Multidimensional Coherent Spectroscopy of Molecular Polaritons: Langevin Approach

Zhang, Zhedong; Nie, Xiaoyu; Lei, Dangyuan; Mukamel, Shaul

doi:10.1103/physrevlett.130.103001

Multidimensional Coherent Spectroscopy of Molecular Polaritons: Langevin Approach

Journal Article · Fri Mar 10 04:00:00 EST 2023 · Physical Review Letters

DOI:https://doi.org/10.1103/physrevlett.130.103001· OSTI ID:2422046

^[1]; ^[2]; Lei, Dangyuan ^[3]; Mukamel, Shaul ^[4]

City Univ. of Hong Kong, Kowloon (Hong Kong); City Univ. of Hong Kong, Shenzhen (China). Shenzhen Research Institute; OSTI
Xi'an Jiaotong Univ., Shaanxi (China)
City Univ. of Hong Kong, Kowloon (Hong Kong)
Univ. of California, Irvine, CA (United States)

We present a microscopic theory for nonlinear optical spectroscopy of N molecules in an optical cavity. Using the Heisenberg-Langevin equation, an analytical expression is derived for the time- and frequency-resolved signals accounting for arbitrary numbers of vibrational excitations. We identify clear signatures of the polariton-polaron interaction from multidimensional projections of the signal, e.g., pathways and timescales. Cooperative dynamics of cavity polaritons against intramolecular vibrations is revealed, along with a crosstalk between long-range coherence and vibronic coupling that may lead to localization effects. Our results further characterize the polaritonic coherence and the population transfer that is slower.

View Accepted Manuscript (DOE)

Research Organization:: Wayne State Univ., Detroit, MI (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC); National Science Foundation (NSF); Hong Kong Research Grants Council

Grant/Contract Number:: SC0022134

OSTI ID:: 2422046

Journal Information:: Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 10 Vol. 130; ISSN 0031-9007; ISSN PRLTAO

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

References (59)

