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arXiv:2604.06142

Light-Induced Quantum Self-Trapping of Vibrational Excitons in an Optical Cavity

Vincent Pouthier, Saad Yalouz

quant-phSubmitted Apr 7, 2026• Announced Apr 8, 2026• 0 citations
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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 \textit{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: \textit{Quantum Self-Trapping} (QST). We employ a generalized Tavis--Cummings model to investigate the transport of vibrational excitons -- \textit{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 -- \textit{i.e.}, an infinite-lifetime 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 new route to control energy flow in quantum systems.

Related papers

Light-induced quantum self-trapping of vibrational excitons in an optical cavity

Vincent Pouthier, Saad Yalouz

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.

Physical Review A•Jun 29, 2026•0 citations

Cavity Quantum Electrodynamics of Molecular Systems : Polarization Effects, Multiple Excitations, and Vibrational Selectivity

Garcia Borges, Lucas

The field of Polaritonic Chemistry studies molecules strongly coupled to the light field of optical cavities. The resulting modification of the potential energy landscape has been demonstrated to enable control over the chemical and physical properties of materials and molecular ensembles. This thesis extends the Tavis–Cummings model to describe molecules under strong light–matter coupling, incorporating static dipole moments and dipole self-energy contributions derived from the Pauli–Fierz Hamiltonian. These additional terms are shown to be essential for reproducing cavity-modified molecular dynamics and spectra. Simulations on the nuclear wavefunction propagation of MgH+ molecules demonstrate the impact of these terms, while an effective two-level system model accurately captures the behavior of large ensembles. Beyond single excitations, the thesis also explores the higher excitation manifolds of the Tavis-Cummings model, which reveals that allowing for more than a single excitation makes the reaction of the involved polaritons entropically more favorable. Open-system simulations highlight how the coherence of the system's initial state governs decay pathways and enables long-lived energy storage. Finally, a multilevel vibrational model coupled to a two-mode cavity is introduced, where a Raman scheme enables selective mixing of vibrational states. The simulation results show that continuous pumping can drive molecules into specific vibrational states while suppressing electronic excitation, both for single molecules and small ensembles. Together, these results provide new theoretical insights into the mechanisms by which optical cavities reshape molecular energy landscapes. The results suggest approaches for controlling photonic, electronic, and vibrational dynamics in strongly coupled systems, contributing to the theoretical foundation of polariton chemistry.

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Molecular Electron Transfer in Optical Cavities: From Excitonic to Vibronic Polaritons

Takumi Hidaka, Tomohiro Fukushima, Nguyen Thanh Phuc

Strong coupling between molecular excitations and quantized electromagnetic fields in optical cavities provides a powerful means to control the physical and chemical properties of molecular systems. Here, we study electron transfer (ET) dynamics in cavity-coupled molecules using the numerically exact hierarchical equations of motion (HEOM) method, which captures nonperturbative and non-Markovian effects beyond standard perturbative theories. We identify distinct resonance and collective effects associated with polariton formation and show that the ET rate saturates in the strong-coupling regime, a feature not captured by perturbative approaches. We further extend the cavity-modified ET model by incorporating the nuclear-coordinate dependence of molecular electric dipole moments, which gives rise to a three-body interaction involving molecular electronic and vibrational degrees of freedom and cavity photons. This vibronic polariton formation leads to non-monotonic, oscillatory dependencies of the ET rate on the light-matter coupling strength and cavity frequency, which we attribute to quantum interference among multiple transfer pathways. These findings establish cavity-modified electron transfer as a multichannel quantum process governed by the interplay of electronic, vibrational, and photonic degrees of freedom.

