stable, clean, and welldispersed BNNT networks. We demonstrated that the
BNNT templates can be utilized to synthesize avariety of MX2NTs including alloys (Fig. 1). The
present methodology will accelerate the growing
efforts to reveal the electronic properties and potential
application of MX2NTs.

Figure 1 (a) Schematic and (b) HAADFSTEM images of a single-walled MoS2NT
coaxially grown on an individual BNNT.

[1] J. Musfeldt et al., Phys. Today 73, 8 (2020) [2] R. Xiang et al., Science 367, 537 (2020) [3] M. Liu et al.,ACS Nano 15, 8418 (2021)
Corresponding Author: Y. Nakanishi and Y. Miyata
Tel: +81-42-677-2498 E-mail: naka24ysk@tmu.ac.jp; miyata-yasumitsu@tmu.ac.jp992P-17
Intercalation of group-XIII metals
in crystalline bundles of WTe atomic wires○Ryusuke Natsui1, Hiroshi Shimizu1, Zheng Liu2, Iori Kikuchi3, Jiang Pu3, Taishi Takenobu3,
Hong En Lim1, Takahiko Endo1, Yusuke Nakanishi1*, and Yasumitsu Miyata1*
12

Department of Physics, Tokyo Metropolitan University, Hachioji 192-0397, Japan
Innovative Functional Materials Research Institute, AIST, Nagoya 463-8560, Japan3
Department of Applied Physics, Nagoya University, Nagoya 464-8603, Japan

Atomically thin wires of transition metal chalcogenides (TMCs) −labeled as MX with M:
transition-metal and X: chalcogen− are quasi-one-dimensional (1D) conductive materials withthe diameter of less than 1 nm (Fig. 1a), which can assemble into van der Waals 3D bundles aswell [1]. Recently, we have developed the wafer-scale growth of 2D and 3D crystalline bundlesof WTe atomic wires using chemical vapor deposition (CVD) [2]. In addition to the tunabledimensionality, assembled TMC wires possess inner hollow spaces to incorporate foreign atoms.
Upon the intercalation of metal atoms, the electronic properties can be drastically changed,
which allows for exploring emergent phenomena such as superconductivity [3].
Here we present the intercalation of group-XIII metals into crystalline bundles of WTe
atomic wires. In and Tl-intercalated samples were first fabricated by vapor-phase intercalation
into CVD-grown WTe bundles. The presence of intercalated In atoms was directly confirmedby cross-sectional HAADF-STEM observation (Fig. 1b, c). In addition, we successfullyintercalated Tl atoms into the bundles. The present results show the possibilities that the electric
properties of WTe bundles can be tuned by intercalating different atoms.

Figure. 1 a Schematic image of an individual WTe atomic wire. b Cross-sectional HAADF−STEM image of Inintercalated WTe bundles. Scale bar = 1 nm. c The structure model corresponding to the region marked by a squarein b.
[1] H. Zhu et. al., Adv. Mater. 29, 1606264 (2017). [2] H. E. Lim et al., Nano Lett. 21, 243 (2021). [3] A. P.
Petrović et al., Phys. Rev. B 82, 235128 (2010).
Corresponding Author: Y. Nakanishi and Y. Miyata,
TEL: +81-42-677-2498, E-mail: naka24ysk@tmu.ac.jp;
Tel: +81-42-677-2508, E-mail: miyata-yasumitsu@tmu.ac.jp100

2P-18
Spontaneous photocurrent of WSe2/CrPS4 hetero-interface
with in-plane polarization and highly air-stability.
○Shuichi Asada1, Keisuke Shinokita1, Kenji Watanabe2,

Takashi Taniguchi2, and Kazunari Matsuda1
12Institute of Advanced Energy, Kyoto University, Uji 611-0011, Japan
National Institute for Materials Science, Tsukuba 305-0044, Japanan der Waa s dW hetero inter aces based on t o di ensiona 2
a ered ateria s ha e
recent attracted tre endous interest, because o the arious ateria co binations and generationo ne
h sica ro erties
stacking ro er se ected 2 a ered ateria s ith di erent
rotationa s
etries ith a articu ar ang e, the s
etr o dW hetero inter ace is reduced toon ha e a sing e irror s
etr , hich induces s ontaneous in ane o arization 1 The, bothin ane o arization has been e eri enta re orted in WSe2 b ack b ack hos horus
o hich are non o arizing ateria s The WSe2
dW hetero inter ace sho s er ro isingresu ts or s ontaneous hoto o taic e ect ithout p n junction and bias o tage o e er, theiser susce tib e to degradation due to o idization, and there ore the a or de ice a ications othis ho e u hotocurrent ro erties are strong re uired
ere, e designed a WSe2 r S dW hetero inter ace ith unia ia s
etr or in ane
o arization, here r S is kno n to be uch higher air stabi it 2 The cr sta direction o eachake as con ir ed b the edge o the ake
The akes ere stacked at the ro er ang e, re ing
on the o tica i age inset o ig 1 a The WSe2 and r S ha e three o d and t o o d rotationasetries, res ecti e , hich can t be co atib e, a though on one irror s
etr re ains in
the dW hetero inter ace This s
etr causes o arization in the direction ara e to the irror
ane As a conse uence, e can e ect the generation o ano a ous hotocurrent igure 1 a
sho s the hotocurrent easured in WSe2 r S dW hetero inter ace, here the e ectrodes ere
abricated in the ara e direction to the irror
ane We obser ed s ontaneous hotocurrent
atde ending on irradiation o aser ight,
hich suggests that the in ane o arization isa so generated on this neco bination
hetero inter ace n the resentation, e i
discuss ore detai ed hoto o taic ro erties
andotentiaa icationo
thishetero inter ace
1 T Aka atsu et al., Science 2,
2
Son et al., ACS Nano , 1
ee et al., ACS Nano , 1

2 21
2 21
2 1

orres onding Author Kazunari Matsuda
Te1ai
atsuda iae k oto u ac j101

2P-19Synthesis of [C60] fullerene nanowhisker-glycine capped ZnS:Mn
composites and their photocatalytic degradation of methylene blue
○ Seung Won Ko1, Hoon Chung1, Weon Bae Ko1,2
1

Department of Convergence Science, Graduate School, Sahmyook University, 815, Hwarang-ro,
Nowon-gu, Seoul 01795, Republic of Korea
2
Department of Chemistry, Sahmyook University, 815, Hwarang-ro, Nowon-gu, Seoul 01795,
Republic of Korea

ZnS:Mn-Gly nanocrystals were synthesized by capping the surface of ZnS:Mn with
L-glycine and were characterized by UV-vis, Raman spectroscopy, XRD, SEM, and TEM [1].
The liquid–liquid interfacial precipitation (LLIP) method was used to create [C60] fullerene
nanowhisker-ZnS:Mn-Gly composites from C60-saturated toluene, the ZnS:Mn-Gly solution,and isopropyl alcohol [2].The product of the hybrid nanocomposites was characterized by
UV-vis, Raman spectroscopy, XRD, SEM, and TEM. The photocatalytic degradation of
methylene blue was confirmed using [C60] fullerene nanowhisker-ZnS:Mn-Gly composites by
UV-vis spectroscopy. The kinetics study for the photocatalytic degradation of MB with the[C60] fullerene nanowhisker-ZnS:Mn-Gly composites as photocatalyst under UV irradiation at
254 nm followed a pseudo first order reaction rate law.
0.0ln(C/C0)

-0.5

-1.0

0.00587 ± 0.01195
Intercept-0.01023 ± 1.65746ESlope
0.99869
R-Square (COD)
-1.5
0

20

40

60

80

100

120

Time (min)Fig. 1 Kinetics study for photocatalytic degradation of methylene blue with [C60] fullerene
nanowhisker-ZnS:Mn-Gly composites under UV irradiation at 254 nm.

