Mixed-halide perovskites represent a particularly relevant case within the family of leadhalide perovskites. Beyond their technological relevance for a variety of optoelectronic devices, photo-induced structural changes characteristic of this type of materials lead to extreme photophysical changes that are currently the subject of an intense debate. Herein
The family of antiferromagnetic layered metal hexathiohypo diphosphates, M2P2S6 represents a versatile class of materials, particularly interesting for fundamental studies on magnetic properties in low dimensional structures, and yet exhibiting great potential for a broad variety of applications including catalysis, energy storage and conversion, and spintronics. In this work, three representatives of this family of 2D materials (M = Fe, Ni, and Mn) are exfoliated in the liquid phase under inert conditions and the nanosheet’s properties are studied in detail for different sizes of all three compounds. Centrifugation-based size selection is performed for this purpose. The exfoliability and structural integrity of the nanosheets is studied by statistical AFM and TEM measurements. Further, we report size and thickness dependent optical properties and spectroscopic metrics for the average material dimensions in dispersion, as well as the nanomaterials’ magnetic response using a combination of cryo-Raman and SQUID measurements. Finally, the material stability is studied semi-quantitatively, using time and temperature dependent extinction and absorbance spectroscopy, enabling the determination of the materials’ half-life, portion of reacted substance and the macroscopic activation energy for the degradation.
The peculiar defect
chemistry of hybrid organic–inorganic
lead halide perovskites is believed to be partially responsible for
the outstanding performance of this solution-processed material in
optoelectronic devices. While most effort has been put on the management
of halide defects (the ones presenting the highest mobility) for CH3NH3PbI3, its bromide counterpart has
not been so widely studied. Although the former is the material of
choice for photovoltaics, the latter is present in most light-emitting
applications. Here, we report how the exposure of CH3NH3PbBr3 single crystals to a bromine atmosphere strongly
affects its emission properties. Such improvement takes place in the
absence of apparent signs of degradation and remains for tens of hours.
We propose an explanation based on the defect structure for this material
where bromine-related defects can act as deep or shallow traps. These
results are of relevance for a material expected to be present in
a new generation of solution-processed light-emitting devices.
The growth of lead halide perovskites within metal-oxide nanoporous films has been recently considered as a means to obtain chemically and photo-stable ligand-free high quality nanocrystals. The growth process, governed by the reactions taking place in nano-reactors dictated by the matrix pore size, has not been explored so far. In this work we use photoluminescence as a tool to monitor the growth of perovskite nanocrystals within the void network of an optically transparent matrix. We consider the effect of different external factors, such as temperature, light illumination or precursor concentration, on the growth dynamics, and discuss a possible formation mechanism of the confined perovskite nanocrystals. Based on this analysis, guidelines that could serve to improve the fabrication and optoelectronic quality of this type of nanocrystals are also proposed.
The disentanglement of single and many particle properties in 2D semiconductors and their dependencies on high carrier concentration is challenging to experimentally study by pure optical means. We establish an electrolyte gated WS2 monolayer field-effect structure capable of shifting the Fermi level from the valence into the conduction band that is suitable to optically trace exciton binding as well as the single-particle band gap energies in the weakly doped regime. Combined spectroscopic imaging ellipsometry and photoluminescence spectroscopies spanning large n- and p-type doping with charge carrier densities up to 1014 cm−2 enable to study screening phenomena and doping dependent evolution of the rich exciton manifold whose origin is controversially discussed in literature. We show that the two most prominent emission bands in photoluminescence experiments are due to the recombination of spin-forbidden and momentum-forbidden charge neutral excitons activated by phonons. The observed interband transitions are redshifted and drastically weakened under electron or hole doping. This field-effect platform is not only suitable for studying exciton manifold but is also suitable for combined optical and transport measurements on degenerately doped atomically thin quantum materials at cryogenic temperatures.
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