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

Wang, Siwei; Scholes, Gregory D.; Hsu, Liang-Yan

doi:10.1063/1.5100014

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

Journal Article · 02 July 2019 · Journal of Chemical Physics

DOI: https://doi.org/10.1063/1.5100014 · OSTI ID:1612286

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Princeton Univ., NJ (United States); Academia Sinica, Taipei (Taiwan)
Princeton Univ., NJ (United States)
Academia Sinica, Taipei (Taiwan)

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.

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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

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Cited by: 31 works

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References (67)

A single-photon transistor using nanoscale surface plasmons Chang, Darrick E.; Sørensen, Anders S.; Demler, Eugene A. Nature Physics, Vol. 3, Issue 11 https://doi.org/10.1038/nphys708	journal	August 2007
Plasmon-coupled resonance energy transfer: A real-time electrodynamics approach Ding, Wendu; Hsu, Liang-Yan; Schatz, George C. The Journal of Chemical Physics, Vol. 146, Issue 6 https://doi.org/10.1063/1.4975815	journal	February 2017
Spontaneous decay in the presence of dispersing and absorbing bodies: General theory and application to a spherical cavity Dung, Ho Trung; Knöll, Ludwig; Welsch, Dirk-Gunnar Physical Review A, Vol. 62, Issue 5 https://doi.org/10.1103/physreva.62.053804	journal	October 2000
Note on the Numerical Solution of Integro-Differential Equations Day, J. T. The Computer Journal, Vol. 9, Issue 4 https://doi.org/10.1093/comjnl/9.4.394	journal	February 1967
Extending the applicability of Redfield theories into highly non-Markovian regimes Montoya-Castillo, Andrés; Berkelbach, Timothy C.; Reichman, David R. The Journal of Chemical Physics, Vol. 143, Issue 19 https://doi.org/10.1063/1.4935443	journal	November 2015
Raman spectra of pyridine adsorbed at a silver electrode Fleischmann, M.; Hendra, P. J.; McQuillan, A. J. Chemical Physics Letters, Vol. 26, Issue 2, p. 163-166 https://doi.org/10.1016/0009-2614(74)85388-1	journal	May 1974
Effects of Donor–Acceptor Quantum Coherence and Non-Markovian Bath on the Distance Dependence of Resonance Energy Transfer Jang, Seogjoo J. The Journal of Physical Chemistry C, Vol. 123, Issue 9 https://doi.org/10.1021/acs.jpcc.8b12481	journal	February 2019
Optical transitions between vibronic states Schwendimann, P.; Sigmund, E. Journal of Physics C: Solid State Physics, Vol. 19, Issue 30 https://doi.org/10.1088/0022-3719/19/30/009	journal	October 1986
Plasmon-Coupled Resonance Energy Transfer II: Exploring the Peaks and Dips in the Electromagnetic Coupling Factor Ding, Wendu; Hsu, Liang-Yan; Heaps, Charles W. The Journal of Physical Chemistry C, Vol. 122, Issue 39 https://doi.org/10.1021/acs.jpcc.8b07210	journal	September 2018
Ultrafast fluorescent decay induced by metal-mediated dipole–dipole interaction in two-dimensional molecular aggregates Hu, Qing; Jin, Dafei; Xiao, Jun Proceedings of the National Academy of Sciences, Vol. 114, Issue 38 https://doi.org/10.1073/pnas.1703000114	journal	September 2017
Characteristic Distance of Resonance Energy Transfer Coupled with Surface Plasmon Polaritons Wu, Jhih-Sheng; Lin, Yen-Cheng; Sheu, Yae-Lin The Journal of Physical Chemistry Letters, Vol. 9, Issue 24 https://doi.org/10.1021/acs.jpclett.8b03429	journal	November 2018
Displaced Fock states and their connection to quasiprobabilities Wunsche, A. Quantum Optics: Journal of the European Optical Society Part B, Vol. 3, Issue 6 https://doi.org/10.1088/0954-8998/3/6/005	journal	December 1991
Strong coupling in molecular exciton-plasmon Au nanorod array systems Fedele, Stefano; Hakami, Manal; Murphy, Antony Applied Physics Letters, Vol. 108, Issue 5 https://doi.org/10.1063/1.4941078	journal	February 2016