[1] J.W. Lee, C.S. Hwang, Bulletin of the Korean Chemical Society, 35, 189 (2014).
[2] K. Miyazawa, Journal of Nanoscience and Nanotechnology, 9, 41 (2009).
Corresponding Author: W. B. Ko
Tel: +82-2-3399-1700, Fax:, +82-2-979-5318,
E-mail: kowb@syu.ac.kr102

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    .*)!#)(*%##)'"$%.* &103

2P-21Fabrication of nanocarbon hybrid structure composed of carbon nanotubes
and carbon foams○Shu Kondo1, Moeri Sugiyama1, Daiki Yamamoto1, Shusaku Karasawa1, Kamal P Sharma1,
Takahiro Saida1,2, Shigeya Naritsuka3, Takahiro Maruyama1,2
1

Department of Applied Chemistry, Meijo University, Japan

2

Nanomaterials Research Center, Meijo University, Japan3

Department of Materials Science and Engineering, Meijo University, Japan

1.

Introduction
Because of their high specific surface areas, Carbon nanotubes (CNTs) are expected as
support materials for catalyst particles in many fields such as batteries, chemical biosensors,and fuel cell. Previous study showed that, by depositing Pt catalysts on CNTs, their activity
was enhanced. Furthermore, to increase the specific surface area, combining CNTs with othernanocarbon materials such as graphene has been attempted. In this study, we attempted tofabricate hybrid structure composed of CNTs and carbon foam to realize a support layer withhigh specific surface area.

2.

Experimental procedure

After cleaning of a melamine foam (~1 cm3), it was introduced into a furnace of a hot-wallchemical vapor deposition (CVD) system. After temperature rise to 300C, ethanol vapor was
introduced into the furnace, and the temperature was further raised to 600C, and kept for 20
min to form a carbon foam. Then, it was treated by O2 plasma, and immersed in aqueous
solution of Co(II) acetate for 24 h. After it was dried in an oven, CNT growth was performedby CVD with ethanol as carbon source. The growth temperature and time were 750C and 10
min, respectively. The samples were characterized by Raman spectroscopy and FESEM.
3.

Result and Discussion
Fig. 1(a) and (b) show Raman spectra of samples grown using 0.01 M and 0.005M ofaqueous solutions of Co(II) acetate, respectively. In both spectra, RBM peaks were observed,
indicating single-walled CNTs (SWCNTs). As theconcentration of Co(II) acetate increased, the
SWCNT diameters were enlarged. Fig.1 (c) and (d)show FESEM images of the samples shown in Fig.
1(a) and (b), respectively. SWCNT growth wereobserved on carbon foams, formed by carbonizationof melamine foams.

Part of this research was supported by the private university
research branding project "Meijo University Brand Building
Program by Creating New Nanomaterials" and JSPS
Bilateral International Joint Research Projects.
[1] T. Onoe et al. Catalysis Commun. 8, 2007, 701.
Corresponding Author: T. Maruyama
Phone: 81-52-838-2386, Fax: 81-52-832-1172
E-mail: takamaru@meijo-u.ac.jp

104

Fig. 1 Raman spectra of the sample
using (a) 0.01 M and (b) 0.005M ofaqueous solutions of Co(II) acetate.
FESEM images of (c) the sample in (a),and (d) the sample in (b).

2P-22Synthesis of aligned carbon nanotubes from nanodiamond seeds
by kite-growth mechanism○

Yuanjia Liu1, Michiharu Arifuku2, Noriko Kiyoyanagi2, Masamitsu Satake2, Taiki Inoue1,
Yoshihiro Kobayashi1
1Department of Applied Physics, Osaka University, Osaka 565-0871, Japan
2
Nippon Kayaku, Tokyo 115-8588, Japan

Carbon nanotubes (CNTs) have received extensive attention due to their extraordinary
thermal, electrical, and mechanical properties. Kite-growth [1] is a process to grow aligned
CNTs by utilizing laminar gas flow and enables the formation of air-suspended CNTs, which
are useful for physical property measurements. In the past research, metal particles are used as
catalysts. However, they inevitably remain as impurities and often lead to defect formation,
which deteriorates the performance of CNTs. In order to overcome these effects, this research
performs metal-free kite-growth of CNTs. Nanodiamond (ND) is stable at high temperatures,
easy to grow low-defect CNTs, and avoids remaining metal impurities. Another advantage of
ND is that CNTs can be synthesized on any kind of substrate (including electrodes), which isconvenient for device fabrication. [2] The results showed over 100 μm-long CNTs were grownby controlling growth conditions.
The kite-growth of aligned CNTs was performed by catalytic chemical vapor deposition(CVD) using ethanol as the carbon source. ND particles dispersed in ethanol were dropped onto
half of the silicon substrates with a 300 nm thick SiO2 layer. In a control experiment, Fe catalyst
was prepared with FeCl3 ethanol solution. The nanotube growth was initiated by introducing
35 sccm H2/Ar bubbling through ethanol and 420 sccm H2/Ar through another gas line atconstant temperature (930ºC). After 30 min of growth, the sample was cooled down in Ar toroom temperature. The whole CVD process was performed at atmospheric pressure. Scanningelectron microscopy (SEM, Hitachi S-4800) was used for observing the morphologies of thesynthesized CNTs. Raman spectra were measured for investigating the CNT structures with alaser excitation wavelength of 633 nm.
The SEM images (Fig. 1) compare the morphology at the tipof CNTs when CNTs are grown using metal catalysts and ND by
kite-growth mechanism. When using Fe as the catalyst (a), it canbe observed that there is a bright particle attached to the tip, whichmeans that the CNT tip has a metal catalyst attached because Fe
has more secondary electron (SE) yield than carbon [3]. The
catalyst is always at the tip of the CNT during the growth process
and moves as the CNT grows. That is, the kite-growth of Fe
catalysts belongs to tip-growth mode, which is consistent with theprevious experimental results. On the other hand, when using ND
as the growth seeds (b), there is no bright particle attached to thetip. This means that the CNT is not grown from metal impurities.
Although some examples of bright tip were also found in thissample, according to statistics, the proportion is less than 5%,
which belongs to the influence of metal impurities. Thus, it canbe concluded that the CNT in this sample is grown from ND. Fi
Fig. 1 SEM images
off CNTsi
CNT
Although the growth efficiency of ND as growth seeds is grown from (a) Fe catalyst andsignificantly lower than metal catalysts, we demonstrate the (b) ND seeds by kite-mechanism.
feasibility of growing CNTs from ND using kite-mechanism.
The white arrow represents the[1] S. Huang et al. Nano Lett., 4, 1025 (2004). [2] D. Takagi et al. J. Am. Chem.
Soc., 131, 6922 (2009). [3] H. Seiler, J. Appl. Phys., 54, R1 (1983).
Corresponding Author: Y. Kobayashi, E-mail: kobayashi@ap.eng.osaka-u.ac.jp

105

direction of gas-flow. Scale bars
are 2 μm. Primary electronenergy is 5 keV.

