Metal-halide perovskite semiconductors are of tremendous interest for a variety of applications. Only recently, solar cells based on a representative of this family have been certified with an efficiency in excess of 24%.[1] Aside from their remarkable success in photovoltaics, metal-halide perovskites are also highly promising as light emitters, e.g., in light-emitting diodes (LEDs) or lasers. [2][3][4] LEDs based on the fruit-fly of these compounds, i.e., methylammonium lead iodide (CH 3 NH 3 PbI 3 or MAPbI 3 ), and other related perovskites have been demonstrated with continuously increasing efficiency. [5][6][7] For lasers, there is the vision that perovskites may overcome/avoid the typical limitations and loss mechanisms present in organic gain media, such as triplet-singlet annihilation or absorption due to triplet excitons and
Cesium lead halide perovskites are of interest for light-emitting diodes and lasers. So far, thin-films of CsPbX 3 have typically afforded very low photoluminescence quantum yields (PL-QY < 20%) and amplified spontaneous emission (ASE) only at cryogenic temperatures, as defect related nonradiative recombination dominated at room temperature (RT). There is a current belief that, for efficient light emission from lead halide perovskites at RT, the charge carriers/excitons need to be confined on the nanometer scale, like in CsPbX 3 nanoparticles (NPs).Here, thin films of cesium lead bromide, which show a high PL-QY of 68% and low-threshold ASE at RT, are presented. As-deposited layers are recrystallized by thermal imprint, which results in continuous films (100% coverage of the substrate), composed of large crystals with micrometer lateral extension. Using these layers, the first cesium lead bromide thin-film distributed feedback and vertical cavity surface emitting lasers with ultralow threshold at RT that do not rely on the use of NPs are demonstrated. It is foreseen that these results will have a broader impact beyond perovskite lasers and will advise a revision of the paradigm that efficient light emission from CsPbX 3 perovskites can only be achieved with NPs.
Grain boundary segregation leads to nanoscale chemical variations that can alter a material's performance by orders of magnitude (e.g., embrittlement). To understand this phenomenon, a large number of grain boundaries must be characterized in terms of both their five crystallographic interface parameters and their atomic-scale chemical composition. We demonstrate how this can be achieved using an approach that combines the accuracy of structural characterization in transmission electron microscopy with the 3D chemical sensitivity of atom probe tomography. We find a linear trend between carbon segregation and the misorientation angle ω for low-angle grain boundaries in ferrite, which indicates that ω is the most influential crystallographic parameter in this regime. However, there are significant deviations from this linear trend indicating an additional strong influence of other crystallographic parameters (grain boundary plane, rotation axis). For high-angle grain boundaries, no general trend between carbon excess and ω is observed; i.e., the grain boundary plane and rotation axis have an even higher influence on the segregation behavior in this regime. Slight deviations from special grain boundary configurations are shown to lead to unexpectedly high levels of segregation.
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