Double-core-hole spectroscopy for chemical analysis with an intense X-ray femtosecond laser

Nora Berrah, Li Fang, Brendan Murphy, Timur Osipov, Kiyoshi Ueda, Edwin Kukk, Raimund Feifel, Peter Van Der Meulen, Peter Salen, Henning T. Schmidt, Richard D. Thomas, Mats Larsson, Robert Richter, Kevin C. Prince, John D. Bozek, Christoph Bostedt, Shin Ichi Wada, Maria N. Piancastelli, Motomichi Tashiro, Masahiro Ehara

Research output: Contribution to journalArticlepeer-review

143 Citations (Scopus)

Abstract

Theory predicts that double-core-hole (DCH) spectroscopy can provide a new powerful means of differentiating between similar chemical systems with a sensitivity not hitherto possible. Although DCH ionization on a single site in molecules was recently measured with double- and single-photon absorption, double-core holes with single vacancies on two different sites, allowing unambiguous chemical analysis, have remained elusive. Here we report that direct observation of double-core holes with single vacancies on two different sites produced via sequential two-photon absorption, using short, intense X-ray pulses from the Linac Coherent Light Source free-electron laser and compare it with theoretical modeling. The observation of DCH states, which exhibit a unique signature, and agreement with theory proves the feasibility of the method. Our findings exploit the ultrashort pulse duration of the free-electron laser to eject two core electrons on a time scale comparable to that of Auger decay and demonstrate possible future X-ray control of physical inner-shell processes.

Original languageEnglish
Pages (from-to)16912-16915
Number of pages4
JournalProceedings of the National Academy of Sciences of the United States of America
Volume108
Issue number41
DOIs
Publication statusPublished - 2011 Oct 11

Keywords

  • Multi-photon ionization
  • Two-photon spectroscopy
  • Ultrafast

ASJC Scopus subject areas

  • General

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