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Development of the spin frustration due to dynamical spin equilibrium and its induced successive magnetic phase transitions

Research Project

Project/Area Number 16K05421
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeMulti-year Fund
Section一般
Research Field Condensed matter physics II
Research InstitutionToyota Physical and Chemical Research Institute

Principal Investigator

Kojima Norimichi  公益財団法人豊田理化学研究所, フェロー事業部門, フェロー (60149656)

Co-Investigator(Kenkyū-buntansha) 岡澤 厚  東京大学, 大学院総合文化研究科, 助教 (30568275)
Research Collaborator Enomoto Masaya  
Project Period (FY) 2016-04-01 – 2019-03-31
Project Status Completed (Fiscal Year 2018)
Budget Amount *help
¥4,420,000 (Direct Cost: ¥3,400,000、Indirect Cost: ¥1,020,000)
Fiscal Year 2018: ¥1,040,000 (Direct Cost: ¥800,000、Indirect Cost: ¥240,000)
Fiscal Year 2017: ¥1,430,000 (Direct Cost: ¥1,100,000、Indirect Cost: ¥330,000)
Fiscal Year 2016: ¥1,950,000 (Direct Cost: ¥1,500,000、Indirect Cost: ¥450,000)
Keywords集積型金属錯体 / スピンクロスオーバー / 動的スピン平衡 / メスバウアー分光 / スピンフラストレーション / 逐次相転移 / 連鎖物性 / 磁気相転移 / 電荷移動相転移 / 混合原子価 / 連結異性 / 光異性化 / 光誘起相転移 / 強磁性 / 電荷移動
Outline of Final Research Achievements

We have synthesized (C6H5)4P[Zn(II)Fe(III)(mto)3](mto = C2O3S) consisting of Fe(III)O3S3 and Zn(II)O6 octahedra and investigated the spin state of the Fe(III) site. ESR and 57Fe Mossbauer spectra revealed that the rapid spin equilibrium in which the high spin state and the low spin state exchange in the time scale of 0.1 ns < τ < 0.1 μs occurs at the Fe(III) site. In the case of (C6H5)4P[Mn(II)Fe(III)(mto)3], there exists a rapid spin equilibrium (τ < 0.1 μs) between the high-spin and low-spin states at the Fe(III) site, which induces the frustration of internal magnetic field between the ferromagnetic and antiferromagnetic interactions at the Mn(II) site. Owing to the frustration of internal magnetic field at the Mn(II) site due to the rapid spin equilibrium at the Fe(III) site, (C6H5)4P[Mn(II)Fe(III)(mto)3] undergoes the successive magnetic phase transitions at 30 K and 23 K. At 30 K, only Mn(II) spin is ordered, while both of the Mn(II) and Fe(III) spins are ordered at 23 K.

Academic Significance and Societal Importance of the Research Achievements

A[Mn(II)Fe(III)(C2O3S)3] (A = cation)において、Fe(III)の動的スピン平衡現象を媒介とした磁性金属イオン間磁気相互作用のフラストレーションが生まれる。A = (C6H5)4Pにおいては、Fe(III)の低スピン状態とMn(II)スピンの間には強磁性相互作用が発現するが、Fe(III)の高スピン状態とMn(II)スピンの間には反強磁性相互作用が発現する。このような動的スピン平衡と連鎖する磁気相互作用のフラストレーションが磁気相転移に与える影響は全く未知の分野であり、分子磁性のみならず広く物性科学に波及効果をもたらすものである。

Report

(4 results)
  • 2018 Annual Research Report   Final Research Report ( PDF )
  • 2017 Research-status Report
  • 2016 Research-status Report
  • Research Products

    (41 results)

All 2018 2017 2016 Other

All Journal Article (12 results) (of which Int'l Joint Research: 3 results,  Peer Reviewed: 12 results,  Open Access: 6 results,  Acknowledgement Compliant: 1 results) Presentation (25 results) (of which Int'l Joint Research: 13 results,  Invited: 5 results) Book (1 results) Remarks (3 results)

  • [Journal Article] Unique Hydration/Dehydration-Induced Vapochromic Behavior of a Charge-Transfer Salt Comprising Viologen and Hexacyanidoferrate(II)2018

