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  Probing the Electronic Structure of Bulk Water at the Molecular Length Scale with Angle-Resolved Photoelectron Spectroscopy

Gozem, S., Seidel, R., Hergenhahn, U., Lugovoy, E., Abel, B., Winter, B., et al. (2020). Probing the Electronic Structure of Bulk Water at the Molecular Length Scale with Angle-Resolved Photoelectron Spectroscopy. The Journal of Physical Chemistry Letters, 11(13), 5162-5170. doi:10.1021/acs.jpclett.0c00968.

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Gozem, Samer1, Autor
Seidel, Robert2, 3, Autor
Hergenhahn, U.4, 5, Autor           
Lugovoy, Evgeny4, 6, Autor
Abel, Bernd4, 6, Autor
Winter, Bernd5, Autor           
Krylov, Anna I.7, 8, Autor
Bradforth, Stephen E.7, Autor
Affiliations:
1Department of Chemistry, Georgia State University, Atlanta, Georgia 30303, United States, ou_persistent22              
2Helmholtz-Zentrum Berlin für Materialien und Energie, 12489 Berlin, Germany, ou_persistent22              
3Humboldt-Universität zu Berlin, Department of Chemistry, 12489 Berlin, Germany, ou_persistent22              
4Leibniz Institute of Surface Engineering IOM), Department of Functional Surfaces, 04318 Leipzig, Germany, ou_persistent22              
5Molecular Physics, Fritz Haber Institute, Max Planck Society, ou_634545              
6University of Leipzig, Wilhelm-Ostwald-Institute for Physical and Theoretical Chemistry, 04318 Leipzig, Germany, ou_persistent22              
7Department of Chemistry, University of Southern California, Los Angeles, CA 90089, United States, ou_persistent22              
8Hamburg Centre for Ultrafast Imaging, Luruper Chaussee 149, Hamburg 22671, Germany, ou_persistent22              

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Schlagwörter: Magnetic properties, Electrical energy, Energy, Kinetics, Molecules
 Zusammenfassung: We report a combined experimental and theoretical study of bulk water photoionization. Angular distributions of photoelectrons produced by ionizing the valence bands of neat water using X-ray radiation (250–750 eV) show a limited (∼20%) decrease in the β anisotropy parameter compared to the gas phase, indicating that the electronic structure of the individual water molecules can be probed. We show that, in the high-energy regime, photoionization of bulk can be described using an incoherent superposition of individual molecules, in contrast to a low-energy regime where photoionization probes delocalized entangled states of molecular aggregates. The two regimes—low versus high energy—are limiting cases where the de Broglie wavelength of the photoelectron is larger or smaller than the intermolecular distance between water molecules, respectively. The comparison of measured and computed anisotropies reveals that the reduction in β at high kinetic energies is mostly due to scattering rather than rehybridization due to solvation.

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Sprache(n): eng - English
 Datum: 2020-03-272020-06-012020-06-012020-07-02
 Publikationsstatus: Erschienen
 Seiten: 9
 Ort, Verlag, Ausgabe: -
 Inhaltsverzeichnis: -
 Art der Begutachtung: Expertenbegutachtung
 Identifikatoren: DOI: 10.1021/acs.jpclett.0c00968
 Art des Abschluß: -

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Titel: The Journal of Physical Chemistry Letters
  Kurztitel : J. Phys. Chem. Lett.
Genre der Quelle: Zeitschrift
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Affiliations:
Ort, Verlag, Ausgabe: Washington, DC : American Chemical Society
Seiten: 9 Band / Heft: 11 (13) Artikelnummer: - Start- / Endseite: 5162 - 5170 Identifikator: CoNE: https://pure.mpg.de/cone/journals/resource/1948-7185