Mechanism of Molecular Polariton Decoherence in the Collective Light–Matter Couplings Regime

Chng, Benjamin X. K.; Ying, Wenxiang; Lai, Yifan; Vamivakas, A. Nickolas; Cundiff, Steven T.; Krauss, Todd D.; Huo, Pengfei

doi:10.1021/acs.jpclett.4c03049

Mechanism of Molecular Polariton Decoherence in the Collective Light–Matter Couplings Regime

Journal Article · Mon Nov 18 00:00:00 EST 2024 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.4c03049· OSTI ID:2477863

^[1]; ^[1]; Lai, Yifan ^[1]; ^[1]; ^[2]; ^[1]; ^[1]

University of Rochester, NY (United States)
University of Michigan, Ann Arbor, MI (United States)

Molecular polaritons, the hybridization of electronic states in molecules with photonic excitation inside a cavity, play an important role in fundamental quantum science and technology. Understanding the decoherence mechanism of molecular polaritons is among the most significant fundamental questions. We theoretically demonstrate that hybridizing many molecular excitons in a cavity protects the overall quantum coherence from phononinduced decoherence. The polariton coherence time can be prolonged up to 100 fs with a realistic collective Rabi splitting and quality factor at room temperature, compared to the typical electronic coherence time which is around 15 fs. Our numerically exact simulations and analytic theory suggest that the dominant decoherence mechanism is the population transfer from the upper polariton state to the dark state manifold. Increasing the collective coupling strength will increase the energy gap between these two sets of states and thus prolong the coherence lifetime. We further derived valuable scaling relations that directly indicate how polariton coherence depends on the number of molecules, Rabi splittings, and light–matter detunings.

View Journal Article

Research Organization:: University of Rochester, NY (United States)

Sponsoring Organization:: Air Force Office of Scientific Research (AFOSR); National Science Foundation (NSF); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0022171

OSTI ID:: 2477863

Alternate ID(s):: OSTI ID: 2525908
OSTI ID: 2479165

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 47 Vol. 15; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (61)

