Ehrenfest+R dynamics. II. A semiclassical QED framework for Raman scattering

Hsing Ta Chen, Tao E. Li, Maxim Sukharev, Abraham Nitzan, Joseph E. Subotnik

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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.

Original languageEnglish (US)
Article number044103
JournalJournal of Chemical Physics
Volume150
Issue number4
DOIs
StatePublished - Jan 28 2019

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ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

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