Nonlinear light scattering in molecules triggered by an impulsive X-ray Raman process.
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 ~N2-scaling difference frequency generation and an incoherent fluorescence ~N-scaling component whereNis the number of active molecules. The former is given by the classical Larmor formula based on the time-dependent charge density. The latter requires additional information about the electronic structure and may be recast in terms of transition amplitudes representing quantum matter pathways.
University of California, Irvine, California 92697-2025.
Konstantin E
KE
Dorfman
University of California, Irvine, California 92697-2025.
Kochise
K
Bennett
University of California, Irvine, California 92697-2025.
Yu
Y
Zhang
University of California, Irvine, California 92697-2025.
Shaul
S
Mukamel