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2021 年度 実施状況報告書

Electron Scattering and Electron Angular Anisotropy in Water and Aqueous Solution

研究課題

研究課題/領域番号 20K15229
研究機関京都大学

研究代表者

THUERMER STEPHAN  京都大学, 理学研究科, 准教授 (40722161)

研究期間 (年度) 2020-04-01 – 2023-03-31
キーワードelectron spectroscopy / electron scattering / liquid water / photoelectron anisotropy
研究実績の概要

The project studies electron scattering and its impact on electron angular distributions in liquids using photoelectron spectroscopy in international collaboration. Electron scattering is crucial for understanding energy deposition, radical formation and biological damage by slow and fast electrons, and a correct interpretation of spectra from liquid water and aqueous solutions.
A novel energy-referencing scheme has been developed to determine accurate ionization energies from aqueous solutions down to a few-10 meV scale. This enables the study of surface-specific effects as well as detection of even small energy shifted due to inelastic electron scattering.
This novel method was then applied to solutions of sodium iodide and tetrabutylammonium iodide, which showed very different concentration-dependent energy shifts. The former is a model system for bulk electronic structure changes while the latter is a surface-active species, which modifies the surface potential of the solution.
Knowledge of electron scattering behavior at low kinetic energies was used to interpret the very first photoelectron circular dichroism from liquid fenchone, a chiral molecule. After careful subtraction of the scattering background signal a significant left / right asymmetry was found. This first result opens the path for studies of biologically relevant molecules in aqueous solutions.

現在までの達成度 (区分)
現在までの達成度 (区分)

1: 当初の計画以上に進展している

理由

Even though the pandemic is still ongoing, effective online collaboration and work sharing with international partners have resulted in good progress of the project. Experimental measurements are ongoing in Germany, while analysis is conducted in Japan. Several topics are already in the wrap-up phase on the way to publishing results while experiments continue in parallel.
The new absolute-energy referencing method developed last year in combination with gained knowledge on electron scattering behavior at low kinetic energies proved to be a crucial basis to study photoemission from a flat jet as well as from chiral molecules, both emerging new fields in liquid-jet spectroscopy.
Overall, the project is progressing smoothly and already more difficult-to-interpret solutes are being studied.

今後の研究の推進方策

While the pandemic situation is slowly relaxing, the collaboration will continue online for the time being. Plans to resume travel for a more direct collaboration and on-site experiments in Germany are underway.
After establishing accurate binding-energy measurements the next goal is to access energies referenced to the Fermi-level (or electrochemical potential), which will make it possible to discern surface- or bulk specific effects of solutes. This promises to open the pathway for quantifying probing depth and a solution's surface potential. In parallel, measurements of calibrated liquid-phase spectra will be undertaken, which are then compared with a physical scattering model to gain insight into then relative probability of electron scattering at different energies.

次年度使用額が生じた理由

The project proposed international collaboration with mainly business travel expenses to join experiments in Europe and discuss with collaboration partners directly. This has unfortunately been made impossible by the ongoing corona pandemic. Thanks to effective online collaboration the research project is not negatively impacted by this. Travel will be resumed for a more effective collaboration as soon as the travel restrictions have been lifted. If possible the expenses will be used for 2-3 business trips to Europe and travel to conferences as originally planned in the proposal.

  • 研究成果

    (13件)

すべて 2022 2021 その他

すべて 国際共同研究 (2件) 雑誌論文 (5件) (うち国際共著 5件、 査読あり 5件、 オープンアクセス 5件) 学会発表 (4件) (うち国際学会 2件) 備考 (2件)

  • [国際共同研究] Fritz Haber Institute/Helmholtz Zentrum Berlin/DESY Hamburg(ドイツ)

    • 国名
      ドイツ
    • 外国機関名
      Fritz Haber Institute/Helmholtz Zentrum Berlin/DESY Hamburg
  • [国際共同研究] Czech Academy of Sciences(チェコ)

    • 国名
      チェコ
    • 外国機関名
      Czech Academy of Sciences
  • [雑誌論文] Quantitative electronic structure and work-function changes of liquid water induced by solute2022

    • 著者名/発表者名
      Credidio Bruno、Pugini Michele、Malerz Sebastian、Trinter Florian、Hergenhahn Uwe、Wilkinson Iain、Thuermer Stephan、Winter Bernd
    • 雑誌名

