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Light-induced quantum self-trapping of vibrational excitons in an optical cavity
Phys. Rev. A 114, 013116 – Published 15 July, 2026
DOI: https://doi.org/10.1103/56c3-drn7
Abstract
In an optical cavity, strong light-matter coupling between excitons and photons has been widely reported as a way to enhance energy delocalization through spatially extended polaritonic states. In contrast, leveraging cavity-mediated light-matter effects to promote the reciprocal phenomenon, namely, energy localization, remains largely underexplored. In the present work, we address this question by focusing on a special form of energy localization arising from nonlinear matter interactions: quantum self-trapping (QST). We employ a generalized Tavis-Cummings model to investigate the transport of vibrational excitons, i.e., vibrons, between two anharmonic vibrational modes and examine their interplay with cavity photons. In the absence of a cavity, the arising of true and complete QST, i.e., a fully stabilized localization, is not possible due to the symmetry of the system. The energy transfer between the two modes still occurs, slowed down by the many-body interactions. Coupling the system to a single-mode cavity strongly alters this behavior, with two emerging regimes. First, at weak light-matter coupling, destructive interference between newly opened transition pathways suppresses energy exchange, leading to cavity-enhanced self-trapping. As the coupling strength increases, these interference effects evolve, leading to cavity-assisted energy transfer, where we observe an acceleration of the vibrational energy flow. Most notably, we identify critical coupling strengths that separate both regimes in which the dynamics almost totally freeze, suggesting the arising of a “stabilized” light-induced QST of many-vibron bound states. These results suggest that optical cavities can not only enhance transport but could also stabilize energy localization phenomena, providing a route to control energy flow in quantum systems.
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References (63)
- Y. Kubo, F. R. Ong, P. Bertet, D. Vion, V. Jacques, D. Zheng, A. Dréau, J.-F. Roch, A. Auffeves, F. Jelezko, J. Wrachtrup, M. F. Barthe, P. Bergonzo, and D. Esteve, Strong coupling of a spin ensemble to a superconducting resonator, Phys. Rev. Lett. 105, 140502 (2010).
- D. Shelton, I. Brener, J. C. Ginn, M. B. Sinclair, D. W. Peters, K. R. Coffey, and G. D. Boreman, Strong coupling between nanoscale metamaterials and phonons, Nano Lett. 11, 2104 (2011).
- I. J. Luxmoore, C. H. Gan, P. Q. Liu, F. Valmorra, P. Li, J. Faist, and G. R. Nash, Strong coupling in the far-infrared between graphene plasmons and the surface optical phonons of silicon dioxide, ACS Photon. 1, 1151 (2014).
- P. Sivarajah, A. Steinbacher, B. Dastrup, J. Lu, M. Xiang, W. Ren, S. Kamba, S. Cao, and K. A. Nelson, THz-frequency magnon-phonon-polaritons in the collective strong-coupling regime, J. Appl. Phys. 125, 213103 (2019).
- Y. Kaluzny, P. Goy, M. Gross, J. M. Raimond, and S. Haroche, Observation of self-induced Rabi oscillations in two-level atoms excited inside a resonant cavity: The ringing regime of superradiance, Phys. Rev. Lett. 51, 1175 (1983).
- M. G. Raizen, R. J. Thompson, R. J. Brecha, H. J. Kimble, and H. J. Carmichael, Normal-mode splitting and linewidth averaging for two-state atoms in an optical cavity, Phys. Rev. Lett. 63, 240 (1989).
- R. J. Thompson, G. Rempe, and H. J. Kimble, Observation of normal-mode splitting for an atom in an optical cavity, Phys. Rev. Lett. 68, 1132 (1992).
- C. Weisbuch, M. Nishioka, A. Ishikawa, and Y. Arakawa, Observation of the coupled exciton-photon mode splitting in a semiconductor quantum microcavity, Phys. Rev. Lett. 69, 3314 (1992).
- D. G. Lidzey, D. Bradley, M. Skolnick, T. Virgili, S. Walker, and D. Whittaker, Strong exciton-photon coupling in an organic semiconductor microcavity, Nature (London) 395, 53 (1998).
- D. G. Lidzey, D. D. Bradley, A. Armitage, S. Walker, and M. S. Skolnick, Photon-mediated hybridization of Frenkel excitons in organic semiconductor microcavities, Science 288, 1620 (2000).
- F. Herrera and F. C. Spano, Cavity-controlled chemistry in molecular ensembles, Phys. Rev. Lett. 116, 238301 (2016).
- G. Groenhof and J. J. Toppari, Coherent light harvesting through strong coupling to confined light, J. Phys. Chem. Lett. 9, 4848 (2018).
- S. Wang, T. Chervy, J. George, J. A. Hutchison, C. Genet, and T. W. Ebbesen, Quantum yield of polariton emission from hybrid light-matter states, J. Phys. Chem. Lett. 5, 1433 (2014).
