Electron Scattering and Electron Angular Anisotropy in Water and Aqueous Solution

• Project/Area Number: 20K15229
• Research Category: Grant-in-Aid for Early-Career Scientists
• Allocation Type: Multi-year Fund
• Review Section: Basic Section 32010:Fundamental physical chemistry-related
• Research Institution: Kyoto University
• Principal Investigator: THUERMER STEPHAN 京都大学, 理学研究科, 准教授 (40722161)
• Project Period (FY): 2020-04-01 – 2024-03-31
• Project Status: Completed (Fiscal Year 2023)
• Budget Amount: ¥4,160,000 (Direct Cost: ¥3,200,000、Indirect Cost: ¥960,000); Fiscal Year 2022: ¥1,170,000 (Direct Cost: ¥900,000、Indirect Cost: ¥270,000); Fiscal Year 2021: ¥1,690,000 (Direct Cost: ¥1,300,000、Indirect Cost: ¥390,000); Fiscal Year 2020: ¥1,300,000 (Direct Cost: ¥1,000,000、Indirect Cost: ¥300,000)
• Keywords: electron spectroscopy / electron scattering / liquid water / photoelectron anisotropy / aqueous solution / synchrotron radiation

Outline of Research at the Start

Important for many chemical and biological processes is a solute’s propensity vs. depth and its orientation at the surface, which is measured with photoelectron spectroscopy by exploiting electron scattering. We quantify how electrons scatter and loose energy in aqueous solutions for this purpose.

Outline of Annual Research Achievements

The project is about electron scattering mechanisms in liquid water and aqueous solutions and its impact on photoelectron angular distributions 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 for interpreting of spectra from aqueous solutions.
The last year had several applications of the newly found understanding of electron scattering. Various surface-active solutes were studied, ranging from atmospherically-relevant organic molecular ions to prototypical species, which change their surface propensity as a function of pH value (i.e., the protonation state of the molecule). The former showed than the presence of multiple surface-active species can have a cooperative effect, strongly enhancing their surface propensity. This has large implications for the availability of species in atmospheric reactions. For the latter, we could show that the photoelectron signal and angular distribution are sensitively dependent on the surface propensity, which can be used as a precise depth scale into the solution. These studies are prepared for publication.
A newly developed method enabled us to study the work function (surface potential) and changes of the electronic structure of an aqueous solution as a function of solute concentration for the first time. This lays the foundation for extracting electrochemically relevant parameters, such as the electrochemical potential from aqueous solution, directly via photoelectron spectroscopy.

