Multiphoton L-shell ionization of H2S using intense x-ray pulses from a free-electron laser

B. F. Murphy, L. Fang, M. H. Chen, J. D. Bozek, E. Kukk, E. P. Kanter, M. Messerschmidt, T. Osipov, N. Berrah

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14 Scopus citations


Sequential multiphoton L-shell ionization of hydrogen sulfide exposed to intense femtosecond pulses of 1.25-keV x rays has been observed via photoelectron, Auger electron, and ion time-of-flight spectroscopies. Monte Carlo simulations based on relativistic Dirac-Hartree-Slater calculations of Auger decay rates in sulfur with single and double L-shell vacancies accurately model the observed spectra. While single-vacancy-only calculations are surprisingly accurate even at the high x-ray intensity used in the experiment, calculations including double-vacancy states improve on yield estimates of highly charged sulfur ions. In the most intense part of the x-ray focal volume, an average molecule absorbs more than five photons, producing multiple L-shell vacancies in 17% of photoionization events according to simulation. For 280-fs pulse duration and ∼1017 Wcm-2 focal intensity, the yield of S13+ is ∼1% of the S3+ yield, in good agreement with simulations. An overabundance of S12+, and S14+ observed in the experimental ion spectra is not predicted by either single-vacancy or double-vacancy calculations.

Original languageEnglish (US)
Article number053423
JournalPhysical Review A - Atomic, Molecular, and Optical Physics
Issue number5
StatePublished - Nov 29 2012
Externally publishedYes

ASJC Scopus subject areas

  • Atomic and Molecular Physics, and Optics


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