Implementing Lattice and Energy Level Matching to Optimize Buried Interfaces for High‐Performance Perovskite Solar Cells

Abstract In n‐i‐p type perovskite solar cells (PSCs), mismatches in energy level and lattice at the buried interface is highly detrimental to device performance. Here, thin PbS interconnect layer in situ coating on the SnO 2 surface is grown. The function of PbS at the interface is different from the commonly used function of crystalline seeds in perovskite bulk. The theoretical calculation show that it helps construct an interconnect structure of SnO 2 /PbS/Perovskite with matched energy level and lattice. This not only increases conductivity of SnO 2 , but also upshifts Fermi energy levels ( E F ) of both SnO 2 and buried perovskite due to charge transfer and perovskite's internal defect changes. Such a suitable energy level arrangement ensures a better energy level match at the interface, favoring efficient charge transfer and less open circuit voltage ( V oc ) loss. Additionally, in situ PL reveals that the template effect of PbS enable perovskite grain to grow bottom‐up because of their highly matched lattice parameters. This growth mode optimizes buried interface contact and crystallinity of perovskite. Ultimately, after PbS modification, a remarkable power conversion efficiency (PCE) exceeding 24% and better device stability are obtained. This work demonstrates an effective interconnect layers strategy to realize ideal interface contact toward high‐performance PSCs.