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2021 Fiscal Year Annual Research Report

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

Research Project

Project/Area Number 21H01907
Research InstitutionOsaka Prefecture University

Principal Investigator

プラシデス コスマス  大阪府立大学, 工学(系)研究科(研究院), 教授 (90719006)

Project Period (FY) 2021-04-01 – 2024-03-31
Keywordscarbon-based / molecular materials / spin liquids / polyaromatics / fullerenes
Outline of Annual Research Achievements

The project targets the synthesis of 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 combining with high-level theory and integrated with a range of state-of-the-art structural and magnetic measurement techniques to identify the new electronic states that arise. To-date, two key research achievements have been reached: (i) the demonstration of the sensitivity of the fragile magnetic states to small perturbations induced by the chemical dopants that lead to transitions to long-range-ordered magnetic states, and (ii) the incorporation of spherical units like C60 to afford hybrid systems, promising candidates of new metallic and superconducting states.

Current Status of Research Progress
Current Status of Research Progress

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

Reason

Progress has been very satisfactory with new directions and opportunities appearing. Work on pi-electron carbon-based molecular materials has led to families of new materials and new properties are emerging. The wealth of reduced pi-electron families of polyaromatic hydrocarbons chemically synthesized in this work has led to numerous investigations of the fragility of the magnetic states with changes in the nature of the dopant and the modified crystalline structures. In addition, first steps towards synthesizing hybrid pi-electron systems have been successful by incorporating fullerenes into the polyaromatic hydrocarbon architectures. Structural and magnetic characterizations are in progress.

Strategy for Future Research Activity

The behavior of the binary phases of reduced polyaromatic hydrocarbons doped with alkali metals will be investigated by a variety of experimental techniques probing accurately both the changes in crystalline structure and the resulting changes in the magnetic properties. Experimental techniques to be used will be synchrotron X-ray and powder neutron diffraction combined with complementary magnetization, EPR, NMR and muSR measurements. The separate thread of hybrid molecular solids will be extended to include the isolation of reduced phases where the number of injected electrons is accurately controlled. The characterization of the line phases resulting as a result of this chemistry will be attempted at first stage by synchrotron X-ray diffraction and by SQUID magnetometry.

  • Research Products

    (10 results)

All 2023 2022 Other

All Int'l Joint Research (1 results) Journal Article (1 results) Presentation (7 results) (of which Int'l Joint Research: 3 results,  Invited: 2 results) Remarks (1 results)

  • [Int'l Joint Research] NCSR Demokritos(ギリシャ)

    • Country Name
      GREECE
    • Counterpart Institution
      NCSR Demokritos
  • [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 Pages: 035110

    • DOI

      10.1103/PhysRevB.107.035110

  • [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
    • 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
    • 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
  • [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
  • [Presentation] Mixed valency in (Sm1-xCax)2.75C602022

    • Author(s)
      Naoya Yoshikane, Kosmas Prassides
    • Organizer
      8th Asian Conference on Coordination Chemistry (ACCC8), online
    • 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
    • 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
    • Int'l Joint Research
  • [Remarks] Electronic Functional Materials Laboratory

    • URL

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

URL: 

Published: 2023-12-25  

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