Enhanced visible light absorption performance of SnS₂ and SnSe₂ via surface charge transfer doping

The layered two-dimensional (2D) SnS₂ and SnSe₂ have received intensive attention due to their sizable band gaps and potential properties. However, it has been shown that the visible light absorption of SnS₂ and SnSe₂ are restricted as photocatalysts and light-harvesting material absorbers for water splitting and high-performance optoelectronic devices. Herein, to enhance the visible light absorption performance of SnS₂ and SnSe₂, we performed a systematic investigation on tuning the electronic and optical properties of monolayers SnS₂ and SnSe₂ via surface charge transfer doping (SCTD) with the adsorption of molybdenum trioxide (MoO₃) and potassium (K) as surface dopants based on density functional theory. Our calculations reveal that MoO₃ molecules and K atoms can draw/donate electrons from/to SnS₂ and SnSe₂ as acceptors and donors, respectively. The adsorption of MoO₃ molecules introduces a new flat impurity state in the gap of the monolayers SnS₂/SnSe₂, and the Fermi level moves correspondingly to the top of valence band, resulting in a p-type doping of the monolayer SnS₂/SnSe₂. With the adsorption of K atoms, the electrons can transfer from K atoms to the monolayer of SnS₂ and SnSe₂, making K an effective electron-donating dopant. Meanwhile, the bandgaps of monolayers SnS₂ and SnSe₂ decrease after the MoO₃ and K doping, which leads to the appearance of appreciable new absorption peaks at around ∼650/480 and ∼600/680 nm, respectively, and yielding an enhanced visible light absorption of SnS₂ and SnSe₂. Our results unveil that SCTD is an effective way to improve the photocatalytic and light-harvesting performance of SnS₂ and SnSe₂, broadening their applications in splitting water and degrading environmental pollutants under sunlight irradiation.