- C. Fábri, B. Lasorne, G. J. Halász, L. S. Cederbaum, and Á. Vibók, Striking generic impact of light-induced non-adiabaticity in polyatomic molecules, J. Phys. Chem. Lett. 11, 5324 (2020).
- C. Fábri, B. Lasorne, G. J. Halász, L. S. Cederbaum, and Á. Vibók, Quantum light-induced nonadiabatic phenomena in the absorption spectrum of formaldehyde: Full- and reduced-dimensionality studies, J. Chem. Phys. 153, 234302 (2020).
- A. Csehi, G. J. Halász, L. S. Cederbaum, and Á. Vibók, Competition between light-induced and intrinsic nonadiabatic phenomena in diatomics, J. Phys. Chem. Lett. 8, 1624 (2017).
- C. Fábri, G. J. Halász, and Á. Vibók, Probing light-induced conical intersections by monitoring multidimensional polaritonic surfaces, J. Phys. Chem. Lett. 13, 1172 (2022).
- G. Sandik, J. Feist, F. J. García-Vidal, and T. Schwartz, Cavity-enhanced energy transport in molecular systems, Nat. Mater. 24, 344 (2025).
- R. Bhuyan, J. Mony, O. Kotov, G. W. Castellanos, J. Goomez Rivas, T. O. Shegai, and K. Borjesson, The rise and current status of polaritonic photochemistry and photophysics, Chem. Rev. 123, 10877 (2023).
- J. Feist and F. J. Garcia-Vidal, Extraordinary exciton conductance induced by strong coupling, Phys. Rev. Lett. 114, 196402 (2015).
- D. Hagenmüller, J. Dubail, F. Mattiotti, G. Pupillo, and J. Schachenmayer, Disorder in cavity-modified transport and chemistry, in Polariton Chemistry: Molecules in Cavities, edited by J. Yuen-Zhou, N. C. Giebink, and R. F. Ribeiro (Wiley, New York, 2025), pp. 193–218.
- J. Schachenmayer, C. Genes, E. Tignone, and G. Pupillo, Cavity-enhanced transport of excitons, Phys. Rev. Lett. 114, 196403 (2015).
- D. M. Coles, Y. Yang, Y. Wang, R. T. Grant, R. A. Taylor, S. K. Saikin, A. Aspuru-Guzik, D. G. Lidzey, J. K.-H. Tang, and J. M. Smith, Strong coupling between chlorosomes of photosynthetic bacteria and a confined optical cavity mode, Nat. Commun. 5, 5561 (2014).
- F. Spano, Optical microcavities enhance the exciton coherence length and eliminate vibronic coupling in J-aggregates, J. Chem. Phys. 142, 184707 (2015).
- G. G. Rozenman, K. Akulov, A. Golombek, and T. Schwartz, Long-range transport of organic exciton-polaritons revealed by ultrafast microscopy, ACS Photon. 5, 105 (2018).
- S. Hou, M. Khatoniar, K. Ding, Y. Qu, A. Napolov, V. M. Menon, and S. R. Forrest, Ultralong-range energy transport in a disordered organic semiconductor at room temperature via coherent exciton-polariton propagation, Adv. Mater. 32, 2002127 (2020).
- M. Balasubrahmaniyam, A. Simkhovich, A. Golombek, G. Sandik, G. Ankonina, and T. Schwartz, From enhanced diffusion to ultrafast ballistic motion of hybrid light–matter excitations, Nat. Mater. 22, 338 (2023).
- E. V. Denning, M. Wubs, N. Stenger, J. Mørk, and P. T. Kristensen, Cavity-induced exciton localization and polariton blockade in two-dimensional semiconductors coupled to an electromagnetic resonator, Phys. Rev. Res. 4, L012020 (2022).
- I. Yu. Chestnov, T. A. Khudaiberganov, A. P. Alodjants, and A. V. Kavokin, Heat-assisted self-localization of exciton polaritons, Phys. Rev. B 98, 115302 (2018).
- V. Rokaj, S. I. Mistakidis, and H. Sadeghpour, Cavity induced collective behavior in the polaritonic ground state, SciPost Phys. 14, 167 (2023).
- M. Sato, B. E. Hubbard, and A. J. Sievers, Colloquium: Nonlinear energy localization and its manipulation in micromechanical oscillator arrays, Rev. Mod. Phys. 78, 137 (2006).
- S. Flach and C. Willis, Discrete breathers, Phys. Rep. 295, 181 (1998).
- S. Flach and A. V. Gorbach, Discrete breathers—advances in theory and applications, Phys. Rep. 467, 1 (2008).
- A. S. Davydov and N. I. Kislukha, Solitary excitons in one-dimensional molecular chains, Phys. Status Solidi B 59, 465 (1973).