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Limits of Memory-Assisted Coherence in Cavity-Embedded Molecules

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Strong light-matter coupling in optical cavities is being widely explored as a strategy for modifying molecular dynamics and enhancing coherence. At the same time, structured vibrational environments can exhibit non-Markovian memory that promotes information backflow and coherence revival. We investigate the competition between these effects in a vibronic molecular system strongly coupled to a lossy optical cavity. Using hierarchical equations of motion to treat structured vibrational baths, we quantify both system coherence and non-Markovianity via the l1 norm of coherence and the Breuer-Laine-Piilo measure, respectively. We find that cavity coupling enhances coherence in overdamped environments but can suppress memory-assisted coherence in resonant underdamped regimes, even in the absence of significant photon loss. This suppression arises from hybridization-induced modification of system-bath information flow. We demonstrate that cavity coupling does not universally protect coherence but establishes limits governed by the competition between vibrational recurrence time scales and polaritonic hybridization.

The Journal of Physical Chemistry Letters•Oct 5, 2026•0 citations

Strong quantum interaction between excitons bound by cavity photon exchange

Anonymous, Cristiano Ciuti

We theoretically predict the interaction between polaritonic excitations arising from the coupling of a cavity photon mode with bound to continuum intersubband transitions in a doped quantum well. The resulting exciton bound by photon exchange, recently demonstrated experimentally, exhibits a binding energy that can be continuously tuned by varying the cavity frequency. We show that polariton-polariton interactions, originating from both Coulomb interactions and Pauli blocking, can be dramatically enhanced by reducing the exciton binding energy, thereby increasing the effective Bohr radius along the growth direction. This regime is reminiscent of Rydberg atoms, where weak binding leads to strong quantum interactions. Our predictions indicate that this physics can give rise to giant quantum optical nonlinearities in the mid and far infrared, a spectral region that remains largely unexplored in quantum optics and offers exciting opportunities for both fundamental studies and applications.

arXiv:2510.24421•Physical review. B./Physical review. B•Aug 3, 2026•0 citations

Unidirectional Dark-to-Bright Rescue in Cavity-Coupled Quantum Transport

Jack Diab, Arpit Arora, Taylor L. Patti +1 more

Strong light-matter coupling in optical microcavities can transport energy ballistically across an emitter array, but the same coupling buries most of the excitation in a manifold of dark states that grows with system size and traps energy outside the transport channel. We show that the off-diagonal (non-Condon) part of the exciton-phonon coupling opens a one-way escape route from this trap, driving population irreversibly from dark states into the radiative channel. This rate is fixed by a photonic-weight conservation law rather than by dark-bright overlap which evacuates the dark manifold at a rate independent of system size. The mechanism contributes to transport with near-complete efficiency with four signatures being single exponential dark state decay, a size scaling efficiency gap, distinct temperature behavior, and a resonance in the escape rate at vibrational bath modes. Beyond polariton transport, it recasts dark states from a parasitic loss channel into an engineered dissipative resource, with implications for light harvesting and dissipation based quantum control.

