Exciton-polaritons are light-matter hybrid quasi-particles that have emerged as a flexible platform for developing quantum technologies and engineering material properties. However, the fundamental mechanistic principles that govern their dynamics and relaxation remain elusive. In this work, we provide the microscopic mechanistic understanding of the exciton-polariton relaxation process that follows from an excitation in the upper polariton. Using both mixed quantum-classical simulations and analytical analysis, we reveal that phonon-induced upper-to-lower polariton relaxation proceeds via two steps: the first step is a vertical inter-band transition from the upper to the lower polariton, which is followed by a second step that is a phonon-induced Fröhlich scattering within the lower polariton. We find that in materials of finite thickness (which include filled cavities), phonon-induced polaritonic intraband Fröhlich scattering is significantly suppressed. We show that the microscopic origin of this suppression is phonon-fluctuations synchronization (or self-averaging) due to the polaritonic spatial delocalization in the quantization direction. Finally, we show that the same phonon fluctuation-synchronization effect plays a central role across polaritonic relaxation pathways, and we derive simple analytical expressions that relate a material's finite thickness to the corresponding relaxation rate constants.
Exciton-polaritons are light-matter hybrid quasi-particles that have emerged as a flexible platform for developing quantum technologies and engineering material properties. However, the fundamental mechanistic principles that govern their dynamics and relaxation remain elusive. In this work, we provide the microscopic mechanistic understanding of the exciton-polariton relaxation process that follows from an excitation in the upper polariton. Using both mixed quantum-classical simulations and analytical analysis, we reveal that phonon-induced upper-to-lower polariton relaxation proceeds via two steps: the first step is a vertical inter-band transition from the upper to the lower polariton, which is followed by a second step that is a phonon-induced Fröhlich scattering within the lower polariton. We find that in materials of finite thickness (which include filled cavities), phonon-induced polaritonic intraband Fröhlich scattering is significantly suppressed. We show that the microscopic origin of this suppression is phonon-fluctuations synchronization (or self-averaging) due to the polaritonic spatial delocalization in the quantization direction. Finally, we show that the same phonon fluctuation-synchronization effect plays a central role across polaritonic relaxation pathways, and we derive simple analytical expressions that relate a material's finite thickness to the corresponding relaxation rate constants.
Exciton-polaritons, hybrid light-matter quasiparticles formed when a material interacts with a confined electric field, have experimentally been shown to exhibit mesoscale coherent quantum propagation that remains robust at room temperature. However, an accurate and direct quantum dynamical simulation of this phenomenon that does not resort to semi-classical approximations is prohibitively expensive computationally, limiting the microscopic understanding of the rich dynamical interplay among phonons, photons, and electrons under collective light-matter coupling. To address this fundamental challenge, we develop a non-Markovian master equation approach which enables the fully quantum mechanical simulation of non-equilibrium exciton-polariton dynamics and captures phonon-induced decoherence and dissipation beyond the conventional Markovian limit. To carry out this task, a procedure is developed in which the wave vector space is coarse-grained and each diagonal element of the density matrix is evolved in parallel. To demonstrate the utility of this approach, we simulate exciton-polariton transport in TIPS-pentacene. We find that our approach reasonably captures the experimentally observed renormalization of the polariton group velocity, which originates from the phonon-induced non-Markovian Lamb shift. We further show that this renormalization cannot be reproduced within conventional Markovian theories.
A full quantum theory beyond the mean-field regime is developed for an exciton-polariton condensate, for a complete understanding of quantum fluctuations. We find an analytical solution for the polariton density matrix, showing the nonlinearity causing fast relaxation correlated with the pump so as to yield the quantum condensation above threshold. Increasing the pump intensity, a nonequilibrium phase transition towards the condensation of the lower polaritons emerges, with a statistics transiting from a thermal, through a super-Poissonian, and towards a nonclassical distribution; the latter two possess off-diagonal long-range order but the last one is beyond. The results signify the role of dark states for polariton fluctuations, and lead to a nonclassical counting statistics of emitted photons, which elaborates the role of the key parameters, e.g., pump, detuning, and temperature.