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107

2P-25
One-pot synthesis of Prussian Blue and nano-carbon composites○Taisei Fujikawa, Yoshimitsu Taniguchi, Shinji Kawasaki, Yosuke Ishii
Department of Life science and Applied Chemistry, Nagoya Institute of Technology,
Nagoya 466-8555, JapanThe recovery and utilization of low-grade heat is an urgent necessity to reduce its
contribution to global warming, but there is the problem that the efficiency of conversion of
low-grade heat to electricity is low. The Thermally Regenerative Electrochemical Cycle(TREC) is one technology that can solve this problem. Prussian blue (PB) analogs are some ofuse commonly for the positive electrode in the system, which offers efficient heat-to-electricity
conversion but low power output, necessitating the use of a conductive supporting material.
Therefore, we used Prussian blue nanocarbon composite as TREC electrode. Nano-carbon
improves the ion transport in the composite due to its excellent electron conductivity and wellordered porous structure, while maintaining the properties of PBA grown on their surface. We
used two nano-carbon materials: single-walled carbon nanotubes (SWCNTs) and reduced
graphite oxides (r-GOs).
The PB-SWCNT composite was obtained by adding a mixture of 1 mM FeCl3 and 1 mM
K3[Fe(CN)6] to SWCNTs dispersion. XRD analysis, thermogravimetric analysis, SEM
measurement, and TEM measurement were performed on the synthesized composite. Fig. 1
shows a tubular structure with bamboo segment-like deposits of PB on SWCNTs bundles. TEM
measurement also showed PB particle layers on the surface of SWCNT bundles. These results
indicate that the PB-SWCNTs composite has a core-shell structure in which PB crystals aredeposited on the surface of SWCNTs. We’ll discuss the TREC electrode properties of PBSWCNT composite at the symposium.

Fig. 1 SEM images of (right) PB-SWCNT and (left) PB-Graphene (r-GO) composites.
[1] Y. Ishii, A. Al-zubaidi, Y. Taniguchi, S. Jindo, S. Kawasaki, Single-walled carbon nanotubes as reducing
agent for the synthesis of Prussian blue-based composite: a quartz crystal microbalance study, NanoscaleAdv., (2021). DOI: 10.1039/d1na00739d
Corresponding Author: S. Kawasaki
E-mail: kawasaki.shinji@nitech.ac.jp1082P-26
A quartz crystal microbalance study of ion adsorption behavior of
single-walled carbon nanotubes○Serina Kanematsu, Shinya Jindo, Yu Takeuchi, Yosuke Ishii, Shinji Kawasaki
Department of Life science and Applied Chemistry, Nagoya Institute of Technology,
Nagoya 466-8555, Japan

Single-walled carbon nanotubes (SWCNTs) have been actively investigated as a newelectrode material for Electric Double Layer Capacitors (EDLCs), because of their highelectrical conductivity, chemical stability, and high theoretical specific surface area.
Unfortunately, many research results show that the current electrode performance of SWCNTs
is not high enough to replace existing EDLC electrode materials. However, most of the previous
studies evaluated the electrode performance of SWCNTs without distinguishing between
SWCNTs of different diameters and electronic states, and the details of the ion adsorption
mechanism of SWCNTs are not clear. If this aspect is clarified, it will be possible to propose
new SWCNT electrodes to improve the performance of EDLCs. In this study, the ion adsorption
behaviors of several kinds of SWCNT samples having different mean tube diameters during theformation of the electric double layer in various electrolytes were investigated by Quartz
Crystal Microbalance (QCM) method.
SWCNTs were deposited as a thin layer on the QCM substrate, then the substrate was usedas the working electrode in a three-electrode cell. Carbon fiber wrapped by Pt mesh andAg/AgCl were used as the counter electrode and Ag/AgCl as the reference electrode,
respectively. Simultaneous Cyclic Voltammetry (CV) and QCM measurements were performed
in 1.0 mol/L MCl / H2O (M = Li, Na, K, Cs)
electrolyte, in order to investigate how the adsorption
behavior on SWCNTs changes depending on theelectrolyte.
Fig. 1 shows changes in mass as a function of
charge obtained by QCM measurements of SWCNTs
having mean tube diameter of 1.5 nm for four different
alkali metal chloride electrolytes. It was found that theminimum point of the mass change data shifts toward
high charge value side with increasing atomic numberof alkali metal of the electrolytes. This can be
explained by the difference of ion adsorptiondesorption behaviors depending on the ion species.
[1] A. Al-zubaidi, M. Takahashi, Y. Ishii, S. Kawasaki,
Switching of alternative electrochemical charging
mechanism inside single-walled carbon nanotubes: a quartz
crystal microbalance study, RSC Advances, 11, 3025330258 (2021).
Corresponding Author: S. Kawasaki
E-mail: kawasaki.shinji@nitech.ac.jp

Fig.1 Change in mass as a function of
charge obtained by QCM measurementsof SWCNTs (d = 1.5 nm) electrode.

109

2P-27
Solar CO2 reduction properties of AgI/SWCNT/AgIO3 andg-C3N4/SWCNT/Cu photocatalysts○Jumpei Hayashi, Kenta Kobayashi, Sae Ishikawa, Shunsuke Sato, Yosuke Ishii,
Shinji Kawasaki
Department of Life Science and Applied Chemistry, Nagoya Institute of Technology,
Nagoya 466-8555, Japan

In recent years, there has been a lot of research on photocatalysts that can reduce CO2 using
solar energy. However, the conversion efficiency and selectivity of the reduction reaction are
still low. In order to overcome this situation, several attempts have been done. One of the mostpromising way is to prepare photocatalysts consisting of two kinds of nanoparticles (NPs)having semiconductor/semiconductor or semiconductor/metal combinations, because these
combinations enable to increase photo-absorption energy range and/or to depress the charge
recombination between the excited electrons and holes. However, it is not easy to prepare suchphotocatalysts having good NP1-NP2 contacts. To help the charge transfer from NP1 to NP2,
it is expected that single-walled carbon nanotubes (SWCNTs) can work as a bridge (i.e.
NP1/SWCNT/NP2). We prepared two types of such composite materials: silver iodide(AgI)/SWCNT/silver iodate (AgIO3) and graphitic carbon nitride (g-C3N4)/SWCNT/copper
nanoparticles (Cu) by using the encapsulation properties of SWCNTs.
We prepared AgI/SWCNT/AgIO3 by unique method using I@SWCNTs.[1] We found that
AgI/SWCNT/AgIO3 can work as a good photocatalyst for CO2 reduction under visible lightirradiation (Fig. 1).
On the other hand, g-C3N4/SWCNT/Cu was prepared by two steps. Firstly, we prepared
SWCNTs including copper(II) acetylacetonate (Cu(acac)2) (Cu(acac)2@SWCNTs). Secondly,
the prepared Cu(acac)2@SWCNTs and melamine, which is the precursor of g-C3N4, were heat
treated. We confirmed that g-C3N4/SWCNT/Cu works as a solar CO2 reduction photocatalyst.

