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Fundamental Principles Underlying the Hierarchy of Matter:
A Comprehensive Experimental Study• Organization
This project is being carried out as a collaboration involving eight participating laboratories, in which
we treat the hierarchy of matter from hadrons to biomolecules with three underlying and interconnected
key concepts: interaction, excitation, and heterogeneity. The project consists of experimental research
conducted using cutting-edge technologies, including lasers, signal processing and data acquisition, andparticle beams at RIKEN RI Beam Factory (RIBF) and RIKEN Rutherford Appleton Laboratory (RAL).

• Physical and chemical views of matter lead to major discoveries
Although this project is based on the physics and chemistry of non-living systems, we constantly keep
all types of matter, including living matter, in our mind. The importance of analyzing matter fromphysical and chemical points of view was demonstrated in the case of DNA. The Watson-Crick model of
DNA was developed based on the X-ray diffraction, which is a physical measurement. The key feature ofthis model is the hydrogen bonding that occurs between DNA base pairs. Watson and Crick learned abouthydrogen bonding in the renowned book “The Nature of the Chemical Bond,” written by their competitor,
L. Pauling, who was a leading authority on chemical bonding. This important lesson in history teaches usthat viewing matter from physical and chemical perspectives can lead to dramatic advances in science.

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• Hierarchy of Matter: Universality vs. Diversity
We believe that the behavior of matter, including biological systems, can be understood throughphysical laws. P. Dirac, a great physicist, stated this universality as follows: “once we know theunderlying physical laws, the rest is chemistry.” On the other hand, P. W. Anderson, another great
physicist, claimed that the interactions among multiple components in complex systems create entirely
new properties in each layer of the hierarchy, with his famous phrase “More is different”. This means thatthe science governing each layer is different, and it is not until we understand this diversity that weunderstand the universal principles completely. Therefore, we have selected “interaction” as the first key
concept of this project. In addition, we selected “excitation” and “heterogeneity” as the other important
key concepts to understand diversity in the hierarchy.

• Three Key Concepts: Interaction, Excitation, and Heterogeneity
The importance of these three key concepts is well illustrated by the photochemical reaction system,
involved in photosynthesis. First, the photosynthesis proceeds in the thylakoid membrane, which has aheterogeneous structure. This heterogeneity is essential for the emergence of the functionality of themembrane. Excitation by light is the most important step in photosynthesis. Finally, important processes,
including electron transport and ATP synthesis, are controlled by various interactions.

㸫4㸫• Three Key Concepts and Sub-projects
The three key concepts are associated with three sub-projects: “Interaction in matter” lead by Dr. Ueno,“Excitation in matter” lead by Dr. Azuma, and “Heterogeneity in matter” lead by Dr. Kim. As mentioned,
the “Interaction” sub-project is the core of this project. To comprehensively understand the nature ofinteractions that take place in each layer, it is essential to collaborate with theory groups. The knowledge
obtained by the “Interaction” sub-group will be applied toward the basic science of excitation. The“Interaction” sub-project investigates the ground state of systems, and the “Excitation” sub-projectfocuses on the excited states of systems. The results obtained by these two sub-projects will be expanded
towards the development of functional materials by the “Heterogeneity” sub-group. A unique point of thisproject is that almost all members participate in more than two sub-projects, which enhances
comprehensive understanding of these concepts.

• Interaction in Matter
The “Interaction” sub-group investigates the diversity of phenomena caused by interactions that occur
in each level in the hierarchy of matter. The strong interaction and the electromagnetic interaction giverise to a variety of phenomena depending on many-body effects, geometry, dimensionality, external
conditions and so on. The interactions studied by each team range from the strong interaction between
quarks to the van der Waals interaction between single-stranded DNA molecules, with a focus on how
interactions in systems with multiple degrees of freedom lead to a diversity of phenomena. This meansthat many-body effects and multiple degrees of freedom are key issues in every layer of the hierarchy.
• Excitation in Matter
Excitation is a key step for the emergence of functionality, but knowledge on this topic is surprisingly
limited. Thus, in this sub-group, we carry out three types of research on excitation, “Exploration of
undetected excited states” in deformed nuclei, “Verification of fundamental principles through excitedstates” in kaonic nuclei, and “Observation of excited state dynamics” in excited molecules in liquids, on
surfaces, and in vacuum. We study excitation over a wide range of energies, sizes, and time scales. At thesame time, we study universality as indicated by the large-scale deformations observed in both

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excited-state nuclei and proteins.
• Heterogeneity in Matter
Heterogeneity is an important spatial property for the emergence of functionality as well as achallenging research target that drives the development of cutting-edge measurement technologies. This
sub-group will apply the results of the “Interaction” and “Excitation” sub-groups toward the developmentof functional materials. In this sense, the “Heterogeneity” sub-group is closely tied to practicalapplications. The main topics investigated are superconducting doped diamond (as “Heterogeneity by
Atomic Scale Doping”), electrical double layers in the field effect transistors (as “Heterogeneity at
Molecular Interfaces”), and lipid membranes in solution (as “Heterogeneity in Biological Systems”),
which are tackled through a wide range of collaborations.
• Goal of the Project
The most important goal of the project is the construction of a new cross-disciplinary research network
based on the bottom-up style research activities at RIKEN, which will drive a dramatic evolution ofscience and lead to unpredictable by-products. This network includes ExpRes Dojo where we share, learn,
and report information on cutting-edge experimental technologies, primarily laser and signal processing
and data acquisition technologies. This consists of school-type meetings and workshops. An important
output of the ExpRes Dojo is the application of new technologies developed thorough the physics andchemistry research to biological systems. At the same time, we nurture young researchers with wider anddeeper views of matter. We believe that the scientific community is one where innovative discoveries are
frequently achieved by newcomers in different research fields. The present project will maintain thediversity of science at RIKEN and ensure an environment in which young researchers with highambitions can easily cross over the boundaries between disciplines.