    • Author(s)
      Rikako Tanaka, Atsushi Okazawa, Hisashi Konaka, Akito Sasaki, Norimichi Kojima, Nobuyuki Matsushita
    • Journal Title

      Inorganic Chemistry

      Volume: 57 Issue: 4 Pages: 2209-2217

    • DOI

      10.1021/acs.inorgchem.7b03100

    • Related Report
      2018 Annual Research Report 2017 Research-status Report
    • Peer Reviewed
  • [Journal Article] Ionic Crystal Containing Protons (H+) as Counter Cations: Preparation and Crystal Structure of a Salt of 4,4'-Bipiperidine-1,1'-diium and Hexacyanidoferrate(II)2018

    • Author(s)
      Rikako Tanaka, Atsushi Okazawa, Norimichi Kojima, Nobuyuki Matsushita
    • Journal Title

      Chemistry Letters

      Volume: 47 Issue: 6 Pages: 697-699

    • DOI

      10.1246/cl.180157

    • NAID

      130007384415

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Structural Insight into Charge Transfer Phase Transition for Unique Iron Mixed-Valence Complex (n-C3H7)4N[FeIIFeIII(dto)3] with 2D Honeycomb Network2018

    • Author(s)
      M. Itoi, A. Okazawa, J. Yamaura, S. Maki, T. Komatsu, N. Kojima, I. Maurien, E. Codjovi, K. Boukheddaden. and F. Varret
    • Journal Title

      Inorg. Chem.

      Volume: 57 Issue: 21 Pages: 13728-13738

    • DOI

      10.1021/acs.inorgchem.8b02211

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] A triplet biradical with double bidentate sites based on tert-butyl pyridyl nitroxide as a candidate for strong ferromagnetic couplers2018

    • Author(s)
      Atsushi Okazawa, Yuutaro Terakado, Takayuki Ishida, Norimichi Kojima
    • Journal Title

      New Journal of Chemistry

      Volume: 42 Issue: 22 Pages: 17874-17878

    • DOI

      10.1039/c8nj04180f

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Effect of Transition Metal Substitution on the Charge-Transfer Phase Transition and Ferromagnetism of Dithiooxalato-Bridged Hetero Metal Complexes, (n-C3H7)4N[FeII1-xMnIIxFeIII(dto)3]2018

    • Author(s)
      Masaya Enomoto, Hiromichi Ida, Atsushi Okazawa, Norimichi Kojima
    • Journal Title

      Crystals

      Volume: 8 Issue: 12 Pages: 446-462

    • DOI

      10.3390/cryst8120446

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Studies on Nanostructure and Magnetic Behaviors of Mn-Doped Black Iron Oxide Magnetic Fluids Synthesized from Iron Sand.2017

    • Author(s)
      A. Taufiq, A.T. Sunaryono, N. Hidayat, A. Hidayat, E. Giri, R. Putra, A. Okazawa, I. Watanabe, N. Kojima, S. Pratapa, Darminto
    • Journal Title

      Nano, World Scientific

      Volume: 12 Issue: 09 Pages: 1750110-1750110

    • DOI

      10.1142/s1793292017501107

    • Related Report
      2017 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Control of Spin-Crossover Phenomena in One-Dimensional Triazole-Coordinated Iron(II) Complexes by Means of Functional Counter Ions2017

    • Author(s)
      A. Sugahara, H. Kamebuchi, A. Okazawa, M. Enomoto, N. Kojima
    • Journal Title

      Inorganics

      Volume: 5

    • Related Report
      2017 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Magnetic Properties of V-substitution Effect an Iron Mixed-Valence Complex2017

    • Author(s)
      N. Shida, Y. Suzawa, M. Inaba, A. Okazawa, N. Kojima, M. Enomoto
    • Journal Title

      Polyhedron

      Volume: 136 Pages: 143-148

    • DOI

      10.1016/j.poly.2017.04.006

    • Related Report
      2017 Research-status Report
    • Peer Reviewed
  • [Journal Article] Small-Angle X-Ray Scattering Study on PVA/Fe3O4 Magnetic Hydrogels2016

    • Author(s)
      Sunaryono, Ahmad Taufiq, Edy Giri Rahman Putra, Atsushi Okazawa, Isao Watanabe, Norimichi Kojima, Supagorn Rugmai, Siriwat Soontaranon, Mohammad Zainuri, Triwikantoro, Suminar Pratapa, Darminto
    • Journal Title

