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Elucidation of the unified mechanism of molecular nuclear-spin-conversion with use of rotationally resolved spectroscopy

Research Project

Project/Area Number 20K05424
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeMulti-year Fund
Section一般
Review Section Basic Section 32010:Fundamental physical chemistry-related
Research InstitutionJapan Atomic Energy Agency

Principal Investigator

Yamakawa Koichiro  国立研究開発法人日本原子力研究開発機構, 原子力科学研究部門 原子力科学研究所 先端基礎研究センター, 研究副主幹 (60633279)

Co-Investigator(Kenkyū-buntansha) 福谷 克之  東京大学, 生産技術研究所, 教授 (10228900)
Project Period (FY) 2020-04-01 – 2023-03-31
Project Status Completed (Fiscal Year 2022)
Budget Amount *help
¥4,290,000 (Direct Cost: ¥3,300,000、Indirect Cost: ¥990,000)
Fiscal Year 2022: ¥390,000 (Direct Cost: ¥300,000、Indirect Cost: ¥90,000)
Fiscal Year 2021: ¥390,000 (Direct Cost: ¥300,000、Indirect Cost: ¥90,000)
Fiscal Year 2020: ¥3,510,000 (Direct Cost: ¥2,700,000、Indirect Cost: ¥810,000)
Keywords核スピン転換 / ラマン分光 / テラヘルツ分光
Outline of Research at the Start

ラマン分光法,テラヘルツ-赤外吸収分光法,多光子共鳴イオン化法を用い,分子固体の内部,表面に捕捉したH2, H2O, CH4の単量体及びクラスターの核スピン転換速度を測定し,転換機構を解明する.研究は次の2段階で進める.
① H2, H2O, CH4単量体の核スピン転換を同一環境下で測定し,二・多原子分子の転換機構の統一的解明を目指す.
② 異種2量体H2-H2O, H2-CH4, H2O-CH4の核スピン転換を観測する.2量体中の両分子の転換を同時観測すると共に,分子間振動モードも測定することで,転換機構を解き明かす.

Outline of Final Research Achievements

Molecules including the hydrogen nuclei in the rotationally symmetric positions are classified into nuclear spin isomers, according to the quantum number of their resultant spin. In the present work, we targeted at the fundamental molecules of hydrogen, water, ammonia, and methane, and observed the interconversion between the nuclear spin isomers by using rotationally resolved spectroscopy. We isolated hydrogen in condensed layers of carbon dioxide, and detected weak infrared absorption by polarized hydrogen. The conversion rate was determined from its time development. In addition, we investigated the oxygen-isotope effect on the conversion rate of water molecules, and found the abnormal temperature dependence of the conversion rate of ammonia. Furthermore, we analyzed the time evolution of the infrared spectrum of crystalline methane on the basis of the nuclear spin conversion, and determined the assignments of absorption signals in a combination-tone region.

Academic Significance and Societal Importance of the Research Achievements

核スピン転換の研究は,分子と凝縮系との間の磁気相互作用とエネルギー授受の究明という基礎物理学的観点,水素の効率的な液化貯蔵に代表される産業的観点,そして宇宙における天体の熱履歴の解明という天文学的観点から,重要な意義を持つ.本研究で行った一連の実験によって,水素,水,アンモニア,メタンという基本的な分子の核スピン転換特性が明らかになり,転換メカニズムの理解が大きく進んだ.さらに,核スピン転換の解析がスペクトルを解釈する上でも有用であることが,本研究により示された.

