Multiple-Dimensionally Controllable Nucleation Sites of Two-Dimensional WS2/Bi2Se3 Heterojunctions Based on Vapor Growth.

Two-dimensional (2D) heterojunctions have attracted great attention due to their excellent optoelectronic properties. Until now, precisely controlling the nucleation density and stacking area of 2D heterojunctions has been of critical importance but still a huge challenge. It hampers the progress of controlled growth of 2D heterojunctions for optoelectronic devices because the potential relation between numerous growth parameters and nucleation density is always poorly understood. Herein, by cooperatively controlling three parameters (substrate temperature, gas flow rate, and precursor concentration) in modified vapor deposition growth, the nucleation density and stacking area of WS2/Bi2Se3 vertical heterojunctions were successfully modulated. High-quality WS2/Bi2Se3 vertical heterojunctions with various stacking areas were effectively grown from single and multiple nucleation sites. Moreover, the potential nucleation mechanism and efficient charge transfer of WS2/Bi2Se3 vertical heterojunctions were systematically studied by utilizing the density functional theory and photoluminescence spectra. This modified vapor deposition strategy and the proposed mechanism are helpful in controlling the nucleation density and stacking area of other heterojunctions, which plays a key role in the preparation of electronic and optoelectronic nanodevices.