Modifying Chemical Landscapes by Coupling to Vacuum Fields Hutchison, James A.; Schwartz, Tal; Genet, Cyriaque Angewandte Chemie, Vol. 124, Issue 7 https://doi.org/10.1002/ange.201107033	journal	January 2012
Ground-State Chemical Reactivity under Vibrational Coupling to the Vacuum Electromagnetic Field Thomas, Anoop; George, Jino; Shalabney, Atef Angewandte Chemie International Edition, Vol. 55, Issue 38 https://doi.org/10.1002/anie.201605504	journal	August 2016
Superradiance: An essay on the theory of collective spontaneous emission Gross, M.; Haroche, S. Physics Reports, Vol. 93, Issue 5 https://doi.org/10.1016/0370-1573(82)90102-8	journal	December 1982
Fluorescence spectroscopy of vibronic polaritons of molecular aggregates in optical microcavities Zhang, Zhedong; Mukamel, Shaul Chemical Physics Letters, Vol. 683 https://doi.org/10.1016/j.cplett.2017.02.022	journal	September 2017
Hybrid Light–Matter States in a Molecular and Material Science Perspective Ebbesen, Thomas W. Accounts of Chemical Research, Vol. 49, Issue 11 https://doi.org/10.1021/acs.accounts.6b00295	journal	October 2016
Cavity Born–Oppenheimer Approximation for Correlated Electron–Nuclear-Photon Systems Flick, Johannes; Appel, Heiko; Ruggenthaler, Michael Journal of Chemical Theory and Computation, Vol. 13, Issue 4 https://doi.org/10.1021/acs.jctc.6b01126	journal	March 2017
Controlling the Photostability of Pyrrole with Optical Nanocavities Gudem, Mahesh; Kowalewski, Markus The Journal of Physical Chemistry A, Vol. 125, Issue 5 https://doi.org/10.1021/acs.jpca.0c09252	journal	January 2021
Cavity Femtochemistry: Manipulating Nonadiabatic Dynamics at Avoided Crossings Kowalewski, Markus; Bennett, Kochise; Mukamel, Shaul The Journal of Physical Chemistry Letters, Vol. 7, Issue 11 https://doi.org/10.1021/acs.jpclett.6b00864	journal	May 2016
Polariton-Assisted Cooperativity of Molecules in Microcavities Monitored by Two-Dimensional Infrared Spectroscopy Zhang, Zhedong; Wang, Kai; Yi, Zhenhuan The Journal of Physical Chemistry Letters, Vol. 10, Issue 15 https://doi.org/10.1021/acs.jpclett.9b00979	journal	July 2019
Cavity-Modified Exciton Dynamics in Photosynthetic Units Sáez-Blázquez, Rocío; Feist, Johannes; Romero, Elisabet The Journal of Physical Chemistry Letters, Vol. 10, Issue 15 https://doi.org/10.1021/acs.jpclett.9b01495	journal	July 2019
Can Ultrastrong Coupling Change Ground-State Chemical Reactions? Martínez-Martínez, Luis A.; Ribeiro, Raphael F.; Campos-González-Angulo, Jorge ACS Photonics, Vol. 5, Issue 1 https://doi.org/10.1021/acsphotonics.7b00610	journal	November 2017
Exact States and Spectra of Vibrationally Dressed Polaritons Zeb, M. Ahsan; Kirton, Peter G.; Keeling, Jonathan ACS Photonics, Vol. 5, Issue 1 https://doi.org/10.1021/acsphotonics.7b00916	journal	November 2017
Generation of Anti-Stokes Fluorescence in a Strongly Coupled Organic Semiconductor Microcavity Georgiou, Kyriacos; Jayaprakash, Rahul; Askitopoulos, Alexis ACS Photonics, Vol. 5, Issue 11 https://doi.org/10.1021/acsphotonics.8b00552	journal	October 2018
Dynamics of the Higher Lying Excited States of Cyanine Dyes. An Ultrafast Fluorescence Study Guarin, Cesar A.; Villabona-Monsalve, Juan. P.; López-Arteaga, Rafael The Journal of Physical Chemistry B, Vol. 117, Issue 24 https://doi.org/10.1021/jp400278t	journal	June 2013
Optimization of Exciton Trapping in Energy Transfer Processes Cao, Jianshu; Silbey, Robert J. The Journal of Physical Chemistry A, Vol. 113, Issue 50 https://doi.org/10.1021/jp9032589	journal	December 2009
Quantum Nonlinear Optics with Polar J-Aggregates in Microcavities Herrera, Felipe; Peropadre, Borja; Pachon, Leonardo A. The Journal of Physical Chemistry Letters, Vol. 5, Issue 21 https://doi.org/10.1021/jz501905h	journal	October 2014
Modified relaxation dynamics and coherent energy exchange in coupled vibration-cavity polaritons Dunkelberger, A. D.; Spann, B. T.; Fears, K. P. Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms13504	journal	November 2016
Suppressing photochemical reactions with quantized light fields Galego, Javier; Garcia-Vidal, Francisco J.; Feist, Johannes Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms13841	journal	December 2016
Coherent coupling of molecular resonators with a microcavity mode Shalabney, A.; George, J.; Hutchison, J. Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms6981	journal	January 2015
Polariton-mediated energy transfer between organic dyes in a strongly coupled optical microcavity Coles, David M.; Somaschi, Niccolo; Michetti, Paolo Nature Materials, Vol. 13, Issue 7 https://doi.org/10.1038/nmat3950	journal	May 2014