Fig. 1 AgI/SWCNT/AgIO3 as a photocatalyst for CO2 reduction.
[1] Al-zubaidi, et al., One-step synthesis of visible light CO2 reduction photocatalyst from carbon nanotubes
encapsulating iodine molecules, Sci. Rep., 11, 10140 (2021).
[2] Y. Ishii, et al., Ultra-fine metal particles dispersed on single-walled carbon nanotubes for energy devices, J.
Mater. Sci., in press.
Corresponding Author: S. Kawasaki
Tel: +81-52-735-5221,
E-mail: kawasaki.shinji@nitech.ac.jp1102P-28Performance and stability evaluation of transparent heater
based on polymer-acid-doped carbon nanotube○Emina Hara1, Rongbin Xie 1, Suguru Noda1,2,*
1

Department of Applied Chemistry and 2Waseda Research Institute for Science and Engineering,
Waseda University, Tokyo 169-8555, Japan

Today, transparent heaters (THs) have gained significant attention as deicers and defoggersof headlights on automobiles. Carbon nanotube transparent conductive film (CNT-TCF) is theone of the promising materials for THs because of its flexibility and transparency. However, its
high sheet resistance required high input voltage (50 V) to obtain enough amount of Joule heat[1]. Recently, our lab developed a highly conductive CNT-TCF by using poly(p-styrenesulfonic acid) (PSS) as a dispersant and dopant of CNT [2]. In this study, CNT-PSS THs was
fabricated and its heating performance and stability to humidity and temperature were evaluated.
CNT-PSS-THs were fabricated as following. 1 mg of CNT were dispersed in PSS acidaqueous solution (2 wt%, 30 mL) by stirring and sonication. After sonication, the dispersion
was centrifuged. The supernatant was diluted with pure water and filtrated to obtain CNT-PSS-TCF. CNT-PSS (T=85 %, Rs= 67 Ω/sq) achieved Tmax =100 °C when 12 V was applied (Fig.
1). Next, the stability test was conducted. CNT-PSS-TCF and pure water were put in a sealedcontainer and left in a constant temperature bath at 85 °C. As a comparison, the humidity testof CNT-HNO3, CNT-SDBS, CNT-PSS-Na were also conducted. Humidity test was conducted
for 5 times on each CNT-TCF. After the 1st humidity test, the resistance of CNT-PSS increasedby 1.3-fold compared to its initial value (Fig. 2). After the 5th humidity test, the resistance of
CNT-HNO3 increased by 2.3-fold while the increase resistance ratio of CNT-PSS stabilized at
1.35 which was almost the same value as those of non-doped samples; CNT-SDBS (1.39) and
CNT-PSS-Na (1.38). No correlation was observed between the changes in ID/IG and resistanceincrease. Changes in the CNT network structure was carefully examined and discussed.

Fig.1 CNT-PSS transparent heater(a) Image (b) Heat performanceFig.2 Resistance of CNT-PSS during the
1st humidity test

[1] D.T.Papanastasiou et.al., Adv. Funct. Mater, 30,1910225 (2020).
[2] R.Xie et.al., Carbon, 164, 150 (2020).
Corresponding Author: S.Noda Tel:, Fax:㸩81-3-5286-2769, E-mail: noda@waseda.jp111

2P-29Aqueous electrolyte batteries using the encapsulation properties ofsingle-walled carbon nanotubes○Yuna Yokoya, Yosuke Ishii, Shinji Kawasaki
Department of Life Science and Applied Chemistry, Nagoya Institute of Technology,
Nagoya 466-8555, Japan

Lithium-ion batteries (LIBs) with high energy density are widely used. However, LIBs havethe problems of (1) flammability and (2) high cost. Therefore, in recent years, aqueous
secondary batteries have been attracting considerable attention because they are much safer
than LIBs. Furthermore, if we can use organic compounds and iodine, which are abundant innature, as electrode materials, we can reduce the cost. However, quinone organic compounds
and iodine have the problems of poor electrical conductivity and insufficient charge-discharge
cyclability. We anticipated that encapsulating these active materials in single-walled carbon
nanotubes (SWCNTs) would offer an effective solution to the problems. Here, we propose two
aqueous solution-based secondary batteries that utilize the encapsulation properties of
SWCNTs. The first is a zinc-iodine battery and the second is a quinone-iodine battery (Fig. 1).
For zinc-iodine battery, zinc metal and porous carbon materials are usually used as the anodeand the cathode, respectively. However, the cycling performance of the battery is usually notvery good because the porous carbon materials cannot hold iodine electrode active species very
firmly. We showed that SWCNT zinc-iodine battery shown in Fig.1 has good cyclability.[1]We also confirmed that charge-discharge cycling performance of quinone-iodine battery is
greatly improved by SWCNTs.[2] In the previous study, phenanthrene quinone (PhQ) andanthraquinone (AQ) were used as anode active materials. Here, we report that we can improvethe electromotive force of the quinone-iodine battery by using 1,5-diaminoanthraquinone (1,5DAAQ) and 2,6-diaminoanthraquinone (2,6-DAAQ), which have lower redox potential.

Fig. 1 Schematic pictures of (right) zinc-iodine battery and (left) quinone-iodine battery.
Al-zubaidi, Y. Yokoya, et al.,                      et al., Safe, economical and fast-charging secondary batteries using single-walled carbon nanotubes, J.
Appl. Phys., 58, SAA02 (2018).

