Theory of molecular emission power spectra. I. Macroscopic quantum electrodynamics formalism

Wang, Siwei; Lee, Ming-Wei; Chuang, Yi-Ting; Scholes, Gregory D.; Hsu, Liang-Yan

doi:10.1063/5.0027796

Title: Theory of molecular emission power spectra. I. Macroscopic quantum electrodynamics formalism

Journal Article · Mon Nov 09 00:00:00 EST 2020 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/5.0027796· OSTI ID:1851998

^[1]; Lee, Ming-Wei ^[2]; Chuang, Yi-Ting ^[3];

^[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

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.

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Research Organization:: Princeton Univ., NJ (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; USDOE

Grant/Contract Number:: SC0015429

OSTI ID:: 1851998

Alternate ID(s):: OSTI ID: 1708962

Journal Information:: Journal of Chemical Physics, Vol. 153, Issue 18; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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