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Probing molecular photoinduced dynamics by ultrafast soft x-rays

Conference paper
Authors T. J. A. Wolf
R. H. Myhre
J. P. Cryan
S. Coriani
Richard J. Squibb
A. Battistoni
N. Berrah
C. Bostedt
P. Bucksbaum
G. Coslovich
Raimund Feifel
K. J. Gaffney
J. Grilj
T. J. Martinez
S. Miyabe
S. P. Moeller
M. Mucke
A. Natan
R. Obaid
T. Osipov
O. Plekan
S. Wang
H. Koch
M. Guhr
Published in 2017 Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC). 25-29 June 2017, Munich, Germany
ISBN 978-1-5090-6736-7
Publisher IEEE
Publication year 2017
Published at Department of Physics (GU)
Language en
Links https://doi.org/10.1109/CLEOE-EQEC....
Subject categories Optics, Electrical Engineering, Electronic Engineering, Information Engineering

Abstract

Summary form only given. Molecules selectively transform light energy from the sun into other forms of energy like heat, electricity, or chemical energy with high quantum efficiency. The energy conversion process is the result of a correlated motion of electrons and nuclei after photoexcitation, often under breakdown of the Born-Oppenheimer approximation. The element and site selectivity of x-rays allows observing molecular processes from a different point of view compared to ultrafast optical probes [1,2]. I will concentrate on time resolved x-ray absorption spectroscopy. The method provides high selectivity on the transient electronic structure of a molecule. Recently, we establishes this method in the soft x-ray domain for probing ππ* to nπ* transitions, a general and important process for molecular energy conversion. Fig. 1 shows a sketch of thymine, used in the experiment, with one of the oxygen 1s core orbitals and the π,n and π* valence orbitals. While valence orbitals are generally delocalized over the whole molecular body, the lone pair n orbital is essentially an oxygen 2p orbital. An x-ray induced transition from the oxygen 1s to the n orbital will result in a strong absorption maximum in the pre-edge region. We use this feature to probe the molecular dynamics after photoexcitation.

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