Corresponding Author: S. Kawasaki
Tel: +81-52-735-5221,
E-mail: kawasaki.shinji@nitech.ac.jp112

2P-30
Selective monolayer growth of WS2 nanoribbons on WxOy nanowires○Hiroo Suzuki1, Misaki Kishibuchi1, Soya Ochiai1, Zheng Liu2, Yasumitsu Miyata3 andYasuhiko Hayashi1
1Graduate School of Natural Science and Technology, Okayama University, Okayama
700-8530, Japan
2
Innovative Functional Materials Research Institute, National Institute of Advanced Industrial
Science and Technology (AIST), Tsukuba 305-8565, Japan3
Department of Physics, Tokyo Metropolitan University, Hachioji 192-0397, Japan
Transition metal dichalcogenides (TMDCs) are promising two-dimensional (2D) materials
for next-generation optoelectronic devices; they can also be a platform for further advances inphysics. Structuring 2D TMDC sheets as nanoribbons has tremendous potential for electronic
state modification. The two strategies for the synthesis of TMDC nanoribbons can beconsidered. One is top-down, and the other is a bottom-up process. The top-down approach by
the conventional lithography technique is frequently used, however, there is a great advantage
in the bottom-up process in terms of the cleanness of the surface and edge.
In this research, we have investigated the growth of WS2 nanoribbons by chemical vapor
deposition (CVD), which is a bottom-up process. The cold-wall CVD system with the infrared
gold image furnace was established for TMDC growth. The aqueous solution of Na2WO4 was
employed as a W source for WS2 and deposited on SiO2/Si substrates by spin-coating. The
vapor of (t-C4H9)2S2 was introduced to a CVD chamber as an S source. From the systematicinvestigation of CVD growth, we found that the fiber-like materials can be grown with arelatively low (t-C4H9)2S2 supply. The atomic
force microscopy (AFM) revealed that the fibers
are around 3 nm in thickness, which is thicker
than monolayer WS2. The fibers showed bothalmost the same Raman and photoluminescence(PL) peaks as monolayer WS2. The
cross-sectional scanning transmission electron
microscopy (STEM) observations revealed thepresence of monolayer WS2 nanoribbons grownon the WxOy nanowires. This method realized thehigh monolayer selection yield on a large scale
and the growth of long (~100 µm) WS2
nanoribbons. Regarding the growth mechanism,
we supposed that the supply of source atoms fromthe vapor-solid bilayer and the chemical reaction
at the atomic-scale interface might cause theself-limiting
growthmechanism.
Opticalspectroscopy
andelectricaltransport
measurements characterized the electronic state of
WS2 nanoribbons.
Fig. 1. (a)Illustration of WS2
nanoribbons grown on WxOy
Corresponding Author: H. Suzuki
nanowires. (b) PL mapping of WS2
Tel: +81-86-251-8133
nanoribbons.
E-mail: hiroo.suzuki@okayama-u.ac.jp1132P-31
Growth and anisotropic optical responses of MoS2 nanoribbons‫ۑ‬Masahiko Kaneda1, Hong En Lim1, Kazuki Hashimoto1, Yusuke Nakanishi1,
Takahiko Endo1, Kenji Watanabe2, Takashi Taniguchi3, Yasumitsu Miyata1
1

Department of Physics, Tokyo Metropolitan University, Hachioji, 192-0397, Japan
2
Research Center for Functional Materials, NIMS, Tsukuba 305-0044, Japan
3
International Center for Materials Nanoarchitectonics, NIMS, Tsukuba 305-0044, Japan
Recent advances in the growth technique of transition metal chalcogenides (TMDCs) enable
the formation of structurally-controlled TMDC nanoribbons (NRs) and their superlattices [1,2].
The TMDC NRs are expected to provide a 1D-2D crossover system to study a wide variety ofphysical properties including electron transport, optical responses, and thermal properties.
However, the study of such properties is still limited due to the short length of the NRs. Herein,
we report the growth of long-length TMDC NRs and their anisotropic photoluminescence (PL)properties.
Long-length, NRs of monolayer MoS2 were grown by metal-organic CVD [2]. First, aribbon-shaped monolayer MoSe2 core with dimensions of 2×20 Pm was grown on a Si substrate.
Next, the chalcogen source was switched from Se to S. This generates the MoS2 NR growing
around the MoSe2 core, forming a MoS2/MoSe2 in-plane heterostructure (Fig. 1a). From Fig.1bd, the MoS2 NR shows the brightest PL intensity when the polarization direction of the linearlypolarized laser was aligned in parallel to the ribbon axis at 0°. In contrast, such polarization
dependence was not observed in that of MoSe2 (Fig.1e). This implies a significantly reduced
1D geometry of the MoS2 fabricated. From the similar trait reported in WSe2 NRs [3], theanisotropic PL response observed can be explained by modulation of optical absorption
coefficient due to the depolarization effect [4,5]. Our results present a useful way of studying
the correlation between structure and physical properties of monolayer TMDCs.

Fig. 1. (a) Structural model and optical image of the MoS2 NR grown, surrounding the ribbon-like MoSe2 core. T
refers to the angle between the polarization direction of the incident laser and the ribbon axis. Scale bar is 10 Pm.
(b, c) PL intensity maps of MoS2 (1.8 eV) irradiated at the polarization angle of 0° and 90°. Scale bars are 1 Pm.
(d) PL spatial intensity profiles of MoS2 (1.8 eV) and (e)PL spatial intensity profiles of MoSe2 (1.56 eV) irradiatedat the polarization angle of 0° and 90°[1] S. Xie  .,   359, 1131-1136 (2018), [2] Y. Kobayashi  .,    13, 7, 7527̽7535 (2019)[3] H. E. Lim  .,      . (2021) DOI: 10.1021/acsanm.1c03160. [4] H. Ajiki and T. Ando,  201, 349-352 (1994), [5] S. Uryu and T. Ando,   74, 155411 (2006).
Corresponding Author: Y. Miyata, Tel: 042-677-2508, E-mail: ymiyata@tmu.ac.jp114

2P-32         

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2P-33
MD evaluation of thermal conductivity of double layer hBN ribbon at
different geometries using energy exchange eHEX algorithm.
○Wataru Yuhara1, Tatiana Zolotoukhina1
1

Department of Mechanical Engineering, University of Toyama, Toyama 930-8555, Japan

Materials with high thermal conductivities (κ) are valuable to solve the challenge of waste
heat dissipation in highly integrated and miniaturized modern devices. Materials with highthermal conductivities (κ) are one of the key solutions to this challenge. All boron nitride(BN) materials, including single atomic layer (1L) BN, are electric insulators and considered
as candidates for waste heat dissipation in power chips as both an insulating layer as well as aheat spreader for local hotspots with high heat flux. Bulk cubic (c) and hexagonal (h) BN
crystals are good thermal conductors with κ of Ң690 and 420 W/mK at room temperature [1].
It was reported that high-quality and surface-clean 1L hBN had a κ of 751±340 W/mK [2].
This κ increase with reduced thickness down to the atomic level is attributed to a decrease in
the number of phonon branches and states. We investigate the thermal conductivity of 2L hBN
samples as related to the in-plane & out-of-plane energy transfer channels, coupling to thesample size and layer interaction. The 1 and 2 layers hBN samples with AA stacking of single
and double-width were used. The eHEX [3] energy exchange algorithm was utilized inmolecular dynamics (MD) simulation to maintain stable heat flow.
The hBN layers were of the 1440 x 173.52 (347.04, double width in y) Å size with AA
stacking and Δz=3.3 Å distance between layers. We utilized the eHEX energy exchange
algorithm at periodic boundary condition in the x-direction with varying periodicity in y.
Calculations were carried in LAMMPS. The conduction area was Lx/2 in the x-direction,
heating and cooling areas were taken to be 8 Å wide. The thermal conductivity of the samples
with x, y periodic BC was found to be low. Ribbon samples of 2 different widths gave valuesof κ varying between 100 and 800 W/mK with time. Increased width of nanoribbon was
associated with a better balance between components of the in-plane values of κ.

