Theory of molecular emission power spectra. I. Macroscopic quantum electrodynamics formalism
Abstract
In this work, we study the emission power spectrum of a molecular emitter with multiple vibrational modes in the framework of macroscopic quantum electrodynamics. The theory we present is general for a molecular spontaneous emission spectrum in the presence of arbitrary inhomogeneous, dispersive, and absorbing media. Moreover, the theory shows that the molecular emission power spectra can be decomposed into the electromagnetic environment factor and lineshape function. In order to demonstrate the validity of the theory, we investigate the lineshape function in two limits. In the incoherent limit (single molecules in a vacuum), the lineshape function exactly corresponds to the Franck–Condon principle. In the coherent limit (single molecules strongly coupled with single polaritons or photons) together with the condition of high vibrational frequency, the lineshape function exhibits a Rabi splitting, the spacing of which is exactly the same as the magnitude of exciton–photon coupling estimated by our previous theory [S. Wang et al., J. Chem. Phys. 151, 014105 (2019)]. Finally, we explore the influence of exciton–photon and electron–phonon interactions on the lineshape function of a single molecule in a cavity. The theory shows that the vibronic structure of the lineshape function does not always disappear as the exciton–photon coupling increases,more »
- Authors:
-
[1];
[4];
[5]
- Academia Sinica, Taipei (Taiwan). Inst. of Atomic and Molecular Sciences; Princeton Univ., NJ (United States). Dept. of Chemistry
- Academia Sinica, Taipei (Taiwan). Inst. of Atomic and Molecular Sciences; National Taiwan Normal Univ., Taipei (Taiwan). Dept. of Chemistry
- Academia Sinica, Taipei (Taiwan). Institute of Atomic and Molecular Sciences
- Princeton Univ., NJ (United States). Dept. of Chemistry
- Academia Sinica, Taipei (Taiwan). Inst. of Atomic and Molecular Sciences
- Publication Date:
- Research Org.:
- Princeton Univ., NJ (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; USDOE
- OSTI Identifier:
- 1851998
- Alternate Identifier(s):
- OSTI ID: 1708962
- Grant/Contract Number:
- SC0015429
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 153; Journal Issue: 18; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; Chemistry; physics; quantum electrodynamics; plasmonics; open quantum systems; Franck Condon principle; phonons; emission spectroscopy; excitons; Purcell effect; spectroscopy; Franck Condon factors
Citation Formats
Wang, Siwei, Lee, Ming-Wei, Chuang, Yi-Ting, Scholes, Gregory D., and Hsu, Liang-Yan. Theory of molecular emission power spectra. I. Macroscopic quantum electrodynamics formalism. United States: N. p., 2020.
Web. doi:10.1063/5.0027796.
Wang, Siwei, Lee, Ming-Wei, Chuang, Yi-Ting, Scholes, Gregory D., & Hsu, Liang-Yan. Theory of molecular emission power spectra. I. Macroscopic quantum electrodynamics formalism. United States. https://doi.org/10.1063/5.0027796
Wang, Siwei, Lee, Ming-Wei, Chuang, Yi-Ting, Scholes, Gregory D., and Hsu, Liang-Yan. Mon .
"Theory of molecular emission power spectra. I. Macroscopic quantum electrodynamics formalism". United States. https://doi.org/10.1063/5.0027796. https://www.osti.gov/servlets/purl/1851998.
@article{osti_1851998,
title = {Theory of molecular emission power spectra. I. Macroscopic quantum electrodynamics formalism},
author = {Wang, Siwei and Lee, Ming-Wei and Chuang, Yi-Ting and Scholes, Gregory D. and Hsu, Liang-Yan},
abstractNote = {In this work, we study the emission power spectrum of a molecular emitter with multiple vibrational modes in the framework of macroscopic quantum electrodynamics. The theory we present is general for a molecular spontaneous emission spectrum in the presence of arbitrary inhomogeneous, dispersive, and absorbing media. Moreover, the theory shows that the molecular emission power spectra can be decomposed into the electromagnetic environment factor and lineshape function. In order to demonstrate the validity of the theory, we investigate the lineshape function in two limits. In the incoherent limit (single molecules in a vacuum), the lineshape function exactly corresponds to the Franck–Condon principle. In the coherent limit (single molecules strongly coupled with single polaritons or photons) together with the condition of high vibrational frequency, the lineshape function exhibits a Rabi splitting, the spacing of which is exactly the same as the magnitude of exciton–photon coupling estimated by our previous theory [S. Wang et al., J. Chem. Phys. 151, 014105 (2019)]. Finally, we explore the influence of exciton–photon and electron–phonon interactions on the lineshape function of a single molecule in a cavity. The theory shows that the vibronic structure of the lineshape function does not always disappear as the exciton–photon coupling increases, and it is related to the loss of a dielectric environment.},
doi = {10.1063/5.0027796},
journal = {Journal of Chemical Physics},
number = 18,
volume = 153,
place = {United States},
year = {Mon Nov 09 00:00:00 EST 2020},
month = {Mon Nov 09 00:00:00 EST 2020}
}
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