Comparison of Different Classical, Semiclassical, and Quantum Treatments of Light–Matter Interactions: Understanding Energy Conservation
Abstract
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. As such, 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. Thus, this benchmark study suggests that the Ehrenfest+R approachmore »
- Publication Date:
- Research Org.:
- Univ. of Pennsylvania, Philadelphia, PA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1595479
- Alternate Identifier(s):
- OSTI ID: 1595481
- Grant/Contract Number:
- SC0019397
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Theory and Computation
- Additional Journal Information:
- Journal Volume: 15; Journal Issue: 3; Journal ID: ISSN 1549-9618
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Li, Tao E., Chen, Hsing-Ta, and Subotnik, Joseph E. Comparison of Different Classical, Semiclassical, and Quantum Treatments of Light–Matter Interactions: Understanding Energy Conservation. United States: N. p., 2019.
Web. doi:10.1021/acs.jctc.8b01232.
Li, Tao E., Chen, Hsing-Ta, & Subotnik, Joseph E. Comparison of Different Classical, Semiclassical, and Quantum Treatments of Light–Matter Interactions: Understanding Energy Conservation. United States. https://doi.org/10.1021/acs.jctc.8b01232
Li, Tao E., Chen, Hsing-Ta, and Subotnik, Joseph E. Tue .
"Comparison of Different Classical, Semiclassical, and Quantum Treatments of Light–Matter Interactions: Understanding Energy Conservation". United States. https://doi.org/10.1021/acs.jctc.8b01232. https://www.osti.gov/servlets/purl/1595479.
@article{osti_1595479,
title = {Comparison of Different Classical, Semiclassical, and Quantum Treatments of Light–Matter Interactions: Understanding Energy Conservation},
author = {Li, Tao E. and Chen, Hsing-Ta and Subotnik, Joseph E.},
abstractNote = {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. As such, 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. Thus, this benchmark study suggests that the Ehrenfest+R approach may be very advantageous for simulating light–matter interactions semiclassically.},
doi = {10.1021/acs.jctc.8b01232},
journal = {Journal of Chemical Theory and Computation},
number = 3,
volume = 15,
place = {United States},
year = {Tue Feb 12 00:00:00 EST 2019},
month = {Tue Feb 12 00:00:00 EST 2019}
}
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Works referencing / citing this record:
Understanding detailed balance for an electron-radiation system through mixed quantum-classical electrodynamics
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