Nonlinear light scattering in molecules triggered by an impulsive X-ray Raman process

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 $\sim N^2$-scaling difference frequency generation and an incoherent fluorescence $\sim N$-scaling component where $N$ is 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.

References in corpus (5)

• Bright Coherent Ultrahigh Harmonics in the keV X-Ray Regime from Mid-Infrared Femtosecond Lasers
• Imaging electronic quantum motion with light
• Superoperator nonequilibrium Green's function theory of many-body systems; Applications to charge transfer and transport in open junctions
• Two-Dimensional Stimulated Resonance Raman Spectroscopy of Molecules with Broadband X-ray Pulses
• Radiation Generated by Charge Migration Following Ionization

Cited by in corpus (4)

• Time-, Frequency-, and Wavevector-Resolved X-Ray Diffraction from Single Molecules
• Detecting Electronic Coherence by Multidimensional Broadband Stimulated X-Ray Raman Signals
• Cascading and Local-Field Effects in Non-Linear Optics Revisited; A Quantum-Field Picture Based on Exchange of Photons
• Collective resonances in ${\chi }^{(3)}$; a QED study