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Double-core-hole spectroscopy for chemical analysis with an intense X-ray femtosecond laser
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2011 (English)In: Proceedings of the National Academy of Sciences of the United States of America, ISSN 0027-8424, E-ISSN 1091-6490, Vol. 108, no 41, 16912-16915 p.Article in journal (Refereed) Published
Abstract [en]

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.

Place, publisher, year, edition, pages
2011. Vol. 108, no 41, 16912-16915 p.
Keyword [en]
multi-photon ionization, ultrafast, two-photon spectroscopy
National Category
Natural Sciences
Identifiers
URN: urn:nbn:se:su:diva-69918DOI: 10.1073/pnas.1111380108ISI: 000295973800015OAI: oai:DiVA.org:su-69918DiVA: diva2:479106
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authorCount :20Available from: 2012-01-17 Created: 2012-01-15 Last updated: 2017-12-08Bibliographically approved

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van der Meulen, PeterSalén, PeterSchmidt, Henning T.Thomas, Richard D.Larsson, Mats
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