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Ultrafast X-ray Auger probing of photoexcited molecular dynamics
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2014 (English)In: Nature Communications, ISSN 2041-1723, E-ISSN 2041-1723, Vol. 5, 4235- p.Article in journal (Refereed) Published
Abstract [en]

Molecules can efficiently and selectively convert light energy into other degrees of freedom. Disentangling the underlying ultrafast motion of electrons and nuclei of the photoexcited molecule presents a challenge to current spectroscopic approaches. Here we explore the photoexcited dynamics of molecules by an interaction with an ultrafast X-ray pulse creating a highly localized core hole that decays via Auger emission. We discover that the Auger spectrum as a function of photoexcitation-X-ray-probe delay contains valuable information about the nuclear and electronic degrees of freedom from an element-specific point of view. For the nucleobase thymine, the oxygen Auger spectrum shifts towards high kinetic energies, resulting from a particular C-O bond stretch in the pi pi* photoexcited state. A subsequent shift of the Auger spectrum towards lower kinetic energies displays the electronic relaxation of the initial photoexcited state within 200 fs. Ab-initio simulations reinforce our interpretation and indicate an electronic decay to the n pi* state.

Place, publisher, year, edition, pages
2014. Vol. 5, 4235- p.
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Physical Sciences
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URN: urn:nbn:se:uu:diva-229972DOI: 10.1038/ncomms5235ISI: 000338840000004OAI: oai:DiVA.org:uu-229972DiVA: diva2:738644
Available from: 2014-08-18 Created: 2014-08-18 Last updated: 2017-12-05Bibliographically approved

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Feifel, RaimundMucke, Melanie
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