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) formation: Comparison with

DOI:10.1103/PhysRevA.98.052514 期刊:Physical Review A 出版年份:2018 更新时间:2025-09-09 09:28:46
摘要: Superexcited states of H2S have been investigated with determining the cross sections for emission of dispersed and nondispersed atomic ?uorescence 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 2b?1 2 (mo) states with a single con?guration and the other eight states in the range 16–25 eV are doubly excited states with multiple con?gurations. 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 ~10?3, whereas those in the photoexcitation of H2O range from ~10?3 to ~10?2. 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 “4a?1 1 (mo(cid:4))” 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 ?uorescence cross sections against the incident photon energy for H2S and H2O.
作者: Kouichi Hosaka,Yutaro Torizuka,Kai Minamizaki,Philipp Schmidt,Andre Knie,Arno Ehresmann,Takeshi Odagiri,Masashi Kitajima,Noriyuki Kouchi
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Investigating the electron correlation in the double photoexcitation of H2S and comparing it with H2O to understand the differences in their electronic structures and the formation of H(2p) atoms.

The study found that the electron correlation in H2S is stronger than in H2O, leading to smaller values of the dipole oscillator strengths for H(2p) formation in H2S. The energy splitting of the doubly excited states in H2S is enhanced compared to H2O, and the border between the inner valence and outer valence ranges becomes more obscure in H2S. The similarity in shape between the inner valence band and inner shell band in the fluorescence cross sections for H2S and H2O indicates that electrons are excited to similar orbitals from the valence or inner shell orbitals.

The study is limited by the energy resolution of the incident photon energy and the complexity of separating the Lyman-α fluorescence from other fluorescences in the nondispersed experiments of H2S. The change of the major fragment atoms from H(2p) to S? in H2S also poses challenges in data interpretation.

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