Publication date: 21st July 2025
Halide perovskites exhibit superior optoelectronic properties and hold great promise in advanced optoelectronic devices. However, they lack precise thickness and interfacial structure control in heterojunctions, critical for modular multilayer architectures such as multiple quantum wells. Vapor-phase deposition method have great advantage in thickness control for perovskites. As a dry processing method, it is also capable of preserving the interfacial structure especially for perovskite heterojunctions. In this work, we demonstrate layer-by-layer heteroepitaxial growth CsPbBr3 deposition on 2D perovskites by thermal evaporation. The strict heteroepitaxial templating, revealed by reciprocal space maps, significantly improved perovskite film quality by reducing energetic disorder, enhancing photoluminescence quantum yield, and improving carrier transport. Angstrom-level thickness control and sub-Angstrom smooth layers enable quantum-confined photoluminescence of CsPbBr3 from monolayer, bilayer, and through to bulk.
Futhermore, we demonstrate that the interfacial structure could be tuned by deposition parameters, controls the electronic structure between type-I and type-II heterojunctions. The interfacial-tunable band offset shift could reach much higher values than what has been achieved in III-V semiconductors. Electron transfer from CsPbBr3 to 2D perovskite for the type-II heterojunction results in observation of charge separation and delayed electron-hole recombination, which is absent in the type-I heterojunction. Our results show that the precise quantum confinement control and large band offset tunability unlock perovskite heterojunctions as platforms for scalable, low-cost modular quantum and superlattice-based optoelectronic applications.
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