      Physical Chemistry Chemical Physics

      巻: 24 ページ: 1310~1325

    • DOI

      10.1039/D1CP03165A

    • 査読あり / オープンアクセス / 国際共著
  • [雑誌論文] Photoelectron circular dichroism in angle-resolved photoemission from liquid fenchone2022

    • 著者名/発表者名
      Pohl Marvin N.、Malerz Sebastian、Trinter Florian、Lee Chin、Kolbeck Claudia、Wilkinson Iain、Thuermer Stephan、Neumark Daniel M.、Nahon Laurent、Powis Ivan、Meijer Gerard、Winter Bernd、Hergenhahn Uwe
    • 雑誌名

      Physical Chemistry Chemical Physics

      巻: 24 ページ: 8081~8092

    • DOI

      10.1039/D1CP05748K

    • 査読あり / オープンアクセス / 国際共著
  • [雑誌論文] Accurate vertical ionization energy and work function determinations of liquid water and aqueous solutions2021

    • 著者名/発表者名
      Thuermer Stephan、Malerz Sebastian、Trinter Florian、Hergenhahn Uwe、Lee Chin、Neumark Daniel M.、Meijer Gerard、Winter Bernd、Wilkinson Iain
    • 雑誌名

      Chemical Science

      巻: 12 ページ: 10558~10582

    • DOI

      10.1039/D1SC01908B

    • 査読あり / オープンアクセス / 国際共著
  • [雑誌論文] Spectroscopic evidence for a gold-coloured metallic water solution2021

    • 著者名/発表者名
      Mason Philip E.、Schewe H. Christian、Buttersack Tillmann、Kostal Vojtech、Vitek Marco、McMullen Ryan S.、Ali Hebatallah、Trinter Florian、Lee Chin、Neumark Daniel M.、Thuermer Stephan、Seidel Robert、Winter Bernd、Bradforth Stephen E.、Jungwirth Pavel
    • 雑誌名

      Nature

      巻: 595 ページ: 673~676

    • DOI

      10.1038/s41586-021-03646-5

    • 査読あり / オープンアクセス / 国際共著
  • [雑誌論文] Following in Emil Fischer’s Footsteps: A Site-Selective Probe of Glucose Acid-Base Chemistry2021

    • 著者名/発表者名
      Malerz Sebastian、Mudryk Karen、Tomanik Lukas、Stemer Dominik、Hergenhahn Uwe、Buttersack Tillmann、Trinter Florian、Seidel Robert、Quevedo Wilson、Goy Claudia、Wilkinson Iain、Thuermer Stephan、Slavicek Petr、Winter Bernd
    • 雑誌名

      The Journal of Physical Chemistry A

      巻: 125 ページ: 6881~6892

    • DOI

      10.1021/acs.jpca.1c04695

    • 査読あり / オープンアクセス / 国際共著
  • [学会発表] Novel energy-referencing approach for measuring accurate vertical ionization energies and work functions of liquid water and aqueous solutions2022

    • 著者名/発表者名
      Florian Trinter
    • 学会等名
      DESY Photon Science Users' Meeting 2022
    • 国際学会
  • [学会発表] How shake-up and shake-off satellites can reveal ultrafast charge delocalization in liquid water2022

    • 著者名/発表者名
      Stephan Thuermer
    • 学会等名
      Molecular Physics and Physical Chemistry with Advanced Photon Sources - 739. WE-Heraeus-Seminar
    • 国際学会
  • [学会発表] Shake-up and shake-off satellites as a probe of ultrafast charge delocalization in liquid water2021

    • 著者名/発表者名
      Stephan Thuermer
    • 学会等名
      第24回XAFS討論会
  • [学会発表] How electron scattering impacts photoelectron spectra of liquid water and aqueous solutions at low energies2021

    • 著者名/発表者名
      Stephan Thuermer
    • 学会等名
      第15回分子科学討論会
  • [備考] Google Scholar User Profile

    • URL

      https://scholar.google.com/citations?user=05yx0h0AAAAJ

  • [備考] University Group Homepage

    • URL

      http://kuchem.kyoto-u.ac.jp/bukka/

URL: 

公開日: 2022-12-28  

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