Ultrafast X-ray Auger probing of photoexcited molecular dynamics.

Citation data:

Nature communications, ISSN: 2041-1723, Vol: 5, Issue: 1, Page: 4235

Publication Year:
2014
Usage 21
Abstract Views 19
Clicks 2
Captures 69
Readers 69
Mentions 3
News Mentions 3
Citations 85
Citation Indexes 85
Repository URL:
http://scholarworks.unist.ac.kr/handle/201301/5164
PMID:
24953740
DOI:
10.1038/ncomms5235
Author(s):
B. K. McFarland; J. P. Farrell; S. Miyabe; F. Tarantelli; A. Aguilar; N. Berrah; C. Bostedt; J. D. Bozek; P. H. Bucksbaum; J. C. Castagna; R. N. Coffee; J. P. Cryan; L. Fang; R. Feifel; K. J. Gaffney; J. M. Glownia; T. J. Martinez; M. Mucke; B. Murphy; A. Natan; T. Osipov; V. S. Petrović; S. Schorb; Th. Schultz; L. S. Spector; M. Swiggers; I. Tenney; S. Wang; J. L. White; W. White; M. Gühr Show More Hide
Publisher(s):
Springer Nature; NATURE PUBLISHING GROUP
Tags:
Chemistry; Biochemistry, Genetics and Molecular Biology; Physics and Astronomy; RESOLVED PHOTOELECTRON-SPECTROSCOPY; FREE-ELECTRON LASER; CONICAL INTERSECTIONS; EXCITED-STATES; RNA BASES; AQUEOUS-SOLUTION; THYMINE; DNA; OPERATION; URACIL
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article description
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.