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Orbital, charge and spin degrees of freedom in molecular solids

Research Project

Project/Area Number 15K05478
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeMulti-year Fund
Section一般
Research Field Functional solid state chemistry
Research InstitutionEhime University

Principal Investigator

Yamamoto Takashi  愛媛大学, 理工学研究科(理学系), 准教授 (20511017)

Project Period (FY) 2015-04-01 – 2020-03-31
Project Status Completed (Fiscal Year 2019)
Budget Amount *help
¥4,940,000 (Direct Cost: ¥3,800,000、Indirect Cost: ¥1,140,000)
Fiscal Year 2018: ¥1,040,000 (Direct Cost: ¥800,000、Indirect Cost: ¥240,000)
Fiscal Year 2017: ¥1,170,000 (Direct Cost: ¥900,000、Indirect Cost: ¥270,000)
Fiscal Year 2016: ¥1,170,000 (Direct Cost: ¥900,000、Indirect Cost: ¥270,000)
Fiscal Year 2015: ¥1,560,000 (Direct Cost: ¥1,200,000、Indirect Cost: ¥360,000)
Keywords分子固体 / 軌道自由度 / 縮退軌道 / 電荷自由度 / 電荷再配列 / スピン自由度 / スピン液体 / 伝導性 / 分子性導体 / 金属ジチオレン錯体 / ジチオレン錯体 / 電子自由度 / 格子自由度 / 分子軌道自由度 / HOMO-LUMO逆転 / 金属ジチオレン錯体塩 / 超伝導 / 電荷整列 / モット絶縁体 / Valence Bond Order / 軌道準位の縮退・逆転 / 超分子化 / 伝導性・磁性 / 電荷不均一化 / 分子性固体 / 有機導体 / 電荷・スピン自由度
Outline of Final Research Achievements

Orbital degeneracy in the two-dimensional molecular solids were examined. (1) Me4P[Pt(dmit)2]2 exhibited the phase transition around 200 K. HOMO and LUMO levels in 50 % of dimers were interchanged below 200 K. The same phenomena were observed in Me4N[Pt(dmit)2]2 and Me4Sb[Pt(dmit)2]2. This result indicates the orbital degeneracy was canceled below the phase transition temperature. (2) The magnetic transition and charge disproportionation were observed at the same transition temperature. (3) In contrast, the interchange of the HOMO and LUMO levels remained below the phase transition temperature of Cs[Pd(dmit)2]2. The vibrational spectroscopy revealed that the competition between several kinds of inter-dimer interactions was canceled below the phase transition temperature. This competition was also observed in EtMe3Sb[Pt(dmit)2]2 at the liquid helium temperature. This result suggests that charge and lattice fluctuation is the driving force of the geometrical frustration.

Academic Significance and Societal Importance of the Research Achievements

本研究により、無機物のような軌道自由度と、大きな格子揺らぎといった分子由来の特性を組み合わせた、新しい物性を開拓できる可能性が広がった。軌道の縮退は分子同士の距離に比例する尺度で評価できることを明らかにしたので、今後の研究の進展により、単一成分の分子結晶を始めとする様々な伝導体・超伝導体における伝導機構の解明が期待される。スピン液体として注目されてきた現象の作動原理を明らかにし、スピンだけでなく格子や電荷の自由度も重要であることを示した。

Report

(6 results)
  • 2019 Annual Research Report   Final Research Report ( PDF )
  • 2018 Research-status Report
  • 2017 Research-status Report
  • 2016 Research-status Report
  • 2015 Research-status Report
  • Research Products

    (34 results)

All 2020 2019 2018 2017 2016 2015 Other

All Int'l Joint Research (1 results) Journal Article (8 results) (of which Int'l Joint Research: 1 results,  Peer Reviewed: 8 results,  Open Access: 5 results,  Acknowledgement Compliant: 1 results) Presentation (20 results) (of which Int'l Joint Research: 4 results,  Invited: 2 results) Book (1 results) Remarks (4 results)

  • [Int'l Joint Research] Max Planck Institute(Germany)

    • Related Report
      2015 Research-status Report
  • [Journal Article] Electrical Resistivity under Uniaxial Pressures of β′′-(bis-ethelenedithio-tetrathiafulvalene)4Pd(CN)4H2O2020

    • Author(s)
      Okii Yuichi、Yamamoto Takashi、Konishi Kensuke、Naito Toshio
    • Journal Title

