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Chemistry of open-shell carbon-based pi-electron molecular materials and development into spin liquids

Research Project

Project/Area Number 21H01907
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Review Section Basic Section 32020:Functional solid state chemistry-related
Research InstitutionOsaka Metropolitan University (2022-2023)
Osaka Prefecture University (2021)

Principal Investigator

プラシデス コスマス  大阪公立大学, 大学院理学研究科, 客員研究員 (90719006)

Project Period (FY) 2021-04-01 – 2024-03-31
Project Status Granted (Fiscal Year 2023)
Budget Amount *help
¥17,290,000 (Direct Cost: ¥13,300,000、Indirect Cost: ¥3,990,000)
Fiscal Year 2023: ¥5,330,000 (Direct Cost: ¥4,100,000、Indirect Cost: ¥1,230,000)
Fiscal Year 2022: ¥5,330,000 (Direct Cost: ¥4,100,000、Indirect Cost: ¥1,230,000)
Fiscal Year 2021: ¥6,630,000 (Direct Cost: ¥5,100,000、Indirect Cost: ¥1,530,000)
Keywordspi-electron systems / Molecular nanocarbons / spin liquids / superconductors / carbon-based / molecular materials / polyaromatics / fullerenes
Outline of Research at the Start

The project targets the synthesis of new crystalline materials whose building blocks are electronically-active π-electron unsaturated organic molecular anions of varying size, shape and electronic structure. We will use the new chemistry we pioneered to control the positioning of the π-electron open-shell building blocks in space and create geometrically frustrated magnetic lattices, which can be hosts of quantum spin liquids. These strongly-correlated Mott insulating phases will be further chemically and physically to turn them into metals and superconductors.

Outline of Annual Research Achievements

The project has developed new crystalline materials families whose building blocks are electronically-active π-electron unsaturated organic molecular anions of varying size, shape, and electronic structure. We have been employing the new chemistry we pioneered in recent years to control the positioning of the pi-electron open-shell building blocks in space and create geometrically-frustrated magnetic lattices, which can act as hosts of quantum spin liquids purely arising from carbon pi-electrons. These strongly-correlated Mott insulating phases are further manipulated chemically and physically to turn them into metals and superconductors. Chemical synthesis is integrated with state-of-the-art structural and magnetic measurement techniques to identify the new electronic states that arise. To date, we have established the fragility of the magnetic states to small perturbations induced by the chemical dopants that lead to transitions to long-range-ordered magnetic states, which were studied by ultralow temperature resonance techniques (NMR and muSR). At the same time, we found that incorporation of high-symmetry fullerene units leads to the isolation of hybrid systems, promising candidates of new electronic states.

Current Status of Research Progress
Current Status of Research Progress

1: Research has progressed more than it was originally planned.

Reason

The purpose of the project is to isolate new families of pi-electron carbon-based molecular materials and explore the emergence of new electronic properties. This is being successfully carried out to an advanced stage. In particular, reduced pi-electron families of polyaromatic hydrocarbons chemically synthesized in this work have allowed us to establish the influence of the nature of the dopant and the modified crystalline structures on the structural and electronic properties. In addition, we have successfully incorporated fullerenes into the polyaromatic hydrocarbon architectures. Structural and magnetic characterizations have been completed for proof-of-concept hybrid systems.

Strategy for Future Research Activity

The research plan for the future years consists of three integrated components:
(A) Chemical synthesis. We will create new binary phases of reduced polyaromatic hydrocarbons and hybrid molecular solids doped with alkali metals.
(B) Structural analysis. We will carry out precise structural determination at low temperature and/or high pressure with synchrotron X-ray and neutron diffraction techniques probing accurately the changes in crystalline structure.
(C) Electronic properties. Detailed characterization of the electronic and magnetic properties will be pursued.

