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, Marc Messerschmidt, T. Osipov, N. Berrah

Research output: Contribution to journalArticle

13 Citations (Scopus)

Abstract

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
Volume86
Issue number5
DOIs
StatePublished - Nov 29 2012
Externally publishedYes

Fingerprint

free electron lasers
ionization
pulses
x rays
sulfur
ions
hydrogen sulfide
simulation
decay rates
photoionization
pulse duration
photoelectrons
photons
estimates
spectroscopy
molecules
electrons

ASJC Scopus subject areas

  • Atomic and Molecular Physics, and Optics

Cite this

Multiphoton L-shell ionization of H2S using intense x-ray pulses from a free-electron laser. / Murphy, B. F.; Fang, L.; Chen, M. H.; Bozek, J. D.; Kukk, E.; Kanter, E. P.; Messerschmidt, Marc; Osipov, T.; Berrah, N.

In: Physical Review A - Atomic, Molecular, and Optical Physics, Vol. 86, No. 5, 053423, 29.11.2012.

Research output: Contribution to journalArticle

Murphy, B. F. ; Fang, L. ; Chen, M. H. ; Bozek, J. D. ; Kukk, E. ; Kanter, E. P. ; Messerschmidt, Marc ; Osipov, T. ; Berrah, N. / Multiphoton L-shell ionization of H2S using intense x-ray pulses from a free-electron laser. In: Physical Review A - Atomic, Molecular, and Optical Physics. 2012 ; Vol. 86, No. 5.
@article{251e494391db4d24a8b25f4a5daff78c,
title = "Multiphoton L-shell ionization of H2S using intense x-ray pulses from a free-electron laser",
abstract = "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.",
author = "Murphy, {B. F.} and L. Fang and Chen, {M. H.} and Bozek, {J. D.} and E. Kukk and Kanter, {E. P.} and Marc Messerschmidt and T. Osipov and N. Berrah",
year = "2012",
month = "11",
day = "29",
doi = "10.1103/PhysRevA.86.053423",
language = "English (US)",
volume = "86",
journal = "Physical Review A - Atomic, Molecular, and Optical Physics",
issn = "1050-2947",
publisher = "American Physical Society",
number = "5",

}

TY - JOUR

T1 - Multiphoton L-shell ionization of H2S using intense x-ray pulses from a free-electron laser

AU - Murphy, B. F.

AU - Fang, L.

AU - Chen, M. H.

AU - Bozek, J. D.

AU - Kukk, E.

AU - Kanter, E. P.

AU - Messerschmidt, Marc

AU - Osipov, T.

AU - Berrah, N.

PY - 2012/11/29

Y1 - 2012/11/29

N2 - 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.

AB - 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.

UR - http://www.scopus.com/inward/record.url?scp=84870573152&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84870573152&partnerID=8YFLogxK

U2 - 10.1103/PhysRevA.86.053423

DO - 10.1103/PhysRevA.86.053423

M3 - Article

VL - 86

JO - Physical Review A - Atomic, Molecular, and Optical Physics

JF - Physical Review A - Atomic, Molecular, and Optical Physics

SN - 1050-2947

IS - 5

M1 - 053423

ER -