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

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

Research output: Contribution to journalArticle

4 Citations (Scopus)

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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Raman scattering
Raman spectra
Spontaneous emission
Electromagnetic fields
spontaneous emission
electromagnetic fields
Trajectories
trajectories

ASJC Scopus subject areas

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

Cite this

Ehrenfest+R dynamics. II. A semiclassical QED framework for Raman scattering. / Chen, Hsing Ta; Li, Tao E.; Sukharev, Maxim; Nitzan, Abraham; Subotnik, Joseph E.

In: Journal of Chemical Physics, Vol. 150, No. 4, 044103, 28.01.2019.

Research output: Contribution to journalArticle

Chen, Hsing Ta ; Li, Tao E. ; Sukharev, Maxim ; Nitzan, Abraham ; Subotnik, Joseph E. / Ehrenfest+R dynamics. II. A semiclassical QED framework for Raman scattering. In: Journal of Chemical Physics. 2019 ; Vol. 150, No. 4.
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