A full quantum theory beyond the mean-field regime is developed for an exciton polariton condensate, to gain a complete understanding of quantum fluctuations. We find analytical solution for the polariton density matrix, showing the polariton nonlinearity causing fast relaxation correlated with the pump so as to yield the condensation at threshold. Increasing the pump intensity, a nonequilibrium phase transition towards the condensation of lower polaritons emerges, with a statistics transiting from a thermal, through a super-Poissonian and to a nonclassical distribution beyond the understanding at the level of off-diagonal long-range order. The results signify the role of dark states for polariton fluctuations, and lead to a nonclassical counting statistics of emitted photons, which elaborates the role of the key parameters, e.g., pump, detuning and temperature.
Quantum-well exciton superradiance and exciton cavity polarization formation both require a substantial spatial coherence area in order to become the dominant exciton field interaction. In both interaction processes the quantum-well (in-plane) momentum is conserved. Momentum scattering, which is due, e.g., to interaction with a phonon reservoir, quickly localizes an initially delocalized exciton and randomizes the excitation momentum. We take a close look at how momentum scattering influences measurements of excitonic superradiance and of exciton cavity polariton splitting. An important conclusion is that, in general, measurements of the emitted light do not correspond to the evolution of the system as a whole. Therefore, e.g., the measured decay rates do not correspond to the true decay rate of the system.
Subwavelength arrays of atoms trapped in optical lattices or tweezers are inherently susceptible to deformations: Optomechanical forces displace atoms within their trapping potential and produce lattice distortions, which in turn modify the optical response of the array. We show that this optomechanical coupling hybridizes collective atomic excitations (polaritons) with phonons, forming polaron-polaritons -- the fundamental quasiparticles governing light-matter interactions in arrays of trapped atoms. Using analytical polaron theory and numerical simulations, we find that: (1) phonons can strongly enhance the decay of subradiant states, but also enable their efficient excitation; (2) transport of dark excitations remains remarkably robust even at low trap frequencies, except when a polariton can resonantly scatter phonons; and (3) motion reduces the reflectivity of a two-dimensional atomic mirror; by identifying design principles that mitigate this degradation, we recover reflectivity above 99% under realistic conditions. Our findings lay the foundation for analyzing motional effects in key applications and suggest new ways to harness them in state-of-the-art experiments.
Self-hybridized exciton polaritons in layered semiconductors emerge from the hybridization of excitonic resonances with confined photonic modes in films and provide a versatile platform for controlling light--matter interactions at the nanoscale. Yet, the nature of exciton--photon interactions and the collective and synchronous strong coupling of multiple excitons to the same photonic mode remain largely unexplored. Here, we use complementary momentum-resolved photoluminescence and cathodoluminescence spectroscopy to compare self-hybridized exciton polaritons in Ruddlesden--Popper perovskite flakes under optical and electron-beam excitation. We find that cathodoluminescence exhibits remarkably larger polaritonic level repulsion than photoluminescence, revealing an enhanced effective coupling strength under electron-beam excitation. We attribute this enhancement to the collective coherent excitation of multiple excitons by fast electrons, which couple to the same photonic mode and increase the interaction strength according to a gN=g1N scaling, with an effective number of up to N≈23 coherently coupled excitonic oscillators. By reducing the electron kinetic energy, we further uncover a crossover to a partially incoherent excitation regime in which higher-order Fabry--Pérot exciton-polariton resonances disappear, leaving only the lowest polariton branches while coherent transition radiation persists. This transition arises because low-energy electrons excite excitons over extended spatial volumes, washing out the phase coherence required to sustain collective coupling and form polaritonic resonances. Our work shows that electron beams can actively modify collective light--matter coupling in layered semiconductors and establishes cathodoluminescence as a route to access excitation regimes beyond all-optical excitation schemes.