Lead researcher
Dr. Reizo Kato㸫6㸫įŋÜůČņä$ęĠñľ

Heterogeneity at Materials Interfaces

Goal of the projectThis project aims at understanding and controlling structures and functions originated in heterogeneity

at a variety of interfaces that encompass (A) interaction of a single dopant with surroundings in solid andliquid materials, (B) structures, functions and reactions of molecular interfaces and (C) development of
new functional devices by controlling interface charge carries.



Organization
The corresponding three sub-projects, such as (A) Atomic-scale interfaces, (B) Molecular interfacesand (C) Device interfaces, make it realized by entanglement of research concepts and research resourcesamong world-leading laboratories in RIKEN Cluster for Pioneering Research (CPR) and top-levelresearch infrastructures in RIKEN Nishina Center (RNC).

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Heterogeneity at the interfaces
Heterogeneity at the interface between two different materials plays pivotal roles in transport of charge,

matter, and energy across the interfaces, chemical reactions and interactions, functions of materials anddevices, and biological activities in living systems. The heterogeneity is frequently associated withfunctions of the materials systems. For example, the doping that effectively modulates electricalproperties of various solids (semiconductor, metal, and superconductor) induces heterogeneous
distribution of atoms/molecules. The heterogeneity is also a key concept in the evolution of matter from
non-living matter to life. Field effect transistor and biological membrane are artificial and natural
examples of functional heterogeneous systems, respectively. The heterogeneity, where the periodicity is
missing to reveal gradients, is a challenging research target of the cutting-edge measurement technology,
mainly due to its structural and phenomenal complexity. Especially, we focus on the heterogeneity atinterfaces in various kinds of materials systems, regarding how it affects the functions accompanying
with the peculiar chemical/physical properties.

Lead researcher
Dr. Yousoo Kim

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THz-STM 1kâ[2]&Æ^ THz\¿>M@1 THz-STM "¼'' ² Ý]# THz yº¬1½-¦ªò#ð"Ø1ý©ðĂ1Ï.
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.óa$THz-STM #/&#°Ô1ln.
#«ûÔò")")rāì1) H. Mashiko et al., Nat. Commun. 9, 1468 (2018).
2) K. Yoshioka et al., Nat. Photon. 10, 762 (2016).
3) K. Yoshioka et al., Nano Lett. 18, 5198 (2018).

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I-2

藤田 誠
東京大学大学院工学系研究科応用化学専攻
113-8656 東京都文京区本郷7-3-1
mfujita@appchem.t.u-tokyo,ac,jp

分子科学研究所 特別研究部門
mfujita@ims.,ac,jp

Coordination Self-Assembly （配位駆動自己集合）
Molecular self-assembly based on coordination chemistry has made an explosive development in recent
years. Over the last >25years, we have been showing that the simple combination of transition-metal’ssquare planer geometry (a 90 degree coordination angle) with pyridine-based bridging ligands gives rise to
the quantitative self-assembly of nano-sized, discrete organic frameworks.

Representative examples

include square molecules (1990), linked-ring molecules (1994), cages (1995), capsules (1999), and tubes(2004) that are self-assembled from simple and small components. Originated from these earlier works,
current interests in our group focus on i) molecular confinement effects in coordination cages, ii) solution
chemistry in crystalline porous complexes (as applied to “crystalline sponge method”),[1] and iii) and giant
self-assemblies[2] (Figure 1), as disclosed in this lecture.

Figure 1. X-ray
structure of M48L96
complex.

Reference[1] Y. Inokuma, S. Yoshioka, J. Ariyoshi, T. Arai, Y. Hitora, K. Takada, S. Matsunaga, K. Rissanen, M.
Fujita Nature 2013, 495, 461-466.
[2] D. Fujita, Y. Ueda, S. Sato, N. Mizuno, T. Kumasaka, M. Fujita, Nature 2016, 540, 563.