Research Products

• [Int'l Joint Research] Fritz Haber Institute/Helmholtz Zentrum Berlin/DESY Hamburg(ドイツ)
• [Int'l Joint Research] J. Heyrovsky Institute of Phys. Chem./University of Chemistry and Technology(チェコ)
• [Int'l Joint Research] Uppsala University(スウェーデン)
• [Int'l Joint Research] Fritz Haber Institute/Helmholtz Zentrum Berlin/DESY Hamburg(ドイツ)
• [Int'l Joint Research] Czech Academy of Sciences(チェコ)
• [Int'l Joint Research] Fritz Haber Institute/Helmholtz Zentrum Berlin/DESY Hamburg(ドイツ)
• [Int'l Joint Research] Czech Academy of Sciences(チェコ)
• [Int'l Joint Research] Fritz Haber Institute/Helmholtz Zentrum Berlin/DESY Hamburg(ドイツ)
• [Int'l Joint Research] Czech Academy of Sciences(チェコ)
• [Journal Article] Radiationless Decay Spectrum of O 1s Double Core Holes in Liquid Water (2024)
  • Author(s): Trinter Florian, Inhester Ludger, Puettner Ralph, Malerz Sebastian, Thuermer Stephan, Marchenko Tatiana, Piancastelli Maria-Novella, Simon Marc, Winter Bernd, Hergenhahn Uwe
  • Journal Title: The Journal of Chemical Physics Volume: - Issue: 19
  • DOI: 10.1063/5.0205994
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Photoelectron spectroscopy from a liquid flatjet (2023)
  • Author(s): Stemer Dominik、Buttersack Tillmann、Haak Henrik、Malerz Sebastian、Schewe Hanns Christian、Trinter Florian、Mudryk Karen、Pugini Michele、Credidio Bruno、Seidel Robert、Hergenhahn Uwe、Meijer Gerard、Thuermer Stephan、Winter Bernd
  • Journal Title: The Journal of Chemical Physics Volume: 158 Issue: 23 Pages: 234202-234202
  • DOI: 10.1063/5.0155182
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] How to measure work functions from aqueous solutions (2023)
  • Author(s): Pugini Michele、Credidio Bruno、Walter Irina、Malerz Sebastian、Trinter Florian、Stemer Dominik、Hergenhahn Uwe、Meijer Gerard、Wilkinson Iain、Winter Bernd、Thuermer Stephan
  • Journal Title: Chemical Science Volume: 14 Issue: 35 Pages: 9574-9588
  • DOI: 10.1039/d3sc01740k
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Absolute Electronic Energetics and Quantitative Work Functions of Liquids from Photoelectron Spectroscopy (2023)
  • Author(s): Winter Bernd、Thuermer Stephan、Wilkinson Iain
  • Journal Title: Accounts of Chemical Research Volume: 56 Issue: 2 Pages: 77-85
  • DOI: 10.1021/acs.accounts.2c00548
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Core-Level Photoelectron Angular Distributions at the Liquid-Vapor Interface (2023)
  • Author(s): Dupuy Remi、Thuermer Stephan、Richter Clemens、Buttersack Tillmann、Trinter Florian、Winter Bernd、Bluhm Hendrik
  • Journal Title: Accounts of Chemical Research Volume: 56 Issue: 3 Pages: 215-223
  • DOI: 10.1021/acs.accounts.2c00678
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Angstrom-Depth Resolution with Chemical Specificity at the Liquid-Vapor Interface (2023)
  • Author(s): Dupuy R.、Filser J.、Richter C.、Buttersack T.、Trinter F.、Gholami S.、Seidel R.、Nicolas C.、Bozek J.、Egger D.、Oberhofer H.、Th?rmer S.、Hergenhahn U.、Reuter K.、Winter B.、Bluhm H.
  • Journal Title: Physical Review Letters Volume: 130 Issue: 15 Pages: 156901-156901
  • DOI: 10.1103/physrevlett.130.156901
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Observation of intermolecular Coulombic decay and shake-up satellites in liquid ammonia (2022)
  • Author(s): Schewe Hanns Christian、Muchova Eva、Belina Michal、Buttersack Tillmann、Stemer Dominik、Seidel Robert、Thuermer Stephan、Slavcek Petr、Winter Bernd
  • Journal Title: Structural Dynamics Volume: 9 Issue: 4 Pages: 044901-044901
  • DOI: 10.1063/4.0000151
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Quantitative electronic structure and work-function changes of liquid water induced by solute (2022)
  • 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 Issue: 3 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 fenchone (2022)
  • 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 Issue: 14 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 solutions (2021)
  • 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 Issue: 31 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 solution (2021)
  • 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 Issue: 7869 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 Chemistry (2021)
  • 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 Issue: 32 Pages: 6881-6892
  • DOI: 10.1021/acs.jpca.1c04695
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Low-energy constraints on photoelectron spectra measured from liquid water and aqueous solutions (2021)
