TY - JOUR
T1 - Mixed quantum-classical electrodynamics
T2 - Understanding spontaneous decay and zero-point energy
AU - Li, Tao E.
AU - Nitzan, Abraham
AU - Sukharev, Maxim
AU - Martinez, Todd
AU - Chen, Hsing Ta
AU - Subotnik, Joseph E.
N1 - Publisher Copyright:
©2018 American Physical Society.
PY - 2018/3/12
Y1 - 2018/3/12
N2 - 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. 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)JCPSA60021-960610.1063/1.436793] that Ehrenfest dynamics can effectively describe some aspects of spontaneous emission and highlights interesting possibilities for studying light-matter interactions with semiclassical mechanics.
AB - 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. 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)JCPSA60021-960610.1063/1.436793] that Ehrenfest dynamics can effectively describe some aspects of spontaneous emission and highlights interesting possibilities for studying light-matter interactions with semiclassical mechanics.
UR - http://www.scopus.com/inward/record.url?scp=85044115422&partnerID=8YFLogxK
U2 - 10.1103/PhysRevA.97.032105
DO - 10.1103/PhysRevA.97.032105
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AN - SCOPUS:85044115422
SN - 2469-9926
VL - 97
JO - Physical Review A
JF - Physical Review A
IS - 3
M1 - 032105
ER -