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.
- Authors:
-
- Univ. of Pennsylvania, Philadelphia, PA (United States)
- Arizona State Univ., Mesa, AZ (United States); Arizona State Univ., Tempe, AZ (United States)
- Publication Date:
- Research Org.:
- Univ. of Pennsylvania, Philadelphia, PA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1613217
- Grant/Contract Number:
- SC0019397
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 150; Journal Issue: 4; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS; Chemistry; Physics; Light scattering; Raman spectroscopy; Raman scattering; Scattering theory; Ehrenfest dynamics; Polarizability; Mixed quantum/classical theory; Quantum electrodynamics
Citation Formats
Chen, Hsing-Ta, Li, Tao E., Sukharev, Maxim, Nitzan, Abraham, and Subotnik, Joseph E. Ehrenfest+R dynamics. II. A semiclassical QED framework for Raman scattering. United States: N. p., 2019.
Web. doi:10.1063/1.5057366.
Chen, Hsing-Ta, Li, Tao E., Sukharev, Maxim, Nitzan, Abraham, & Subotnik, Joseph E. Ehrenfest+R dynamics. II. A semiclassical QED framework for Raman scattering. United States. https://doi.org/10.1063/1.5057366
Chen, Hsing-Ta, Li, Tao E., Sukharev, Maxim, Nitzan, Abraham, and Subotnik, Joseph E. Thu .
"Ehrenfest+R dynamics. II. A semiclassical QED framework for Raman scattering". United States. https://doi.org/10.1063/1.5057366. https://www.osti.gov/servlets/purl/1613217.
@article{osti_1613217,
title = {Ehrenfest+R dynamics. II. A semiclassical QED framework for Raman scattering},
author = {Chen, Hsing-Ta and Li, Tao E. and Sukharev, Maxim and Nitzan, Abraham and Subotnik, Joseph E.},
abstractNote = {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.},
doi = {10.1063/1.5057366},
journal = {Journal of Chemical Physics},
number = 4,
volume = 150,
place = {United States},
year = {Thu Jan 24 00:00:00 EST 2019},
month = {Thu Jan 24 00:00:00 EST 2019}
}
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