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Advanced Photonics

Perturbation-driven echo-like superfluorescence in perovskite superlattices

Qiangqiang Wang, Jiqing Tan, Jie Qi, Hongxing Dong, Yong‐Sheng Hu, Chun Lan Zhou, Saifeng Zhang, Yichi Zhong, Shuang Liang, Long Zhang, Wei Xie, Hongxing Xu

Published Oct 6, 2023• 13 citations
Publisher

Abstract

The collective response of macroscopic quantum states under perturbation is widely used to study quantum correlations and cooperative properties, such as defect-induced quantum vortices in Bose–Einstein condensates and the non-destructive scattering of impurities in superfluids. Superfluorescence (SF), as a collective effect rooted in dipole–dipole cooperation through virtual photon exchange, leads to the macroscopic dipole moment (MDM) in high-density dipole ensembles. However, the perturbation response of the MDM in SF systems remains unknown. Echo-like behavior is observed in a cooperative exciton ensemble under a controllable perturbation, corresponding to an initial collapse followed by a revival of the MDM. Such a dynamic response could refer to a phase transition between the macroscopic coherence regime and the incoherent classical state on a time scale of 10 ps. The echo-like behavior is absent above 100 K due to the instability of MDM in a strongly dephased exciton ensemble. Experimentally, the MDM response to perturbations is shown to be controlled by the amplitude and injection time of the perturbations.

