An ensemble of emitters can behave differently from its individual constituents when it interacts coherently via common vacuum light modes. One example of a many-body collective coupling is so-called superfluorescent coupling, where the excited emitters are initially fully uncorrelated and coherence is established through spontaneously triggered correlations from quantum fluctuations. Subsequently, the coupled emitters emit a strong superfluorescent pulse. Since this phenomenon requires low inhomogeneity and a fine balance of interactions between the resonant emitters and their decoupling from the environment, superfluorescence has only been observed in a limited number of systems, such as certain atomic and molecular gases and a few solid-state systems.
Here, we investigate densely packed arrays of fully inorganic cesium lead halide perovskite quantum dots, known as superlattices. These quantum dots obtain exceptional optical properties such as an lowest bright triplet state with an ultrafast radiative decay that is 1000x faster compared to other conventional nanocrystals at cryogenic temperatures. The resulting high oscillator strength and a long exciton dephasing time are key ingredients for strong light-matter interactions. In a solvent-drying-induced assembly process, perovskite quantum dots form densely packed cuboidal superlattices that show key signatures of superfluorescence. We observe a more than twenty-fold accelerated radiative decay with dynamically red-shifted emission, extension of the first-order coherence time by more than a factor of four, photon bunching and an intensity-dependent time delay after which the photon burst is emitted. Also, at high excitation density, the superfluorescent decay exhibits a Burnham-Chiao ringing behavior, reflecting the coherent Rabi-type interaction.
Lead-halide perovskites are currently the highest-performing solution-processable semiconductors for solar energy conversion, with record efficiencies rapidly approaching that of the Shockley-Queisser limit for single-junction solar cells. Further progress in the development of lead-halide perovskite solar cells must overcome this limit, which largely stems from the ultrafast relaxation of high-energy hot carriers above the bandedge. In this contribution, we use a highly-specialized pump-push-probe technique to unravel the key parameters which control hot carrier cooling in bulk and nanocrystal (NC) lead bromide perovskites with different material composition, NC diameter and surface treatment. All samples exhibit slower cooling for higher hot carrier densities, which we assign to a phonon bottleneck mechanism. By comparing this density-dependent cooling behavior in the different samples, we find that the weak quantum confinement of electronic states and the surface defects in the NCs play no observable role in the hot carrier relaxation. Meanwhile, in accordance with our previous observations for bulk perovskites, we show that the cation plays a critical role towards carrier cooling in the perovskite NCs, as evidenced by the faster overall cooling in the hybrid FAPbBr3 NCs with respect to the all-inorganic CsPbBr3 NCs. These observations highlight the crucial role of the cations toward the phononic properties of lead-halide perovskites, and further point towards the defect tolerance of these emerging solution-processed semiconductors.
Colloidal nanocrystal layers deposited onto the enclosure of InGaN light emitting diodes are demonstrated to operate as
nano-phosphors for color conversion with high color stability. Dependent on the choice of the nanocrystal materials,
either CdSe/ZnS or PbS nanocrystals are applied, the diode emission at 470 nm is converted to the red or to infrared
light, with similar quantum efficiencies. The color conversion is further improved by dielectric mirrors with high
reflectivity at the emission band of the nanocrystals, resulting in an almost doubling of the nanocrystal light extraction from the devices, which increases the nanocrystal device efficiency up to 19.1%.