Quantum dynamics of a molecular emitter strongly coupled with surface plasmon polaritons: A macroscopic quantum electrodynamics approach
Abstract
In this work, we study a molecular emitter above a silver surface in the framework of macroscopic quantum electrodynamics and explore the population dynamics including non-Markovian effects. The theory we present is general for molecular fluorescence in the presence of dielectrics with any space-dependent, frequency-dependent, or complex dielectric functions. Furthermore, the proposed theory allows us to calculate the memory kernel of polaritons using computational electrodynamics packages. In the limit of a high vibration frequency, the different strengths of exciton-polariton couplings lead to distinct characteristics in the population dynamics, e.g., Franck-Condon-Rabi oscillation. (The frequency of Rabi oscillation is dependent on the Franck-Condon factor.) Additionally, in a specific condition, we derive a parameter-free formula that can be used to estimate the exciton-polariton coupling between a molecular emitter and a nanocavity, and the coupling estimated by our theory is in good agreement with the reported experimental results.
- Authors:
-
- Princeton Univ., NJ (United States); Academia Sinica, Taipei (Taiwan)
- Princeton Univ., NJ (United States)
- Academia Sinica, Taipei (Taiwan)
- Publication Date:
- Research Org.:
- Princeton Univ., NJ (United States); Energy Frontier Research Centers (EFRC) (United States). Bioinspired Light-Escalated Chemistry (BioLEC)
- Sponsoring Org.:
- Academia Sinica; Taiwan Ministry of Science and Technology (MOST); USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1612286
- Alternate Identifier(s):
- OSTI ID: 1530640
- Grant/Contract Number:
- SC0015429; MOST 106-2113-M-001-036- MY3
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 151; Journal Issue: 1; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; Chemistry; Physics; Nano optics; Green-functions technique; Purcell factor; Surface optics; Quantum electrodynamics; Molecular fluorescence; Open quantum systems; Exciton dynamics; Surface plasmon polaritons
Citation Formats
Wang, Siwei, Scholes, Gregory D., and Hsu, Liang-Yan. Quantum dynamics of a molecular emitter strongly coupled with surface plasmon polaritons: A macroscopic quantum electrodynamics approach. United States: N. p., 2019.
Web. doi:10.1063/1.5100014.
Wang, Siwei, Scholes, Gregory D., & Hsu, Liang-Yan. Quantum dynamics of a molecular emitter strongly coupled with surface plasmon polaritons: A macroscopic quantum electrodynamics approach. United States. https://doi.org/10.1063/1.5100014
Wang, Siwei, Scholes, Gregory D., and Hsu, Liang-Yan. Tue .
"Quantum dynamics of a molecular emitter strongly coupled with surface plasmon polaritons: A macroscopic quantum electrodynamics approach". United States. https://doi.org/10.1063/1.5100014. https://www.osti.gov/servlets/purl/1612286.
@article{osti_1612286,
title = {Quantum dynamics of a molecular emitter strongly coupled with surface plasmon polaritons: A macroscopic quantum electrodynamics approach},
author = {Wang, Siwei and Scholes, Gregory D. and Hsu, Liang-Yan},
abstractNote = {In this work, we study a molecular emitter above a silver surface in the framework of macroscopic quantum electrodynamics and explore the population dynamics including non-Markovian effects. The theory we present is general for molecular fluorescence in the presence of dielectrics with any space-dependent, frequency-dependent, or complex dielectric functions. Furthermore, the proposed theory allows us to calculate the memory kernel of polaritons using computational electrodynamics packages. In the limit of a high vibration frequency, the different strengths of exciton-polariton couplings lead to distinct characteristics in the population dynamics, e.g., Franck-Condon-Rabi oscillation. (The frequency of Rabi oscillation is dependent on the Franck-Condon factor.) Additionally, in a specific condition, we derive a parameter-free formula that can be used to estimate the exciton-polariton coupling between a molecular emitter and a nanocavity, and the coupling estimated by our theory is in good agreement with the reported experimental results.},
doi = {10.1063/1.5100014},
journal = {Journal of Chemical Physics},
number = 1,
volume = 151,
place = {United States},
year = {Tue Jul 02 00:00:00 EDT 2019},
month = {Tue Jul 02 00:00:00 EDT 2019}
}
Web of Science
Figures / Tables:
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