We report the one-pot synthesis of colloidal Mn-doped cesium lead halide (CsPbX 3 ) perovskite nanocrystals and efficient intraparticle energy transfer between the exciton and dopant ions resulting in intense sensitized Mn luminescence. Mn-doped CsPbCl 3 and CsPb(Cl/Br) 3 nanocrystals maintained the same lattice structure and crystallinity as their undoped counterparts with nearly identical lattice parameters at ∼0.2% doping concentrations and no signature of phase separation. The strong sensitized luminescence from d−d transition of Mn 2+ ions upon band-edge excitation of the CsPbX 3 host is indicative of sufficiently strong exchange coupling between the charge carriers of the host and dopant d electrons mediating the energy transfer, essential for obtaining unique properties of magnetically doped quantum dots. Highly homogeneous spectral characteristics of Mn luminescence from an ensemble of Mn-doped CsPbX 3 nanocrystals and well-defined electron paramagnetic resonance spectra of Mn 2+ in host CsPbX 3 nanocrystal lattices suggest relatively uniform doping sites, likely from substitutional doping at Pb 2+ . These observations indicate that CsPbX 3 nanocrystals, possessing many superior optical and electronic characteristics, can be utilized as a new platform for magnetically doped quantum dots expanding the range of optical, electronic, and magnetic functionality.

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Stacking solar cells with decreasing band gaps to form tandems presents the possibility of overcoming the single-junction Shockley-Queisser limit in photovoltaics. The rapid development of solution-processed perovskites has brought perovskite single-junction efficiencies >20%. However, this process has yet to enable monolithic integration with industry-relevant textured crystalline silicon solar cells. We report tandems that combine solution-processed micrometer-thick perovskite top cells with fully textured silicon heterojunction bottom cells. To overcome the charge-collection challenges in micrometer-thick perovskites, we enhanced threefold the depletion width at the bases of silicon pyramids. Moreover, by anchoring a self-limiting passivant (1-butanethiol) on the perovskite surfaces, we enhanced the diffusion length and further suppressed phase segregation. These combined enhancements enabled an independently certified power conversion efficiency of 25.7% for perovskite-silicon tandem solar cells. These devices exhibited negligible performance loss after a 400-hour thermal stability test at 85°C and also after 400 hours under maximum power point tracking at 40°C.

The high-temperature, all-inorganic CsPbI3 perovskite black phase is metastable relative to its yellow, nonperovskite phase at room temperature. Because only the black phase is optically active, this represents an impediment for the use of CsPbI3 in optoelectronic devices. We report the use of substrate clamping and biaxial strain to render black-phase CsPbI3 thin films stable at room temperature. We used synchrotron-based, grazing incidence, wide-angle x-ray scattering to track the introduction of crystal distortions and strain-driven texture formation within black CsPbI3 thin films when they were cooled after annealing at 330°C. The thermal stability of black CsPbI3 thin films is vastly improved by the strained interface, a response verified by ab initio thermodynamic modeling.

Cesium lead halide (CsPbX) nanocrystals have emerged as a new family of materials that can outperform the existing semiconductor nanocrystals due to their superb optical and charge-transport properties. However, the lack of a robust method for producing quantum dots with controlled size and high ensemble uniformity has been one of the major obstacles in exploring the useful properties of excitons in zero-dimensional nanostructures of CsPbX. Here, we report a new synthesis approach that enables the precise control of the size based on the equilibrium rather than kinetics, producing CsPbX quantum dots nearly free of heterogeneous broadening in their exciton luminescence. The high level of size control and ensemble uniformity achieved here will open the door to harnessing the benefits of excitons in CsPbX quantum dots for photonic and energy-harvesting applications.

Thermally-induced tensile strain that remains in perovskite films following annealing results in increased ion migration and is a known factor in the instability of these materials. Previously-reported strain regulation methods for perovskite solar cells (PSCs) have utilized substrates with high thermal expansion coefficients that limits the processing temperature of perovskites and compromises power conversion efficiency. Here we compensate residual tensile strain by introducing an external compressive strain from the hole-transport layer. By using a hole-transport layer with high thermal expansion coefficient, we compensate the tensile strain in PSCs by elevating the processing temperature of hole-transport layer. We find that compressive strain increases the activation energy for ion migration, improving the stability of perovskite films. We achieve an efficiency of 16.4% for compressively-strained PSCs; and these retain 96% of their initial efficiencies after heating at 85°C for 1000 hoursthe most stable wide-bandgap perovskites (above 1.75 eV) reported so far.

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