Band alignment engineering of 2D/3D halide perovskite lateral heterostructures

Two-dimensional (2D)/three-dimensional (3D) halide perovskite heterostructures have been extensively studied for their ability to combine the outstanding long-term stability of 2D perovskites with the superb optoelectronic properties of 3D perovskites. While current studies mostly focus on vertically stacked 2D/3D perovskite heterostructures, a theoretical understanding regarding the optoelectronic properties of 2D/3D perovskite lateral heterostructures is still lacking. Herein, we construct a series of 2D/3D perovskite lateral heterostructures to study their optoelectronic properties and interfacial charge transfer using density functional theory (DFT) calculations. We find that the band alignments of 2D/3D heterostructures can be regulated by varying the quantum-well thickness of 2D perovskites. Moreover, decreasing the 2D component ratio in 2D/3D heterostructures can be favorable to form type-I band alignment, whereas a large component ratio of 2D perovskites tends to form type-II band alignment. We can improve the amount of charge transfer at the 2D/3D perovskite interfaces and the light absorption of 2D perovskites by increasing quantum-well thickness. These present findings can provide a clear designing principle for achieving 3D/2D perovskite lateral heterostructures with tunable optoelectronic properties.