- A. Scott, Davydov's soliton, Phys. Rep. 217, 1 (1992).
- J. Eilbeck, P. Lomdahl, and A. Scott, The discrete self-trapping equation, Physica D 16, 318 (1985).
- A. J. Sievers and S. Takeno, Intrinsic localized modes in anharmonic crystals, Phys. Rev. Lett. 61, 970 (1988).
- J. C. Kimball, C. Y. Fong, and Y. R. Shen, Anharmonicity, phonon localization, two-phonon bound states, and vibrational spectra, Phys. Rev. B 23, 4946 (1981).
- B. N. J. Persson, Application of a boson Hubbard model to vibrational dynamics in adsorbate layers, Phys. Rev. B 46, 12701 (1992).
- C. Falvo, Linear and non-linear infrared response of one-dimensional vibrational Holstein polarons in the anti-adiabatic limit: Optical and acoustical phonon models, J. Chem. Phys. 148, 074103 (2018).
- V. Pouthier, Two-vibron bound states in -helix proteins: The interplay between the intramolecular anharmonicity and the strong vibron-phonon coupling, Phys. Rev. E 68, 021909 (2003).
- F. Bogani, G. Cardini, V. Schettino, and P. L. Tasselli, Vibrational relaxation and dephasing of two-phonon bound states in molecular crystals, Phys. Rev. B 42, 2307 (1990).
- E. Wright, J. Eilbeck, M. Hays, P. Miller, and A. Scott, The quantum discrete self-trapping equation in the Hartree approximation, Physica D 69, 18 (1993).
- L. Bernstein, J. C. Eilbeck, and A. C. Scott, The quantum theory of local modes in a coupled system of nonlinear oscillators, Nonlinearity 3, 293 (1990).
- A. Scott, J. Eilbeck, and H. Gilhøj, Quantum lattice solitons, Physica D 78, 194 (1994).
- J. Dorignac, J. C. Eilbeck, M. Salerno, and A. C. Scott, Quantum signatures of breather-breather interactions, Phys. Rev. Lett. 93, 025504 (2004).
- L. Proville, Biphonons in the Klein-Gordon lattice, Phys. Rev. B 71, 104306 (2005).
- C. Falvo, V. Pouthier, and J. Eilbeck, Fast energy transfer mediated by multi-quanta bound states in a nonlinear quantum lattice, Physica D 221, 58 (2006).
- V. Pouthier, Boundary-induced energy localization in a nonlinear quantum lattice, Phys. Rev. B 76, 224302 (2007).
- R. A. Pinto, M. Haque, and S. Flach, Edge-localized states in quantum one-dimensional lattices, Phys. Rev. A 79, 052118 (2009).
- R. A. Pinto, J. P. Nguenang, and S. Flach, Boundary effects on quantum -breathers in a Bose–Hubbard chain, Physica D 238, 581 (2009).
- V. Pouthier, Quantum self-trapping on a star graph, Phys. Rev. E 105, 044304 (2022).
- V. Pouthier, Two-exciton bound state quantum self-trapping in an extended star graph, J. Chem. Phys. 156, 155101 (2022).
- L. Bernstein, Quantizing a self-trapping transition, Physica D 68, 174 (1993).
- V. Pouthier, Multi-quanta energy relaxation in a nonlinear quantum dimer coupled to a phonon bath, Physica D 221, 13 (2006).
- M. Tavis and F. W. Cummings, Exact solution for an -molecule—radiation-field Hamiltonian, Phys. Rev. 170, 379 (1968).
- M. Tavis and F. W. Cummings, Approximate solutions for an -molecule-radiation-field Hamiltonian, Phys. Rev. 188, 692 (1969).
- F. J. Hernández and F. Herrera, Multi-level quantum Rabi model for anharmonic vibrational polaritons, J. Chem. Phys. 151, 144116 (2019).
- T. E. Li, A. Nitzan, and J. E. Subotnik, Polariton relaxation under vibrational strong coupling: Comparing cavity molecular dynamics simulations against Fermi's golden rule rate, J. Chem. Phys. 156, 134106 (2022).
- J. del Pino, J. Feist, and F. J. Garcia-Vidal, Quantum theory of collective strong coupling of molecular vibrations with a microcavity mode, New J. Phys. 17, 053040 (2015).
- O. Mulken, V. Bierbaun, and A. Blumen, Coherent exciton transport in dendrimers and continuous-time quantum walks, J. Chem. Phys. 124, 124905 (2006).
- C. Cohen-Tannoudji, J. Dupont-Roc, and G. Grynberg, Atom-Photon Interactions: Basic Processes and Applications (Wiley, New York, 1998).
- O. Mülken and A. Blumen, Efficiency of quantum and classical transport on graphs, Phys. Rev. E 73, 066117 (2006).