      NANO

      Volume: 11 Issue: 03 Pages: 1650027-1650027

    • DOI

      10.1142/s1793292016500272

    • Related Report
      2016 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Dynamical Behavior of the Charge Transfer Phase Transition in Dithiooxalato-Bridged Iron Mixed-Valence System2016

    • Author(s)
      M. Enomoto, I. Watanabe, N. Kojima
    • Journal Title

      Current Inorganic Chemistry

      Volume: 6 Issue: 1 Pages: 49-60

    • DOI

      10.2174/1877944105666150910200754

    • Related Report
      2016 Research-status Report
    • Peer Reviewed / Open Access / Acknowledgement Compliant
  • [Journal Article] Synthesis and Magnetic Properties of Linear Two-Coordinate Monomeric Diaryliron(II) Complexes Bearing Fused-Ring Bulky “Rind” Groups2016

    • Author(s)
      Shun Goda, Masanori Nikai, Mikinao Ito, Daisuke Hashizume, Kohei Tamao, Atsushi Okazawa, Norimichi Kojima, Hiroyuki Fueno, Kazuyoshi Tanaka, Yoshio Kobayashi, and Tsukasa Matsuo
    • Journal Title

      Bulletin of the Chemical Society of Japan

      Volume: 印刷中 Issue: 6 Pages: 636-638

    • DOI

      10.1246/cl.160216

    • NAID

      130005155021

    • Related Report
      2016 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Magnetic property and M&#246;ssbauer analysis of SrSn1-xFexO3 prepared by a sol-gel method2016

    • Author(s)
      Kiyoshi Nomura, Shigeyo Suzuki, Yuya Koike, Hongling Li, Atsushi Okazawa, Norimichi Kojima
    • Journal Title

      Hyperfine Interactions

      Volume: 237 Issue: 1

    • DOI

      10.1007/s10751-016-1260-2

    • Related Report
      2016 Research-status Report
    • Peer Reviewed / Open Access
  • [Presentation] Control of Spin-Crossover Transition for Iron(II) Complexes by Means of Functional Counter Ions2018

    • Author(s)
      N. Kojima, A. Sugahara, H. Kamebuchi
    • Organizer
      International Conference on Coordination Chemistry (ICCC2018, Sendai, Japan)
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 多重機能性スピンクロスオーバー錯体の開発と将来の課題2018

    • Author(s)
      小島憲道
    • Organizer
      大阪大学基礎工学研究科・未来研究推進センター・シンポジウム「機能性分子錯体の化学・物理の新しい展開」
    • Related Report
      2018 Annual Research Report
    • Invited
  • [Presentation] Progress of multifunctional phenomena coupled with spin, photon and charge based on iron mixed-valence system2018

    • Author(s)
      N. Kojima
    • Organizer
      The 9th TOYOTA RIKEN International Workshop (Nagoya, 2018)
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Study on the structural evolution of thiolate-protected gold clusters by means of 197Au M&ouml;ssbauer spectroscopy2018

    • Author(s)
      N. Kojima, Y. Kobayashi, M. Seto, Y. Negishi, T. Tsukuda
    • Organizer
      The 9th TOYOTA RIKEN International Workshop (Nagoya, 2018)
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Spin dynamics in tripyrazolylmethane iron(II) complexes showing static and dynamic spin-crossover phenomena2018

    • Author(s)
      A. Okazawa, H. Kobayashi, .I. Kawasaki, I. Watanabe, N. Kojima
    • Organizer
      The 9th TOYOTA RIKEN International Workshop (Nagoya, 2018)
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Molecular Ferroelectrics Studied using mSR2018

    • Author(s)
      F. Pratt, A. Berliel, l. Watanabe, Y. Miyazaki, N. Kojima
    • Organizer
      4th International Conference on Functional Materials Science 2018 (Bali, Indonesia)
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 集積型金属錯体における動的スピン平衡と連鎖する磁気物性2018

    • Author(s)
      小島憲道
    • Organizer
      京都大学複合原子力科学研究所専門研究会「短寿命RIを用いた核分光と核物性研究」
    • Related Report
      2018 Annual Research Report
  • [Presentation] 結晶構造解析とDFT計算による鉄混合原子価錯体(n-C3H7)4N[FeIIFeIII(dto)3]の光誘起電荷移動相転移の可能性の検討2018

