Unraveling segregation behavior of inactive secondary phase driven by ion-competition reaction for perovskite-2D PbI2 heterojunction solar cells

Abstract

The undesired segregation of inactive secondary phase that randomly distributed across the perovskite film is detrimental to charge-carrier transport dynamics and light stability. However, in-depth studies for understanding the underlying chemical reaction mechanism and the relationship between phase structural configuration and physical properties are still lacking. Herein, the segregation behavior of the inactive secondary phase and the underlying microcosmic mechanism regarding ionic chemical replacement reaction and lattice reconfiguration process are systematically elaborated. A high-quality perovskite-PbI2 heterojunction film is constructed via converting the three-dimensional PbI2 photoactive phase into a two-dimensional inactive phase, alleviating the energetic disorder of carrier dynamics and photochemical dissociation. The resultant perovskite solar cells achieve an efficiency of 24.23% with excellent light-resistance. The dissociation energetics of phase dimensional structure is theoretically analyzed. This work provides new insights into crystal structure design for constructing high-quality perovskite heterojunction devices.