Tuning the Coherent Propagation of Organic Exciton‐Polaritons through Dark State Delocalization Pandya, Raj; Ashoka, Arjun; Georgiou, Kyriacos Advanced Science, Vol. 9, Issue 18 https://doi.org/10.1002/advs.202105569	journal	April 2022
Polariton Dynamics under Strong Light-Molecule Coupling Schwartz, Tal; Hutchison, James A.; Léonard, Jérémie ChemPhysChem, Vol. 14, Issue 1 https://doi.org/10.1002/cphc.201200734	journal	December 2012
Dissipation equation of motion approach to open quantum systems Yan, YiJing; Jin, Jinshuang; Xu, Rui-Xue Frontiers of Physics, Vol. 11, Issue 4 https://doi.org/10.1007/s11467-016-0513-5	journal	May 2016
Quantum tunnelling in a dissipative system Caldeira, A. O.; Leggett, A. J. Annals of Physics, Vol. 149, Issue 2 https://doi.org/10.1016/0003-4916(83)90202-6	journal	September 1983
Theoretical Advances in Polariton Chemistry and Molecular Cavity Quantum Electrodynamics Mandal, Arkajit; Taylor, Michael A. D.; Weight, Braden M. Chemical Reviews, Vol. 123, Issue 16 https://doi.org/10.1021/acs.chemrev.2c00855	journal	August 2023
Polariton-Mediated Electron Transfer via Cavity Quantum Electrodynamics Mandal, Arkajit; Krauss, Todd D.; Huo, Pengfei The Journal of Physical Chemistry B, Vol. 124, Issue 29 https://doi.org/10.1021/acs.jpcb.0c03227	journal	June 2020
Molecular Polaritons Generated from Strong Coupling between CdSe Nanoplatelets and a Dielectric Optical Cavity Qiu, Liangyu; Mandal, Arkajit; Morshed, Ovishek The Journal of Physical Chemistry Letters, Vol. 12, Issue 20 https://doi.org/10.1021/acs.jpclett.1c01104	journal	May 2021
Tuning and Enhancing Quantum Coherence Time Scales in Molecules via Light-Matter Hybridization Hu, Wenxiang; Gustin, Ignacio; Krauss, Todd D. The Journal of Physical Chemistry Letters, Vol. 13, Issue 49 https://doi.org/10.1021/acs.jpclett.2c02877	journal	December 2022
Investigating New Reactivities Enabled by Polariton Photochemistry Mandal, Arkajit; Huo, Pengfei The Journal of Physical Chemistry Letters, Vol. 10, Issue 18 https://doi.org/10.1021/acs.jpclett.9b01599	journal	August 2019
Tracking Polariton Relaxation with Multiscale Molecular Dynamics Simulations Groenhof, Gerrit; Climent, Clàudia; Feist, Johannes The Journal of Physical Chemistry Letters, Vol. 10, Issue 18 https://doi.org/10.1021/acs.jpclett.9b02192	journal	August 2019
Quantum Control of Ultrafast Internal Conversion Using Nanoconfined Virtual Photons Avramenko, Aleksandr G.; Rury, Aaron S. The Journal of Physical Chemistry Letters, Vol. 11, Issue 3 https://doi.org/10.1021/acs.jpclett.9b03447	journal	January 2020
Decoupling from a Thermal Bath via Molecular Polariton Formation Takahashi, Shota; Watanabe, Kazuya The Journal of Physical Chemistry Letters, Vol. 11, Issue 4 https://doi.org/10.1021/acs.jpclett.9b03789	journal	February 2020
Room-Temperature Polariton Lasing from CdSe Core-Only Nanoplatelets Freire-Fernández, Francisco; Sinai, Nathan G.; Hui Tan, Max Jin ACS Nano, Vol. 18, Issue 23 https://doi.org/10.1021/acsnano.4c03164	journal	May 2024
Controlling Exciton Propagation in Organic Crystals through Strong Coupling to Plasmonic Nanoparticle Arrays Berghuis, Anton Matthijs; Tichauer, Ruth H.; de Jong, Lianne M. A. ACS Photonics, Vol. 9, Issue 7 https://doi.org/10.1021/acsphotonics.2c00007	journal	June 2022
Polaritonic Chemistry with Organic Molecules Feist, Johannes; Galego, Javier; Garcia-Vidal, Francisco J. ACS Photonics, Vol. 5, Issue 1 https://doi.org/10.1021/acsphotonics.7b00680	journal	October 2017
Theory of Nanoscale Organic Cavities: The Essential Role of Vibration-Photon Dressed States Herrera, Felipe; Spano, Frank C. ACS Photonics, Vol. 5, Issue 1 https://doi.org/10.1021/acsphotonics.7b00728	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
Bose–Einstein condensation of exciton polaritons Kasprzak, J.; Richard, M.; Kundermann, S. Nature, Vol. 443, Issue 7110 https://doi.org/10.1038/nature05131	journal	September 2006
An electrically pumped polariton laser Schneider, Christian; Rahimi-Iman, Arash; Kim, Na Young Nature, Vol. 497, Issue 7449 https://doi.org/10.1038/nature12036	journal	May 2013
All-optical polariton transistor Ballarini, D.; De Giorgi, M.; Cancellieri, E. Nature Communications, Vol. 4, Issue 1 https://doi.org/10.1038/ncomms2734	journal	April 2013
Strong coupling between chlorosomes of photosynthetic bacteria and a confined optical cavity mode Coles, David M.; Yang, Yanshen; Wang, Yaya Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms6561	journal	November 2014