      Journal of the Physical Society of Japan

      Volume: 89 Issue: 3 Pages: 034709-034709

    • DOI

      10.7566/jpsj.89.034709

    • NAID

      210000158043

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Electronic Inhomogeneity in Organic Charge Transfer Salt κ-(BEDT-TTF)2Cu[N(CN)2]I Probed by Polarized Femtosecond Spectroscopy2020

    • Author(s)
      Tsuchiya Satoshi、Kuwae Ryota、Kodama Takumi、Nakamura Yusuke、Kurihara Megumi、Yamamoto Takashi、Naito Toshio、Toda Yasunori
    • Journal Title

      Journal of the Physical Society of Japan

      Volume: 89 Issue: 6 Pages: 064712-064712

    • DOI

      10.7566/jpsj.89.064712

    • NAID

      40022254224

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Charge and Lattice Fluctuations in Molecule-Based Spin Liquids2017

    • Author(s)
      Yamamoto Takashi、Fujimoto Takashi、Naito Toshio、Nakazawa Yasuhiro、Tamura Masafumi、Yakushi Kyuya、Ikemoto Yuka、Moriwaki Taro、Kato Reizo
    • Journal Title

      Scientific Reports

      Volume: 7 Issue: 1 Pages: 1-10

    • DOI

      10.1038/s41598-017-13118-4

    • Related Report
      2017 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Dye-Sensitized Molecular Charge Transfer Complexes: Magnetic and Conduction Properties in the Photoexcited States of Ni(dmit)2 Salts Containing Photosensitive Dyes2017

    • Author(s)
      Yamamoto Ryoma、Yamamoto Takashi、Ohara Keishi、Naito Toshio
    • Journal Title

      Magnetochemistry

      Volume: 3 Issue: 2 Pages: 1-16

    • DOI

      10.3390/magnetochemistry3020020

    • Related Report
      2017 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Anisotropic Field Dependence of the Superconducting Transition in the Magnetic Molecular Superconductor κ-(BETS)2FeBr42017

    • Author(s)
      S. Fukuoka, S. Yamashita, Y. Nakazawa, T. Yamamoto, H. Fujiwara
    • Journal Title

      J. Phys. Soc. Jpn.

      Volume: 86 Issue: 1 Pages: 1-6

    • DOI

      10.7566/jpsj.86.014706

    • NAID

      210000134228

    • Related Report
      2017 Research-status Report
    • Peer Reviewed
  • [Journal Article] Intra- versus Inter-dimer Charge Inhomogeneity in the Triangular Lattice Compounds of β'-Cs[Pd(dmit)2]2: A Degree of Freedom Characteristic of an Interchange of Energy Levels in the Molecular Orbitals2016

    • Author(s)
      T. Yamamoto, M. Tamura, K. Yakushi, and R. Kato
    • Journal Title

      Journal of the Physical Society of Japan

      Volume: 85 Issue: 10 Pages: 104711-13

    • DOI

      10.7566/jpsj.85.104711

    • NAID

      210000134128

    • Related Report
      2016 Research-status Report
    • Peer Reviewed / Acknowledgement Compliant
  • [Journal Article] Direct observation of collective modes coupled to molecular orbital-driven charge transfer2015

    • Author(s)
      T. Ishikawa, S. A. Hayes, S. Keskin, G. Corthey, M. Hada, K. Pichugin, A. Marx, J. Hischt, K. Shionuma, K. Onda, Y. Okimoto, S. Koshihara, T. Yamamoto, H. Cui, M. Nomura, Y. Oshima, M. Abdel-Jawad. R. Kato and R. J. Miller
    • Journal Title

      Science

      Volume: 350 Issue: 6267 Pages: 1501-1505

    • DOI

      10.1126/science.aab3480

    • Related Report
      2015 Research-status Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Activation energy for photoconduction in molecular crystals2015

    • Author(s)
      N. Nagayama, T. Yamamoto, and T. Naito
    • Journal Title

      CheM

      Volume: 2 Pages: 74-80

    • Related Report
      2015 Research-status Report
    • Peer Reviewed / Open Access
  • [Presentation] 縮退に近い軌道を有する 白金ジチオレン錯体塩の相転移2019

    • Author(s)
      山本貴, 高杉滉, 平賀大貴, 内藤俊雄, 売市幹大, 手島史綱, 田中清尚, 加藤礼三
    • Organizer
      日本物理学会秋季大会
    • Related Report
      2019 Annual Research Report
  • [Presentation] 非ダイマーモット型の有機超伝導体 における 一軸圧縮効果2019

