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.

Photonic nanostructures are created in organo-metal halide perovskites by thermal nanoimprint lithography at a temperature of 100 °C. The imprinted layers are significantly smoothened compared to the initially rough, polycrystalline layers and the impact of surface defects is substantially mitigated upon imprint. As a case study, 2D photonic crystals are shown to afford lasing with ultralow lasing thresholds at room temperature.

Thermal management in devices like solar cells, light-emitting diodes, and lasers based on hybrid halide perovskite thin films is expected to be of paramount importance for optimal performance and reliability. As of yet, experimental data of thermal properties of non-iodine-based hybrid halide perovskites is very scarce. Here the thermal conductivity of methylammonium lead halide perovskite (CH3NH3PbX3 X= I, Br, and Cl) single crystals and thin films is analyzed by scanning near-field thermal microscopy. The thermal conductivity of CH3NH3PbX3 single crystals with X= I, Br, and Cl is found to be 0.34 ± 0.12, 0.44 ± 0.08, and 0.50 ± 0.05 W/(mK) at room temperature, respectively. Strikingly, similar thermal conductivities are determined for the corresponding thin-film samples. The thermal conductivity of MAPbI3 in the cubic phase (T > 55 °C) increases to (1.1 ± 0.1) W/(mK). In addition, the temperature dependence of the thermal conductivities and of thermal expansion coefficients of MAPbI3 around the phase transition from the tetragonal to cubic phase is presented.

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Hybrid perovskite semiconductors hold great promise as low‐cost, yet high performance gain media for lasers. Distributed feedback (DFB) resonator structures are a key to unlock low laser threshold levels, which are essential on the way to the first electrically operated perovskite laser diode. Here, the first DFB lasers based on methylammonium lead bromide (MAPbBr3) thin films, with a linear photonic grating imprinted into the MAPbBr3 active layers is presented. High‐Q Bragg resonator gratings with a periodicity of 300 nm are directly patterned by thermal nanoimprinting into thin films of MAPbBr3 at a temperature as low as 100 °C. A notable effect of the imprinting process is a substantial flattening of the initially very rough polycrystalline perovskite layers to layers consisting of large crystals on the order of tens of microns with a surface roughness of 0.6 nm. The smooth surface affords a significantly lowered threshold for the onset of amplified spontaneous emission due to reduced scattering. In optically pumped DFB laser structures, very low lasing thresholds of 3.4 µJ cm−2 are achieved. It is foreseen that these results will influence research on perovskite‐based optoelectronic devices beyond lasers, e.g., light emitting diodes and solar cells.

We have tested nanoimprint lithography, a new and promising technique for nanometer-scale pattern definition. Preliminary experiments reveal that, besides severe sticking and adhesion problems, the problem of material transport is one inherent to this technique. There are clear indications that most of the effects found may be understood in terms of material transport. We performed experiments within a well defined pressure and temperature window which ranged from 60 to 100 bar and from 50 to 90 °C above the glass transition temperature of the poly(methylmethacrylate)-like polymer used. As a result, the quality of imprint is evaluated with respect to full area pattern transfer, based on a qualitative scanning electron microscope investigation of the fully imprinted area of 2 cm × 2 cm patterned with features of different size and shape. Optimum conditions for imprint quality are found around 100 bar and 90 °C above Tg for the specific polymer used. Although material transport will limit nanoimprint performance in general, it is found that periodic patterns and isolated or small area negative stamp relief patterns are most suitable for high quality nanoimprinting.

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Perovskites have high potential for future electronic devices, in particular, in the field of opto-electronics. However, the electronic and optic properties of these materials highly depend on the morphology and thus on the preparation; in particular, highly crystalline layers with large crystals and without pinholes are required. Here, nanoimprint is used to improve the morphology of such layers in a thermal imprint step. Two types of material are investigated, MAPbI3 and MAPbBr3, with MA being methylammonium, CH3NH3+. The perovskite layers are prepared from solution, and the crystal size of the domains is substantially increased by imprinting them at temperatures of 100–150 °C. Although imprint is performed under atmospheric conditions which, in general, enhances the degradation, the stamp that covers the layer under elevated temperature is able to protect the perovskite largely from decomposition. Comparing imprinting experiments with pure annealing at a similar temperature and time proves this. Furthermore, imprint is capable of patterning the surface of the perovskite layers; lines and spaces of 150 nm width were reproducibly obtained under imprint at 150 °C. Moreover, a through-layer patterning is possible by using the partial cavity filling approach. Although not yet optimized, this simple way to define isolated perovskite patterns within a layer simply by thermal nanoimprint is of impact for the preparation of devices, as patterning of perovskite layers by conventional techniques is limited.