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࣒ࣜ࢘-229 (229Th) ཎᏊ᰾ࡢ➨୍ບ㉳≧ែࡀ㏻ᖖࡢ keV ~ MeV ࢆ኱ࡁࡃୗᅇࡿ 8 eV ⛬ᗘ࡛࠶ࡿࡇ࡜ࡀศ࠿ࡗ࡚ࡁࡓ[1] (ᅗ 1)ࠋࡇࡢ 229Th ࡢᇶᗏ≧ែ࡜➨୍ບ㉳≧ែࡢ㛫ࡢ㑄⛣ࡣ 150
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᫬ィࢆୖᅇࡾࠊ3000 ൨ᖺ࡛ 1 ⛊ࡎࢀࡿ⛬ᗘࡢṇ☜ࡉࡀᮇᚅ࡛ࡁࠊ୍⯡┦ᑐㄽ࡟ࡼࡿ㔜ຊ࣏ࢸࣥࢩࣕࣝィ ࢆ฼⏝ࡋࡓ ᆅᏛ➼ࠊᛂ⏝࣭ᇶ♏ศ㔝࡛ᵝࠎ࡞฼⏝ࡀᮇᚅ࡛ࡁࡿ[2]ࠋ
 ࡇࡢບ㉳࢚ࢿࣝࢠ࣮   ࡜࠸࠺್ࡀࡣࡗ
ࡁࡾࡋ࡚ࡁࡓࡢࡣࡇࡢᩘᖺࡢࡇ࡜࡛࠶ࡾࠊࡑ
ࡢᑑ࿨ࡣᮍࡔᮍ☜ᐃ࡛࠶ࡿࠋࡘࡲࡾࠊ┤᥋ບ㉳ࡸගᏊᨺฟ⬺ບ㉳ࡢ ᐃࡀᡂຌࡋࡓ౛ࡣ
ᮍࡔ࡞࠸ࠋᒸᒣ኱ࢆ୰ᚰ࡜ࡋࡓࢢ࣮ࣝࣉ࡛ࡣ
᭱㏆ $ " 㧗㍤ᗘᨺᑕගࢆ฼⏝ࡋ࡚➨୍ບ㉳≧ែ࡬⬟ືⓗ࡞ບ㉳ࢆึࡵ࡚ᐇ⌧ࡋᅗ 1㸸 229Th ཎᏊ᰾‽఩ ࠊ⌧ᅾᇶᗏ≧ែ࡬ࡢ┿✵⣸እගᨺฟ⬺ບ㉳ࡢศග ᐃࢆ⾜ࡗ࡚࠸ࡿࠋᮏㅮ₇࡛ࡣࠊୡ⏺ⓗ࡞◊✲ࡢ≧ἣࢆྵࡵࠊᡃࠎࡢࢢ࣮ࣝࣉࡢ◊✲ࡢ⌧≧ࢆ⤂௓ࡍࡿࠋཧ⪃ᩥ⊩
[1] (#"$"%&!&'$       E. Peik and C. Tamm, Europhys. Lett. 61, 181 (2003).

[3] %'&!&'$   

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kandori@nitech.ac.jp<ODQJTHî,)í.1TÕÖ
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S@TÄjÕÖ,$' ÂÀ 
JTHÄjÕÖ VÈ alternating access model &Ï*)ëz Bì[1]N?Q ÆYa.1T)-4:8,0DQ3U`´|l)¿ÄjÕÖ ¯)alternating access model ÄjÕÖ,¼â´.MU7%VÄjÕÖ,0DQ3Uç '+ (% Ï) z A GBKÙ§N?Q)[1]
N?Q ¦] 0DQ3UR
IQ,Ê (2 5U@
áà,g)GBKÙ§É&W({ÕÖ,Û   ) ë Unbound, Bound,
Energized & Release statesì*N?Q&ÄjÕÖßÍ 0DQ3Uci«ë® 3  4 âì.1
T ÕÖ^¿s)«)bêj.1TJTH$nhh GB
KÙ§N?Q+bêjB@P/LJTH­¥fËÁ$Î [1-3]
SAH6TÌå¡Ø,Â)<ODQ£Ä)SAH6T ( 2002 <ODQSAH6T ³Î*3  bÜ\ "(SAH6T b_Xr¤=UQ¨µ,ä#)[4]¹Ñ© S
AH6T¶»,é<ODQJTHM2C9L,ÒÐ[1] Kandori et al. Chem. Rev. (2018) 118, 10646. [2] Inoue et. al. Nat. Commun. (2013) 4, 1678. [3]Kato et al. Nature (2015) 521, 48. [4] Kandori, Bull. Chem. Soc. Jpn. (2020) 93, 76.

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ࢆ⌮ゎࡍࡓࡵࡢ㔜せ࡞⣲㐣⛬࡛࠶ࡿࠋᮏࣉࣟࢪ࢙ࢡࢺ࡛ࡣࠊ࣊
࣊ࢸࣟ⏺㠃ศᏊ⣔࡟࠾ࡅࡿ㔞Ꮚ≧ែບ㉳࡜ࠊࡑࢀ࡟క࠺ᵝࠎ࡞࢚ࢿࣝࢠ࣮⣲㐣⛬ࡢ⌮ゎ࡜ไᚚࢆ┠ᣦࡋ࡚࠸ࡿࠋࡢ㑅ᢥⓗບ᭷ᶵⓎගࢲ࢖࣮࢜ࢻ࠿ࡽࡢⓎගࡣࠊ㟁ὶ࡟ࡼࡾᙧᡂࡉࢀࡓ୍㔜㡯ບ㉳Ꮚࡶࡋࡃࡣ୕㔜㡯ບ㉳Ꮚ
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ࡿࡇ࡜ࡀ㛗ᖺࡢ㔜せ࡞ㄢ㢟࡛࠶ࡾࠊᢏ⾡㠉᪂ࡀồࡵࡽࢀ࡚ࡁࡓࠋᮏ◊✲࡛ࡣࠊ㉮ᰝᆺࢺࣥࢿࣝ㢧ᚤ㙾 670 ࡟ࡼࡿ༢୍ศᏊⓎග

