Superfluorescence from lead halide perovskite quantum dot superlattices

Abstract

An ensemble of emitters can behave very differently from its individual constituents when they interact coherently via a common light field. After excitation of such an ensemble, collective coupling can give rise to a many-body quantum phenomenon that results in short, intense bursts of light-so-called superfluorescence 1. Because this phenomenon requires a fine balance of interactions between the emitters and their decoupling from the environment, together with close identity of the individual emitters, superfluorescence has thus far been observed only in a limited number of systems, such as certain atomic and molecular gases and a few solid-state systems 2-7. The generation of superfluorescent light in colloidal nanocrystals (which are bright photonic sources practically suited for optoelectronics 8,9) has been precluded by inhomogeneous emission broadening, low oscillator strength, and fast exciton dephasing. Here we show that caesium lead halide (CsPbX 3 , X = Cl, Br) perovskite nanocrystals 10-13 that are self-organized into highly ordered three-dimensional superlattices exhibit key signatures of superfluorescence. These are dynamically red-shifted emission with more than 20-fold accelerated radiative decay, extension of the first-order coherence time by more than a factor of four, photon bunching, and delayed emission pulses with Burnham-Chiao ringing behaviour 14 at high excitation density. These mesoscopically extended coherent states could be used to boost the performance of opto-electronic devices 15 and enable entangled multi-photon quantum light sources 16,17. Spontaneous emission of photons-such as happens in the process of fluorescence that is commonly used in displays and lighting-occurs because of coupling between excited two-level systems (TLS) and the vacuum modes of the electromagnetic field, effectively stimulated by its zero-point fluctuations. In 1954, Dicke predicted 18 that an ensemble of N identical TLS confined in a volume smaller than about λ 3 (where λ is the corresponding emission wavelength of the TLS) can exhibit coherent and cooperative spontaneous emission. This so-called superradiant emission results from the coherent coupling between individual TLS through the common vacuum modes, effectively leading to a single giant emitting dipole from all participating TLS. Superradiant emission has been observed in distinctly different physical systems, such as molecular aggregates and crystals 19 , nitrogen vacancy centres in diamond 20 and epitaxially grown quantum dots 21 (QDs). In the case when the excited TLS are initially fully uncorrelated, the coherence can be established only through spontaneously triggered correlations due to quantum fluctuations rather than by coherent excitation. When this occurs, a so-called superfluorescence (SF) pulse is emitted 1 (Fig. 1, illustrated for the present study). Both superradiant emission and coherent SF bursts are characterized by an accelerated radiative decay time τ SF ∝ τ SE /N, where the exponential decay time τ SE of spontaneous emission fr...

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