Highly Orientated Perovskite Quantum Dot Solids for Efficient Solar Cells

Abstract Perovskite quantum dots (PQDs) have emerged as competitive optoelectronic materials for photovoltaic applications due to their ideal bandgap energy, high defect tolerance, and solution processability. However, the highly dynamic surface and imperfect cubic structure of PQDs generally result in unfavorable charge‐carrier transport within the PQD solids and serious nonradiative recombination. Herein, a highly orientated PQD solid is demonstrated using precursor engineering accompanied by a chemical stripping treatment (CST). A combination of systematic experimental studies and theoretical calculations is conducted to fundamentally understand the resurfacing of PQDs using the CST approach. The results reveal that the highly ordered PQDs can result in a high orientation of PQD solids, significantly promoting charge‐carrier transport within the PQD solids. Meanwhile, the ideal cubic‐structured PQD with an iodine‐rich surface dramatically decreases surface trap states, thereby substantially diminishing trap‐assisted nonradiative recombination. Consequently, the inorganic PQD solar cell delivers a power conversion efficiency of up to 16.25%. This work provides a feasible avenue to construct highly orientated PQD solids with improved photophysical properties for high‐performance optoelectronic devices.