Report

(2 results)
  • 2022 Annual Research Report
  • 2021 Annual Research Report
  • Research Products

    (31 results)

All 2024 2023 2022 Other

All Int'l Joint Research (6 results) Journal Article (6 results) (of which Int'l Joint Research: 6 results,  Peer Reviewed: 6 results,  Open Access: 3 results) Presentation (18 results) (of which Int'l Joint Research: 7 results,  Invited: 11 results) Remarks (1 results)

  • [Int'l Joint Research] NCSR Demokritos/Univ of Thessaloniki(ギリシャ)

    • Related Report
      2022 Annual Research Report
  • [Int'l Joint Research] Univ Fribourg(スイス)

    • Related Report
      2022 Annual Research Report
  • [Int'l Joint Research] Ruder Boskovic Institute(クロアチア)

    • Related Report
      2022 Annual Research Report
  • [Int'l Joint Research] University of Technology(キプロス)

    • Related Report
      2022 Annual Research Report
  • [Int'l Joint Research] HPSTAR Beijing(中国)

    • Related Report
      2022 Annual Research Report
  • [Int'l Joint Research] NCSR Demokritos(ギリシャ)

    • Related Report
      2021 Annual Research Report
  • [Journal Article] On the Structural and Vibrational Properties of Solid Endohedral Metallofullerene Li@C602024

    • Author(s)
      Vrankic Martina、Nakagawa Takeshi、Menelaou Melita、Takabayashi Yasuhiro、Yoshikane Naoya、Matsui Keisuke、Kokubo Ken、Kato Kenichi、Kawaguchi-Imada Saori、Kadobayashi Hirokazu、Arvanitidis John、Kubota Yoshiki、Prassides Kosmas
    • Journal Title

      Inorganics

      Volume: 12 Issue: 4 Pages: 99-99

    • DOI

      10.3390/inorganics12040099

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Isosymmetric Lattice Collapse in Mixed-Valence Rare-Earth Fullerides at High Pressure─Coupling of Lattice and Electronic Degrees of Freedom2023

    • Author(s)
      Yoshikane Naoya、Matsui Keisuke、Nakagawa Takeshi、Yamaoka Hitoshi、Hiraoka Nozomu、Ishii Hirofumi、Arvanitidis John、Prassides Kosmas
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 127 Issue: 21 Pages: 10375-10383

    • DOI

      10.1021/acs.jpcc.3c01626

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Mixed orbital states and modulated crystal structures in La1-xCaxMnO3 deduced from synchrotron X-ray diffraction2023

    • Author(s)
      Pissas Michael、Stamopoulos Dimosthenis、Prassides Kosmas
    • Journal Title

      Communications Physics

      Volume: 6 Issue: 1 Pages: 188-188

    • DOI

      10.1038/s42005-023-01304-y

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Electron injection into superconducting trivalent fullerides close to the Mott transition boundary2023

    • Author(s)
      Matsui Keisuke、Yoshikane Naoya、Terzidou Anastasia G.V.、Arvanitidis John、Kawaguchi Shogo、Kubota Yoshiki、Prassides Kosmas
    • Journal Title

      Modern Physics Letters B

      Volume: N/A Issue: 21

    • DOI

      10.1142/s0217984923420010

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Instability of the Pa-3 fulleride Cs3C60 at ambient pressure and superconducting state of the fcc phase2023

    • Author(s)
      Yue Changming、Nomura Yusuke、Prassides Kosmas、Werner Philipp
    • Journal Title

      Physical Review B

      Volume: 108 Issue: 22

    • DOI

      10.1103/physrevb.108.l220508

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Evolution of the magnetic structure in overdoped antiferromagnetic La1-xCaxMnO3 (0.51 < x < 0.69) manganites: A neutron diffraction study2023

    • Author(s)
      Pissas M.、Stamopoulos D.、Arulraj A.、Prassides K.
    • Journal Title

      Physical Review B

      Volume: 107 Issue: 3 Pages: 35110-35110

    • DOI

      10.1103/physrevb.107.035110

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Presentation] Electron injection into superconducting fullerides close to the Mott transition boundary2024

    • Author(s)
      Keisuke Matsui, Kosmas Prassides
    • Organizer
      The 66th Fullerenes-Nanotubes-Graphene General Symposium, Tokyo, Japan
    • Related Report
      2022 Annual Research Report
  • [Presentation] Spontaneous magnetoelastic effects in Prussian blue analogue molecular magnets2023

    • Author(s)
      Kosmas Prassides
    • Organizer
      2023 Joint CTMNM/NAGC Conference, Spetses, Greece
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Coupling of structural and electronic behaviors in mixed-valence RE2.75C602023

    • Author(s)
      Naoya Yoshikane, Kosmas Prassides
    • Organizer
      2023 Joint CTMNM/NAGC Conference, Spetses, Greece
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Coupling of lattice and electronic degrees of freedom in mixed-valence rare-earth fullerides2023

