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

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

doi:10.1063/1.5057366

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 language	English (US)
Article number	044103
Journal	Journal of Chemical Physics
Volume	150
Issue number	4
DOIs	https://doi.org/10.1063/1.5057366
State	Published - Jan 28 2019

ASJC Scopus subject areas

General Physics and Astronomy
Physical and Theoretical Chemistry

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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.",

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AU - Subotnik, Joseph E.

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

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