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Ehrenfest+R dynamics. II. A semiclassical QED framework for Raman scattering
Hsing-Ta Chen1, Tao E Li1, Maxim Sukharev2
1Department of Chemistry, University of Pennsylvania, Philadelphia, Pennsylvania 19104, USA.
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.
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