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⇥ගࡢࡳ⏕ࡌࡿ࡜࠸࠺᪂ࡋ࠸Ⓨගᶵᵓࢆぢฟࡋࡓࠋ
୍᪉ࠊ ࢆ⏝࠸ࡓᒁᡤ᣺ືศගἲࡢ㛤Ⓨࡣࠊࢼࣀࢫࢣ࣮ࣝ⾲㠃࣭⏺㠃࡟࠾ࡅࡿ໬Ꮫⓗ࡞᝟ሗᚓࡿࡓࡵࡢ㔜せ࡞ᣮᡓ࡛࠶ࡿࠋᮏ◊✲࡛ࡣࠊ ᥈㔪࡟ࡼࡿ࣐ࣛࣥಙྕࡢቑᙉ⌧㇟ࢆ฼⏝ࡋࡓ  ᥈㔪ቑᙉ࣐ࣛࣥศගἲ㸦 㸧ࢆ㛤Ⓨࡋࠊ༢୍ศᏊ᣺ື࣮ࣔࢻࡢ✵㛫ศᕸࢆྍど໬ࡍࡿࡇ࡜࡟ᡂຌࡋ
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௒ᅇࡣ࢝࢖ࣛࣝ࡞ᵓ㐀ࡀືⓗ࡟ไᚚฟ᮶ࡿศᏊ࣮ࣔࢱ࣮ࢆ⏝࠸࡚ࠊ ຠᯝ࡟ࡼࡿ෌ᵓᡂྍ
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[Pt(dmdt)2][Pd(dddt)2] Ì:>5LNÍ]#HOMO  LUMO "4DK8O 'iPc"¸0fs-!*Ì-#ÅZ©+!#47<>?9 Ñz©0~¬ -#ÓsR"[Pd(dddt)2] A2J?9Ñz·ÔEO=KJ3NhÌÕl¼0Àb[2]d#µPj­ DFT Â¶}Ós¸£É0_!Á 0¿ Xq*) ½r Diamond Light Source ! -`Ö¹q~ÒÓsR"¸£É0¥}-!e¸mÇ[FNBÂ¶0®A2J?9Ñz· 
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ISCOM2019, Tomar, Portugal, September 26 (2019): Plenary talk2) R. Kato, H. B. Cui, T. Tsumuraya, T. Miyazaki, and Y. Suzumura, J. Am. Chem. Soc., 139,
1770-1773 (2017).
3) B. Zhou, S. Ishibashi, T. Ishii, T. Sekine, R. Takehara, K. Miyagawa, K. Kanoda, E. Nishibori,and A. Kobayashi, Chem.Commun., 55, 3327-3330 (2019).
4) R. Kato and Y. Suzumura, submitted to J. Phys. Soc. Jpn.

