Probing electronic and vibrational dynamics in molecules by time-resolved photoelectron, Auger-electron, and X-ray photon scattering spectroscopy.
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 photoelectron 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.
Chemistry Department, University of California, Irvine, California 92697-2025, USA. kcbennet@uci.edu smukamel@uci.edu mkowalew@uci.edu.
Kochise
K
Bennett
Markus
M
Kowalewski
Shaul
S
Mukamel
D000171:Acrolein / Q000737:chemistry*; D004583:Electrons; D007536:Isomerism; D056951:Photoelectron Spectroscopy / Q000379:methods*; D011789:Quantum Theory; D013997:Time Factors; D014965:X-Rays
D000171:Acrolein