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Title: Quantum dynamics of a molecular emitter strongly coupled with surface plasmon polaritons: A macroscopic quantum electrodynamics approach

Journal Article · · Journal of Chemical Physics
DOI: https://doi.org/10.1063/1.5100014 · OSTI ID:1612286

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.

Research Organization:
Princeton Univ., NJ (United States); Energy Frontier Research Centers (EFRC) (United States). Bioinspired Light-Escalated Chemistry (BioLEC)
Sponsoring Organization:
Academia Sinica; Taiwan Ministry of Science and Technology (MOST); USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0015429; MOST 106-2113-M-001-036- MY3
OSTI ID:
1612286
Alternate ID(s):
OSTI ID: 1530640
Journal Information:
Journal of Chemical Physics, Vol. 151, Issue 1; ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 31 works
Citation information provided by
Web of Science

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Cited By (3)


Figures / Tables (5)