2013/03/31 by Konstantin E. Dorfman, Kochise Bennett, Yu Zhang +1 · 10 citations
Biochemistry, Genetics and Molecular Biology · Physics and Astronomy · #Computer science #Laser-Matter Interactions and Applications #Materials science #Molecular physics #Molecule #Nonlinear system #Optics #Physics #Process (computing) #Protein Interaction Studies and Fluorescence Analysis #Quantum mechanics #Raman scattering #Raman spectroscopy #Scattering #Spectroscopy and Quantum Chemical Studies #physics.chem-ph #physics.optics #quant-ph
paper · pdf · doi:10.1103/physreva.87.053826
published in Physical Review A 87(5), 53826 (American Physical Society)
arxiv created 2013/04/19 · openalex publication_date 2013/05/22 · arxiv updated 2013/05/27 · openalex created_date 2025/10/10 · openalex updated_date 2026/08/05
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 \ensuremath∼N2-scaling difference-frequency-generation and an incoherent fluorescence \ensuremath∼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 carries additional information about the electronic structure and may be recast in terms of transition amplitudes representing quantum matter pathways.