The role of structural and dynamical disorder in semiconductors is a topic of fundamental relevance because of its contribution to the spectral line shape of the photoluminescence, and it plays a major role in ruling the carrier transport properties at the band edge. In this regard, a class of semiconductors, i.e., halide perovskites, deeply investigated in the last decade, shows a peculiar degree of disorder, which has only been recently under investigation. The interest to study disorder in halide perovskites is related to the large set of innovative applications of this class of materials, spanning from energy harvesting to high brilliance incoherent and coherent light emitters. In this perspective, we show that quantitative information on the disorder in halide perovskites can be extracted by deep analysis of the photoluminescence in different experimental conditions. Our study, conducted on a large set of samples of a metal halide perovskite, CsPbBr3, prepared with various synthesis/deposition methods, clarifies the relative weight of the static and dynamic contributions. A comparison with theoretical predictions is provided, gaining insights into the exciton/carrier–phonon interaction in metal halide perovskites.
Owing to their ability to generate non‐classical light states, quantum dots (QDs) are very promising candidates for the large‐scale implementation of quantum information technologies. However, the high photon collection efficiency demanded by these technologies may be impossible to reach for “standalone” semiconductor QDs, embedded in a high‐refractive index medium. In this work a novel laser writing technique is presented, enabling the direct fabrication of a QD self‐aligned—with a precision of ±30 nm—to a dielectric microsphere. The presence of the microsphere leads to an enhancement of the QD luminescence collection by a factor 7.3 ± 0.7 when an objective with 0.7 numerical aperture is employed. This technique exploits the possibility of breaking the N−H bonds in GaAs1−xNx:H by a laser light, obtaining a lower‐bandgap material, GaAs1−xNx. The microsphere, deposited on top of a GaAs1−xNx:H/GaAs quantum well, is used to generate a photonic nanojet, which removes hydrogen exactly below the microsphere, creating a GaAs1−xNx QD at a predefined distance from the sample surface. Second‐order autocorrelation measurements confirm the ability of the QDs obtained with this technique to emit single photons.
Caesium lead halide perovskites were recently demonstrated to be a relevant class of semiconductors for photonics and optoelectronics. Unlike CsPbBr3 and CsPbI3, the realization of high-quality thin films of CsPbCl3, particularly interesting for highly efficient white LEDs when coupled to converting phosphors, is still a very demanding task. In this work we report the first successful deposition of nanocrystalline CsPbCl3 thin films (70–150 nm) by radio frequency magnetron sputtering on large-area substrates. We present a detailed investigation of the optical properties by high resolution photoluminescence (PL) spectroscopy, resolved in time and space in the range 10–300 K, providing quantitative information concerning carriers and excitons recombination dynamics. The PL is characterized by a limited inhomogeneous broadening (~15 meV at 10 K) and its origin is discussed from detailed analysis with investigations at the micro-scale. The samples, obtained without any post-growth treatment, show a homogeneous PL emission in spectrum and intensity on large sample areas (several cm2). Temperature dependent and time-resolved PL spectra elucidate the role of carrier trapping in determining the PL quenching up to room temperature. Our results open the route for the realization of large-area inorganic halide perovskite films for photonic and optoelectronic devices.
In recent years, dielectric microspheres have been used in conjunction with optical microscopes to beat the diffraction limit and to obtain super-resolution imaging. We investigate, for the first time, the use of microspheres on quantum dots (QDs) to enhance the light coupling efficiency. We demonstrate the enhancement of the QD luminescence collection in terms of extraction and directionality, as well as the enhancement of spatial resolution. In particular, we find that a dielectric microsphere, placed on top of an epitaxial QD, increases the collected radiant energy by about a factor of 42, when a low numerical aperture objective is used. Moreover, if two or more QDs are present below the microsphere, the modification of the far field emission pattern allows selective collection of the luminescence from a single QD by simply changing the collection angle. Dielectric microspheres present a simple and efficient tool to improve the QD spectroscopy, and potentially QD based devices.
Inorganic metal halide perovskites are relevant semiconductors for optoelectronic devices. The successful deposition of thin films of CsPbBr3 and CsPbCl3 has recently been obtained by Radio-Frequency magnetron sputtering. In this work we compare the morphological, structural and optical characteristics of the two materials obtained with this deposition technique. A detailed photoluminescence (PL) spectroscopy study of the as-grown samples was conducted at the macro and micro scale in a wide temperature range (10-300 K) to fully characterize the PL on sample areas of square centimeters, to assess the origin of the inhomogeneous broadening and to quantify the PL quantum yield quenching. Our results prove that this technique allows for the realization of high quality nanometric films with controlled thickness of relevance for optoelectronic applications.
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