DOI
10.1117/1.ap.5.5.055001

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The collective response of macroscopic quantum states under perturbation is widely used to study quantum correlations and cooperative properties, such as defect-induced quantum vortices in Bose–Einstein condensates and the non-destructive scattering of impurities in superfluids. Superfluorescence (SF), as a collective effect rooted in dipole–dipole cooperation through virtual photon exchange, leads to the macroscopic dipole moment (MDM) in high-density dipole ensembles. However, the perturbation response of the MDM in SF systems remains unknown. Echo-like behavior is observed in a cooperative exciton ensemble under a controllable perturbation, corresponding to an initial collapse followed by a revival of the MDM. Such a dynamic response could refer to a phase transition between the macroscopic coherence regime and the incoherent classical state on a time scale of 10 ps. The echo-like behavior is absent above 100 K due to the instability of MDM in a strongly dephased exciton ensemble. Experimentally, the MDM response to perturbations is shown to be controlled by the amplitude and injection time of the perturbations.
Superfluorescence is a quantum optical phenomenon in which an initially excited ensemble of incoherent dipoles first acquire macroscopic coherence and then collectively recombine and radiate a burst of photons. This process is a symmetry breaking macroscopic quantum phase transition similar to superconductivity and Bose-Einstein condensation. Since quantum coherence is extremely fragile at high temperatures, similar to other macroscopic quantum phase transitions, superfluorescence has been almost always observed at cryogenic temperatures. In this presentation I will first present our results on room temperature superfluorescence in lead-halide perovskites and then present the mechanism that enables this exotic quantum phase transition at room temperature.
Superfluorescence (SF) is the emission from a dense coherent system in population inversion formed from an initially incoherent ensemble. This is characterized by an induction time (${\ensuremath{\tau}}_{\mathrm{D}}$) for the spontaneous development of the macroscopic quantum coherence. Here we report detailed observation of SF on an ultrafast timescale from a quantum ensemble of coherent excitons in highly excited intrinsic-bulk ZnTe single crystal at 5 K, showing a characteristic ${\ensuremath{\tau}}_{\mathrm{D}}$ from 40 ps to 10 ps, quantum noise and fluctuations, and quantum beating and ringing. From this clear observation of SF from a spontaneous coherence of excitons bound to impurities and defect states, we infer that this is indicative of the formation of a spontaneous Bose-Einstein condensation (BEC) of excitons on an ultrafast timescale. The population density and dephasing time (T2{T}_{2}T2​ or T2∗{T}_{2}^{*}T2∗​) of exciton are two controlling factors in the generation of SF from the BEC.
Metal halide perovskites (MHPs) have emerged as promising platforms for cooperative quantum emission. Superfluorescence is particularly intriguing because it arises from spontaneous synchronization of initially incoherent emitters into a macroscopic quantum state, producing delayed, intense, ultrafast bursts of coherent light. While superfluorescence has been demonstrated in perovskite nanocrystal superlattices and thin films, the mechanisms that enable its emergence at elevated temperatures, and the boundaries that separate cooperative from non-cooperative emission regimes, remain insufficiently understood.[1],[2] Addressing these knowledge gaps is essential for advancing superfluorescence toward quantum photonic applications.[3] In this talk, I present how our work tackles the challenges of identifying, and controlling superfluorescence in quasi-2D perovskite thin films. We demonstrate clear evidence to distinguish superfluorescence from amplified spontaneous emission and spontaneous emission. A comprehensive experimental phase map is constructed to reveal when and how macroscopic coherence forms, how it decays, and under what conditions it transitions into non-cooperative regimes.[4] Using quasi-2D PBA:CsPbBr3 thin films, we demonstrate superfluorescence with the lowest threshold fluence reported at 78 K in metal halide perovskites. Temperature and fluence dependent steady state and ultrafast spectroscopies resolve cooperative emission from 78 to 180 K, including a sharper coupled emission band, a delayed emission peak, ultrafast radiative lifetimes, quadratic like intensity scaling, and Burnham-Chiao ringing. We also map a phase diagram that delineates spontaneous emission, superfluorescence, and amplified spontaneous emission, and we observe deviations from ideal superfluorescence at high fluences and elevated temperatures, reflecting competing many-body and dephasing processes.[4] To interpret these observations, we introduce the ab initio quantum model Superfluorescence Non-Approximating Integrating Large Solver (SNAILS), which tracks emission density, inter emitter correlations, excited state populations, and trace distance under varying pumping and dephasing conditions.[4] Simulations reproduce delayed cooperative bursts when dephasing is weak and show rapid suppression of correlations and loss of delay when dephasing is stronger. Trace distance dynamics identify synchronization plateaus during cooperative emission and prolonged plateaus linked to subradiant or dark states under high dephasing, establishing a unified framework for cooperative emission and its breakdown in perovskite thin films. Overall, this work clarifies the optical and dynamical conditions required for macroscopic coherence in perovskites. The combined insights from phase mapping, ultrafast spectroscopy, and quantum modeling highlight strategies for lowering threshold fluence, mitigating dephasing, and extending superfluorescence toward higher temperatures.
Superfluorescence, the cooperative burst of spontaneous emission from an ensemble of dipoles, arises when microscopic oscillators spontaneously synchronize their phases. Here we show that this process can be reversed in time within quantum materials. Coherent multidimensional spectroscopy of halide perovskite quantum dots reveals a delayed cooperative absorption burst, the mirror image of superfluorescent emission, driven by transient polaron fields that phase-lock unit-cell dipoles within 100 fs. The effect scales systematically with quantum-dot size and halide composition, reaching near-unity coherence fidelity even at 300 K. A microscopic exciton-polaron model reproduces the buildup and decay of the coherent state, identifying lattice polarons as the mediators of synchronization. These results demonstrate that many-body temporal coherence can self-organize and persist at room temperature, opening routes toward engineered collective optical states and superabsorbing quantum devices.
Macroscopic coherence of Bose condensates is a fundamental and practical phenomenon in many-body systems, such as the long-range correlation of exciton-polariton condensates with a dipole density typically below the exciton Mott-transition limit. Here we extend the macroscopic coherence of electron-hole-photon interacting systems to a new region in the phase diagram-the high-density plasma region, where long-range correlation is generally assumed to be broken due to the rapid dephasing. Nonetheless, a cooperative state of electron-hole plasma does emerge through the sharing of the superfluorescence field in an optical microcavity. In addition to the in situ coherence of e-h plasma, a long-range correlation is formed between two 8-μm-spaced plasma ensembles even at room temperature. Quantized and self-modulated correlation modes are generated for e-h ensembles in the plasma region. By controlling the distance between the two ensembles, multiple coupling regimes are revealed, from strong correlation to perturbative phase correlation and finally to an incoherent classical case, which has potential implications for tunable and high-temperature-compatible quantum devices.