Abstract
The time- and frequency-resolved nonlinear light scattering (NLS) signals from a time-evolving charge distribution of valence electrons prepared by impulsive x-ray pulses are calculated using a superoperator Green's function formalism. The signal consists of a coherent -scaling difference-frequency-generation and an incoherent fluorescence -scaling component, where is the number of active molecules. The former is given by the classical Larmor formula based on the time-dependent charge density. The latter carries additional information about the electronic structure and may be recast in terms of transition amplitudes representing quantum matter pathways.
- Received 31 December 2012
DOI:https://doi.org/10.1103/PhysRevA.87.053826
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