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
Room-temperature polariton lasing in an organic single-crystal microcavity Kéna-Cohen, S.; Forrest, S. R. Nature Photonics, Vol. 4, Issue 6 https://doi.org/10.1038/nphoton.2010.86	journal	April 2010
Molecular polariton electroabsorption Cheng, Chiao-Yu; Krainova, Nina; Brigeman, Alyssa N. Nature Communications, Vol. 13, Issue 1 https://doi.org/10.1038/s41467-022-35589-4	journal	December 2022
Quantum dynamical effects of vibrational strong coupling in chemical reactivity Lindoy, Lachlan P.; Mandal, Arkajit; Reichman, David R. Nature Communications, Vol. 14, Issue 1 https://doi.org/10.1038/s41467-023-38368-x	journal	May 2023
Ultrafast imaging of polariton propagation and interactions Xu, Ding; Mandal, Arkajit; Baxter, James M. Nature Communications, Vol. 14, Issue 1 https://doi.org/10.1038/s41467-023-39550-x	journal	June 2023
Multi-scale molecular dynamics simulations of enhanced energy transfer in organic molecules under strong coupling Sokolovskii, Ilia; Tichauer, Ruth H.; Morozov, Dmitry Nature Communications, Vol. 14, Issue 1 https://doi.org/10.1038/s41467-023-42067-y	journal	October 2023
Quantum computing with exciton-polariton condensates Ghosh, Sanjib; Liew, Timothy C. H. npj Quantum Information, Vol. 6, Issue 1 https://doi.org/10.1038/s41534-020-0244-x	journal	February 2020
From enhanced diffusion to ultrafast ballistic motion of hybrid light–matter excitations Balasubrahmaniyam, Mukundakumar; Simkhovich, Arie; Golombek, Adina Nature Materials, Vol. 22, Issue 3 https://doi.org/10.1038/s41563-022-01463-3	journal	January 2023
A room-temperature organic polariton transistor Zasedatelev, Anton V.; Baranikov, Anton V.; Urbonas, Darius Nature Photonics, Vol. 13, Issue 6 https://doi.org/10.1038/s41566-019-0392-8	journal	March 2019
Quantum coherences reveal excited-state dynamics in biophysical systems Wang, Lili; Allodi, Marco A.; Engel, Gregory S. Nature Reviews Chemistry, Vol. 3, Issue 8 https://doi.org/10.1038/s41570-019-0109-z	journal	June 2019
Polariton condensates for classical and quantum computing Kavokin, Alexey; Liew, Timothy C. H.; Schneider, Christian Nature Reviews Physics, Vol. 4, Issue 7 https://doi.org/10.1038/s42254-022-00447-1	journal	April 2022
An analysis of electronic dephasing in the spin-boson model Hwang, Hyonseok; Rossky, Peter J. The Journal of Chemical Physics, Vol. 120, Issue 24 https://doi.org/10.1063/1.1742979	journal	June 2004
Theory of open quantum systems with bath of electrons and phonons and spins: Many-dissipaton density matrixes approach Yan, YiJing The Journal of Chemical Physics, Vol. 140, Issue 5 https://doi.org/10.1063/1.4863379	journal	February 2014
Multi-scale dynamics simulations of molecular polaritons: The effect of multiple cavity modes on polariton relaxation Tichauer, Ruth H.; Feist, Johannes; Groenhof, Gerrit The Journal of Chemical Physics, Vol. 154, Issue 10 https://doi.org/10.1063/5.0037868	journal	March 2021
Local molecular probes of ultrafast relaxation channels in strongly coupled metalloporphyrin-cavity systems Avramenko, Aleksandr G.; Rury, Aaron S. The Journal of Chemical Physics, Vol. 155, Issue 6 https://doi.org/10.1063/5.0055296	journal	August 2021
Resonance theory and quantum dynamics simulations of vibrational polariton chemistry Ying, Wenxiang; Huo, Pengfei The Journal of Chemical Physics, Vol. 159, Issue 8 https://doi.org/10.1063/5.0159791	journal	August 2023
Quantum dynamics simulations of the 2D spectroscopy for exciton polaritons Mondal, M. Elious; Koessler, Eric R.; Provazza, Justin The Journal of Chemical Physics, Vol. 159, Issue 9 https://doi.org/10.1063/5.0166188	journal	September 2023
Room-temperature strong coupling between CdSe nanoplatelets and a metal–DBR Fabry–Pérot cavity Morshed, Ovishek; Amin, Mitesh; Cogan, Nicole M. B. The Journal of Chemical Physics, Vol. 161, Issue 1 https://doi.org/10.1063/5.0210700	journal	July 2024
Non-equilibrium rate theory for polariton relaxation dynamics Lai, Yifan; Ying, Wenxiang; Huo, Pengfei The Journal of Chemical Physics, Vol. 161, Issue 10 https://doi.org/10.1063/5.0231396	journal	September 2024
Manipulating molecules with quantum light Kowalewski, Markus; Mukamel, Shaul Proceedings of the National Academy of Sciences, Vol. 114, Issue 13 https://doi.org/10.1073/pnas.1702160114	journal	March 2017