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RI࣭㔜࢖࢜ࣥࣅ࣮࣒ࢆ⏝࠸ࡓᏛ㝿ⓗ㛤Ⓨ◊✲ᙜࢢ࣮ࣝࣉ࡛ࡣࠊ㝧Ꮚ㐣๫ Zr RI࡛ணゝࡉࢀ࡚࠸ࡿ≉␗᰾ᵓ㐀Ⓨ⌧ࡢ᭷↓ཬࡧࡑࢀࢆᑟࡃ┦஫స⏝ 㸦ከయຠᯝ㸧ࡢゎ᫂࡟ྥࡅࠊ◊✲ᐊ⊂⮬ࡢᢏ⾡㛤Ⓨ࡜ࡋ࡚ 1) GeV ࢚ࢿࣝࢠ࣮ RI ࣅ࣮࣒ࢆ⏝࠸ࡓ᪂つ࣮ࣞࢨ࣮᰾ศග⿦⨨ࡢ㛤Ⓨࢆ㐍ࡵࡿ୍᪉ࠊศ㔝㛫ᢏ⾡㐃ᦠ◊✲࡜ࡋ࡚ 2) 㔜࢖࢜ࣥࣅ࣮࣒ࡢ┤᥋ࢻ࣮ࣉ࡟ࡼࡿࢲ࢖ࣖࣔࣥࢻࡢ㉸ఏᑟᛶࡢ◊✲㸦ຍ⸨㸦♩㸧◊࡜ࡢඹྠ◊✲㸧ࠊ
࠾ࡼࡧ 3) ㉸ὶື He ୰ࡢ୙⣧≀ཎᏊࡀ♧ࡍ᥃ࡅ㞳ࢀࡓ྾཰࣭Ⓨගࢫ࣌ࢡࢺࣝࡢືⓗኚ໬࡟㛵ࡍࡿ◊✲㸦⏣ཎ◊࡜ࡢඹྠ◊✲㸧ࡢ஧ࡘࡢ ࣊ࢸࣟ⏺㠃 ◊✲ࢆྜࢃࡏࡓୗグࡢィ 3 ࡘࡢㄢ㢟ࢆ୰ᚰ࡟◊✲ࢆ㐍ࡵ࡚࠸ࡿࠋ௒ᅇࡣ㐍ᒎࡢ࠶ࡗࡓ 1) ࡜ᅄⱞඵⱞࡢ 2) ࢆ୰ᚰ࡟ሗ࿌ࡍࡿࠋ
1) ࡛ࡣ Zr ࡟ඛࢇࡌ࡚ࠊࡲࡎࡣᢅ࠸ࡸࡍ࠸ Ba+ ࢆ⏝࠸ࡓ⿦⨨㛤Ⓨࢆ⾜ࡗࡓࠋdye ࣮ࣞࢨ࣮ࢆ
ග※࡜ࡋࠊ5d 2D5/2 ࠿ࡽ 6p 2P3/2 ≧ែ࡬ບ㉳ࡋࡓཎᏊ࠿ࡽࡢ 6p 2P3/2–6s 2S1/2 ⮬↛ᨺฟගほ ࢆᐇ᪋ࡋࡓࠋ㛤Ⓨࡢᮎࠊྠ఩యࢩࣇࢺཬࡧ㉸ᚤ⣽ᵓ㐀ศ⿣ࢆほ ࡍࡿࡇ࡜ࡀ࡛ࡁࠊࡘ࠸࡟⿦⨨㛤Ⓨ୍࡛ᒣ㉺࠼ࡿࡇ࡜ࡀ࡛ࡁࡓࠋࡇࡢ࠶࡜ࠊ㛤Ⓨࢆ㐍ࡵ࡚ࡁࡓ (a) ECLD ග※ࢆ⏝࠸࡚ Zr ᐇ㦂࡛ࡢບ㉳㌿⛣
࡜ྠࡌ㌿⛣㸦Ba ࡢሙྜ 6s 2S1/2–6p 2P3/2㸧࡛ࡢศග ᐃࠊཬࡧ (b) ࣅ࣮࣒⢏Ꮚ࡜ࡢྠᮇ ᐃࡢࢩࢫࢸ࣒ࡢᑟධࡋ࡟ࡼࡿࣂࢵࢡࢢࣛ࢘ࣥࢻࡢపῶ໬ࢆ⾜ࡗࡓ࡜ࡇࢁ࡛⿦⨨㛤Ⓨࡢᡂᯝࢆㄽᩥ࡟ࡲ࡜ࡵ
ࡿணᐃ࡛࠶ࡿࠋ୪⾜ࡋࠊZr ࡢ RI ࣅ࣮࣒ࢆ⏝࠸ࡓ࢜ࣥࣛ࢖ࣥᐇ㦂࡟ྥࡅࠊ(c) ග※㛤Ⓨ࡜(d) Ⲵ㟁ኚ᥮⿦⨨ࡢ㛤Ⓨࢆ㐍ࡵ࡚࠸ࡿࠋ (c) ࡛ࡣ Zr+ ࡢศග࡟ᚲせ࡞⊃⥺ᖜ 357 nm ࣮ࣞࢨ࣮ගࢆฟຊࡍࡿ
➨஧ḟ㧗ㄪἼⓎ⏕ჾࡢ㛤Ⓨࢆ㐍ࡵࠊ஧ಸἼࡢⓎ⏕ࢆ☜ㄆࡋࡓ࡜ࡇࢁࡲ࡛㐍ࢇࡔࠋ(d) ࡛ࡣ࢜ࣥࣛ࢖
ࣥᐇ㦂࡟࠾࠸࡚๓ẁࡢ SLOWRI ⿦⨨࠿ࡽ2 ౯ࠊ3 ౯ࡢRI࢖࢜ࣥࡀ౪⤥ࡉࢀࡿࡇ࡜ࡀ᝿ᐃࡉࢀࡿࡓ
ࡵࠊ1 ౯࢖࢜ࣥࢆᚓࡿࡓࡵࡢⲴ㟁ኚ᥮⿦⨨ࡢタィࢆ㐍ࡵ࡚࠸ࡿࠋ࡞࠾ࠊ࢜ࣇࣛ࢖ࣥᐇ㦂⏝ࡢ (e) ࢖࢜ࣥ※㛤Ⓨ࡜ࡋ࡚ࠊHe ࢞ࢫ୰ࡢ࣮ࣞࢨ࣮࢔ࣈ࣮ࣞࢩࣙࣥ࡜㧗࿘Ἴ࢖࢜ࣥ࢞࢖ࢻࢆ⤌ࡳྜࢃࡏࡓࢩ
ࢫࢸ࣒ࢆᵓ⠏ࡋࡓࠋZr ࢆࡣࡌࡵࠊWࠊTa ࡞࡝ࡢ㧗⼥Ⅼ㔠ᒓࡢ࢖࢜ࣥࣅ࣮࣒ࡢ⏕ᡂࡀ☜ㄆ῭࡛࠶ࡿࠋ
2) ࡛ࡣ RNC ࢖࢜ࣥ※ࢳ࣮࣒ࡢ༠ຊࡢࡶ࡜ࠊ࢖࢜ࣥࣅ࣮࣒┤᥋ᑟධ࡟ࡼࡗ࡚ࢲ࢖ࣖࣔࣥࢻࡢ
㟁Ẽఏᑟࢆไᚚࡍࡿ᪉ἲࢆ᳨ウࡋࡓࠋ௒ᖺᗘࡣ CVD ἲ࡟ࡼࡿ㉸ఏᑟⓎ⌧ࡀ☜ㄆࡉࢀ࡚࠸ࡿ࣍࢘⣲࡟ࡘ࠸࡚ࠊ࢖࢜ࣥࣅ࣮࣒ὀධࢲ࢖ࣖࣔࣥࢻࡢ≀ᛶࢆホ౯ࡋࡓࠋ≉࡟ࠊ࣍࢘⣲ὀධᚋ࡟ࢲ࢖ࣖࣔࣥ
ࢻࡀᏳᐃ࡞ ᗘ࣭ᅽຊ㡿ᇦ࡟࠾࠸࡚࢔ࢽ࣮ࣝࢆ⾜࠸ࠊᵓ㐀࣭≀ᛶࡢኚ໬ࢆㄪ࡭ࡓࠋ㟁Ẽఏᑟ࡟ࡣ࢟ࣕࣜ࢔ࢻ࣮ࣉࡉࢀࡓ༙ᑟయࡢ࣍ࢵࣆࣥࢢఏᑟࡢഴྥࡀ⌧ࢀ࡚࠸ࡿࡀࠊ㉸ఏᑟࡣ⌧ࢀ࡚࠸࡞࠸ࠋ
ࡇࢀࡣࠊࢲ࢖ࣖࣔࣥࢻ୰࡟⏕ᡂࡉࢀࡿ❅⣲–✵Ꮝᑐࡀ࢔ࢡࢭࣉࢱ࣮࡜ࡋ࡚ࡢ࣍࢘⣲ࡢᐤ୚ࢆ┦ẅࡋ࡚࠸ࡿࡢࡀཎᅉࡢ୍ࡘ࡛࠶ࡿ࡜⪃࠼ࡽࢀࡿࠋࡇࡢ௬ㄝࢆ᳨ドࡍࡿࡓࡵ࡟ࠊ❅⣲୙⣧≀ࡢᑡ࡞࠸ IIᆺࢲ࢖ࣖࣔࣥࢻࢆ౑ࡗࡓ࣍࢘⣲ὀධᐇ㦂ࢆ⌧ᅾ㐍ࡵ࡚࠸ࡿࠋ

