Ehrenfest+R dynamics. II. A semiclassical QED framework for Raman scattering
Abstract
In Paper I [Chen et al., J. Chem. Phys. 150, 044102 (2019)], we introduced Ehrenfest+R dynamics for a two-level system and showed how spontaneous emission can be heuristically included such that, after averaging over an ensemble of Ehrenfest+R trajectories, one can recover both coherent and incoherent electromagnetic fields. In the present paper, we now show that Ehrenfest+R dynamics can also correctly describe Raman scattering, whose features are completely absent from standard Ehrenfest dynamics. Ehrenfest+R dynamics appear to be quantitatively accurate both for resonant and off-resonant Raman signals, as compared with Kramers–Heisenberg–Dirac theory.
Document Details
- Document Type
- Pub Defense Publication
- Publication Date
- Jan 24, 2019
- Source ID
- 10.1063/1.5057366
Entities
People
- Abraham Nitzan
- Hsing-Ta Chen
- Joseph E Subotnik
- Maxim Sukharev
- Tao E Li
Organizations
- Air Force Office of Scientific Research
- Arizona State University
- German Research Foundation
- National Science Foundation
- United States Department of Energy
- University of Pennsylvania