Report

(4 results)
  • 2022 Annual Research Report   Final Research Report ( PDF )
  • 2021 Research-status Report
  • 2020 Research-status Report
  • Research Products

    (13 results)

All 2022 2021 2020

All Journal Article (5 results) (of which Peer Reviewed: 5 results) Presentation (8 results) (of which Int'l Joint Research: 2 results,  Invited: 3 results)

  • [Journal Article] Nuclear-spin conversion analysis of ν2 + ν4 combination band of crystalline methane in phase II2021

    • Author(s)
      Takeru Sugimoto, Koichiro Yamakawa
    • Journal Title

      J. Chem. Phys.

      Volume: 154 Pages: 1-4

    • Related Report
      2020 Research-status Report
    • Peer Reviewed
  • [Journal Article] 凝縮系での分子の振動回転および核スピン転換に関する理論・分光研究2020

    • Author(s)
      山川紘一郎
    • Journal Title

      しょうとつ

      Volume: 17 Pages: 86-101

    • Related Report
      2020 Research-status Report
    • Peer Reviewed
  • [Journal Article] その場テラヘルツ・赤外吸収分光装置の開発2020

    • Author(s)
      山川紘一郎, 那須裕一, 清水元希
    • Journal Title

      分光研究

      Volume: 69 Pages: 105-106

    • Related Report
      2020 Research-status Report
    • Peer Reviewed
  • [Journal Article] Fast nuclear-spin conversion of H2 trapped and polarized in a CO2 matrix2020

    • Author(s)
      Koichiro Yamakawa, Atsuki Ishibashi, Toshinobu Namiyoshi, Yuichi Azuma, Ichiro Arakawa
    • Journal Title

      Physical Review B Rapid Communication

      Volume: 102 Pages: 1-5

    • Related Report
      2020 Research-status Report
    • Peer Reviewed
  • [Journal Article] Terahertz and mid-infrared spectroscopy of matrix-isolated clusters and matrix-sublimation ice of D2O2020

    • Author(s)
      Koichiro Yamakawa, Hirokazu Nasu, Natsumi Suzuki, Genki Shimizu, Ichiro Arakawa
    • Journal Title

      Journal of Chemical Physics

      Volume: 152 Pages: 1-13

    • Related Report
      2020 Research-status Report
    • Peer Reviewed
  • [Presentation] 水素結合クラスターの超高真空下テラヘルツ・赤外分光2022

    • Author(s)
      山川紘一郎,那須裕一,鈴木菜摘,清水元希,荒川一郎
    • Organizer
      第32回MRS年次大会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 分子の核スピン異性化とクラスター化に関するテラヘルツ・赤外分光研究2022

    • Author(s)
      山川紘一郎
    • Organizer
      2022年度日本分光学会年次講演会
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] Infrared-spectroscopic study of the photolysis in CO-X ice with use of isotopologues2022

    • Author(s)
      Akemi Hirayama, Ichiro Arakawa, Koichiro Yamakawa
    • Organizer
      22nd International Vacuum Conference
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Non-destructive observation of nuclear spin conversion in diatomic and polyatomic molecules2022

    • Author(s)
      Koichiro Yamakawa
    • Organizer
      1st Workshop on Molecular Dynamics at Surfaces
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] その場テラヘルツ・赤外分光法を用いた分子の振動・核スピンダイナミクスの研究2022

    • Author(s)
      山川紘一郎
    • Organizer
      日本物理学会第77回年次大会
    • Related Report
      2021 Research-status Report
    • Invited
  • [Presentation] 希ガス凝縮層中に分離した多原子分子の核スピン転換2021

    • Author(s)
      川邉裕之,荒川一郎,山川紘一郎
    • Organizer
      2021年日本表面真空学会学術講演会
    • Related Report
      2021 Research-status Report
  • [Presentation] 二酸化炭素凝縮層中に捕捉した水素の核スピン転換2021

    • Author(s)
      山川紘一郎,石橋篤季,波吉敏信,荒川一郎,
    • Organizer
      日本物理学会第76回年次大会
    • Related Report
      2020 Research-status Report
  • [Presentation] マトリックス分離した水素の核スピン転換の非破壊観測2020

    • Author(s)
      山川紘一郎,石橋篤季,波吉敏信,荒川一郎
    • Organizer
      第3回ハイドロジェノミクス研究会
    • Related Report
      2020 Research-status Report

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Published: 2020-04-28   Modified: 2024-01-30  

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