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㔜࠸ࢡ࢛࣮ࢡࢆྵࡴࣂࣜ࢜ࣥບ㉳≧ែࡢ◊✲ᡃࠎࡣࠊ᪂㡿ᇦ㛤ᣅㄢ㢟ࠕ≀㉁㝵ᒙࡢཎ⌮ࢆ᥈ồࡍࡿ⥲ྜⓗᐇ㦂◊✲㸦≀㉁㝵ᒙཎ⌮◊✲㸧ࠖ࡟ಀࡿࠊ㔜࠸ࢡ࢛࣮ࢡࢆྵࡴࢳ࣮࣒ࣕࣂࣜ࢜ࣥບ㉳≧ែࡢ⏕ᡂ࡜ᔂቯࢆ㏻ࡋ࡚ෆ㒊ᵓ㐀ࢆㄪ࡭ࡿ◊✲ࢆ⾜࠺ࠋ◊✲࡟⏝࠸ࡿࢫ࣌ࢡࢺ࣓࣮ࣟࢱࢆ㛤Ⓨ୰࡛௒ᖺᗘࡣ  ᖺ┠࡟ᙜࡓࡿࠋ
௒ᖺᗘࡢᡂᯝ࡜ࡋ࡚ࠊࢫ࣌ࢡࢺ࣓࣮ࣟࢱ࡟⏝࠸ࡿ௨ୗࡢ᳨ฟჾ㛤Ⓨ࡟ࡘ࠸࡚ྲྀࡾୖࡆࡿࠋ
㧗㏿ࢱ࢖࣑ࣥࢢ᳨ฟჾ㸦㸧ࡢ㛤Ⓨ㸸ࢳ࣮࣒ࣕࣂࣜ࢜ࣥࡢ⏕ᡂ཯ᛂ࡟క࠺ᩓ஘⢏Ꮚࡢ㆑ูࡢࡓࡵ࡟⢏Ꮚࡢ㏿ᗘࡢ᝟ሗࡀᚲせ࡛ࠊ㣕⾜᫬㛫ᐃࡢࡓࡵࡢࢱ࢖࣑ࣥࢢ᳨ฟჾࡢ᫬㛫ศゎ⬟ࡀ⢏Ꮚ㆑ูࡢᛶ⬟ࢆỴᐃࡍࡿࠋࡑࡢᇶ‽᫬㛫㸦ࢱ࢖࣒ࢮࣟ㸧ࢆ ᐃࡍࡿ᳨ฟჾࡀ  ࡛࠶ࡿࠋ㏻ᖖ㧗㏿ࣉࣛࢫࢳࢵࢡࢩࣥࢳ࣮ࣞࢱࡀ౑ࢃࢀࡿࡀࠊᡃࠎࡣࠊ
ࢳ࢙ࣞࣥࢥࣇග㍽ᑕయ࡜ࡋ࡚ࡢ࢔ࢡࣜࣝࢆ⏝࠸ࡓᅗ 㸸ᨵⰋ๓ᚋࡢ๓⨨ቑᖜჾಙྕ ᳨ฟჾࢆ㛤Ⓨࡋࡓࠋ㍽ᑕࡢᣦྥᛶ࡜༶Ⓨᛶࢆ฼⏝ࡍࡿࡇ࡜࡛ࠊ&( ⛬ᗘࡢ㧗᫬㛫ศゎ⬟ࢆ㐩ᡂࡋࡓࠋ௒ᖺᗘࡢㄢ㢟࡜ࡋ࡚ࠊࣜࣥࢠࣥࢢࡢᑡ
࡞࠸ฟຊἼᙧ㸦ᅗ 㸧ࡢ๓⨨ቑᖜᅇ㊰ࢆ㛤Ⓨࡋࠊ* ࡢ㠀ᖖ࡟㧗࠸⧞ࡾ㏉ࡋ஦㇟㢖ᗘ࡛ࡶ㧗ศゎ⬟ࢆ⥔ᣢ࡛ࡁࡿぢ㏻ࡋࡀ❧ࡗࡓࠋࢩࣥࢳ࣮ࣞࢩࣙࣥࣇ࢓࢖ࣂ࣮ࢺࣛࢵ࣮࢝㸦㸧ࡢ㛤Ⓨ㸸⏕ᡂ᩿㠃✚ࡢᑠࡉ࠸ࢳ࣮࣒ࣕࣂࣜ࢜ࣥࡢ⏕ᡂࡢࡓࡵ࡟  ࡢ኱ᙉᗘ㧗࢚ࢿࣝࢠ࣮ȧ୰㛫Ꮚࣅ࣮࣒ࢆ฼⏝ࡍࡿࠋẖ⛊  ༓୓ಶࡢȧࣅ࣮࣒⢏Ꮚ࡜ࡇࢀ࡟క࠺㧗࠸㢖ᗘ㸦 *㸧࠿ࡘ⢏Ꮚከ㔜ᗘ㸦஦㇟ᙜࡓࡾᖹᆒ

