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Metal halide perovskites have arisen as a new family of semiconductors for radiation detectors due to their high stopping power, large and balanced electron–hole mobility-lifetime (μτ) product, and tunable bandgap. Here, we report a simple and low-cost solution processing approach using additive-assisted inverse temperature crystallization (ITC) to grow cesium lead bromide (CsPbBr3) single crystals with low-defect density. Crystals grown from precursor solutions without additives tend to grow fastest along the [002] direction, resulting in crystals shaped as small elongated bars. The addition of choline bromide (CB) proves to mediate the crystallization process to produce large single crystals with a cuboid shape, allowing for more practical fabrication of gamma-ray detectors. This new additive-assisted growth method also improves the resulting crystal quality to yield a reduction in the density of trap states by over one order of magnitude, relative to a crystal grown without CB. The detector fabricated from a CB-assisted solution-grown perovskite CsPbBr3 single crystal is able to acquire an energy spectrum from a cesium-137 (137Cs) source with a resolution of 5.5% at 662 keV.

The efficiencies of green and red perovskite light-emitting diodes (PeLEDs) have been increased close to their theoretical upper limit, while the efficiency of blue PeLEDs is lagging far behind. Here we report enhancing the efficiency of sky-blue PeLEDs by overcoming a major hurdle of low photoluminescence quantum efficiency in wide-bandgap perovskites. Blending phenylethylammonium chloride into cesium lead halide perovskites yields a mixture of two-dimensional and three-dimensional perovskites, which enhances photoluminescence quantum efficiency from 1.1% to 19.8%. Adding yttrium (III) chloride into the mixture further enhances photoluminescence quantum efficiency to 49.7%. Yttrium is found to incorporate into the three-dimensional perovskite grain, while it is still rich at grain boundaries and surfaces. The yttrium on grain surface increases the bandgap of grain shell, which confines the charge carriers inside grains for efficient radiative recombination. Record efficiencies of 11.0% and 4.8% were obtained in sky-blue and blue PeLEDs, respectively., Despite the rapid progress on perovskite light emitting diodes (PeLEDs), the efficiency of blue PeLEDs is lagging behind. Here Wang et al. employ yttrium (III) chloride additive to yield enhanced photoluminescence in the perovskite materials and thus record high device efficiencies for sky-blue and blue PeLEDs.

The influence of metal ions on perovskite properties and resulting device performance has been undeniable in progressing the field of inorganic and organic–inorganic hybrid perovskites. Here we provide a review on the capacity of metal ions to impart a broad range of effects from controlling crystallization to the alloying, doping, and passivation of perovskite materials. Although some metal ions have already proved effective in modulating bandgaps through alloying, their ability to control crystallization, carrier concentration, and emissive effects still require significant improvements in fundamental understanding. This presents enormous opportunities in research that may afford novel properties and applications through unparalleled control of perovskite materials.

Summary Organic-inorganic halide perovskites are promising semiconductors to mate with silicon in tandem photovoltaic cells due to their solution processability and tunable complementary bandgaps. Herein, we show that a combination of two additives, MACl and MAH2PO2, in the perovskite precursor can significantly improve the grain morphology of wide-bandgap (1.64–1.70 eV) perovskite films, resulting in solar cells with increased photocurrent while reducing the open-circuit voltage deficit to 0.49–0.51 V. The addition of MACl enlarges the grain size, while MAH2PO2 reduces non-radiative recombination through passivation of the perovskite grain boundaries, with good synergy of functions from MACl and MAH2PO2. Matching the photocurrent between the two sub-cells in a perovskite/silicon monolithic tandem solar cell by using a bandgap of 1.64 eV for the top cell results in a high tandem Voc of 1.80 V and improved power conversion efficiency of 25.4%.

Tailoring the doping of semiconductors in heterojunction solar cells shows tremendous success in enhancing the performance of many types of inorganic solar cells, while it is found challenging in perovskite solar cells because of the difficulty in doping perovskites in a controllable way. Here, a small molecule of 4,4',4″,4″'-(pyrazine-2,3,5,6-tetrayl) tetrakis (N,N-bis(4-methoxyphenyl) aniline) (PT-TPA) which can effectively p-dope the surface of FAx MA1- x PbI3 (FA: HC(NH2 )2 ; MA: CH3 NH3 ) perovskite films is reported. The intermolecular charge transfer property of PT-TPA forms a stabilized resonance structure to accept electrons from perovskites. The doping effect increases perovskite dark conductivity and carrier concentration by up to 4737 times. Computation shows that electrons in the first two layers of octahedral cages in perovskites are transferred to PT-TPA. After applying PT-TPA into perovskite solar cells, the doping-induced band bending in perovskite effectively facilitates hole extraction to hole transport layer and expels electrons toward cathode side, which reduces the charge recombination there. The optimized devices demonstrate an increased photovoltage from 1.12 to 1.17 V and an efficiency of 23.4% from photocurrent scanning with a stabilized efficiency of 22.9%. The findings demonstrate that molecular doping is an effective route to control the interfacial charge recombination in perovskite solar cells which is in complimentary to broadly applied defect passivation techniques.