    • Author(s)
      Kosmas Prassides
    • Organizer
      International Conference on Quantum Materials, Superstripes 2023, Ischia, Italy
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Structural changes induced by alkali metal substitution in Prussian Blue analogues2023

    • Author(s)
      Marina Nishiura, Kosmas Prassides
    • Organizer
      2023 Summer School of Young Coordination Chemists, Kyushu, Japan
    • Related Report
      2022 Annual Research Report
  • [Presentation] Effect of electron injection into superconducting trivalent fullerides close to the Mott transition boundary2023

    • Author(s)
      Keisuke Matsui, Kosmas Prassides
    • Organizer
      9th TKU-ECUST-KISTymposium on Advanced Materials and Applications, Hyogo, Japan
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] Search for superconducting fullerides by alkaline-earth doping2023

    • Author(s)
      Mizuki Suzuki, Kosmas Prassides
    • Organizer
      9th TKU-ECUST-KISTymposium on Advanced Materials and Applications, Hyogo, Japan
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] Alkali-intercalation chemistry of hybrid molecular solids derived from C60 and polyaromatic hydrocarbons2023

    • Author(s)
      Akane Matsumoto, Kosmas Prassides
    • Organizer
      9th TKU-ECUST-KISTymposium on Advanced Materials and Applications, Hyogo, Japan
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] Development of Pentavalent Fulleride Systems: Synthesis, Structural Studies and Electronic Properties2023

    • Author(s)
      Keisuke Matsui, Kosmas Prassides
    • Organizer
      International Symposium of the Graduate School of Engineering, Osaka Metropolitan University: World-Leading Engineering Research
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] Pressure Induced Self-doping in Mixed-valent Molecular Solids, RE2.75C602023

    • Author(s)
      Naoya Yoshikane, Kosmas Prassides
    • Organizer
      International Symposium of the Graduate School of Engineering, Osaka Metropolitan University: World-Leading Engineering Research
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] Something old, something new, something blue2023

    • Author(s)
      Kosmas Prassides
    • Organizer
      Phase Transition and Dynamical Properties of Spin Transition Materials (PDSTM 2023), Tokyo, Japan
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Superconductivity and quantum magnetism in π-electron systems: a personal ongoing voyage into the unexpected2022

    • Author(s)
      Kosmas Prassides
    • Organizer
      Seminar, Department of Chemistry, University of Crete
    • Related Report
      2021 Annual Research Report
    • Invited
  • [Presentation] Searching for the Hebel-Slichter coherence peak across the superconductivity dome of fullerides2022

    • Author(s)
      Kosmas Prassides
    • Organizer
      Superstripes 2022 International Conference, Frascati, Rome,Italy
    • Related Report
      2021 Annual Research Report
    • Invited
  • [Presentation] Synthesis and structural study of pentavalent fullerides2022

    • Author(s)
      Keisuke Matsui, Kosmas Prassides
    • Organizer
      2022 Summer School of the Young Coordination Chemists’ Association of Japan, held at Tokyo Institute of Technology
    • Related Report
      2021 Annual Research Report
  • [Presentation] Exploration of the Calcium-C60 Binary Phase Field2022

    • Author(s)
      Mizuki Suzuki, Kosmas Prassides
    • Organizer
      2022 Summer School of the Young Coordination Chemists’ Association of Japan, held at Tokyo Institute of Technology
    • Related Report
      2021 Annual Research Report
  • [Presentation] Mixed valency in (Sm1-xCax)2.75C602022

    • Author(s)
      Naoya Yoshikane, Kosmas Prassides
    • Organizer
      8th Asian Conference on Coordination Chemistry (ACCC8), online
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Structural control of Prussian blue analogues by alkali metal substitution2022

    • Author(s)
      Marina Nishiura, Kosmas Prassides
    • Organizer
      8th Asian Conference on Coordination Chemistry (ACCC8), online
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Ab initio structural investigation of C60/PAH co-adducts - new structures from powder diffraction data2022

    • Author(s)
      Akane Matsumoto, Kosmas Prassides
    • Organizer
      8th Asian Conference on Coordination Chemistry (ACCC8), online
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research
  • [Remarks] Electronic Functional Materials Laboratory

    • URL

      http://mtr1.osakafu-u.ac.jp/prassides-lab/

    • Related Report
      2021 Annual Research Report

URL: 

Published: 2021-04-28   Modified: 2024-12-25  

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