Mixing molecular cations in hybrid lead halide perovskites is a highly effective approach to enhance the stability and performance of optoelectronic devices based on these compounds. In this work, we prepare and study novel mixed 3D methylammonium (MA)−ethylammonium (EA) MA 1−x EA x PbI 3 (x < 0.4) hybrid perovskites. We use a suite of different techniques to determine the structural phase diagram, cation dynamics, and photoluminescence properties of these compounds. Upon introduction of EA, we observe a gradual lowering of the phase-transition temperatures, indicating stabilization of the cubic phase. For mixing levels higher than 30%, we obtain a complete suppression of the low-temperature phase transition and formation of a new tetragonal phase with a different symmetry. We use broad-band dielectric spectroscopy to study the dielectric response of the mixed compounds in an extensive frequency range, which allows us to distinguish and characterize three distinct dipolar relaxation processes related to the molecular cation dynamics. We observe that mixing increases the rotation barrier of the MA cations and tunes the dielectric permittivity values. For the highest mixing levels, we observe the signatures of the dipolar glass phase formation. Our findings are supported by density functional theory calculations. Our photoluminescence measurements reveal a small change of the band gap upon mixing, indicating the suitability of these compounds for optoelectronic applications.
Spatial changes of properties of Gd3Ga5O12 (GGG) single crystals caused by diffusion of cobalt ions during high-temperature annealing (1200 • C, 24 h) in Co3O4 powder are investigated. The registration of these changes was carried out by optical spectrophotometry, microscopy and micro-Raman scattering methods. Changes in structure of near-surface layers of the crystal were investigated by X-ray diffraction technique. It was shown that the additional absorption induced by annealing is related to intra-center optical transitions in Co 2+ ions, which occupy tetrahedral positions in the garnet structure at the distances of 250-500 µm from the crystal surface. The dependence of induced absorption with depth has got a non-monotonous character with a maximum at 400 µm. A comparison of the results obtained by different methods allows to suppose that the thermal treatment of GGG in the presence of cobalt ions leads to formation of the structurally and chemically non-uniform layer with a width about 500 µm.
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