Science (New York, N.Y.) · 2025
Layer-by-layer epitaxial growth of perovskite heterostructures with tunable band offsets.
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Lu Yang, Jung Young-Kwang, Dubajic Milos, Li Xinjuan, Maqbool Shabnum, Gu Qichun, Bai Xinyu, Boeije Yorrick, Chua Xian Wei, Mirabelli Alessandro J, Kang Taeheon, Sonneveld Lars, Zhang Youcheng, Selby Thomas A, Mamak Capucine, Tang Kan, Yu Zhongzheng, Liu Tianjun, Anaya Miguel, Barlow Stephen, Marder Seth R, Ehrler Bruno, Ducati Caterina, Friend Richard H, Stranks Samuel D
Аннотация
Halide perovskites exhibit superior optoelectronic properties but lack precise thickness and band offset control in heterojunctions, which is critical for modular multilayer architectures such as multiple quantum wells. We demonstrate vapor-phase, layer-by-layer heteroepitaxial growth exemplified by CsPbBr3 deposition on single crystals of PEA2PbBr4 (PEA: 2-phenylethylammonium). Angstrom-level thickness control and subangstrom smooth layers enable quantum-confined photoluminescence of CsPbBr3 from monolayer, bilayer, and through to bulk. The interfacial structure controls the electronic structure from a Cs‒PEA-terminated interface (type II heterojunction) to a PEA‒PEA-terminated interface (type I heterojunction), with a layer-tunable band offset shift exceeding 0.5 electron volts. Electron transfer from CsPbBr3 to PEA2PbBr4 for a type II Cs‒PEA heterojunction results in delayed electron-hole recombination beyond 10 microseconds. Precise quantum confinement control and large band offset tunability unlock perovskite heterojunctions as platforms for scalable, superlattice-based optoelectronic applications.