Theory of multichromophoric coherent resonance energy transfer: A polaronic quantum master equation approach Jang, Seogjoo The Journal of Chemical Physics, Vol. 135, Issue 3 https://doi.org/10.1063/1.3608914	journal	July 2011
Theory of vibronic intensity borrowing. Comparison of Herzberg‐Teller and Born‐Oppenheimer coupling Orlandi, G.; Siebrand, W. The Journal of Chemical Physics, Vol. 58, Issue 10 https://doi.org/10.1063/1.1679014	journal	May 1973
Self-Coupling of a Two-Level System by a Mirror Morawitz, H. Physical Review, Vol. 187, Issue 5 https://doi.org/10.1103/physrev.187.1792	journal	November 1969
Green-function approach to the radiation-field quantization for homogeneous and inhomogeneous Kramers-Kronig dielectrics Gruner, T.; Welsch, D. -G. Physical Review A, Vol. 53, Issue 3 https://doi.org/10.1103/physreva.53.1818	journal	March 1996
Solutions of integral and integro-differential equation systems by using differential transform method Arikoglu, Aytac; Ozkol, Ibrahim Computers & Mathematics with Applications, Vol. 56, Issue 9 https://doi.org/10.1016/j.camwa.2008.05.017	journal	November 2008
Resonant excitation transfer: A quantum electrodynamical study Andrews, David L.; Sherborne, Brad S. The Journal of Chemical Physics, Vol. 86, Issue 7 https://doi.org/10.1063/1.451910	journal	April 1987
Lifetime of an emitting molecule near a partially reflecting surface Chance, R. R.; Prock, A.; Silbey, R. The Journal of Chemical Physics, Vol. 60, Issue 7 https://doi.org/10.1063/1.1681437	journal	April 1974
Single-molecule strong coupling at room temperature in plasmonic nanocavities Chikkaraddy, Rohit; de Nijs, Bart; Benz, Felix Nature, Vol. 535, Issue 7610 https://doi.org/10.1038/nature17974	journal	June 2016
Effect of surface plasmons on transitions in molecules Philpott, Michael R. The Journal of Chemical Physics, Vol. 62, Issue 5 https://doi.org/10.1063/1.430708	journal	March 1975
Near-Zone Mediation of RET by One and Two Proximal Particles Salam, A. The Journal of Physical Chemistry A, Vol. 123, Issue 13 https://doi.org/10.1021/acs.jpca.9b00827	journal	March 2019
Reversible dynamics of single quantum emitters near metal-dielectric interfaces González-Tudela, A.; Huidobro, P. A.; Martín-Moreno, L. Physical Review B, Vol. 89, Issue 4 https://doi.org/10.1103/physrevb.89.041402	journal	January 2014
Control of the absorption of a four-level quantum system near a plasmonic nanostructure Carreño, F.; Antón, M. A.; Yannopapas, V. Physical Review B, Vol. 95, Issue 19 https://doi.org/10.1103/physrevb.95.195410	journal	May 2017
A new hybrid exchange–correlation functional using the Coulomb-attenuating method (CAM-B3LYP) Yanai, Takeshi; Tew, David P.; Handy, Nicholas C. Chemical Physics Letters, Vol. 393, Issue 1-3, p. 51-57 https://doi.org/10.1016/j.cplett.2004.06.011	journal	July 2004
Plasmonics for improved photovoltaic devices Atwater, Harry A.; Polman, Albert Materials for Sustainable Energy https://doi.org/10.1142/9789814317665_0001	book	October 2010
Spontaneous emission interference in negative-refractive-index waveguides Li, Gao-xiang; Evers, Jörg; Keitel, Christoph H. Physical Review B, Vol. 80, Issue 4 https://doi.org/10.1103/physrevb.80.045102	journal	July 2009
Classical Aspects of Energy Transfer in Molecular Systems Kuhn, Hans The Journal of Chemical Physics, Vol. 53, Issue 1 https://doi.org/10.1063/1.1673749	journal	July 1970
Purcell Factor: A Tunable Metric for Plasmon-Coupled Fluorescence Emission Enhancements in Cermet Nanocavities Srinivasan, Venkatesh; Ramamurthy, Sai Sathish The Journal of Physical Chemistry C, Vol. 120, Issue 5 https://doi.org/10.1021/acs.jpcc.5b11311	journal	December 2015
Principles of Nano-Optics Novotny, Lukas; Hecht, Bert Cambridge University Press https://doi.org/10.1017/CBO9780511813535	book	January 2006
Plasmon-Coupled Resonance Energy Transfer Hsu, Liang-Yan; Ding, Wendu; Schatz, George C. The Journal of Physical Chemistry Letters, Vol. 8, Issue 10 https://doi.org/10.1021/acs.jpclett.7b00526	journal	May 2017