Simulating molecular polaritons in the collective regime using few-molecule models Pérez-Sánchez, Juan B.; Koner, Arghadip; Stern, Nathaniel P. Proceedings of the National Academy of Sciences, Vol. 120, Issue 15 https://doi.org/10.1073/pnas.2219223120	journal	April 2023
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
Comment on ‘Quantum theory of collective strong coupling of molecular vibrations with a microcavity mode’ Martínez-Martínez, Luis A.; Yuen-Zhou, Joel New Journal of Physics, Vol. 20, Issue 1 https://doi.org/10.1088/1367-2630/aaa751	journal	February 2018
Chemical Dynamics in Condensed Phases Nitzan, Abraham Oxford University Press https://doi.org/10.1093/oso/9780198529798.001.0001	book	April 2006
Polaritons and excitons: Hamiltonian design for enhanced coherence Scholes, Gregory D. Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 476, Issue 2242 https://doi.org/10.1098/rspa.2020.0278	journal	October 2020
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
Exciton-polariton integrated circuits Liew, T. C. H.; Kavokin, A. V.; Ostatnický, T. Physical Review B, Vol. 82, Issue 3 https://doi.org/10.1103/PhysRevB.82.033302	journal	July 2010
When polarons meet polaritons: Exciton-vibration interactions in organic molecules strongly coupled to confined light fields Wu, Ning; Feist, Johannes; Garcia-Vidal, Francisco J. Physical Review B, Vol. 94, Issue 19 https://doi.org/10.1103/PhysRevB.94.195409	journal	November 2016
Reversible Switching of Ultrastrong Light-Molecule Coupling Schwartz, T.; Hutchison, J. A.; Genet, C. Physical Review Letters, Vol. 106, Issue 19 https://doi.org/10.1103/PhysRevLett.106.196405	journal	May 2011
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
Observation of the coupled exciton-photon mode splitting in a semiconductor quantum microcavity Weisbuch, C.; Nishioka, M.; Ishikawa, A. Physical Review Letters, Vol. 69, Issue 23 https://doi.org/10.1103/PhysRevLett.69.3314	journal	December 1992
Relationship between Quantum Decoherence Times and Solvation Dynamics in Condensed Phase Chemical Systems Prezhdo, Oleg V.; Rossky, Peter J. Physical Review Letters, Vol. 81, Issue 24 https://doi.org/10.1103/PhysRevLett.81.5294	journal	December 1998
Room-Temperature Polariton Lasing in Semiconductor Microcavities Christopoulos, S.; von Högersthal, G. Baldassarri Höger; Grundy, A. J. D. Physical Review Letters, Vol. 98, Issue 12 https://doi.org/10.1103/PhysRevLett.98.126405	journal	March 2007
Exciton-polariton Bose-Einstein condensation Deng, Hui; Haug, Hartmut; Yamamoto, Yoshihisa Reviews of Modern Physics, Vol. 82, Issue 2 https://doi.org/10.1103/RevModPhys.82.1489	journal	May 2010
Quantum Dissipative Systems Weiss, Ulrich https://doi.org/10.1142/8334	book	March 2012
Time Evolution of a Quantum System in Contact with a Nearly Gaussian-Markoffian Noise Bath Tanimura, Yoshitaka; Kubo, Ryogo Journal of the Physical Society of Japan, Vol. 58, Issue 1 https://doi.org/10.1143/JPSJ.58.101	journal	January 1989
Bose–Einstein Condensation of Exciton-Polaritons in Organic Microcavities Keeling, Jonathan; Kéna-Cohen, Stéphane Annual Review of Physical Chemistry, Vol. 71, Issue 1 https://doi.org/10.1146/annurev-physchem-010920-102509	journal	April 2020
Photocurrent generation following long-range propagation of organic exciton–polaritons Liu, Bin; Huang, Xinjing; Hou, Shaocong Optica, Vol. 9, Issue 9 https://doi.org/10.1364/OPTICA.461025	journal	September 2022
Origin of the asymmetric light emission from molecular exciton–polaritons Neuman, Tomáš; Aizpurua, Javier Optica, Vol. 5, Issue 10 https://doi.org/10.1364/OPTICA.5.001247	journal	January 2018
Polariton Spectra under the Collective Coupling Regime. I. Efficient Simulation of Linear Spectra and Quantum Dynamics Mondal, Elious; Vamivakas, Nickolas; Cundiff, Steven https://doi.org/10.26434/chemrxiv-2024-8kfcb	preprint	October 2024

Similar Records

Quantum dynamics simulations of the 2D spectroscopy for exciton polaritons

Journal Article · Thu Aug 31 20:00:00 EDT 2023 · Journal of Chemical Physics · OSTI ID:2422069

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Cavities
Coupling reactions
Molecules
Phonons
Polariton
Decoherence
Polaritons

Mechanism of Molecular Polariton Decoherence in the Collective Light–Matter Couplings Regime

Citation Formats

References (61)

Similar Records

Related Subjects