Electron correlation in double photoexcitation of H2S as studied by H(2p) formation: Comparison with H2O

Kouichi Hosaka, Yutaro Torizuka, Kai Minamizaki, Philipp Schmidt, Andre Knie, Arno Ehresmann, Takeshi Odagiri, Masashi Kitajima, and Noriyuki Kouchi
Phys. Rev. A 98, 052514 – Published 29 November 2018

Abstract

Superexcited states of H2S have been investigated with determining the cross sections for emission of dispersed and nondispersed atomic fluorescence against the incident photon energy in the range 11–40 eV to address the ionization and excitation of the valence electrons. This method enables us to extract the discrete electronic state from the superposition with continuous electronic states. The cross sections for H(2p) formation have been put on an absolute scale. Ten superexcited states have been found, two in the range 13–15 eV are singly excited 2b21(mo) states with a single configuration and the other eight states in the range 16–25 eV are doubly excited states with multiple configurations. State-resolved dipole oscillator strengths for H(2p) formation in the photoexcitation of H2S have been determined. Similar experiments have been performed for H2O. The state-resolved dipole oscillator strengths for H(2p) formation in the photoexcitation of H2S are 103, whereas those in the photoexcitation of H2O range from 103 to 102. It is found that major fragment atoms are H(2p) atoms in the photoexcitation of H2O and S* in the photoexcitation of H2S. The superexcited states of H2O and H2S are compared based on the similarity and difference of the electronic structures. It turns out from the comparison that (i) the smaller values of the dipole oscillator strengths for H(2p) formation in the photoexcitation of H2S are related to the change of the major fragment atoms and (ii) the energy splitting of the doubly excited “4a11(mo)” states of H2S is enhanced in comparison with that of the doubly excited “2a11(mo)” states of H2O. This enhancement is caused by the stronger electron correlation in H2S than in H2O. The similarity in shape is indicated between the inner valence band and inner shell band in the fluorescence cross sections against the incident photon energy for H2S and H2O.

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  • Received 26 June 2018
  • Revised 2 October 2018

DOI:https://doi.org/10.1103/PhysRevA.98.052514

©2018 American Physical Society

Physics Subject Headings (PhySH)

Atomic, Molecular & Optical

Authors & Affiliations

Kouichi Hosaka1,*, Yutaro Torizuka1, Kai Minamizaki1, Philipp Schmidt2, Andre Knie2, Arno Ehresmann2, Takeshi Odagiri3, Masashi Kitajima1, and Noriyuki Kouchi1

  • 1Department of Chemistry, Tokyo Institute of Technology, Meguro-ku, Tokyo 152-8551, Japan
  • 2Institute of Physics and Center for Interdisciplinary Nanostructure Science and Technology (CINSaT), University of Kassel, Heinrich-Plett-Straße 40, D-34132 Kassel, Germany
  • 3Department of Materials and Life Sciences, Sophia University, Chiyoda-ku, Tokyo 102-8554, Japan

  • *hosakak@chem.titech.ac.jp

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Issue

Vol. 98, Iss. 5 — November 2018

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