Schwingungsstruktur der Elektronenübergänge bei mehratomigen Molekülen Herzberg, G.; Teller, E. Zeitschrift für Physikalische Chemie, Vol. 21B, Issue 1 https://doi.org/10.1515/zpch-1933-2136	journal	January 1933
Generalized effective mode volume for leaky optical cavities Kristensen, P. T.; Van Vlack, C.; Hughes, S. Optics Letters, Vol. 37, Issue 10 https://doi.org/10.1364/ol.37.001649	journal	January 2012
Plasmonics for improved photovoltaic devices Atwater, Harry A.; Polman, Albert Nature Materials, Vol. 9, Issue 3, p. 205-213 https://doi.org/10.1038/nmat2629	journal	February 2010
Increased light harvesting in dye-sensitized solar cells with energy relay dyes Hardin, Brian E.; Hoke, Eric T.; Armstrong, Paul B. Nature Photonics, Vol. 3, Issue 7 https://doi.org/10.1038/nphoton.2009.96	journal	June 2009
A unified theory of radiative and radiationless molecular energy transfer Andrews, D. L. Chemical Physics, Vol. 135, Issue 2 https://doi.org/10.1016/0301-0104(89)87019-3	journal	August 1989
Non-Markovian dynamics in plasmon-induced spontaneous emission interference Thanopulos, I.; Yannopapas, V.; Paspalakis, E. Physical Review B, Vol. 95, Issue 7 https://doi.org/10.1103/physrevb.95.075412	journal	February 2017
Spectral properties of a strongly coupled quantum-dot–metal-nanoparticle system Hakami, Jabir; Wang, Ligang; Zubairy, M. Suhail Physical Review A, Vol. 89, Issue 5 https://doi.org/10.1103/physreva.89.053835	journal	May 2014
Lasing action in strongly coupled plasmonic nanocavity arrays Zhou, Wei; Dridi, Montacer; Suh, Jae Yong Nature Nanotechnology, Vol. 8, Issue 7 https://doi.org/10.1038/nnano.2013.99	journal	June 2013
The enhancement of Raman scattering, resonance Raman scattering, and fluorescence from molecules adsorbed on a rough silver surface Weitz, D. A.; Garoff, S.; Gersten, J. I. The Journal of Chemical Physics, Vol. 78, Issue 9 https://doi.org/10.1063/1.445486	journal	May 1983
Influence of a dielectric interface on fluorescence decay time Drexhage, K. H. Journal of Luminescence, Vol. 1-2 https://doi.org/10.1016/0022-2313(70)90082-7	journal	January 1970
Increased light harvesting in dye-sensitized solar cells with energy relay dyes Hardin, Brian E.; Hoke, Eric T.; Armstrong, Paul B. Nature Photonics, Vol. 3, Issue 11 https://doi.org/10.1038/nphoton.2009.212	journal	November 2009
Coherent Coupling of Molecular Excitons to Electronic Polarizations of Noble Metal Nanoparticles Wiederrecht, Gary P.; Wurtz, Gregory A.; Hranisavljevic, Jasmina Nano Letters, Vol. 4, Issue 11 https://doi.org/10.1021/nl0488228	journal	November 2004
Correlation-Dependent Coherent to Incoherent Transitions in Resonant Energy Transfer Dynamics Nazir, Ahsan Physical Review Letters, Vol. 103, Issue 14 https://doi.org/10.1103/physrevlett.103.146404	journal	October 2009
The rotating-wave approximation: consistency and applicability from an open quantum system analysis Fleming, Chris; Cummings, N. I.; Anastopoulos, Charis Journal of Physics A: Mathematical and Theoretical, Vol. 43, Issue 40 https://doi.org/10.1088/1751-8113/43/40/405304	journal	September 2010
Plasmonic Purcell factor and coupling efficiency to surface plasmons. Implications for addressing and controlling optical nanosources Francs, G. Colas des; Barthes, J.; Bouhelier, A. Journal of Optics, Vol. 18, Issue 9 https://doi.org/10.1088/2040-8978/18/9/094005	journal	August 2016
Intermolecular energy transfer in the presence of dispersing and absorbing media Dung, Ho Trung; Knöll, Ludwig; Welsch, Dirk-Gunnar Physical Review A, Vol. 65, Issue 4 https://doi.org/10.1103/physreva.65.043813	journal	April 2002
Theory of coherent resonance energy transfer for coherent initial condition Jang, Seogjoo The Journal of Chemical Physics, Vol. 131, Issue 16 https://doi.org/10.1063/1.3247899	journal	October 2009
