Abstract
AbstractDouble perovskites are considered for future photovoltaic and electro‐optic applications as a toxic‐free alternative to lead halide perovskites. Alas, due to the lower efficiency of lead‐free devices, material properties need to improve to compete. In this work, the self‐healing and annealing of crystal voids is reported. Experiments are conducted on nanocrystals and in situ a transmission electron microscopy (TEM) microscope. The setup enables creation of crystal voids and to monitor their dynamics in real time. Void trajectories and velocities are calculated for TEM videos. An inaccessible, protected volume for migration near the nanocrystal outer surface is discovered, confining the migration of voids to inner crystal parts. Once surface passivation in the form of organic ligands is removed, void dynamics changes, to enable annealing of the voids and self‐healing of the crystal. It is determined that surface ligand protection against void migration is extending several atomic layers below the crystal surface. Modeling based on these results predict equilibrium positions for the voids, which are discovered in the data. The study suggests that tuning of organic ligand density influences structural stability and crystal defect tolerance in double perovskites. Engineering surfaces with inherent self‐healing properties may increase efficiencies in future devices based on these materials.
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