quant-pharXiv:2608.05312•Aug 7, 2026•0 citations
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 \textit{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: \textit{Quantum Self-Trapping} (QST). We employ a generalized Tavis--Cummings model to investigate the transport of vibrational excitons -- \textit{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 -- \textit{i.e.}, an infinite-lifetime 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 new route to control energy flow in quantum systems.
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.
The field of Polaritonic Chemistry studies molecules strongly coupled to the light field of optical cavities. The resulting modification of the potential energy landscape has been demonstrated to enable control over the chemical and physical properties of materials and molecular ensembles. This thesis extends the Tavis–Cummings model to describe molecules under strong light–matter coupling, incorporating static dipole moments and dipole self-energy contributions derived from the Pauli–Fierz Hamiltonian. These additional terms are shown to be essential for reproducing cavity-modified molecular dynamics and spectra. Simulations on the nuclear wavefunction propagation of MgH+ molecules demonstrate the impact of these terms, while an effective two-level system model accurately captures the behavior of large ensembles. Beyond single excitations, the thesis also explores the higher excitation manifolds of the Tavis-Cummings model, which reveals that allowing for more than a single excitation makes the reaction of the involved polaritons entropically more favorable. Open-system simulations highlight how the coherence of the system's initial state governs decay pathways and enables long-lived energy storage. Finally, a multilevel vibrational model coupled to a two-mode cavity is introduced, where a Raman scheme enables selective mixing of vibrational states. The simulation results show that continuous pumping can drive molecules into specific vibrational states while suppressing electronic excitation, both for single molecules and small ensembles. Together, these results provide new theoretical insights into the mechanisms by which optical cavities reshape molecular energy landscapes. The results suggest approaches for controlling photonic, electronic, and vibrational dynamics in strongly coupled systems, contributing to the theoretical foundation of polariton chemistry.
Strong coupling between molecular excitations and quantized electromagnetic fields in optical cavities provides a powerful means to control the physical and chemical properties of molecular systems. Here, we study electron transfer (ET) dynamics in cavity-coupled molecules using the numerically exact hierarchical equations of motion (HEOM) method, which captures nonperturbative and non-Markovian effects beyond standard perturbative theories. We identify distinct resonance and collective effects associated with polariton formation and show that the ET rate saturates in the strong-coupling regime, a feature not captured by perturbative approaches. We further extend the cavity-modified ET model by incorporating the nuclear-coordinate dependence of molecular electric dipole moments, which gives rise to a three-body interaction involving molecular electronic and vibrational degrees of freedom and cavity photons. This vibronic polariton formation leads to non-monotonic, oscillatory dependencies of the ET rate on the light-matter coupling strength and cavity frequency, which we attribute to quantum interference among multiple transfer pathways. These findings establish cavity-modified electron transfer as a multichannel quantum process governed by the interplay of electronic, vibrational, and photonic degrees of freedom.
Strong light-matter coupling in optical cavities is being widely explored as a strategy for modifying molecular dynamics and enhancing coherence. At the same time, structured vibrational environments can exhibit non-Markovian memory that promotes information backflow and coherence revival. We investigate the competition between these effects in a vibronic molecular system strongly coupled to a lossy optical cavity. Using hierarchical equations of motion to treat structured vibrational baths, we quantify both system coherence and non-Markovianity via the l1 norm of coherence and the Breuer-Laine-Piilo measure, respectively. We find that cavity coupling enhances coherence in overdamped environments but can suppress memory-assisted coherence in resonant underdamped regimes, even in the absence of significant photon loss. This suppression arises from hybridization-induced modification of system-bath information flow. We demonstrate that cavity coupling does not universally protect coherence but establishes limits governed by the competition between vibrational recurrence time scales and polaritonic hybridization.
We theoretically predict the interaction between polaritonic excitations arising from the coupling of a cavity photon mode with bound to continuum intersubband transitions in a doped quantum well. The resulting exciton bound by photon exchange, recently demonstrated experimentally, exhibits a binding energy that can be continuously tuned by varying the cavity frequency. We show that polariton-polariton interactions, originating from both Coulomb interactions and Pauli blocking, can be dramatically enhanced by reducing the exciton binding energy, thereby increasing the effective Bohr radius along the growth direction. This regime is reminiscent of Rydberg atoms, where weak binding leads to strong quantum interactions. Our predictions indicate that this physics can give rise to giant quantum optical nonlinearities in the mid and far infrared, a spectral region that remains largely unexplored in quantum optics and offers exciting opportunities for both fundamental studies and applications.
Strong light-matter coupling in optical microcavities can transport energy ballistically across an emitter array, but the same coupling buries most of the excitation in a manifold of dark states that grows with system size and traps energy outside the transport channel. We show that the off-diagonal (non-Condon) part of the exciton-phonon coupling opens a one-way escape route from this trap, driving population irreversibly from dark states into the radiative channel. This rate is fixed by a photonic-weight conservation law rather than by dark-bright overlap which evacuates the dark manifold at a rate independent of system size. The mechanism contributes to transport with near-complete efficiency with four signatures being single exponential dark state decay, a size scaling efficiency gap, distinct temperature behavior, and a resonance in the escape rate at vibrational bath modes. Beyond polariton transport, it recasts dark states from a parasitic loss channel into an engineered dissipative resource, with implications for light harvesting and dissipation based quantum control.