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Chemical Physics Letters

Theory of time-resolved resonance scattering

Jacqueline O. Berg, Charles A. Langhoff, G. Wilse Robinson

Published Dec 1, 1974• 78 citations
Publisher
DOI
10.1016/0009-2614(74)85112-2

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Time resolved resonance and near-resonance light scattering is analyzed by means of Green’s operator formalism. We study the process of a photon wavepacket colliding with and scattered from a given molecule. Two decay components similar to those observed by Williams, Rousseau, and Dworetsky are obtained under appropriate conditions. Unlike other recent treatments of this problem, the light pulse is not treated as a pure quantum state (minimum uncertainty wavepacket) but rather as a mixture having characteristic time and energy profiles. It is shown that the nature of the light pulse may strongly influence the ratio of the short time to the long time decay intensities.
We develop a framework to evaluate the time-dependent resonant inelastic x-ray scattering (RIXS) signal with the use of nonequilibrium dynamical mean-field theory simulations. The approach is based on the solution of a time-dependent impurity model which explicitly incorporates the probe pulse. It avoids the need to compute four-point correlation functions and can in principle be combined with different impurity solvers. This opens a path to study time-resolved RIXS processes in multiorbital systems. The approach is exemplified with a study of the RIXS signal of a melting Mott antiferromagnet.