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| 001 | 630677 | ||
| 005 | 20250723105959.0 | ||
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| 100 | 1 | _ | |a Thuermer, Stephan |0 P:(DE-H253)PIP1086906 |b 0 |e Corresponding author |
| 245 | _ | _ | |a Low-Energy Photoelectron Spectroscopy and Scattering from Aqueous Solutions and the Role of Solute Surface Activity |
| 260 | _ | _ | |a Washington, DC |c 2025 |b ACS Publications |
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| 520 | _ | _ | |a Experimental insights into low-kinetic-energy electron scattering in aqueous solutions are essential for an improved understanding of electron-driven chemistry and radiobiology, and the development and informed application of aqueous-phase electron-based spectroscopy and dichroism methods. Generally, in aqueous environments and for electron kinetic energies below 12–15 eV, significant and, thus far, incompletely understood low-energy-transfer inelastic electron scattering with solvent molecules preponderates. This leads to cascades of tens-of-meV kinetic-energy losses that distort nascent photoelectron spectra, prevent direct and accurate electron-binding-energy measurements, and limit possibilities to determine electron-scattering cross sections at especially low electron kinetic energies. Here, we quantify aqueous-phase inelastic-scattering-based energy losses using 1–30 eV kinetic energy photoelectrons and liquid-jet photoemission spectroscopy, specifically by photoionizing an exemplary surface-active solute and comparing the results with those from the homogeneously distributed aqueous solvent. Thereby, we identify a general ≳17 eV electron-kinetic-energy requirement for the direct and accurate measurement of aqueous-phase electron binding energies, irrespective of interfacial concentration profiles. Further, at electron kinetic energies from 10 eV down to a few-eV above the ionization threshold, we observe and quantify lower degrees of scattering for photoelectrons generated from surface-active solutes, allowing moderately distorted surface-active-solute photoemission peaks to be resolved down to just few-eV electron kinetic energies. These results demonstrate that liquid-jet photoemission spectroscopy can be used to probe interfacial surface-active-solute dynamics and dichroism effects close to ionization thresholds, in stark contrast to similar experiments on homogeneously distributed solution components. Furthermore, they offer novel insights into low-electron-kinetic-energy scattering in aqueous environments, thereby addressing the current lack of reliable experimental data in this critical energy range. |
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| 700 | 1 | _ | |a Stemer, Dominik |0 P:(DE-H253)PIP1096040 |b 1 |
| 700 | 1 | _ | |a Trinter, Florian |0 P:(DE-H253)PIP1017364 |b 2 |
| 700 | 1 | _ | |a Kiyan, Igor Yu |0 P:(DE-HGF)0 |b 3 |
| 700 | 1 | _ | |a Winter, Bernd |0 P:(DE-H253)PIP1023483 |b 4 |
| 700 | 1 | _ | |a Wilkinson, Iain |0 P:(DE-H253)PIP1086922 |b 5 |e Corresponding author |
| 773 | _ | _ | |a 10.1021/jacs.5c04263 |g Vol. 147, no. 23, p. 19868 - 19877 |0 PERI:(DE-600)1472210-0 |n 23 |p 19868 - 19877 |t Journal of the American Chemical Society |v 147 |y 2025 |x 0002-7863 |
| 856 | 4 | _ | |u https://pubs.acs.org/doi/full/10.1021/jacs.5c04263 |
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