    • Author(s)
      山本 貴, 沖井 優一, 東澤 玲央, 内藤 俊雄, 圷 広樹, 中澤 康浩
    • Organizer
      高圧討論会
    • Related Report
      2019 Annual Research Report
  • [Presentation] Hidden Ordered States Characteristic of Interchange of MO Levels in Molecule-Based Conductors2018

    • Author(s)
      Takashi Yamamoto, Toshio Naito, Yasuhiro Nakazawa, Masafumi Tamura, Kyuya Yakushi and Reizo Kato
    • Organizer
      The 8th TOYOTA RIKEN International Workshop, Nagakute, Aichi, Japan, Oct. 24-26, 2018
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Interplay between spin, charge, lattice and orbital in molecule-based frustrated spin system2018

    • Author(s)
      Takashi Yamamoto, Toshio Naito, Yasuhiro Nakazawa, Masafumi Tamura, Kyuya Yakushi and Reizo Kato
    • Organizer
      The 43rd International Conference on Coordination Chemistry (ICCC 2018), Sendai, Miyagi, Japan,Jul. 30-Aug. 4, 2018
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] kappa-型(ET)2Cu[N(CN)2]I 塩の物性と二次元電子構造2018

    • Author(s)
      嵐育未、山本 貴、中村 祐介、内藤 俊雄
    • Organizer
      第12回分子科学討論会2018福岡(2018年9月10日(月)―13日(木);福岡国際会議場)
    • Related Report
      2018 Research-status Report
  • [Presentation] 分子結晶の電荷の揺らぎを利用した光励起状態に固有の金属状態2018

    • Author(s)
      内藤俊雄、山本澪馬、張明楊、山本貴
    • Organizer
      2018年日本化学会中国四国支部大会 愛媛大会
    • Related Report
      2018 Research-status Report
  • [Presentation] Me4Sb[Pt(dmit)2]2のラマンスペクトル2018

    • Author(s)
      平賀 大貴、山本 貴、内藤 俊雄、売市 幹大、加藤 礼三
    • Organizer
      2018年日本化学会中国四国支部大会 愛媛大会
    • Related Report
      2018 Research-status Report
  • [Presentation] π共役系を縮小した新規TTP, DTEDT 系導体の合成、構造と物性2018

    • Author(s)
      木下 直哉、Mohamad Safuwan bin Alias、白旗 崇、山本 貴、内藤 俊雄、山田 順一、御崎 洋二
    • Organizer
      2018年日本化学会中国四国支部大会 愛媛大会
    • Related Report
      2018 Research-status Report
  • [Presentation] HOMO-LUMO逆転した二次元系に特有な磁性と電荷の協奏現象2018

    • Author(s)
      山本 貴・内藤 俊雄・藤本 尚史・中澤 康浩・田村 雅史・池本 夕佳・森脇 太郎・薬師 久弥・加藤 礼三
    • Organizer
      日本化学会第98春季年会2018
    • Related Report
      2017 Research-status Report
  • [Presentation] κ型(ET)2Cu[N(CN)2]I塩の物性と二次元電子構造2018

    • Author(s)
      山本貴, 中村祐介, 内藤俊雄
    • Organizer
      日本物理学会 第73回年次大会
    • Related Report
      2017 Research-status Report
  • [Presentation] Photo-induced dynamics of Me4P[Pt(dmit)2]22017

    • Author(s)
      Tadahiko Ishikawa, Takashi Yamamoto, et. al.
    • Organizer
      6th international Conference on Photoinduced Phase Transtions
    • Place of Presentation
      SENDAI INTERNATIONAL CENTER (宮城県 仙台市)
    • Year and Date
      2017-06-04
    • Related Report
      2016 Research-status Report
    • Int'l Joint Research
  • [Presentation] 振動領域時間分解分光から見たMe4P[Pt(dmit)2]2の光誘起ダイナミクス2017

    • Author(s)
      石川忠彦, 卜澤陽平, 田中誠一, 恩田健, 沖本洋一, 腰原伸也, 山本貴, 野村光城, 加藤礼三
    • Organizer
      日本物理学会 第72回年次大会
    • Place of Presentation
      大阪大学 (大阪府 豊中市)
    • Year and Date
      2017-03-17
    • Related Report
      2016 Research-status Report
  • [Presentation] 振動分光によるMe4N[Pt(dmit)2]2およびMe4P[Pd(dmit)2]2の分子非対称化の研究2017