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Fig1 Thermal conductivity in hBN 2 layer interacting system (T=300 K, conduction area in x) [1] P. Q. Jiang, X. Qian, R. G. Yang, and L. Lindsay, Phys. Rev. Mater. 2, 064005 (2018).
[2] Q. Cai, D. Scullion, W. Gan, A. Falin, S. Zhang, K.Watanabe, T. Taniguchi, etc., Sci. Adv., 5, eaav0129 (2019).
[3] P.Wirnsberger, D.Frenkel, C. Dellago, J. Chem.Phys., 143, 124104 (2015).
Corresponding Author: T. Zolotoukhina
Tel: +81-76-445-6739, Fax: +81-76-445-6739,

E-mail: zolotu@eng.u-toyama.ac.jp

116



2P-34Temperature Dependency on the Layer Spacing of Graphene Oxide
Polyethyleneimine Composite Membranes○Norihiro Fukaya1, K. Kanishka H. De Silva2, Masamichi Yoshimura2, Hiroya Tanaka1
1

2

Toyota Central R&D Labs., Inc., Nagakute 480-1192, Japan
Graduate School of Engineering, Toyota Technological Institute, Nagoya 468-8511, Japan

Two-dimensional membranes have attracted much interest in the filtering and transport ofchemical and molecular species [1, 2]. Graphene oxide (GO) has huge potential because its
permeability and selectivity can be controlled with its functional groups. In particular, theadaptation capability has been programmed in the membrane formed by GO and
Polyethyleneimine (PEI). In this presentation, we study temperature dependency on theinterlayer spacing of the GO-PEI membranes to prove its suitability of selective ion
permeability and water permeability.
The membranes were prepared by vacuum filtration of suspension of GO (0.1 mg/mL) andPEI (2 mg/mL) on filters (Anodisc, pore size 100 nm). For reference, we also made GO
membranes (w/o PEI) via the same process. Figures 1a and 1b show XRD spectra of GO and
GO-PEI membranes heated at different temperatures in air, respectively. In Fig. 1a, peak
position shifts to wide angle with the increase of temperature. This means that the interlayer
spacing of GO decreases with the increasing temperature due to the removal of oxygen groups.
In Fig 1b, the peak of the curves is located at a lower angle (5~7q) due to the insertion of
PEI between the GO layers. In addition, a new peak appears around 22q from 150℃ to 200℃.
This angle coincides with reduced GOs. It can be understood that the PEI enhanced the
reduction of GO, and reduced GOs were obtained at lower temperatures than those w/o PEI.
In conclusion, we explored the temperature dependency of interlayer spacing of the GO and
GO-PEI membranes via variable temperature XRD analysis. Moreover, we reveal that PEI
plays
y an important role in removingg the oxygenyg ggroups in GO.

Fig. 1. XRD patterns of (a) GO and (b) GO-PEI heated at different temperatures (r.t.= room temperature).
[1] D. V. Andreeva et al., Nat. Nanotechnol. 16, 174 (2021).
[2] H. Huang et al., J. Membr. Sci. 572, 12 (2019).
Corresponding Author: N. Fukaya
Tel: +81-561-71-8137, E-mail: fukaya@mosk.tytlabs.co.jp1172P-35
Effect of iron ion beam irradiation on MoS2 fluorescence○Takumi Hidaka1,2, Kosuke Nakamura1, Tomoaki Nishimura2, Kazuyuki Takai1,2
1Graduate School of Science and Engineering, Hosei University, Tokyo 184-8584. Japan
2
Research Center of Ion Beam Technology, Hosei University, Tokyo 184-8584. Japan

Intensity (arb.unit)A

D/A

In 2D material, defects and impurities significantly affect the electronic properties comparedto 3D materials due to its low-dimensional structure. Meanwhile, ion beam implantation is oneof the methods that can quantitatively and reproducibly introduce defects and impurities intomaterials. We can achieve the maximum implanted ion distribution on 2D materials by using asacrificial layer [1]. It is not well known yet how chemical properties of the implanted ion
affects on 2D materials in spite of many reports on the ion-dose dependence on 2D materials.
In this study, Fe+ as a magnetic impurity that can cause spin scattering were introduced by ion
beam irradiation into 1L-MoS2 in which fluorescence strongly correlates with the degree of
freedom of spin. The irradiation effects on structural and electronic properties were investigatedusing Photoluminescence (PL).
Cr / NaCl of 10 nm / 250 nm was deposited as a sacrificial layer on 1L-MoS2 obtained by thecleavage method on a SiO2 / Si substrate. The film thickness of the sacrificial layer was
optimized using Monte Carlo simulation for Fe+ distribution by SRIM2013. Fe+ irradiation to
the sample was performed at an acceleration voltage of 200 keV with a dose of 1012, 1013 cm-2.
MoS2 before and after Fe+ irradiation was measured by low temperature PL at 77 K using aspectrometer (LabRAMHR, Horiba).
In addition to the characteristic peaks of MoS2: A (1.89 -1.91 eV) and B (~2.06 eV), the Dpeaks (1.71 - 1.78 eV) which does not appear at room temperature also appeared at 77 K after
the irradiation (Fig. 1). The D peaks are attributed to the physisorption of O2 and N2 in the air
at the S defects introduced by Fe+ irradiation, resulting in the formation of new defect levels[2]. The D / A ratio increased as the irradiation dose increased (Fig. 2). This is attributed to theincrease in the amount of adsorbed molecules caused by the increase in defect sites due to Fe+
irradiation. All the peaks slightly shifted to the higher energy side by Fe+ irradiation (Fig.2).
This suggests that the lattice constant changes due to the compressive strain caused by the
introduced defects, resulting in the changes of the band gap.
3
Pristine

1.5

D

position (eV)

0

12

10

1013 B
11.55

1.75

1.95

2.15

2.1

B
1.9
1.7

A
D

13
Pristine
12
10
12
-2
Log [Dose (cm )]Energy (eV)Fig. 1 PL spectra for MoS2 before and after
Fe+ irradiation at 77 K
[1] K. Nakamura et al, FNTG Symposium (2019)[2] S. Tongay et al, Sci. Rep. (2013)

118

14

Fig. 2 (a) Change of D peak intensity (b)ࠐ), B(‫)ݔ‬, D(□)
change of peak position of A(ࠐupon Fe+ irradiation at 77 K

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120

2P-38
Electrical Conductivity of Nanodiamond Hydrogels #1:
their measurements by using interdigitated electrodes.
○ Kazuya Yamaguchi1, Masaya Yabuki1, Toshihiko Tanaka1, Tetsuya Aoyama2,
Yasuhiro F. Miura3, Yoshiya Akagi3, Eiji Osawa4
1

