Ultrafast X-ray Auger probing of photoexcited molecular dynamics

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 and M. Gühr ()
Additional contact information
B. K. McFarland: PULSE Institute, SLAC National Accelerator Laboratory
J. P. Farrell: PULSE Institute, SLAC National Accelerator Laboratory
S. Miyabe: PULSE Institute, SLAC National Accelerator Laboratory
F. Tarantelli: Biologia e Biotecnologie, Universita di Perugia, and ISTM-CNR
A. Aguilar: Advanced Light Source, Lawrence Berkeley National Lab
N. Berrah: Western Michigan University
C. Bostedt: LCLS, SLAC National Accelerator Laboratory
J. D. Bozek: LCLS, SLAC National Accelerator Laboratory
P. H. Bucksbaum: PULSE Institute, SLAC National Accelerator Laboratory
J. C. Castagna: LCLS, SLAC National Accelerator Laboratory
R. N. Coffee: LCLS, SLAC National Accelerator Laboratory
J. P. Cryan: PULSE Institute, SLAC National Accelerator Laboratory
L. Fang: Western Michigan University
R. Feifel: Uppsala University
K. J. Gaffney: PULSE Institute, SLAC National Accelerator Laboratory
J. M. Glownia: PULSE Institute, SLAC National Accelerator Laboratory
T. J. Martinez: PULSE Institute, SLAC National Accelerator Laboratory
M. Mucke: Uppsala University
B. Murphy: Western Michigan University
A. Natan: PULSE Institute, SLAC National Accelerator Laboratory
T. Osipov: Western Michigan University
V. S. Petrović: PULSE Institute, SLAC National Accelerator Laboratory
S. Schorb: LCLS, SLAC National Accelerator Laboratory
Th. Schultz: Max-Born-Institut, Max-Born-Strasse 2a
L. S. Spector: PULSE Institute, SLAC National Accelerator Laboratory
M. Swiggers: LCLS, SLAC National Accelerator Laboratory
I. Tenney: PULSE Institute, SLAC National Accelerator Laboratory
S. Wang: PULSE Institute, SLAC National Accelerator Laboratory
J. L. White: PULSE Institute, SLAC National Accelerator Laboratory
W. White: LCLS, SLAC National Accelerator Laboratory
M. Gühr: PULSE Institute, SLAC National Accelerator Laboratory

Nature Communications, 2014, vol. 5, issue 1, 1-7

Abstract: 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.

Date: 2014
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DOI: 10.1038/ncomms5235

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