⢏Ꮚ㸧ࡢᩓ஘⢏Ꮚࡢ㌶㐨ࢆ ᐃࡍࡿᚲせࡀ࠶ࡿࠋᡃࠎࡣ  ੈᚄࡢࢩࣥࢳ࣮ࣞࢩࣙࣥࣇ࢓࢖ࣂ࣮ࢆࢩ࣮ࢺ≧࡟୪࡭ࡓᅗ 㸸㛤Ⓨࡋࡓ  ࡢࣅ࣮࣒ヨ㦂㸦'$  ᪋タ࡟࡚㸧⢏Ꮚ㣕㊧᳨ฟჾ㸦㸧ࢆ㛤Ⓨࡋࡓࠋ᫖ᖺᗘࡲ࡛࡟⏝ពࡋࡓヨ㦂ჾࢆᇶ࡟ᐇᶵࢆసᡂࡋࡓࠋࣅ࣮࣒ヨ㦂ࢆ⾜࠸ᡤᮇࡢᛶ⬟ࢆ☜ㄆࡋࡓ㸦ᅗ㸰㸧
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ÌMµA                        7ÁS¢¥¼GÀ¥Ó¹Wp²~eq¦¯7ÁS¢¥¼GÀ¥ÏNitric Oxide Reductaes: NORÐe[Y7!
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#^f{'¸m(Q)-Tp V !$¸mmØ!$1) T. Sekiguchi, et al., Angew. Chem. Int. Ed., 57(20), 5626-5629 (2018); M. Tamura et al., J. Phys.
Chem. Lett., 10(10), 2470-2474 (2019); S. Ishiuchi et al., Phys. Chem. Chem. Phys., 21(2), 561-571(2019). 2) M. C. Rose and R. W. Henkens, BBA, 372(2), 426-435(1974). 3) Varma, S. et al. J. Mol.
Biol. 376(1), 13–22 (2008).