Entangled photons enabled time-frequency-resolved coherent Raman spectroscopy and applications to electronic coherences at femtosecond scale Zhang, Zhedong; Peng, Tao; Nie, Xiaoyu Light: Science & Applications, Vol. 11, Issue 1 https://doi.org/10.1038/s41377-022-00953-y	journal	September 2022
Nonlinear plasmon-exciton coupling enhances sum-frequency generation from a hybrid metal/semiconductor nanostructure Zhong, Jin-Hui; Vogelsang, Jan; Yi, Jue-Min Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-15232-w	journal	March 2020
Cavity frequency-dependent theory for vibrational polariton chemistry Li, Xinyang; Mandal, Arkajit; Huo, Pengfei Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-21610-9	journal	February 2021
Enhanced nonlinear interaction of polaritons via excitonic Rydberg states in monolayer WSe2 Gu, Jie; Walther, Valentin; Waldecker, Lutz Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-22537-x	journal	April 2021
Turning a molecule into a coherent two-level quantum system Wang, Daqing; Kelkar, Hrishikesh; Martin-Cano, Diego Nature Physics, Vol. 15, Issue 5 https://doi.org/10.1038/s41567-019-0436-5	journal	February 2019
Elementary processes of photochemical reactions Franck, J.; Dymond, E. G. Transactions of the Faraday Society, Vol. 21, Issue February https://doi.org/10.1039/TF9262100536	journal	January 1926
Photon echoes of polyatomic molecules in condensed phases Yan, Yi Jing; Mukamel, Shaul The Journal of Chemical Physics, Vol. 94, Issue 1 https://doi.org/10.1063/1.460376	journal	January 1991
Optical microcavities enhance the exciton coherence length and eliminate vibronic coupling in J-aggregates Spano, F. C. The Journal of Chemical Physics, Vol. 142, Issue 18 https://doi.org/10.1063/1.4919348	journal	May 2015
Non-adiabatic dynamics of molecules in optical cavities Kowalewski, Markus; Bennett, Kochise; Mukamel, Shaul The Journal of Chemical Physics, Vol. 144, Issue 5 https://doi.org/10.1063/1.4941053	journal	February 2016
Communication: The origin of many-particle signals in nonlinear optical spectroscopy of non-interacting particles Mukamel, Shaul The Journal of Chemical Physics, Vol. 145, Issue 4 https://doi.org/10.1063/1.4960049	journal	July 2016
Monitoring polariton dynamics in the LHCII photosynthetic antenna in a microcavity by two-photon coincidence counting Zhang, Zhedong; Saurabh, Prasoon; Dorfman, Konstantin E. The Journal of Chemical Physics, Vol. 148, Issue 7 https://doi.org/10.1063/1.5004432	journal	February 2018
Effect of molecular Stokes shift on polariton dynamics Hulkko, E.; Pikker, S.; Tiainen, V. The Journal of Chemical Physics, Vol. 154, Issue 15 https://doi.org/10.1063/5.0037896	journal	April 2021
Super-reaction: The collective enhancement of a reaction rate by molecular polaritons in the presence of energy fluctuations Thanh Phuc, Nguyen The Journal of Chemical Physics, Vol. 155, Issue 1 https://doi.org/10.1063/5.0052226	journal	July 2021
Atoms and molecules in cavities, from weak to strong coupling in quantum-electrodynamics (QED) chemistry Flick, Johannes; Ruggenthaler, Michael; Appel, Heiko Proceedings of the National Academy of Sciences, Vol. 114, Issue 12 https://doi.org/10.1073/pnas.1615509114	journal	March 2017
Multidimensional photon correlation spectroscopy of cavity polaritons Dorfman, Konstantin E.; Mukamel, Shaul Proceedings of the National Academy of Sciences, Vol. 115, Issue 7 https://doi.org/10.1073/pnas.1719443115	journal	January 2018
Two-dimensional infrared spectroscopy of vibrational polaritons Xiang, Bo; Ribeiro, Raphael F.; Dunkelberger, Adam D. Proceedings of the National Academy of Sciences, Vol. 115, Issue 19 https://doi.org/10.1073/pnas.1722063115	journal	April 2018
Quantum theory of collective strong coupling of molecular vibrations with a microcavity mode Pino, Javier del; Feist, Johannes; Garcia-Vidal, Francisco J. New Journal of Physics, Vol. 17, Issue 5 https://doi.org/10.1088/1367-2630/17/5/053040	journal	May 2015
Exact Solution for an N -Molecule—Radiation-Field Hamiltonian Tavis, Michael; Cummings, Frederick W. Physical Review, Vol. 170, Issue 2 https://doi.org/10.1103/PhysRev.170.379	journal	June 1968
Quantum control with quantum light of molecular nonadiabaticity Csehi, András; Vibók, Ágnes; Halász, Gábor J. Physical Review A, Vol. 100, Issue 5 https://doi.org/10.1103/PhysRevA.100.053421	journal	November 2019
Absorption and photoluminescence in organic cavity QED Herrera, Felipe; Spano, Frank C. Physical Review A, Vol. 95, Issue 5 https://doi.org/10.1103/PhysRevA.95.053867	journal	May 2017
Probing biological light-harvesting phenomena by optical cavities Caruso, Filippo; Saikin, Semion K.; Solano, Enrique Physical Review B, Vol. 85, Issue 12 https://doi.org/10.1103/PhysRevB.85.125424	journal	March 2012