  • Author(s): Malerz Sebastian、Trinter Florian、Hergenhahn Uwe、Ghrist Aaron、Ali Hebatallah、Nicolas Christophe、Saak Clara-Magdalena、Richter Clemens、Hartweg Sebastian、Nahon Laurent、Lee Chin、Goy Claudia、Neumark Daniel M.、Meijer Gerard、Wilkinson Iain、Winter Bernd、Thuermer Stephan
  • Journal Title: Physical Chemistry Chemical Physics Volume: 23 Issue: 14 Pages: 8246-8260
  • DOI: 10.1039/d1cp00430a
  • Peer Reviewed / Open Access / Int'l Joint Research
• [Journal Article] Valence Photoelectron Spectra of Liquid Methanol and Ethanol Measured Using He II Radiation (2021)
  • Author(s): Thuermer Stephan、Shinno Takatoshi、Suzuki Toshinori
  • Journal Title: The Journal of Physical Chemistry A Volume: 125 Issue: 12 Pages: 2492-2503
  • DOI: 10.1021/acs.jpca.1c00288
  • Peer Reviewed
• [Presentation] How to measure work functions from aqueous solutions (2023)
  • Author(s): Stephan Thuermer
  • Organizer: 第17回分子科学討論会
• [Presentation] Photoelectron spectroscopy of Liquids: Accessing Electronic Energetics and Surface Properties (2023)
  • Author(s): Stephan Thuermer
  • Organizer: UVSOR-III+MAX IV International Workshop
  • Int'l Joint Research / Invited
• [Presentation] Shake-up and shake-off satellites as probe of ultrafast charge delocalization in liquid water (2023)
  • Author(s): Florian Trinter, Bernd Winter, Stephan Thuermer
  • Organizer: XXXIII International Conference on Photonic, Electronic and Atomic Collisions
  • Int'l Joint Research
• [Presentation] Photoelectron Circular Dichroism from Aqueous-Phase Biomolecules (2023)
  • Author(s): M. Pugini, K. Mudryk, D. Stemer, L. Tomanik, S. Malerz, F. Trinter, T. Buttersack, U. Hergenhahn, I. Wilkinson, S. Thuermer, P. Slavicek, G. Meijer, B. Winter
  • Organizer: DESY Photon Science Users' Meeting 2023
  • Int'l Joint Research
• [Presentation] Expanding Liquid-Jet Photoelectron Spectroscopy to Liquid Flatjets (2023)
  • Author(s): Stemer Dominik、Buttersack Tillmann、Haak Henrik、Malerz Sebastian、Schewe Hanns Christian、Trinter Florian、Mudryk Karen、Pugini Michele、Credidio Bruno、Seidel Robert、Hergenhahn Uwe、Meijer Gerard、Thuermer Stephan、Winter Bernd
  • Organizer: BESSY user meeting 2023
  • Int'l Joint Research
• [Presentation] Photoelectron Circular Dichroism from Aqueous-Phase Biomolecules (2023)
  • Author(s): M. Pugini, D. Stemer, K. Mudryk, L. Tomanik, S. Malerz, F. Trinter, T. Buttersack, U. Hergenhahn, I. Wilkinson, S. Thuermer, P. Slavicek, B. Winter, G. Meijer
  • Organizer: DESY Photon Science Users' Meeting 2023
  • Int'l Joint Research
• [Presentation] Core-ionization of Liquid Ammonia: Intermolecular Coulombic Decay and Shake-up Satellites (2022)
  • Author(s): S. Thuermer
  • Organizer: 第２５回 XAFS 討論会
• [Presentation] Measuring Fermi-referenced ionization energies and work functions from aqueous solution (hot topics) (2022)
  • Author(s): S. Thuermer
  • Organizer: International Workshop on Photoionization (IWP) Resonant Inelastic X-ray Scattering (RIXS) 2022
  • Int'l Joint Research
• [Presentation] Photoemission Studies On A Liquid Jet At The Petra III Beamline P04 (2022)
  • Author(s): F. Trinter, S.Malerz, K. Mudryk, D. Stemer, M. Pugini, T. Buttersack, M.N. Pohl, I. Wilkinson, U. Hergenhahn, S. Thuermer, B. Winter
  • Organizer: SNI2022
  • Int'l Joint Research
• [Presentation] Photoemission from aqueous solutions at PETRA III beamline P04: Towards detecting Photoelectron Circular Dichroism (PECD) (2022)
  • Author(s): S. Malerz, F. Trinter, U. Hergenhahn, T. Buttersack, D. Stemer, K. Mudryk, M. Pohl, G. Meijer, I. Wilkinson, S. Thuermer, B. Winter
  • Organizer: 14th International Conference on Synchrotron Radiation Instrumentation (SRI) 2022
  • Int'l Joint Research
• [Presentation] Novel energy-referencing approach for measuring accurate vertical ionization energies and work functions of liquid water and aqueous solutions (2022)
  • 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 water (2022)
  • 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 water (2021)
  • 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 energies (2021)
  • 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] Kyoto University Activity Dtabase
  • URL: https://kdb.iimc.kyoto-u.ac.jp/profile/ja.7b8f7b2e37181b16.html
• [Remarks] Kyoto University Activity Dtabase
  • URL: https://kdb.iimc.kyoto-u.ac.jp/profile_private/en.7b8f7b2e37181b16.html
• [Remarks] University Group Homepage
  • URL: http://kuchem.kyoto-u.ac.jp/bukka/