    • Author(s)
      山本 貴,高杉 滉,内藤 俊雄,加藤 礼三
    • Organizer
      第11回分子科学討論会
    • Related Report
      2017 Research-status Report
  • [Presentation] Vibrational Spectra of [M(dmit)2] Salts2017

    • Author(s)
      Koh Takasugi, Takashi Yamamoto, Toshio Naito, Reizo Kato
    • Organizer
      12th International Symposium on Crystalline Organic Metals, Superconductors and Magnets (ISCOM2017)
    • Related Report
      2017 Research-status Report
    • Int'l Joint Research
  • [Presentation] (C7H13NH)[Pd(dmit)2]2およびMe4N[Pt(dmit)2]2の分子振動2016

    • Author(s)
      高杉滉, 山本貴, 内藤俊雄
    • Organizer
      日本化学会中四国支部大会
    • Place of Presentation
      香川大学 (香川県 高松市)
    • Year and Date
      2016-11-05
    • Related Report
      2016 Research-status Report
  • [Presentation] Uniaxial Strain Effects on β"-type BEDT-TTF salts2016

    • Author(s)
      OKII, Yuichi; YAMAMOTO, Takashi; NAITO, Toshio; KONISHI, Kensuke
    • Organizer
      日本化学会第96春季年会
    • Place of Presentation
      同志社大学(京都府・京田辺市)
    • Year and Date
      2016-03-24
    • Related Report
      2015 Research-status Report
  • [Presentation] 光照射下の銅 (II)ジチオレン錯体塩の磁性 ・伝導2015

    • Author(s)
      野間博貴 , 小原敬士 , 山本 貴, 内藤俊雄
    • Organizer
      2015年 日本化学会中国四国支部大会
    • Place of Presentation
      岡山大学(岡山県・岡山市)
    • Year and Date
      2015-11-14
    • Related Report
      2015 Research-status Report
  • [Presentation] 光照射下におけるBPY[Ni(dmit)2]6・3CH3CN単結晶の伝導挙動2015

    • Author(s)
      山本 澪馬, 山本 貴, 内藤 俊雄
    • Organizer
      2015年 日本化学会中国四国支部大会
    • Place of Presentation
      岡山大学(岡山県・岡山市)
    • Year and Date
      2015-11-14
    • Related Report
      2015 Research-status Report
  • [Presentation] 高い光伝導を示すNMQ[Ni(dmit)2]の伝導機構に関する研究2015

    • Author(s)
      長山直樹、山本貴、内藤俊雄
    • Organizer
      2015年 日本化学会中国四国支部大会
    • Place of Presentation
      岡山大学(岡山県・岡山市)
    • Year and Date
      2015-11-14
    • Related Report
      2015 Research-status Report
  • [Presentation] κ-(ET)2Cu[N(CN)2] Iの多様な物性2015

    • Author(s)
      中村祐介、山本 貴、内藤俊雄、小西健介
    • Organizer
      第9回分子科学討論会2015
    • Place of Presentation
      東京工業大学(東京都・目黒区)
    • Year and Date
      2015-09-16
    • Related Report
      2015 Research-status Report
  • [Book] “Diversity in the Electronic Phase due to Interchange of MO Levels in [M(dmit)2] Anion Salts (M = Pd and Pt)” in Functional Materials: Advances and Applications in Energy Storage and Conversion2018

    • Author(s)
      T. Yamamoto
    • Total Pages
      73
    • Publisher
      Pan Stanford Publishing
    • ISBN
      9780429468131
    • Related Report
      2018 Research-status Report
  • [Remarks] 分子結晶におけるスピン液体の起源を解明

    • URL

      https://www.ehime-u.ac.jp/data_relese/data_relese-64678/

    • Related Report
      2017 Research-status Report
  • [Remarks] 分子結晶におけるスピン液体の起源を解明

    • URL

      http://www.spring8.or.jp/ja/news_publications/press_release/2017/171010/

    • Related Report
      2017 Research-status Report
  • [Remarks] 分子結晶におけるスピン液体の起源を解明

    • URL

      http://www.riken.jp/pr/press/2017/

    • Related Report
      2017 Research-status Report
  • [Remarks] 分子が変形する様子を2兆分の1秒刻みでコマ撮り撮影―光機能性物質の動作メカニズム解明に成功―

    • URL

      http://www.titech.ac.jp/news/2015/032959.html

    • Related Report
      2015 Research-status Report

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Published: 2015-04-16   Modified: 2021-02-19  

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