    • Author(s)
      糸井充穂, 岡澤厚, 山浦淳一, 真木祥千子, 小松徳太郎, I. Maurin, E. Codjovi, K. Boukheddaden, 小島;憲道
    • Organizer
      日本物理学会・第74回年次大会
    • Related Report
      2018 Annual Research Report
  • [Presentation] Crystal structure construction of organic salts comprising proton, H+, as a counter cation2018

    • Author(s)
      R. Tanaka, A. Okazawa, N. Kojima, N. Matsushita
    • Organizer
      Annual Meeting of the Chemical Society of Japan, (Funahashi, Chiba)
    • Related Report
      2017 Research-status Report
  • [Presentation] Progress of Multifunctional Phenomena Coupled with Spin, Photon and Charge Based on Organic-Inorganic Hybrid System2017

    • Author(s)
      N. Kojima
    • Organizer
      International Conference on Smart Materials (Bangkok, Thailand)
    • Place of Presentation
      Bangkok, Thailand
    • Year and Date
      2017-03-16
    • Related Report
      2016 Research-status Report
    • Int'l Joint Research
  • [Presentation] Progress of Multi Functional Properties of Organic-Inorganic Hybrid System, A[FeIIFeIIIX3] (A = (CnH2n+1)4N, Spiropyran; X = C2O2S2, C2O3S)2017

    • Author(s)
      N. Kojima
    • Organizer
      International Congress on Chemistry and Materials Science, (Ankara, Turkey)
    • Related Report
      2017 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Control of charge transfer phase transition and ferromagnetism for iron mixed-valence complexes by means of photo-isomerization2017

    • Author(s)
      N. Kojima, J. Yoshida, A. Okazawa, M. Enomoto, Y. Kobayashi
    • Organizer
      International Conference on the Applications of the Mossbauer Effect (St. Petersburg, Russia)
    • Related Report
      2017 Research-status Report
    • Int'l Joint Research
  • [Presentation] 鉄混合原子価錯体の電子状態および相転移のメスバウアー分光法による解析2017

    • Author(s)
      小島憲道
    • Organizer
      メスバウアー分光研究会(東京理科大学)
    • Related Report
      2017 Research-status Report
  • [Presentation] 鉄混合原子価錯体における連結異性と電荷移動相転移に及ぼす効果のメスバウアー分光研究2017

    • Author(s)
      小島憲道
    • Organizer
      京都大学原子炉実験所専門研究会「短寿命RIを用いた核分光と核物性研究」
    • Related Report
      2017 Research-status Report
  • [Presentation] メスバウアー分光から見た鉄混合原子価錯体の電荷移動相転移と磁性2016

    • Author(s)
      小島憲道, 吉田順哉, 岡澤厚, 榎本真哉,小林義男
    • Organizer
      平成28年度KUR専門研究会「短寿命RIを用いた核分光と核物性研究」
    • Place of Presentation
      京都大学原子炉実験所、大阪府
    • Year and Date
      2016-12-20
    • Related Report
      2016 Research-status Report
  • [Presentation] Study on the Structural Evolution of Thiolate-protected Gold Clusters by Means of 197Au M&ouml;ssbauer Spectroscopy2016

    • Author(s)
      N. Kojima
    • Organizer
      International Conference on Atomic and Nuclear Physics
    • Place of Presentation
      Atlanta, USA
    • Year and Date
      2016-11-17
    • Related Report
      2016 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] ビピリジン骨格を有する有機アクセプター分子と鉄錯体ドナーからなるベイポクロ ミック電荷移動塩における構造未知相の粉末 X 線構造解析2016

    • Author(s)
      田中李叶子、小中尚、佐々木明登、岡澤厚、小島憲道、松下信之
    • Organizer
      日本結晶学会平成28年度年会
    • Place of Presentation
      茨城県立県民文化センター、水戸市
    • Year and Date
      2016-11-17
    • Related Report
      2016 Research-status Report
  • [Presentation] イオン交換膜を利用したスピンクロスオーバー錯体膜の開発とプロトンの流れの可視化2016

