Comparison of Different Classical, Semiclassical, and Quantum Treatments of Light–Matter Interactions: Understanding Energy Conservation

Li, Tao E.; Chen, Hsing-Ta; Subotnik, Joseph E.

doi:10.1021/acs.jctc.8b01232

Comparison of Different Classical, Semiclassical, and Quantum Treatments of Light–Matter Interactions: Understanding Energy Conservation

Journal Article · Tue Feb 12 00:00:00 EST 2019 · Journal of Chemical Theory and Computation

DOI:https://doi.org/10.1021/acs.jctc.8b01232· OSTI ID:1595479

^[1]; Chen, Hsing-Ta ^[2]; Subotnik, Joseph E. ^[2]

Univ. of Pennsylvania, Philadelphia, PA (United States); University of pennsylvania
Univ. of Pennsylvania, Philadelphia, PA (United States)

The optical response of an electronic two-level system (TLS) coupled to an incident continuous wave (cw) electromagnetic (EM) field is simulated explicitly in one dimension by the following five approaches: (i) the coupled Maxwell-Bloch equations, (ii) the optical Bloch equation (OBE), (iii) Ehrenfest dynamics, (iv) the Ehrenfest+R approach, and (v) classical dielectric theory (CDT). Our findings are as follows: (i) standard Ehrenfest dynamics predict the correct optical signals only in the linear response regime where vacuum fluctuations are not important; (ii) both the coupled Maxwell-Bloch equations and CDT predict incorrect features for the optical signals in the linear response regime due to a double-counting of self-interaction; (iii) by exactly balancing the effects of self-interaction versus the effects of quantum fluctuations (and insisting on energy conservation), the Ehrenfest+R approach generates the correct optical signals in the linear regime and slightly beyond, yielding, e.g., the correct ratio between the coherent and incoherent scattering EM fields. Furthermore, Ehrenfest+R dynamics agree with dynamics from the quantum OBE, but whereas the latter is easily applicable only for a single TLS in vacuum, the former should be applicable to large systems in environments with arbitrary dielectrics. Hence, this benchmark study suggests that the Ehrenfest+R approach may be very advantageous for simulating light-matter interactions semiclassically.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Pennsylvania, Philadelphia, PA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0019397

OSTI ID:: 1595479

Alternate ID(s):: OSTI ID: 1595481

Journal Information:: Journal of Chemical Theory and Computation, Journal Name: Journal of Chemical Theory and Computation Journal Issue: 3 Vol. 15; ISSN 1549-9618

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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