Interfacial Strain Release from the WS 2 /CsPbBr 3 van der Waals Heterostructure for 1.7 V Voltage All‐Inorganic Perovskite Solar Cells

Perovskite lattice distortion induced by residual tensile strain from the thermal expansion mismatch between the electron‐transporting layer (ETL) and perovskite film causes a sluggish charge extraction and transfer dynamics in all‐inorganic CsPbBr 3 perovskite solar cells (PSCs) because of their higher crystallization temperatures and thermal expansion coefficients. Herein, the interfacial strain is released by fabricating a WS 2 /CsPbBr 3 van der Waals heterostructure owing to their matched crystal lattice structure and the atomically smooth dangling bond‐free surface to act as a lubricant between ETL and CsPbBr 3 perovskite. Arising from the strain‐released interface and condensed perovskite lattice, the best device achieves an efficiency of 10.65 % with an ultrahigh open‐circuit voltage of 1.70 V and significantly improved stability under persistent light irradiation and humidity (80 %) attack over 120 days.