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Non-equilibrium x-ray spectroscopy using direct quantum dynamics
被引:17
|作者:
Northey, T.
[1
]
Duffield, J.
[1
]
Penfold, T. J.
[1
]
机构:
[1] Newcastle Univ, Chem Sch Nat & Environm Sci, Newcastle Upon Tyne NE1 7RU, Tyne & Wear, England
关键词:
FREE-ELECTRON LASER;
STATE MOLECULAR-DYNAMICS;
ABSORPTION SPECTROSCOPY;
GAUSSIAN WAVEPACKETS;
EXTREME-ULTRAVIOLET;
WATER WINDOW;
SCATTERING;
SIMULATIONS;
OPERATION;
SPECTRUM;
D O I:
10.1063/1.5047487
中图分类号:
O64 [物理化学(理论化学)、化学物理学];
学科分类号:
070304 ;
081704 ;
摘要:
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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