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A low defect density in metal halide perovskite single crystals is critical to achieve high performance optoelectronic devices. Here we show the reduction of defect density in perovskite single crystals grown by a ligand-assisted solution process with 3‐(decyldimethylammonio)‐propane‐sulfonate inner salt (DPSI) as an additive. DPSI ligands anchoring with lead ions on perovskite crystal surfaces not only suppress nucleation in solution, but also regulate the addition of proper ions to the growing surface, which greatly enhances the crystal quality. The grown CH3NH3PbI3 crystals show better crystallinity and a 23-fold smaller trap density of 7 × 1010 cm−3 than the optimized control crystals. The enhanced material properties result in significantly suppressed ion migration and superior X-ray detection sensitivity of CH3NH3PbI3 detectors of (2.6 ± 0.4) × 106 µC Gy−1air cm−2 for 60 kVp X-ray and the lowest detectable dose rate reaches (5.0 ± 0.7) nGy s−1, which enables reduced radiation dose to patients in medical X-ray diagnostics., The performance of a metal halide perovskite single crystal is governed by the defect density. Here, the authors report a high quality single crystal perovskite grown by a ligand-assisted solution process with DPSI achieving 23-fold smaller trap density than that without DPSI.

Grain boundaries have been established to impact charge transport, recombination and thus the power conversion efficiency of metal halide perovskite thin film solar cells. As a special category of grain boundaries, ferroelastic twin boundaries have been recently discovered to exist in both CH3NH3PbI3 thin films and single crystals. However, their impact on the carrier transport and recombination in perovskites remains unexplored. Here, using the scanning photocurrent microscopy, we find that twin boundaries have negligible influence on the carrier transport across them. Photoluminescence (PL) imaging and the spatial-resolved PL intensity and lifetime scanning confirm the electronically benign nature of the twin boundaries, in striking contrast to regular grain boundaries which block the carrier transport and behave as the non-radiative recombination centers. Finally, the twin-boundary areas are found still easier to degrade than grain interior., Grain boundaries are known to be generally detrimental to the operation of metal halide perovskite solar cells. Here Xiao et al. show with scanning photocurrent microscopy that ferroelastic twin boundaries are benign to the electrical properties in crystalline samples, in contrast to grain boundaries.

Identifying the origin of intrinsic instability for organic–inorganic halide perovskites (OIHPs) is crucial for their application in electronic devices, including solar cells, photodetectors, radiation detectors, and light-emitting diodes, as their efficiencies or sensitivities have already been demonstrated to be competitive with commercial available devices. Here we show that free charges in OIHPs, whether generated by incident light or by current-injection from electrodes, can reduce their stability, while efficient charge extraction effectively stabilizes the perovskite materials. The excess of both holes and electrons reduce the activation energy for ion migration within OIHPs, accelerating the degradation of OIHPs, while the excess holes and electrons facilitate the migration of cations or anions, respectively. OIHP solar cells capable of efficient charge-carrier extraction show improved light stability under regular operation conditions compared to an open-circuit condition where the photo-generated charges are confined in the perovskite layers., Optoelectronic devices based on organic–inorganic halide perovskites show promising performance, but their poor stability impedes the commercialization. Here Lin et al. show that excess free charges are detrimental and efficient charge-carrier extraction is necessary for improved device stability.

Photon recycling, that is, iterative self-absorption and re-emission by the photoactive layer itself, has been speculated to contribute to the high open-circuit voltage in several types of high efficiency solar cells. For organic–inorganic halide perovskites that have yielded highly efficient photovoltaic devices, however, it remains unclear whether the photon recycling effect is significant enough to improve solar cell efficiency. Here we quantitatively evaluate the re-absorption and re-emission processes to determine photon recycling efficiency in hybrid perovskite with its single crystals by measuring the ratio of the re-emitted photons to the initially excited photons, which is realized by modulating their polarization to differentiate them. The photon recycling efficiencies are revealed to be less than 0.5% in CH3NH3PbI3 and CH3NH3PbBr3 single crystals under excitation intensity close to one sun, highlighting the intrinsically long carrier recombination lifetime instead of the photon-recycling-induced photon propagation as the origin of their long carrier diffusion length., Fang et al. develop a method to determine the photon recycling efficiency for organic-inorganic hybrid single crystal perovskites by differentiating between emitted and re-absorbed photons based on their polarization difference. For these systems efficiencies of less than 0.5% are reported.

The efficiency of perovskite solar cells has surged in the past few years, while the bandgaps of current perovskite materials for record efficiencies are much larger than the optimal value, which makes the efficiency far lower than the Shockley–Queisser efficiency limit. Here we show that utilizing the below-bandgap absorption of perovskite single crystals can narrow down their effective optical bandgap without changing the composition. Thin methylammonium lead triiodide single crystals with tuned thickness of tens of micrometers are directly grown on hole-transport-layer covered substrates by a hydrophobic interface confined lateral crystal growth method. The spectral response of the methylammonium lead triiodide single crystal solar cells is extended to 820 nm, 20 nm broader than the corresponding polycrystalline thin-film solar cells. The open-circuit voltage and fill factor are not sacrificed, resulting in an efficiency of 17.8% for single crystal perovskite solar cells., Thin films of halide perovskites are promising for solar cell technology but they do not perform well at the band edge due to the low optical absorption. Herein, Chen et al. fabricate a high efficiency single crystal perovskite solar cell with thicker single crystals to harvest the below-bandgap photons.