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Title: Inner-shell photoionization and core-hole decay of Xe and XeF2

Abstract

In this work, photoionization cross sections and partial ion yields of Xe and XeF2 from Xe 3d5/2, Xe 3d3/2, and F 1s subshells in the 660–740 eV range are compared to explore effects of the F ligands. The Xe 3d-$$ϵ$$f continuum shape resonances dominate the photoionization cross sections of both the atom and molecule, but prominent resonances appear in the XeF2 cross section due to nominal excitation of Xe 3d and F 1s electrons to the lowest unoccupied molecular orbital (LUMO), a delocalized anti-bonding MO. Comparisons of the ion products from the atom and molecule following Xe 3d photoionization show that the charge-state distribution of Xe ions is shifted to lower charge states in the molecule along with production of energetic F+ and F2+ ions. This suggests that, in decay of a Xe 3d core hole, charge is redistributed to the F ligands and the system dissociates due to Coulomb repulsion. The ion products from excitation of the F 1s-LUMO resonance are different and show strong increases in the yields of Xe+ and F+ ions. The subshell ionization thresholds, the LUMO resonance energies, and their oscillator strengths are calculated by relativistic coupled-cluster methods and agree well with measurements.

Authors:
 [1];  [2]; ORCiD logo [1];  [1];  [3];  [4]
+ Show Author Affiliations
  1. Argonne National Lab. (ANL), Argonne, IL (United States)
  2. Univ. of Wisconsin-Madison, Stoughton, WI (United States). Synchrotron Radiation Center (SRC)
  3. Univ. of Texas, Austin, TX (United States)
  4. Department of Chemistry and Biochemistry, The University of Texas at Austin, Austin, Texas 78712, USA
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; National Science Foundation (NSF)
OSTI Identifier:
1392461
Alternate Identifier(s):
OSTI ID: 1228186
Grant/Contract Number:  
AC02-06CH11357; CHE-1361031
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 142; Journal Issue: 22; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Southworth, Stephen H., Wehlitz, Ralf, Picón, Antonio, Lehmann, C. Stefan, Cheng, Lan, and Stanton, John F. Inner-shell photoionization and core-hole decay of Xe and XeF2. United States: N. p., 2015. Web. doi:10.1063/1.4922208.
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Southworth, Stephen H., Wehlitz, Ralf, Picón, Antonio, Lehmann, C. Stefan, Cheng, Lan, & Stanton, John F. Inner-shell photoionization and core-hole decay of Xe and XeF2. United States. https://doi.org/10.1063/1.4922208
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Southworth, Stephen H., Wehlitz, Ralf, Picón, Antonio, Lehmann, C. Stefan, Cheng, Lan, and Stanton, John F. Tue . "Inner-shell photoionization and core-hole decay of Xe and XeF2". United States. https://doi.org/10.1063/1.4922208. https://www.osti.gov/servlets/purl/1392461.
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@article{osti_1392461,
title = {Inner-shell photoionization and core-hole decay of Xe and XeF2},
author = {Southworth, Stephen H. and Wehlitz, Ralf and Picón, Antonio and Lehmann, C. Stefan and Cheng, Lan and Stanton, John F.},
abstractNote = {In this work, photoionization cross sections and partial ion yields of Xe and XeF2 from Xe 3d5/2, Xe 3d3/2, and F 1s subshells in the 660–740 eV range are compared to explore effects of the F ligands. The Xe 3d-$ϵ$f continuum shape resonances dominate the photoionization cross sections of both the atom and molecule, but prominent resonances appear in the XeF2 cross section due to nominal excitation of Xe 3d and F 1s electrons to the lowest unoccupied molecular orbital (LUMO), a delocalized anti-bonding MO. Comparisons of the ion products from the atom and molecule following Xe 3d photoionization show that the charge-state distribution of Xe ions is shifted to lower charge states in the molecule along with production of energetic F+ and F2+ ions. This suggests that, in decay of a Xe 3d core hole, charge is redistributed to the F ligands and the system dissociates due to Coulomb repulsion. The ion products from excitation of the F 1s-LUMO resonance are different and show strong increases in the yields of Xe+ and F+ ions. The subshell ionization thresholds, the LUMO resonance energies, and their oscillator strengths are calculated by relativistic coupled-cluster methods and agree well with measurements.},
doi = {10.1063/1.4922208},
journal = {Journal of Chemical Physics},
number = 22,
volume = 142,
place = {United States},
year = {Tue Jun 09 00:00:00 EDT 2015},
month = {Tue Jun 09 00:00:00 EDT 2015}
}
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https://doi.org/10.1063/1.4922208
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