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 superfluorescence¹. 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^2,3,4,5,6,7. 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 (CsPbX₃, X = Cl, Br) perovskite nanocrystals^10,11,12,13 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 behaviour¹⁴ at high excitation density. These mesoscopically extended coherent states could be used to boost the performance of opto-electronic devices¹⁵ and enable entangled multi-photon quantum light sources^16,17.

Fully-inorganic cesium lead halide perovskite nanocrystals (NCs) have shown to exhibit outstanding optical properties such as wide spectral tunability, high quantum yield, high oscillator strength as well as blinking-free single photon emission and low spectral diffusion. Here, we report measurements of the coherent and incoherent exciton dynamics on the 100 fs to 10 ns timescale, determining dephasing and density decay rates in these NCs. The experiments are performed on CsPbBr₂Cl NCs using transient resonant three-pulse four-wave mixing (FWM) in heterodyne detection at temperatures ranging from 5 K to 50 K. We found a low-temperature exciton dephasing time of 24.5±1.0 ps, inferred from the decay of the photon-echo amplitude at 5 K, corresponding to a homogeneous linewidth (FWHM) of 54±5 μeV. Furthermore, oscillations in the photon-echo signal on a picosecond timescale are observed and attributed to coherent coupling of the exciton to a quantized phonon mode with 3.45 meV energy.

Microcavities with embedded optically active materials allow to create exciton–polariton condensates in the strong light–matter interaction regime. These condensates exhibit quantum fluid properties up to room temperature, and, when crystal-like lattices are imprinted in the cavity, they can be used to emulate and study solid-state physics toy models. Here, we demonstrate room temperature polariton condensation in a nano-fabricated two-dimensional Lieb lattice with an organic polymer. We exploit the tunability of our open cavity to selectively condense into the s-, p- and d-lattice band manifolds. Furthermore, we interferometrically measure long-range first-order coherence across the lattice and assess the influence of the disorder in the system. These are key first steps to investigate extended topological polariton systems at ambient conditions.

A common signature of nearly all nanoscale emitters is fluorescence intermittency, which is a rapid switching between “on”-states exhibiting a high photon emission rate and “off”-states with a much lower rate. One consequence of fluorescence intermittency occurring on time scales longer than the exciton decay time is the so-called delayed photon emission, manifested by a long radiative decay component. Besides their dominant fast radiative decay, fully inorganic cesium lead halide perovskite quantum dots exhibit a long fluorescence decay component at cryogenic temperatures that is often attributed to the decay of the dark exciton. Here, we show that its origin is delayed photon emission by investigating temporal variations in fluorescence intensity and concomitant decay times found in single CsPbBr₃ perovskite quantum dots. We attribute the different intensity levels of the intensity trace to a rapid switching between a high-intensity exciton state and an Auger-reduced low-intensity trion state that occurs when the excitation is sufficiently strong. Surprisingly, we observe that the exponent of this power-law-dependent delayed emission is correlated with the emission intensity, which cannot be explained with existing charge carrier trapping models. Our analysis reveals that the long decay component is mainly governed by delayed emission, which is present in both the exciton and trion state. The absence of a fine structure in trions clarifies the vanishing role of the dark exciton state for the long decay component. Our findings are essential for the development of a complete photophysical model that captures all observed features of fluorescence variations in colloidal nanocrystals.