㸫29㸫

O-11
⏣ཎኴᖹ

⌮໬Ꮫ◊✲ᡤ ⏣ཎศᏊศග◊✲ᐊᇸ⋢┴࿴ගᕷᗈἑ      ࢸࣛ࣊ࣝࢶ᰾㐠ືࡢᐇ᫬㛫ほ㢦෗┿㈞௜ࡅ

࡟ࡼࡿ໬Ꮫ⤖ྜ⏕ᡂࢲ࢖ࢼ࣑ࢡࢫࡢ㏣㊧໬Ꮫ཯ᛂ࡛ࡣ໬Ꮫ⤖ྜࡢ㛤⿣ࡸ⏕ᡂ࡟࡜ࡶ࡞ࡗ࡚ศᏊࡢᵓ㐀ࡀኚ໬ࡋࠊ᪂ࡋ࠸≀㉁ࡀ⏕ᡂࡍࡿࠋࡇࡢ໬Ꮫ཯ᛂࡢ㛫࡟ศᏊࡢᙧࡀ࡝ࡢࡼ࠺࡟ኚ໬ࡋ࡚࠸ࡃࡢ࠿ࠊࡑࡢ୍㒊ጞ⤊ࢆࣜ࢔ࣝࢱ࢖࣒࡛ほ ࡍࡿࡇ࡜ࡣ໬Ꮫ⪅ࡢክࡢ୍ࡘ࡜ゝ࠼ࡿࠋࡇࡢࡼ࠺࡞ศᏊࡢ
ኚ໬ࡢ୰࡛ࡶ໬Ꮫ⤖ྜࡢ⏕ᡂ࡟క࠺ᵓ㐀ኚ໬ࡢ㐣⛬ࢆ┤᥋ほ ࡍࡿࡇ࡜ࡣࠊࡑࢀࢆ௵
ពࡢࢱ࢖࣑ࣥࢢ࡛㛤ጞࡉࡏࡿᡭẁࡀ࡞࠿ࡗࡓࡇ࡜ࠊࡑࡋ࡚ࡑࢀࡼࡗ࡚㉳ࡿᵓ㐀ኚ໬ࡣࣇ࢙࣒ࢺ⛊㹼ࣆࢥ⛊㡿ᇦ࡛㠀ᖖ࡟㏿ࡃ㉳ࡿࡇ࡜࠿ࡽࠊ୍⯡࡟ᴟࡵ࡚㞴ࡋ࠸ࠋᡃࠎࡣ௒ᅇࠊᐩᒣ኱Ꮫࡢࢢ࣮ࣝࣉ࡜ඹྠ࡛ࠊ⣸እගࢆ྾཰ࡍࡿࡇ࡜࡛㔠ཎᏊ㛫࡟ඹ᭷⤖ྜࡀ⏕ᡂࡍࡿศᏊ㞟ྜయ࡛࠶ࡿࢪࢩ࢔ࣀ㔠㘒యࡢ୕㔞యࢆྲྀࡾୖࡆࠊ໬Ꮫ⤖ྜᙧᡂ࡜ࡑࢀ࡟క࠺ᵓ㐀ኚ໬ࢆ◊✲ࡋࡓࠋࡇࡢ⣔ࡢࢲ࢖ࢼ࣑ࢡࢫ࡟ࡘ࠸࡚ࡣࠊᐇࡣ௨๓࡟
ᡃࠎࡀึࡵ࡚㟁Ꮚ྾཰ࡢࣇ࢙࣒ࢺ⛊᫬㛫ศゎ ᐃࢆ⏝࠸࡚◊✲ࢆ⾜࠸ࠊࡑࡢᶵᵓ࡟ࡘ
࠸࡚ሗ࿌ࡋࡓࡀ>@ࠊࡑࡢᚋࠊ௚ࡢࢢ࣮ࣝࣉࡀ ; ⥺⮬⏤࣮ࣞࢨ࣮ࢆ⏝࠸ࡓᐇ㦂ࢆ⾜࠸ࠊᡃࠎ࡜␗࡞ࡿ୺ᙇࢆ⾜ࡗࡓࡓࡵ>@ࠊㄽத࡟࡞ࡗ࡚࠸ࡓࠋࡑࡇ࡛ࠊᡃࠎࡣ⌮◊࡛㛤Ⓨࡋࡓࣇ࢙࣒ࢺ⛊᫬㛫㡿ᇦ࣐ࣛࣥศගࢆ⏝࠸࡚ࢸࣛ࣊ࣝࢶ㡿ᇦࡢ᰾Ἴ᮰㐠ືࡢᐇ᫬㛫ほࢆ⾜࠸ࠊࡇࡢၥ㢟࡟Ỵ╔ࢆࡘࡅࡿࡇ࡜ࢆヨࡳࡓ>@ࠋᚓࡽࢀࡓࢸࣛ࣊ࣝࢶ㡿ᇦࡢࣇ࢙࣒ࢺ⛊࣐ࣛࣥࢫ࣌ࢡࢺࣝ࡜⌮ㄽィ⟬࡜ࡢẚ㍑࡟ࡼࡗ࡚ࠊ㔠㸫㔠㛫ࡢ⤖ྜࡢ⏕ᡂ࡟కࡗ࡚⣙  ࣆࢥ⛊௨ෆ࡟㔠ཎᏊ㛫㊥㞳ࡢ཰⦰ࡀ㉳ࡇࡾࠊ⥆࠸࡚᪂ࡓ࡞ᙉ࠸⤖ྜࡢᙧᡂࢆ
཯ᫎࡋ࡚ࠊ⣙  ࣆࢥ⛊࠿ࡅ࡚ࢪࢩ࢔ࣀ㔠㘒య୕㔞యࡀ᭤ࡀࡗࡓᙧ≧࠿ࡽ┤⥺ᆺࡢᵓ㐀࡬࡜ኚᙧࡋ࡚࠸ࡃࡇ࡜ࡀ♧ࡉࢀࡓࠋࡇࡢ⤖ᯝࡣᡃࠎࡢ᭱ึ࡟ᥦၐࡋࡓᶵᵓࡀṇࡋ࠿ࡗࡓࡇ࡜ࢆព࿡ࡋ࡚࠸ࡿࠋཧ⪃ᩥ⊩  0,ZDPXUD67DNHXFKL.1R]DNLDQG77DKDUD-$P&KHP6RF    .+.LP-*.LP61R]DZD76DWR.<2DQJ7:.LP+.L--R63DUN&6RQJ7
6DWR.2JDZD77RJDVKL.7RQR0<DEDVKL7,VKLNDZD-.LP55\RR-.LP+,KHH
DQG6$GDFKLNature    + .XUDPRFKL 6 7DNHXFKL 0 ,ZDPXUD . 1R]DNL DQG 7 7DKDUD J. Am. Chem. Soc
  

㸫30㸫

O-12
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