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arXiv:2204.13528

Quantum Fluctuations and Coherence of a Molecular Polariton Condensate

Zhedong Zhang, Shixuan Zhao, Dangyuan Lei

Published Apr 28, 2022• 0 citations
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Abstract

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.

DOI
10.48550/arxiv.2204.13528

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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.
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.
Polariton condensates provide a versatile platform for exploring non-equilibrium phase transitions and collective phenomena in open quantum systems. Near the condensation threshold, these systems are particularly sensitive to fluctuations and instabilities, which can strongly influence the condensate formation. Using optical trapping and homodyne detection, we directly access the photon statistics and second-order correlation function g(2)(0)g^{(2)}(0)g(2)(0) of the condensate. We show that polariton condensation near the threshold is not a purely static transition, but instead undergoes a dynamical regime characterized by stochastic hopping between condensed and non-condensed states. These intermittent dynamics are accompanied by a gradual reduction of g(2)(0)g^{(2)}(0)g(2)(0) towards unity, revealing the progressive build-up of coherence even in the presence of strong temporal fluctuations. Numerical simulations, based on a stochastic Truncated Wigner description of the driven-dissipative polariton field, reproduce these dynamics and capture the essential role of noise and reservoir interactions. This work demonstrates that the observed temporal hopping is an intrinsic feature of polariton condensation, providing a dynamical perspective that goes beyond static descriptions of the condensation phase transition.
In this Letter, we give an analytical quantum description of a nonequilibrium polariton Bose-Einstein condensate (BEC) based on the solution of the master equation for the full polariton density matrix in the limit of fast thermalization. We find the density matrix of a nonequilibrium BEC, that takes into account quantum correlations between all polariton states. We show that the formation of BEC is accompanied by the build-up of cross-correlations between the ground state and the excited states reaching their highest values at the condensation threshold. Despite the nonequilibrium nature of polariton systems, we show the average population of polariton states exhibits the Bose-Einstein distribution with an almost zero effective chemical potential above the condensation threshold similar to an equilibrium BEC. We demonstrate that above threshold the effective temperature of polaritons drops below the reservoir temperature.
We measure the full photon-number distribution emitted from a Bose condensate of microcavity exciton polaritons confined in a micropillar cavity. The statistics are acquired by means of a photon-number-resolving transition edge sensor. We directly observe that the photon-number distribution evolves with the nonresonant optical excitation power from geometric to quasi-Poissonian statistics, which is canonical for a transition from a thermal to a coherent state. Moreover, the photon-number distribution allows one to evaluate the higher-order photon correlations, shedding further light on the coherence formation and phase transition of the polariton condensate. The experimental data are analyzed in terms of thermal-coherent states, which gives direct access to the thermal and coherent fraction from the measured distributions. These results pave the way for a full understanding of the contribution of interactions in light-matter condensates in the coherence buildup at threshold.
Polariton condensates provide a versatile platform for exploring non-equilibrium phase transitions and collective phenomena in open quantum systems. Near the condensation threshold, these systems are particularly sensitive to fluctuations and instabilities, yet how these dynamics govern the initial formation of the condensate remains poorly understood. To address this, we directly access the photon statistics and second-order correlation function g (2) (0) of the condensate by using optical trapping and homodyne detection. We show that polariton condensation near the threshold is not a purely static transition, but instead undergoes a dynamical regime characterized by stochastic hopping between condensed and non-condensed states. These intermittent dynamics are accompanied by a gradual reduction of g (2) (0) toward unity, revealing the progressive build-up of coherence even in the presence of strong temporal fluctuations. Numerical simulations, based on a stochastic truncated Wigner description of the driven-dissipative polariton field, reproduce these dynamics and capture the essential role of noise and reservoir interactions. This work demonstrates that the observed temporal hopping is an intrinsic feature of polariton condensation, challenging traditional static descriptions of phase transitions and offering a framework for controlling noise and coherence in driven-dissipative quantum technologies.
Bose-Einstein condensate of exciton polaritons in a semiconductor microcavity is a macroscopically populated coherent quantum state subject to concurrent pumping and decay. Debates about the fundamental nature of the condensed phase in this open quantum system still persist. Here, we gain a new insight into the spontaneous condensation process by imaging long-lifetime exciton polaritons in a high-quality inorganic microcavity in the single-shot optical excitation regime, without averaging over multiple condensate realisations. In this highly non-stationary regime, a condensate is strongly influenced by the `hot' incoherent reservoir, and reservoir depletion is critical for the transition to the ground energy and momentum state. Condensates formed by more photonic exciton polaritons exhibit dramatic reservoir-induced density filamentation and shot-to-shot fluctuations. In contrast, condensates of more excitonic quasiparticles display smooth density and are second-order coherent. Our observations show that the single-shot measurements offer a unique opportunity to study formation of macroscopic phase coherence during a quantum phase transition in a solid state system.