Non-equilibrium x-ray spectroscopy using direct quantum dynamics
Advances in experimental methodology aligned with technological developments, such as 3rd generation light sources, X-ray Free Electron Lasers, and High Harmonic Generation, have led to a paradigm shift in the capability of X-ray spectroscopy to deliver high temporal and spectral resolution on an ex...
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Veröffentlicht in: | The Journal of chemical physics 2018-09, Vol.149 (12), p.124107-124107 |
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Format: | Artikel |
Sprache: | eng |
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Zusammenfassung: | Advances in experimental methodology aligned with technological developments, such as 3rd
generation light sources, X-ray Free Electron Lasers, and High Harmonic Generation, have
led to a paradigm shift in the capability of X-ray spectroscopy to deliver high temporal
and spectral resolution on an extremely broad range of samples in a wide array of
different environments. Importantly, the complex nature and high information content of
this class of techniques mean that detailed theoretical studies are often essential to
provide a firm link between the spectroscopic observables and the underlying molecular
structure and dynamics. In this paper, we present approaches for simulating dynamical
processes in X-ray spectroscopy based upon on-the-fly quantum dynamics
with a Gaussian basis set. We show that it is possible to provide a fully quantum
description of X-ray spectra without the need of precomputing highly multidimensional
potential energy surfaces. It is applied to study two different dynamical situations,
namely, the core-hole lifetime dynamics of the water monomer and the dissociation of
CF4+
recently studied using pump-probe X-ray spectroscopy. Our results compare favourably to
previous experiments, while reducing the computational effort, providing the scope to
apply them to larger systems. |
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ISSN: | 0021-9606 1089-7690 |
DOI: | 10.1063/1.5047487 |