Coherent Emission from a Disordered Organic Semiconductor Induced by Strong Coupling with Surface Plasmons Aberra Guebrou, S.; Symonds, C.; Homeyer, E. Physical Review Letters, Vol. 108, Issue 6 https://doi.org/10.1103/PhysRevLett.108.066401	journal	February 2012
Subradiance in a Large Cloud of Cold Atoms Guerin, William; Araújo, Michelle O.; Kaiser, Robin Physical Review Letters, Vol. 116, Issue 8 https://doi.org/10.1103/PhysRevLett.116.083601	journal	February 2016
Cavity-Controlled Chemistry in Molecular Ensembles Herrera, Felipe; Spano, Frank C. Physical Review Letters, Vol. 116, Issue 23 https://doi.org/10.1103/PhysRevLett.116.238301	journal	June 2016
Dark Vibronic Polaritons and the Spectroscopy of Organic Microcavities Herrera, Felipe; Spano, Frank C. Physical Review Letters, Vol. 118, Issue 22 https://doi.org/10.1103/PhysRevLett.118.223601	journal	May 2017
Collective Jahn-Teller Interactions through Light-Matter Coupling in a Cavity Vendrell, Oriol Physical Review Letters, Vol. 121, Issue 25 https://doi.org/10.1103/PhysRevLett.121.253001	journal	December 2018
Langevin Approach to Quantum Optics with Molecules Reitz, Michael; Sommer, Christian; Genes, Claudiu Physical Review Letters, Vol. 122, Issue 20 https://doi.org/10.1103/PhysRevLett.122.203602	journal	May 2019
Exact Potential Energy Surface for Molecules in Cavities Lacombe, Lionel; Hoffmann, Norah M.; Maitra, Neepa T. Physical Review Letters, Vol. 123, Issue 8 https://doi.org/10.1103/PhysRevLett.123.083201	journal	August 2019
Catalysis by Dark States in Vibropolaritonic Chemistry Du, Matthew; Yuen-Zhou, Joel Physical Review Letters, Vol. 128, Issue 9 https://doi.org/10.1103/PhysRevLett.128.096001	journal	February 2022
Experimental Evidence for Subradiance Pavolini, D.; Crubellier, A.; Pillet, P. Physical Review Letters, Vol. 54, Issue 17 https://doi.org/10.1103/PhysRevLett.54.1917	journal	April 1985
Temperature-dependent superradiant decay of excitons in small aggregates Spano, Francis C.; Kuklinski, Jan R.; Mukamel, Shaul Physical Review Letters, Vol. 65, Issue 2 https://doi.org/10.1103/PhysRevLett.65.211	journal	July 1990
Cavity-Induced Modifications of Molecular Structure in the Strong-Coupling Regime Galego, Javier; Garcia-Vidal, Francisco J.; Feist, Johannes Physical Review X, Vol. 5, Issue 4 https://doi.org/10.1103/PhysRevX.5.041022	journal	November 2015
Nonlinear optics of semiconductor and molecular nanostructures; a common perspective Axt, V. M.; Mukamel, S. Reviews of Modern Physics, Vol. 70, Issue 1 https://doi.org/10.1103/RevModPhys.70.145	journal	January 1998
Manipulating optical nonlinearities of molecular polaritons by delocalization Xiang, Bo; Ribeiro, Raphael F.; Li, Yingmin Science Advances, Vol. 5, Issue 9 https://doi.org/10.1126/sciadv.aax5196	journal	September 2019
Nonlinear infrared polaritonic interaction between cavities mediated by molecular vibrations at ultrafast time scale Xiang, Bo; Wang, Jiaxi; Yang, Zimo Science Advances, Vol. 7, Issue 19 https://doi.org/10.1126/sciadv.abf6397	journal	May 2021
Photon-mediated interactions between quantum emitters in a diamond nanocavity Evans, R. E.; Bhaskar, M. K.; Sukachev, D. D. Science, Vol. 362, Issue 6415 https://doi.org/10.1126/science.aau4691	journal	September 2018
Stochastic Liouville, Langevin, Fokker–Planck, and Master Equation Approaches to Quantum Dissipative Systems Tanimura, Yoshitaka Journal of the Physical Society of Japan, Vol. 75, Issue 8 https://doi.org/10.1143/JPSJ.75.082001	journal	August 2006
H- and J-Aggregate Behavior in Polymeric Semiconductors Spano, Frank C.; Silva, Carlos Annual Review of Physical Chemistry, Vol. 65, Issue 1 https://doi.org/10.1146/annurev-physchem-040513-103639	journal	April 2014
Dynamics of Light Harvesting in Photosynthesis Cheng, Yuan-Chung; Fleming, Graham R. Annual Review of Physical Chemistry, Vol. 60, Issue 1 https://doi.org/10.1146/annurev.physchem.040808.090259	journal	May 2009

Similar Records

Enabling multiple intercavity polariton coherences by adding quantum confinement to cavity molecular polaritons

Journal Article · Mon Dec 26 23:00:00 EST 2022 · Proceedings of the National Academy of Sciences of the United States of America · OSTI ID:1906876

Related Subjects

74 ATOMIC AND MOLECULAR PHYSICS
Atoms
ions
& molecules in cavities
Chemical physics & physical chemistry
Molecules
Organic microcavities
Physics
Polaritons
light-matter interaction

Multidimensional Coherent Spectroscopy of Molecular Polaritons: Langevin Approach

Citation Formats

References (59)

Similar Records

Related Subjects