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

Abstract

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.

Authors:
 [1];  [1];  [2];  [3];  [1];  [1]
  1. Univ. of Pennsylvania, Philadelphia, PA (United States). Dept. of Chemistry
  2. Arizona State Univ., Tempe, AZ (United States). Dept. of Physics; Arizona State Univ., Mesa, AZ (United States). College of Integrative Sciences and Arts
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE), and Dept. of Chemistry
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF); US Air Force Office of Scientific Research (AFOSR)
OSTI Identifier:
1436986
Alternate Identifier(s):
OSTI ID: 1425531
Grant/Contract Number:  
AC02-76SF00515; FA9950-13-1-0157; FA9550-15-1-0189; 2014113; CHE1665291
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review A
Additional Journal Information:
Journal Volume: 97; Journal Issue: 3; Journal ID: ISSN 2469-9926
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS

Citation Formats

Li, Tao E., Nitzan, Abraham, Sukharev, Maxim, Martinez, Todd, Chen, Hsing-Ta, and Subotnik, Joseph E. Mixed quantum-classical electrodynamics: Understanding spontaneous decay and zero-point energy. United States: N. p., 2018. Web. doi:10.1103/physreva.97.032105.
Li, Tao E., Nitzan, Abraham, Sukharev, Maxim, Martinez, Todd, Chen, Hsing-Ta, & Subotnik, Joseph E. Mixed quantum-classical electrodynamics: Understanding spontaneous decay and zero-point energy. United States. doi:10.1103/physreva.97.032105.
Li, Tao E., Nitzan, Abraham, Sukharev, Maxim, Martinez, Todd, Chen, Hsing-Ta, and Subotnik, Joseph E. Mon . "Mixed quantum-classical electrodynamics: Understanding spontaneous decay and zero-point energy". United States. doi:10.1103/physreva.97.032105. https://www.osti.gov/servlets/purl/1436986.
@article{osti_1436986,
title = {Mixed quantum-classical electrodynamics: Understanding spontaneous decay and zero-point energy},
author = {Li, Tao E. and Nitzan, Abraham and Sukharev, Maxim and Martinez, Todd and Chen, Hsing-Ta and Subotnik, Joseph E.},
abstractNote = {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.},
doi = {10.1103/physreva.97.032105},
journal = {Physical Review A},
number = 3,
volume = 97,
place = {United States},
year = {2018},
month = {3}
}

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