Mixed quantum-classical electrodynamics: Understanding spontaneous decay and zero-point energy

Li, Tao E.; Nitzan, Abraham; Sukharev, Maxim; Martinez, Todd; Chen, Hsing-Ta; Subotnik, Joseph E.

doi:10.1103/physreva.97.032105

Mixed quantum-classical electrodynamics: Understanding spontaneous decay and zero-point energy

Journal Article · Mon Mar 12 00:00:00 EDT 2018 · Physical Review A

DOI:https://doi.org/10.1103/physreva.97.032105· OSTI ID:1436986

Li, Tao E. ^[1]; Nitzan, Abraham ^[1]; Sukharev, Maxim ^[2]; Martinez, Todd ^[3]; Chen, Hsing-Ta ^[1]; Subotnik, Joseph E. ^[1]

Univ. of Pennsylvania, Philadelphia, PA (United States). Dept. of Chemistry
Arizona State Univ., Tempe, AZ (United States). Dept. of Physics; Arizona State Univ., Mesa, AZ (United States). College of Integrative Sciences and Arts
SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE), and Dept. of Chemistry

The dynamics of an electronic two-level system coupled to an electromagnetic field are simulated explicitly for one- and three-dimensional systems through semiclassical propagation of the Maxwell-Liouville equations. Here, we consider three flavors of mixed quantum-classical dynamics: (i) the classical path approximation (CPA), (ii) Ehrenfest dynamics, and (iii) symmetrical quasiclassical (SQC) dynamics. Our findings are as follows: (i) The CPA fails to recover a consistent description of spontaneous emission, (ii) a consistent “spontaneous” emission can be obtained from Ehrenfest dynamics, provided that one starts in an electronic superposition state, and (iii) spontaneous emission is always obtained using SQC dynamics. Using the SQC and Ehrenfest frameworks, we further calculate the dynamics following an incoming pulse, but here we find very different responses: SQC and Ehrenfest dynamics deviate sometimes strongly in the calculated rate of decay of the transient excited state. Nevertheless, our work confirms the earlier observations by Miller [J. Chem. Phys. 69, 2188 (1978)] that Ehrenfest dynamics can effectively describe some aspects of spontaneous emission and highlights interesting possibilities for studying light-matter interactions with semiclassical mechanics.

View Accepted Manuscript (DOE)

Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: National Science Foundation (NSF); US Air Force Office of Scientific Research (AFOSR); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1436986

Alternate ID(s):: OSTI ID: 1425531

Journal Information:: Physical Review A, Journal Name: Physical Review A Journal Issue: 3 Vol. 97; ISSN PLRAAN; ISSN 2469-9926

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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