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Author

Schultz, Thomas
CRASY(Correlated Rotational Alignment Spectroscopy)
Research Interests
  • Correlated spectroscopy

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Ultrafast X-ray Auger probing of photoexcited molecular dynamics

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Title
Ultrafast X-ray Auger probing of photoexcited molecular dynamics
Author
McFarland B.K.Farrell J.P.Miyabe S.Tarantelli F.Aguilar A.Berrah N.Bostedt C.Bozek J.D.Bucksbaum P.H.Castagna J.C.Coffee R.N.Cryan J.P.Fang L.Feifel R.Gaffney K.J.Glownia J.M.Martinez T.J.Mucke M.Murphy B.Natan A.Osipov T.Petrovic V.S.Schorb S.Schultz, ThomasSpector L.S.Swiggers M.Tenney I.Wang S.White J.L.White W.Guhr M.
Keywords
RESOLVED PHOTOELECTRON-SPECTROSCOPY; FREE-ELECTRON LASER; CONICAL INTERSECTIONS; EXCITED-STATES; RNA BASES; AQUEOUS-SOLUTION; THYMINE; DNA; OPERATION; URACIL
Issue Date
201406
Publisher
NATURE PUBLISHING GROUP
Citation
NATURE COMMUNICATIONS, v.5, no., pp. -
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 pp 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 nφ* state.
URI
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DOI
http://dx.doi.org/10.1038/ncomms5235
ISSN
2041-1723
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