Department of Chemistry and Biochemistry, National Institute of Technology,
Fukushima College, 30 Aza-nagao, Tairakamiarakawa, Iwaki, Fukushima, 970-8034, Japan2
Ultrahigh Precision Optics Tech. Team, RIKEN RAP, 2-1 Hirosawa, Wako, Saitama, Japan
3
Hamamatsu University School of Medicine, 1-20-1 Handayama,
Higashi-ku, Hamamatsu City, Shizuoka, Japan
4
Nano Carbon Research Institute Ltd., Asama Research Extension Center,
Shinshu University, 3-15-1 Tokida, Ueda, Nagano, JapanThe solid surfaces of diamond often take mobile electrons due to its negative electron
affinity and they have attracted much attention to apply them to device applications including
sensors.1 The interfacial water on the surfaces also have a high conductivity due to their
protons.2 We consider that electrons or protons in their interfacial water also account for the
conductivity of the hydrogels.
Recently we have found the high electrical conductivity of nanodiamond (ND) hydrogels.
To reduce the sampling amount of ND, we have developed a measurement method using acommercial interdigitated Au electrodes (Metrohm Drop Sens IDEAU200, Spain). They
consist of two interdigitated Au electrodes with two connection tracks on a ceramic substrate.
The substrate dimensions are small : L 22.8 mm x W 7.6 mm x H 1 mm and the interdigitatedarea is only 6.5 x 6.5 mm2. Hence, we can measure the conductivity of a tiny liquid droplet
down to ~0.03g, if their calibration are done with some standard KCl solutions; a cell constantand the resistance of Au electrode (nearly 15) are obtained.Fig.1Impedance spectra wererecorded with an LCR meter from 1 to 106 Hz and the resistance of Au electrode wassubtracted, thus the DC conductivity of samples being calculated (up to at least 1.9 mS/cm asshown in #2 presentation.), which is significantly larger than those reported value for pellets
of diamond particles with saturated water vapour.

Figure. 1 Measured resistance vs. specific resistance of the standard KCL solutions.
[1] T.Kondo, I. Neitze, V. N. Mochalin, J. Urai,1 M. Yuasa, Y. Gogotsi, J. Appl. Phys. 113, 214307 (2013)[2] V. G. Artemov,E. Uykur, P. O. Kapralov, A. Kiselev, K. Stevenson, H. Ouerdane, M. Dressel, J. Phys. Chem.
Lett. 2020, 11, 3623−3628.
Corresponding Author:Toshihiko Tanaka / Tel: +81-246-46-0810 / E-mail: ttanaka@fukushima-nct.ac.jp1212P-39
Electrical Conductivity of Nanodiamond Hydrogels #2:
their temperature dependence○ Masaya Yabuki1, Kazuya Yamaguchi1, Toshihiko Tanaka1, Tetsuya Aoyama2,○ Yasuhiro F. Miura3, Yoshiya Akagi3, Eiji Osawa4
1

Department of Chemistry and Biochemistry, National Institute of Technology,
Fukushima College, 30 Aza-nagao, Tairakamiarakawa, Iwaki, Fukushima, 970-8034, Japan2
Ultrahigh Precision Optics Tech. Team, RIKEN RAP, 2-1 Hirosawa, Wako, Saitama, Japan
3
Hamamatsu University School of Medicine, 1-20-1 Handayama,
Higashi-ku, Hamamatsu City, Shizuoka, Japan
4
Nano Carbon Research Institute Ltd., Asama Research Extension Center,
Shinshu University, 3-15-1 Tokida, Ueda, Nagano, Japan
Here we have measured the high electrical conductivity of nanodiamond(ND) hydrogels1
by using interdigitated electrodes explained in #1 presentation. The measured values havereached at least 1.9 mS/cm (presumably up to 7mS/cm) at room temperature, being
significantly higher than those reported values for the interfacial water of pellets of diamondparticles (5, 40, 80, 120,or 200 nm) with saturated water vapour.2 What are the charge carriers
for our cases? Are these similar to those for the pellets? Or are there any difference?
We
concentratedanND@
solution( NanoAmando ,NanoCarbon
Research Institute Ltd., containing
EDIANsfrom 2.5 to ~35wt% andcooled while its conductivity was
being measured by an LCR meter. The
conductivity decreased as shown in
Fig.1, its slope indicating nearly 0.21
eV of activation energy. This value isslightly different from 0.17 eV thatreported2, where Artemov et al.
suggested protons as carriers becauseof the value. Lower temperatures givea larger slope, indicating significant
larger activation energy nearly 0.7 eV.
Hence, we have to determine the Figure 1. Temperature dependence of the electricalcarriers carefully. One possibility is conductivity   S/cm  of the ND hydrogel (~ 35%)
proton conduction and we have to through cooling it.
explain the larger slope in this case. Otherwise, we have to postulate another possibility. Petit,
et al. demonstrated the solvated electrons in the interfacial water of hydrogenated ND and
NanoAmando is similar to hydrogenated ND because of their rich CH terminations.3 Hence,
we also have to consider this possibility. We will discuss them here.
[1]E. Ōsawa, D. Ho, H. Huang, M.V. Korobov, N.N. Rozhkova, Dia. Rel. Mat. 18 , 904(2009)[2]V. G. Artemov, E. Uykur, P. O. Kapralov, A. Kiselev, K. Stevenson, H. Ouerdane, M. Dressel, J. Phys. Chem.
Lett. 2020, 11, 3623(2020),;[3]T. Petit, et al., J. Phys. Chem. C, 121, 5185(2017)
Corresponding Author:Toshihiko Tanaka / Tel: +81-246-46-0810 / E-mail: ttanaka@fukushima-nct.ac.jp

122

発表索引
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126

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         A  $ $     &$*               -90 
 -                        $ &  JJ---0>0J*  K  A  F0       F J           02022 年 2 月 23 日 発行

第62回フラーレン・ナノチューブ・グラフェン総合シンポジウム
講演要旨集
㲉フラーレン・ナノチューブ・グラフェン学会㲊
〒464-8601 愛知県名古屋市千種区不老町
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未来エレクトロニクス集積研究センター 大野研究室内
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名古屋大学消費生活協同組合

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ஸশဗઝ฾॒๦
㕲಑ଭӨԔՂԑԱԋՇ ؄‫׮י‬؉՛‫؞ؖנ׾‬NIRvana® HS؄‫׮י‬؉՛‫׾‬ӼӿӺӨԶՄՇӨӲӨԶՉՀՀӨԀӾӺՌӿӻӼӨՄԺՌԵՀՇӨӴӻӼӺӺӨԶՄՇӨӲӨӼӺӺՌӼӺӺӨՄԺՌԵՀՇӨӴ໣ఀ֩ၥ‫־‬ഞ֖‫ؗ‬՛‫׾‬ԔՂՈԵԷՆԱՈԵӨԦԸԺՀԵӨԡԵԱԴӨӲԔԦԡӴӨՁՃԴԵဩఐ
ؓ‫׶ؠ‬ԡԞԔ

