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Optics and Spectroscopy

Effect of vibrations on the absorption spectrum of a single-mode vibronic system interacting with a quasiresonant light field

Alexei D. Kiselev

Published Jan 1, 1991• 0 citations
OpenAlex

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Possibility of coherent excitation of molecular vibrations in a resonance light field

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The problem of resonant interaction between an electromagnetic radiation field and a vibronic system, such as a molecule or a localized electronphonon system, is considered. The vibronic coupling is assumed to result from displaced and distorted potential energy surfaces for the vibrational motion in the electronic quantum states involved in the resonant interaction with the radiation field. Furthermore, the vibrational energy relaxation is taken into account without assumptions about Markovian-type relaxation. In order to study correlation properties of higher than second order in the electric field strength of the light emitted a method of calculation of the expectation value of an arbitrary product combination of effective time evolution operators of the vibronic system is developed. The calculations are performed by utilizing Feynman's disentangling and operator ordering techniques and yield closed solutions in the low-temperature limit. The theory is used for studying the intensity and the normally ordered intensity correlation function of the resonance fluorescence light from a two-atom molecule excited by a relatively weak laser field, which undergoes phase fluctuations. It is shown that the vibronic coupling can give rise to an anticorrelation effect which is substantially stronger than in the case of resonance fluorescence from an atom. For the case of small vibrational damping a general formula which directly connects the asymptotic long-time behaviour of the normalized intensity correlation function with the vibrational relaxation in the molecule is deduced. It should be convenient for the determination of very small vibrational decay rates.

Physica Scripta•Sep 1, 1983•5 citations

Optical Manifestations of Energy and Phase Relaxation in Vibronic Systems

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Using the model of displaced potential energy surfaces, we studied the spectrum of the resonance fluorescence light from vibronic systems. In this model, equal vibrational frequencies in the two electronic quantum states allow many vibronic transitions to be in resonance with a monochromatic driving laser field tuned to the electronic transition frequency. Level splittings in the strong-field case give rise to a multiple-line spectrum of the scattered light. In particular, the Rayleigh component consists of a superimposed series of triplets, whereas the Raman part is built up by superimposed quadruplets.

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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.

quant-pharXiv:2604.06142•Apr 8, 2026•0 citations

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
The problem of resonant interaction between an electromagnetic radiation field and a vibronic system, such as a molecule or a localized electronphonon system, is considered. The vibronic coupling is assumed to result from displaced and distorted potential energy surfaces for the vibrational motion in the electronic quantum states involved in the resonant interaction with the radiation field. Furthermore, the vibrational energy relaxation is taken into account without assumptions about Markovian-type relaxation. In order to study correlation properties of higher than second order in the electric field strength of the light emitted a method of calculation of the expectation value of an arbitrary product combination of effective time evolution operators of the vibronic system is developed. The calculations are performed by utilizing Feynman's disentangling and operator ordering techniques and yield closed solutions in the low-temperature limit. The theory is used for studying the intensity and the normally ordered intensity correlation function of the resonance fluorescence light from a two-atom molecule excited by a relatively weak laser field, which undergoes phase fluctuations. It is shown that the vibronic coupling can give rise to an anticorrelation effect which is substantially stronger than in the case of resonance fluorescence from an atom. For the case of small vibrational damping a general formula which directly connects the asymptotic long-time behaviour of the normalized intensity correlation function with the vibrational relaxation in the molecule is deduced. It should be convenient for the determination of very small vibrational decay rates.
Using the model of displaced potential energy surfaces, we studied the spectrum of the resonance fluorescence light from vibronic systems. In this model, equal vibrational frequencies in the two electronic quantum states allow many vibronic transitions to be in resonance with a monochromatic driving laser field tuned to the electronic transition frequency. Level splittings in the strong-field case give rise to a multiple-line spectrum of the scattered light. In particular, the Rayleigh component consists of a superimposed series of triplets, whereas the Raman part is built up by superimposed quadruplets.
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.