Probing Electronic and Vibrational Dynamics in Molecules by Time-Resolved Photoelectron Auger-Electron and X-ray Photon Scattering Spectroscopy

摘要

We present a unified description for time-resolved electron and photon scattering spectroscopies from molecules prepared in nonstationary states. Signals are expressed in terms of superoperator Green’s functions and a systematic procedure for treating various degrees of freedom consistently at different levels of theory is developed. The standard Fermi Golden Rule expressions for photelectron spectra, which are limited to broad, slowly-varying signals, are obtained as a limiting case of our more general theory that applies to broader parameter regimes.