    • Author(s)
      小島憲道
    • Organizer
      第25回ポリマー材料フォーラム
    • Place of Presentation
      名古屋国際会議場、名古屋市
    • Year and Date
      2016-11-10
    • Related Report
      2016 Research-status Report
    • Invited
  • [Presentation] ビピリジン骨格を有する有機アクセプターと鉄錯体ドナーからなる電荷移動塩における固相合成相の結晶構造2016

    • Author(s)
      田中李叶子、岡澤厚、小島憲道、松下信之
    • Organizer
      第 25 回有機結晶シンポジウム
    • Place of Presentation
      京都大学、京都市
    • Year and Date
      2016-09-18
    • Related Report
      2016 Research-status Report
  • [Presentation] 鎖状二価カチオンがもたらす鉄混合原子価錯体における磁性層の歪みによる電荷移動挙動の変化2016

    • Author(s)
      矢口寛、佐々木翔太郎、榎本真哉、岡澤厚、小島憲道
    • Organizer
      錯体化学会第66回討論会
    • Place of Presentation
      福岡大学、福岡市
    • Year and Date
      2016-09-10
    • Related Report
      2016 Research-status Report
  • [Presentation] ベイポクロミック鉄錯体電荷移動塩の粉末X線構造解析による結晶構造解明2016

    • Author(s)
      田中李叶子、小中尚、佐々木明登、岡澤厚、小島憲道、松下信之
    • Organizer
      錯体化学会第66回討論会
    • Place of Presentation
      福岡大学、福岡市
    • Year and Date
      2016-09-10
    • Related Report
      2016 Research-status Report
  • [Presentation] Synthesis, Crystal Structures, and Magnetic Properties of Copper(II) Complexes with Bischelate and High-spin Biradical Ligand2016

    • Author(s)
      A. Okazawa, T. Ishida, K. Ogawa, N. Kojima
    • Organizer
      International Conference on Molecular Magnetism 2016 (ICMM2016)
    • Place of Presentation
      Sendai, Japan
    • Year and Date
      2016-09-04
    • Related Report
      2016 Research-status Report
    • Int'l Joint Research
  • [Presentation] The Charge Transfer Phase Transition in an Iron Mixed-Valence Complex with Specific2016

    • Author(s)
      M. Enomoto, M. Shirakawa, H. Izawa, K. Sato, A. Okazawa, N. Kojima
    • Organizer
      International Conference on Molecular Magnetism 2016 (ICMM2016),
    • Place of Presentation
      Sendai, Japan
    • Year and Date
      2016-09-04
    • Related Report
      2016 Research-status Report
    • Int'l Joint Research
  • [Presentation] Magnetic Properties of Substitution Effect in an Iron Mixed-Valence Complex2016

    • Author(s)
      N. Shida, Y. Suzawa, A. Okazawa, N. Kojima, M. Enomoto
    • Organizer
      International Conference on Molecular Magnetism 2016 (ICMM2016),
    • Place of Presentation
      Sendai, Japan
    • Year and Date
      2016-09-04
    • Related Report
      2016 Research-status Report
    • Int'l Joint Research
  • [Presentation] Dynamical Behavior of the Charge Transfer Phase Transition in Dithiooxalato-Bridged Iron Mixed-Valence System2016

    • Author(s)
      N. Kojima, M. Enomoto, A. Okazawa, M. Itoi, I. Watanabe
    • Organizer
      XXIII International Symposium on the Jahn-Teller Effect
    • Place of Presentation
      Tartu, Estonia
    • Year and Date
      2016-08-27
    • Related Report
      2016 Research-status Report
    • Int'l Joint Research
  • [Book] “Nafion: Properties, Structure and Applications,” ed. A. Sutton2016

    • Author(s)
      H. Kamebuchi, M. Enomoto, N. Kojima
    • Publisher
      Nova Science Publishers
    • Related Report
      2016 Research-status Report
  • [Remarks] 豊田理化学研究所

    • URL

      https://www.toyotariken.jp/info/index.html

    • Related Report
      2018 Annual Research Report
  • [Remarks] 豊田理化学研究所

    • URL

      http://www.toyotariken.jp/info/index.html

    • Related Report
      2017 Research-status Report
  • [Remarks] 豊田理化学研究所HP

    • URL

      http://www.toyotariken.jp/info/index.html

    • Related Report
      2016 Research-status Report

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Published: 2016-04-21   Modified: 2020-03-30  

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