Our previous study [S. Wang et al., J. Chem. Phys. 153, 184102 (2020)] has shown that in a complex dielectric environment, molecular emission power spectra can be expressed as the product of the lineshape function and the electromagnetic environment factor (EEF). In this work, we focus on EEFs in a vacuum–NaCl–silver system and investigate molecular emission power spectra in the strong exciton–polariton coupling regime. A numerical method based on computational electrodynamics is presented to calculate the EEFs of single-molecule emitters in a dispersive and lossy dielectric environment with arbitrary shapes. The EEFs in the far-field region depend on the detector position, emission frequency, and molecular orientation. We quantitatively analyze the asymptotic behavior of the EFFs in the far-field region and qualitatively provide a physical picture. The concept of EEF should be transferable to other types of spectra in a complex dielectric environment. Finally, our study indicates that molecular emission power spectra cannot be simply interpreted by the lineshape function (quantum dynamics of a molecular emitter), and the effect of the EEFs (photon propagation in a dielectric environment) has to be carefully considered.
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21 August 2021
Research Article|
August 16 2021
Theory of molecular emission power spectra. II. Angle, frequency, and distance dependence of electromagnetic environment factor of a molecular emitter in plasmonic environments
Special Collection:
2021 JCP Emerging Investigators Special Collection
Ming-Wei Lee;
Ming-Wei Lee
Institute of Atomic and Molecular Sciences, Academia Sinica
, Taipei 10617, Taiwan
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Yi-Ting Chuang;
Yi-Ting Chuang
Institute of Atomic and Molecular Sciences, Academia Sinica
, Taipei 10617, Taiwan
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Liang-Yan Hsu
Liang-Yan Hsu
a)
Institute of Atomic and Molecular Sciences, Academia Sinica
, Taipei 10617, Taiwan
a)Author to whom correspondence should be addressed: [email protected]
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a)Author to whom correspondence should be addressed: [email protected]
Note: This paper is part of the 2021 JCP Emerging Investigators Special Collection.
J. Chem. Phys. 155, 074101 (2021)
Article history
Received:
May 17 2021
Accepted:
August 02 2021
Connected Content
This is a companion to:
Theory of molecular emission power spectra. I. Macroscopic quantum electrodynamics formalism
Citation
Ming-Wei Lee, Yi-Ting Chuang, Liang-Yan Hsu; Theory of molecular emission power spectra. II. Angle, frequency, and distance dependence of electromagnetic environment factor of a molecular emitter in plasmonic environments. J. Chem. Phys. 21 August 2021; 155 (7): 074101. https://doi.org/10.1063/5.0057018
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