skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

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

References (66)

A single-photon transistor using nanoscale surface plasmons journal August 2007
Plasmon-coupled resonance energy transfer: A real-time electrodynamics approach journal February 2017
Spontaneous decay in the presence of dispersing and absorbing bodies: General theory and application to a spherical cavity journal October 2000
Note on the Numerical Solution of Integro-Differential Equations journal February 1967
Extending the applicability of Redfield theories into highly non-Markovian regimes journal November 2015
Raman spectra of pyridine adsorbed at a silver electrode journal May 1974
Effects of Donor–Acceptor Quantum Coherence and Non-Markovian Bath on the Distance Dependence of Resonance Energy Transfer journal February 2019
Optical transitions between vibronic states journal October 1986
Plasmon-Coupled Resonance Energy Transfer II: Exploring the Peaks and Dips in the Electromagnetic Coupling Factor journal September 2018
Ultrafast fluorescent decay induced by metal-mediated dipole–dipole interaction in two-dimensional molecular aggregates journal September 2017
Characteristic Distance of Resonance Energy Transfer Coupled with Surface Plasmon Polaritons journal November 2018
Displaced Fock states and their connection to quasiprobabilities journal December 1991
Strong coupling in molecular exciton-plasmon Au nanorod array systems journal February 2016
Theory of multichromophoric coherent resonance energy transfer: A polaronic quantum master equation approach journal July 2011
Theory of vibronic intensity borrowing. Comparison of Herzberg‐Teller and Born‐Oppenheimer coupling journal May 1973
Self-Coupling of a Two-Level System by a Mirror journal November 1969
Green-function approach to the radiation-field quantization for homogeneous and inhomogeneous Kramers-Kronig dielectrics journal March 1996
Solutions of integral and integro-differential equation systems by using differential transform method journal November 2008
Resonant excitation transfer: A quantum electrodynamical study journal April 1987
Lifetime of an emitting molecule near a partially reflecting surface journal April 1974
Single-molecule strong coupling at room temperature in plasmonic nanocavities journal June 2016
Effect of surface plasmons on transitions in molecules journal March 1975
Near-Zone Mediation of RET by One and Two Proximal Particles journal March 2019
Reversible dynamics of single quantum emitters near metal-dielectric interfaces journal January 2014
Control of the absorption of a four-level quantum system near a plasmonic nanostructure journal May 2017
A new hybrid exchange–correlation functional using the Coulomb-attenuating method (CAM-B3LYP) journal July 2004
Spontaneous emission interference in negative-refractive-index waveguides journal July 2009
Classical Aspects of Energy Transfer in Molecular Systems journal July 1970
Purcell Factor: A Tunable Metric for Plasmon-Coupled Fluorescence Emission Enhancements in Cermet Nanocavities journal December 2015
Principles of Nano-Optics book January 2006
Plasmon-Coupled Resonance Energy Transfer journal May 2017
Schwingungsstruktur der Elektronenübergänge bei mehratomigen Molekülen journal January 1933
Generalized effective mode volume for leaky optical cavities journal January 2012
Plasmonics for improved photovoltaic devices journal February 2010
Increased light harvesting in dye-sensitized solar cells with energy relay dyes journal June 2009
A unified theory of radiative and radiationless molecular energy transfer journal August 1989
Non-Markovian dynamics in plasmon-induced spontaneous emission interference journal February 2017
Spectral properties of a strongly coupled quantum-dot–metal-nanoparticle system journal May 2014
Lasing action in strongly coupled plasmonic nanocavity arrays journal June 2013
The enhancement of Raman scattering, resonance Raman scattering, and fluorescence from molecules adsorbed on a rough silver surface journal May 1983
Influence of a dielectric interface on fluorescence decay time journal January 1970
Increased light harvesting in dye-sensitized solar cells with energy relay dyes journal November 2009
Coherent Coupling of Molecular Excitons to Electronic Polarizations of Noble Metal Nanoparticles journal November 2004
Correlation-Dependent Coherent to Incoherent Transitions in Resonant Energy Transfer Dynamics journal October 2009
The rotating-wave approximation: consistency and applicability from an open quantum system analysis journal September 2010
Plasmonic Purcell factor and coupling efficiency to surface plasmons. Implications for addressing and controlling optical nanosources journal August 2016
Intermolecular energy transfer in the presence of dispersing and absorbing media journal April 2002
Theory of coherent resonance energy transfer for coherent initial condition journal October 2009
Quantum interference between decay channels of a three-level atom in a multilayer dielectric medium journal June 2001
Electromagnetic theory of enhanced Raman scattering by molecules adsorbed on rough surfaces journal October 1980
Transformation Optics Approach to Plasmon-Exciton Strong Coupling in Nanocavities journal August 2016
A practical method for the use of curvilinear coordinates in calculations of normal-mode-projected displacements and Duschinsky rotation matrices for large molecules journal November 2001
Variation of the Fluorescence Decay Time of a Molecule in Front of a Mirror journal March 1968
Lessons from nature about solar light harvesting journal September 2011
Nanoscale imaging and spontaneous emission control with a single nano-positioned quantum dot journal February 2013
Study of the Franck-Condon and Herzberg-Teller Approximations journal October 1974
Review Label-free detection with high-Q microcavities: a review of biosensing mechanisms for integrated devices journal January 2012
A single-photon transistor using nano-scale surface plasmons text January 2007
Correlation-dependent coherent to incoherent transitions in resonant energy transfer dynamics text January 2009
The Rotating-Wave Approximation: Consistency and Applicability from an Open Quantum System Analysis text January 2010
Extending the applicability of Redfield theories into highly non-Markovian regimes text January 2015
JUNO and Neutrinoless Double Beta Decay text January 2015
Plasmonic Purcell factor and coupling efficiency to surface plasmons. Implications for addressing and controlling optical nanosources text January 2016
Transformation Optics Approach to Plasmon-Exciton Strong Coupling in Nanocavities text January 2016
Non-Markovian dynamics in plasmon-induced spontaneous emission interference text January 2017
Spontaneous decay in the presence of dispersing and absorbing bodies: general theory and application to a spherical cavity text January 2000

Cited By (3)


Figures / Tables (5)