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Energy-Dependent Relative Cross Sections in Carbon 1s Photoionization: Separation of Direct Shake and Inelastic Scattering Effects in Single Molecules
Sorbonne Univ, LCPMR, CNRS, UMR7614, Paris, France;LOrme Merisiers, Synchrotron Soleil, F-91192 Gif Sur Yvette, France.
Univ Oulu, Fac Sci, Nano & Mol Syst Res Unit, POB 3000, Oulu 90014, Finland.ORCID iD: 0000-0002-2970-7494
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and Condensed Matter Physics.ORCID iD: 0000-0002-9647-0394
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Inorganic Chemistry. Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and Condensed Matter Physics.ORCID iD: 0000-0002-9188-9604
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2019 (English)In: Journal of Physical Chemistry A, ISSN 1089-5639, E-ISSN 1520-5215, Vol. 123, no 35, p. 7619-7635Article in journal (Refereed) Published
Abstract [en]

We demonstrate that the possibility of monitoring relative photoionization cross sections over a large photon energy range allows us to study and disentangle shake processes and intramolecular inelastic scattering effects. In this gas-phase study, relative intensities of the carbon 1s photoelectron lines from chemically inequivalent carbon atoms in the same molecule have been measured as a function of the incident photon energy in the range of 300-6000 eV. We present relative cross sections for the chemically shifted carbon 1s lines in the photoelectron spectra of ethyl trifluoroacetate (the "ESCA" molecule). The results are compared with those of methyl trifluoroacetate and S-ethyl trifluorothioacetate as well as a series of chloro-substituted ethanes and 2-butyne. In the soft X-ray energy range, the cross sections show an extended X-ray absorption fine structure type of wiggles, as was previously observed for a series of chloroethanes. The oscillations are damped in the hard X-ray energy range, but deviations of cross-section ratios from stoichiometry persist, even at high energies. The current findings are supported by theoretical calculations based on a multiple scattering model. The use of soft and tender X-rays provides a more complete picture of the dominant processes accompanying photoionization. Such processes reduce the main photoelectron line intensities by 20-60%. Using both energy ranges enabled us to discern the process of intramolecular inelastic scattering of the outgoing electron, whose significance is otherwise difficult to assess for isolated molecules. This effect relates to the notion of the inelastic mean free path commonly used in photoemission studies of clusters and condensed matter.

Place, publisher, year, edition, pages
AMER CHEMICAL SOC , 2019. Vol. 123, no 35, p. 7619-7635
National Category
Theoretical Chemistry Physical Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-394685DOI: 10.1021/acs.jpca.9b05063ISI: 000484884200011PubMedID: 31386367OAI: oai:DiVA.org:uu-394685DiVA, id: diva2:1366662
Conference
64th Pacific Conference on Spectroscopy and Dynamics (PCSD), JAN 19-22, 2017, Pacific Grove, CA
Funder
Knut and Alice Wallenberg FoundationAvailable from: 2019-10-30 Created: 2019-10-30 Last updated: 2019-10-30Bibliographically approved

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Söderström, JohanLindblad, AndreasMårtensson, NilsSvensson, Svante

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