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Halide perovskite light absorbers have great advantages for photovoltaicssuch as efficient solar energy absorption, but charge accumulation andrecombination at the interface with an electron transport layer (ETL) remains amajor challenge in realizing their full potential. Here we report theexperimental realization of a zipper-like interdigitated interface between aPb-based halide perovskite light absorber and an oxide ETL by the PbO cappingof the ETL surface, which produces an atomically thin two-dimensional metalliclayer that can significantly enhance the perovskite/ETL charge extractionprocess. As the atomistic origin of the emergent two-dimensional interfacialmetallicity, first-principles calculations performed on the representativeMAPbI$_3$/TiO$_2$ interface identify the interfacial strain induced by thesimultaneous formation of stretched I-substitutional Pb bonds (and thus Pb-I-Pbbonds bridging MAPbI$_3$ and TiO$_2$) and contracted substitutional Pb-O bonds.Direct and indirect experimental evidences for the presence of interfacialmetallic states are provided, and a non-conventional defect-passivating natureof the strained interdigitated perovskite/ETL interface is emphasized. It isexperimentally demonstrated that the PbO capping method is generally applicableto other ETL materials including ZnO and SrTiO$_3$, and that the zipper-likeinterdigitated metallic interface leads to about two-fold increase in chargeextraction rate. Finally, in terms of the photovoltaic efficiency, we observe avolcano-type behavior with the highest performance achieved at themonolayer-level PbO capping. The method established here might prove to be ageneral interface engineering approach to realize high-performance perovskitesolar cells.

acs nano

Strain-induced metallization and defect suppression at zipper-like  interdigitated atomically thin interfaces enabling high-efficiency halide  perovskite solar cells