Quantum interference between decay channels of a three-level atom in a multilayer dielectric medium Li, Gao-xiang; Li, Fu-li; Zhu, Shi-yao Physical Review A, Vol. 64, Issue 1 https://doi.org/10.1103/physreva.64.013819	journal	June 2001
Electromagnetic theory of enhanced Raman scattering by molecules adsorbed on rough surfaces Gersten, Joel; Nitzan, Abraham The Journal of Chemical Physics, Vol. 73, Issue 7 https://doi.org/10.1063/1.440560	journal	October 1980
Transformation Optics Approach to Plasmon-Exciton Strong Coupling in Nanocavities Li, Rui-Qi; Hernángomez-Pérez, D.; García-Vidal, F. J. Physical Review Letters, Vol. 117, Issue 10 https://doi.org/10.1103/physrevlett.117.107401	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 Reimers, Jeffrey R. The Journal of Chemical Physics, Vol. 115, Issue 20 https://doi.org/10.1063/1.1412875	journal	November 2001
Variation of the Fluorescence Decay Time of a Molecule in Front of a Mirror Drexhage, K. H.; Kuhn, H.; Schäfer, F. P. Berichte der Bunsengesellschaft für physikalische Chemie, Vol. 72, Issue 2 https://doi.org/10.1002/bbpc.19680720261	journal	March 1968
Lessons from nature about solar light harvesting Scholes, Gregory D.; Fleming, Graham R.; Olaya-Castro, Alexandra Nature Chemistry, Vol. 3, Issue 10 https://doi.org/10.1038/nchem.1145	journal	September 2011
Nanoscale imaging and spontaneous emission control with a single nano-positioned quantum dot Ropp, Chad; Cummins, Zachary; Nah, Sanghee Nature Communications, Vol. 4, Issue 1 https://doi.org/10.1038/ncomms2477	journal	February 2013
Study of the Franck-Condon and Herzberg-Teller Approximations Lin, S. H.; Eyring, H. Proceedings of the National Academy of Sciences, Vol. 71, Issue 10 https://doi.org/10.1073/pnas.71.10.3802	journal	October 1974
Review Label-free detection with high-Q microcavities: a review of biosensing mechanisms for integrated devices Vollmer, Frank; Yang, Lan Nanophotonics, Vol. 1, Issue 3-4 https://doi.org/10.1515/nanoph-2012-0021	journal	January 2012
A single-photon transistor using nano-scale surface plasmons Chang, D. E.; Sørensen, A. S.; Demler, E. A. arXiv https://doi.org/10.48550/arxiv.0706.4335	text	January 2007
Correlation-dependent coherent to incoherent transitions in resonant energy transfer dynamics Nazir, Ahsan arXiv https://doi.org/10.48550/arxiv.0906.0592	text	January 2009
The Rotating-Wave Approximation: Consistency and Applicability from an Open Quantum System Analysis Fleming, Chris; Cummings, N. I.; Anastopoulos, Charis arXiv https://doi.org/10.48550/arxiv.1003.1749	text	January 2010
Extending the applicability of Redfield theories into highly non-Markovian regimes Montoya-Castillo, Andrés; Berkelbach, Timothy C.; Reichman, David R. arXiv https://doi.org/10.48550/arxiv.1507.02755	text	January 2015
JUNO and Neutrinoless Double Beta Decay Ge, Shao-Feng; Rodejohann, Werner arXiv https://doi.org/10.48550/arxiv.1507.05514	text	January 2015
Plasmonic Purcell factor and coupling efficiency to surface plasmons. Implications for addressing and controlling optical nanosources Francs, G. Colas des; Barthes, J.; Bouhelier, A. arXiv https://doi.org/10.48550/arxiv.1603.09403	text	January 2016
Transformation Optics Approach to Plasmon-Exciton Strong Coupling in Nanocavities Li, Rui-Qi; Hernangómez-Pérez, D.; García-Vidal, F. J. arXiv https://doi.org/10.48550/arxiv.1605.09443	text	January 2016
Non-Markovian dynamics in plasmon-induced spontaneous emission interference Thanopulos, I.; Yannopapas, V.; Paspalakis, E. arXiv https://doi.org/10.48550/arxiv.1701.04440	text	January 2017
Spontaneous decay in the presence of dispersing and absorbing bodies: general theory and application to a spherical cavity Dung, Ho Trung; Knoll, Ludwig; Welsch, Dirk-Gunnar arXiv https://doi.org/10.48550/arxiv.quant-ph/0003138	text	January 2000

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Related Subjects

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