Nuclear Dynamical Correlation Effects in X-ray Spectroscopy from a Theoretical Time-Domain Perspective.
To date X-ray spectroscopy has become a routine tool that can reveal highly local and element-specific information on the electronic structure of atoms in complex environments. Here, we focus on nuclear dynamical correlation effects in X-ray spectra and develop a rigorous time-correlation function method employing ground state classical molecular dynamics simulations. The importance of nuclear correlation phenomena is demonstrated by comparison against the results from the conventional sampling approach performed on the same data set for gas phase water. In contrast to the first-order absorption, second-order resonant inelastic scattering spectra exhibit pronounced fingerprints of nuclear motions. The developed methodology is not biased to a particular electronic structure method and, owing to its generality, can be applied to, e.g., X-ray photoelectron and Auger spectroscopies.
Institute of Physics, University of Rostock , Albert-Einstein-Str. 23-24, 18059 Rostock, Germany.
Sven
S
Karsten
Institute of Physics, University of Rostock , Albert-Einstein-Str. 23-24, 18059 Rostock, Germany.
Sergei D
http://orcid.org/0000-0002-6631-4868
SD
Ivanov
Chemistry Department, Faculty of Science, King Abdulaziz University , 21589 Jeddah, Saudi Arabia.
Saadullah G
SG
Aziz
Institute of Physics, University of Rostock , Albert-Einstein-Str. 23-24, 18059 Rostock, Germany.
Sergey I
SI
Bokarev
Institute of Physics, University of Rostock , Albert-Einstein-Str. 23-24, 18059 Rostock, Germany.
Oliver
O
Kühn