Abstract：
: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 ππ* 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 nπ* state.
journal_name
Nat Communjournal_title
Nature communicationsauthors
McFarland BK,Farrell JP,Miyabe S,Tarantelli F,Aguilar A,Berrah N,Bostedt C,Bozek JD,Bucksbaum PH,Castagna JC,Coffee RN,Cryan JP,Fang L,Feifel R,Gaffney KJ,Glownia JM,Martinez TJ,Mucke M,Murphy B,Natan A,Osipov T,doi
10.1038/ncomms5235subject
Has Abstractpub_date
2014-06-23 00:00:00pages
4235issn
2041-1723pii
ncomms5235journal_volume
5pub_type
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