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.
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.
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.
Successful deposition of CsPbX3 (X = Br, Cl) thin films (50-500 nm) on several kind of substrates has been realized by Radio-Frequency Magnetron Sputtering. The technique allows for high homogeneity of the samples on large areas (several cm2) not only in terms of morphology but also referring to the optical properties. In particular, high resolution (in space, spectrum and time) photoluminescence studies in a wide temperature range (10-300 K) reveal that the low inhomogeneous broadening comes from a submicron size disorder while no significant contribution arises from a micrometric or even larger disorder. Given the relevance of inorganic halide perovskites for innovative optoelectronic devices, our results prove the scalability of this technique. Moreover, the successful deposition on several different substrates open the route for an easy integration in multi-layered structures.
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