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2021 Fiscal Year Research-status Report

Electron Scattering and Electron Angular Anisotropy in Water and Aqueous Solution

Research Project

Project/Area Number 20K15229
Research InstitutionKyoto University

Principal Investigator

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

Project Period (FY) 2020-04-01 – 2023-03-31
Keywordselectron spectroscopy / electron scattering / liquid water / photoelectron anisotropy
Outline of Annual Research Achievements

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.

Current Status of Research Progress
Current Status of Research Progress

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

Reason

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.

Strategy for Future Research Activity

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.

Causes of Carryover

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.

  • Research Products

    (13 results)

All 2022 2021 Other

All Int'l Joint Research (2 results) Journal Article (5 results) (of which Int'l Joint Research: 5 results,  Peer Reviewed: 5 results,  Open Access: 5 results) Presentation (4 results) (of which Int'l Joint Research: 2 results) Remarks (2 results)

  • [Int'l Joint Research] Fritz Haber Institute/Helmholtz Zentrum Berlin/DESY Hamburg(ドイツ)

    • Country Name
      GERMANY
    • Counterpart Institution
      Fritz Haber Institute/Helmholtz Zentrum Berlin/DESY Hamburg
  • [Int'l Joint Research] Czech Academy of Sciences(チェコ)

    • Country Name
      CZECH
    • Counterpart Institution
      Czech Academy of Sciences
  • [Journal Article] Quantitative electronic structure and work-function changes of liquid water induced by solute2022

    • Author(s)
      Credidio Bruno、Pugini Michele、Malerz Sebastian、Trinter Florian、Hergenhahn Uwe、Wilkinson Iain、Thuermer Stephan、Winter Bernd
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: 24 Pages: 1310~1325

    • DOI

      10.1039/D1CP03165A

    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Photoelectron circular dichroism in angle-resolved photoemission from liquid fenchone2022

    • Author(s)
      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
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: 24 Pages: 8081~8092

    • DOI

      10.1039/D1CP05748K

    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Accurate vertical ionization energy and work function determinations of liquid water and aqueous solutions2021

    • Author(s)
      Thuermer Stephan、Malerz Sebastian、Trinter Florian、Hergenhahn Uwe、Lee Chin、Neumark Daniel M.、Meijer Gerard、Winter Bernd、Wilkinson Iain
    • Journal Title

      Chemical Science

      Volume: 12 Pages: 10558~10582

    • DOI

      10.1039/D1SC01908B

    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Spectroscopic evidence for a gold-coloured metallic water solution2021

    • Author(s)
      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
    • Journal Title

      Nature

      Volume: 595 Pages: 673~676

    • DOI

      10.1038/s41586-021-03646-5

    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Following in Emil Fischer’s Footsteps: A Site-Selective Probe of Glucose Acid-Base Chemistry2021

    • Author(s)
      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
    • Journal Title

      The Journal of Physical Chemistry A

      Volume: 125 Pages: 6881~6892

    • DOI

      10.1021/acs.jpca.1c04695

    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Presentation] Novel energy-referencing approach for measuring accurate vertical ionization energies and work functions of liquid water and aqueous solutions2022

    • Author(s)
      Florian Trinter
    • Organizer
      DESY Photon Science Users' Meeting 2022
    • Int'l Joint Research
  • [Presentation] How shake-up and shake-off satellites can reveal ultrafast charge delocalization in liquid water2022

    • Author(s)
      Stephan Thuermer
    • Organizer
      Molecular Physics and Physical Chemistry with Advanced Photon Sources - 739. WE-Heraeus-Seminar
    • Int'l Joint Research
  • [Presentation] Shake-up and shake-off satellites as a probe of ultrafast charge delocalization in liquid water2021

    • Author(s)
      Stephan Thuermer
    • Organizer
      第24回XAFS討論会
  • [Presentation] How electron scattering impacts photoelectron spectra of liquid water and aqueous solutions at low energies2021

    • Author(s)
      Stephan Thuermer
    • Organizer
      第15回分子科学討論会
  • [Remarks] Google Scholar User Profile

    • URL

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

  • [Remarks] University Group Homepage

    • URL

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

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Published: 2022-12-28  

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