The 2D InSe/WS2 Heterostructure with Enhanced Optoelectronic Performance in the Visible Region*

Two-dimensional (2D) InSe and WS2 exhibit promising characteristics for optoelectronic applications. However, they both have poor absorption of visible light due to wide bandgaps: 2D InSe has high electron mobility but low hole mobility, while 2D WS2 is on the contrary. We propose a 2D heterostructure composed of their monolayers as a solution to both problems. Our first-principles calculations show that the heterostructure has a type-II band alignment as expected. Consequently, the bandgap of the heterostructure is reduced to 2.19 eV, which is much smaller than those of the monolayers. The reduction in bandgap leads to a considerable enhancement of the visible-light absorption, such as about fivefold (threefold) increase in comparison to monolayer InSe (WS2) at the wavelength of 490 nm. Meanwhile, the type-II band alignment also facilitates the spatial separation of photogenerated electron-hole pairs; i.e., electrons (holes) reside preferably in the InSe (WS2) layer. As a result, the two layers complement each other in carrier mobilities of the heterostructure: the photogenerated electrons and holes inherit the large mobilities from the InSe and WS2 monolayers, respectively.