࿃ၥ‫־‬ഞ֖‫ׯי؃‬ԤԢԌӽӸӺไ໗

量子効率グラフQuantum Eﬃciency (%)‫ח‬،‫צ؟‬՛‫ب؜׬‬፯Ք؊‫פ׸؀׽מ‬ଅ൩ԟԙ‫ؖי‬՛‫ץب׭‬ਸֲ‫ؠ׽פ؏׮‬Քࡴഓஶ౒ຍ‫ؖי‬՛‫ץب׭‬ਸֲ‫ؠ׽פ؏׮‬Ք໤ጉဃཕԟԙ‫ؖי‬՛‫ץب׭‬ਸֲ‫ؠ׽פ؏׮‬Ք࿵໲৑໐ᅑೕ୯‫ؖי‬՛‫ץب׭‬Քඳᆀཉኜ‫ؖי‬՛‫ץب׭‬ՔԔՂӷԥԺՊՃ‫ؖי‬՛‫ץب׭‬Ӡ֩֨

100
90
80
70
60
50
40
30
20
10
0.8

0.9

1.0

1.1

1.2

1.3

1.4

1.5

1.6

1.7

Wavelength (μm)౗ዻ
640 x 512 x InGaAs

素子サイズ
波長範囲

20μm x 20μm

FRAME

1

FRAME

0.9 〜 1.7 μm-55℃(-50℃空冷 )

-80℃

-190℃

ダークチャージ

700 e-/p/sec

300 e-/p/sec<8 e-/p/sec

読み出しノイズダイナミックレンジ
フレームレート<60 e-rms<120 e-rms

15 e-rms

インターフェース

USB3.016 Bit (>15Bit@1 素子 )250 fps

110 fps

2.77 fps@250KHz
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2

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冷却温度

ԝԔԡՊԱՂԱԄԀӾӺԙԝԝԔԡՊԱՂԱԄԀӾӺREADOUTԝԔԡՊԱՂԱӨԒԢREADOUT‫ؠ׼ؗ‬

Integrate While Read (IWR) mode
for maximum duty cycle

ZZZSLMFRMS‫ بי׵ء׻‬Ք ‫ؘ׭‬؆‫ب‬খಠवೂӨӨ،‫׹بؖؠ׹׮بיب׽׮ب؟‬ÆӻԁӺӷӺӺӻӽӠဪੜဒሟဥતဪཕ༂ӨӽӷӾӷӽӨཕ༂‫י‬՛‫׽׮‬ӨӨ ӨԣԏԙӨӺӽӷԀԁӺԃӷӺԀӽӻӠԐԋԧӨӺӽӷԀԁӺԃӷӺԀӽӼ∈⇭∑⇧⇍∙⇞ ⊡⇟∄∞⇮↙⇭⇜⇊∙↚ቇҥદ˺⊡‴⁄″⁀⁅⁁⁀ ឬ᪦ඬ∁∈⇞⇰⇊⇜∞
ᧈⅾↃग़᫑ⅳ↎↏ⅳ↕ⅹ↹↭ↈ‴⁄″⁀⁅⁁⁀ឬ᪦ඬ∁∈⇞⇰⇊⇜∞↖ૼ↎↙∈⇭∑ⅻᛓဃↆ↭ↆ↎⅛ɼ↙ཎᧈ‣†ᩓൢ⇎⇳∑⇔∞ⅺ↸ឬ᪦ඬਰѣ↧↝‫٭‬੭јྙⅻ‫ˌ‗‧‫‬ɥ℉‒໯ᬛ↙⇎⇳∑⇔∞∓⇟ⅻ‫ↄݱ‬ⅾ⅚‫↎ↆܭܤ‬ਰࠢⅻࢽ↸↻↺⅛․†ᡫࠝ↖↞⅚෩˳↝ᆔ᫏↚↷→↕ਰࠢⅻ‫ↆܭܤ‬ᩊⅳ⅛
℉‒வˑ⇁‫٭‬ⅷ↕↱ɟ‫↝ܭ‬ਰࠢ⇁̬↓ೞᏡⅻ↓ⅳ↕ⅳ↺⅛
‥†⇞∋∞∑≋⁩⁓⁦⁦⁷⁥⁗⁕≌↚↷↺ႆਰСࣂⅻӧᏡ
℉‒⁆⁡⁦⁓⁞˴⇞∋∞∑↖ↂ↝ϼྸⅻ‫ܦ‬ʕↈ↺↗ⅳⅵऴ‫إ‬ⅻᛯ૨↚ਫ਼᠍↖ⅼ↺⅛․•⁝›⁬ឬ᪦ඬ∁∈⇞⇰⇊⇜∞‴⁄″⁀⁅⁁⁀‒⁅⁁⁀※‸※‷⁄‒⁅‸⁊․‧•„‧‧•…•⁝›⁬ឬ᪦ඬ∁∈⇞⇰⇊⇜∞‴⁄″⁀⁅⁁⁀‒⁅⁁⁀※‸※‷⁄‒⁅‸⁊‣‧•››

ɼ↙⇈⇽∐⇗∞⇝∍∙
Ў૝⇑∞∂∙⇰⇴⇧∋∞⇼ ஊೞ᫊૰ ໯ೞ᫊૰ ⇡∏∅⇩⇕ ⇡∇∙⇮ ज़ή˳ ᚡ᥵஬૰ᄬࣱብ ብ஛ϫ᣿ ᣠ҄ᤧ ᣿‫ޓ‬ᣠ҄ཋ ⇝∐⇑ ⇈∑∅⇰ ⇑∞∂∙⇼∏⇩⇕∃∐∄∞ ∏⇬⇩⇕⇟ ᙌኡ ⇻⇇∙⇭∞⇝∍∙ᄂᄶд ᩓ൷ ⇻⇉∏∞ ήᚑ‫ ۥ‬ᚑ‫ٳ˳ ∙⇧⇕∕ ۥ‬ᚮૺᕤ ഫᄶⅼብ ⇝∉∙⇽∞Ҟ‫ ˳ݰ‬ᩓ‫ؕ܇‬Ⴔ ෩୒ ᝮ᣿‫ ޓ‬᣿‫ܰ ޓ‬ჽ ⇥⇊∊ ႆᣞᓏ᫏ ↌↝˂ʐ҄⇎∄∑⇞∍∙ᙌд ᠾᕤ ⇮⇰∞ ∏⇬⇩⇕⇟ မ᩿෇ࣱд ⇕∐∞∆ ʐ෩ ↌↝˂᪥ᮏᅜෆ㈍኎⥲௦⌮ᗑᮾிᮏ♫䠖䛈㻝㻟㻢㻙㻜㻜㻣㻝㻌ᮾி㒔Ụᮾ༊டᡞ㻝㻙㻞㻤㻙㻢 䝍䝙䝡䝹㻟㻲㻌㻌ᢏ⾡≀ὶ䝉䞁䝍䞊䠖䛈㻞㻣㻞㻙㻜㻝㻠㻢㻌༓ⴥ┴ᕷᕝᕷᗈᑿ㻞㻙㻝㻙㻥㻌㻌኱㜰ᨭᗑ䠖䛈㻡㻟㻟㻙㻜㻜㻟㻝㻌኱㜰ᗓ኱㜰ᕷᮾᾷᕝ༊すῐ㊰㻝㻙㻝㻙㻟㻢㻌᪂኱㜰䝡䝹⚟ᒸႠᴗᡤ䠖
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