Colloidal CsPbX 3 (X = Br, Cl, and I) perovskite nanocrystals exhibit tunable bandgaps over the entire visible spectrum and high photoluminescence quantum yields in the green and red regions. However, the lack of highly efficient blue-emitting perovskite nanocrystals limits their development for optoelectronic applications. Herein, neodymium (III) (Nd 3+) doped CsPbBr 3 nanocrystals are prepared through the ligand-assisted reprecipitation method at room temperature with tunable photoemission from green to deep blue. A blue-emitting nanocrystal with a central wavelength at 459 nm, an exceptionally high photoluminescence quantum yield of 90%, and a spectral width of 19 nm is achieved. First principles calculations reveal that the increase in photoluminescence quantum yield upon doping is driven by an enhancement of the exciton binding energy due to increased electron and hole effective masses and an increase in oscillator strength due to shortening of the Pb-Br bond. Putting these results together, an all-perovskite white light-emitting diode is successfully fabricated, demonstrating that B-site composition engineering is a reliable strategy to further exploit the perovskite family for wider optoelectronic applications.

Nanocrystals based on metal-halide perovskites offer a promising material platform for highly efficient lighting. Using transient optical spectroscopy, we study excitation recombination dynamics in manganese-doped CsPb(Cl,Br)3 perovskite nanocrystals. We find an increase in the intrinsic excitonic radiative recombination rate upon doping, which is typically a challenging material property to tailor.Supported by ab initio calculations, we can attribute the enhanced emission rates to increased exciton localization through lattice periodicity breaking from Mn dopants, which increases exciton effective masses and overlap of electron and hole wavefunctions and thus the oscillator strength. Our report of a fundamental strategy for improving luminescence efficiencies in perovskite nanocrystals will be valuable for maximizing efficiencies in light-emitting applications.

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Detecting low dose rates of X-rays is critical for making safer radiology instruments, but is limited by the absorber materials available. Here, we develop bismuth oxyiodide (BiOI) single crystals into effective X-ray detectors. BiOI features complex lattice dynamics, owing to the ionic character of the lattice and weak van der Waals interactions between layers. Through use of ultrafast spectroscopy, first-principles computations and detailed optical and structural characterisation, we show that photoexcited charge-carriers in BiOI couple to intralayer breathing phonon modes, forming large polarons, thus enabling longer drift lengths for the photoexcited carriers than would be expected if self-trapping occurred. This, combined with the low and stable dark currents and high linear X-ray attenuation coefficients, leads to strong detector performance. High sensitivities reaching 1.1  × 103 μC Gyair−1 cm−2 are achieved, and the lowest dose rate directly measured by the detectors was 22 nGyair s−1. The photophysical principles discussed herein offer new design avenues for novel materials with heavy elements and low-dimensional electronic structures for (opto)electronic applications.

Metal-halide perovskite nanocrystals have demonstrated excellent optoelectronic properties for light-emitting applications. Isovalent doping with various metals (M 2+ ) can be used to tailor and enhance their light emission. Although crucial to maximize performance, an understanding of the universal working mechanism for such doping is still missing. Here, we directly compare the optical properties of nanocrystals containing the most commonly employed dopants, fabricated under identical synthesis conditions. We show for the first time unambiguously, and supported by first-principles calculations and molecular orbital theory, that element-unspecific symmetry-breaking rather than element-specific electronic effects dominate these properties under device-relevant conditions. The impact of most dopants on the perovskite electronic structure is predominantly based on local lattice periodicity breaking and resulting charge carrier localization, leading to enhanced radiative recombination, while dopant-specific hybridization effects play a secondary role. Our results suggest specific guidelines for selecting a dopant to maximize the performance of perovskite emitters in the desired optoelectronic devices.