Oxidation-induced graded bandgap narrowing in Two-dimensional tin sulfide for high-sensitivity broadband photodetection.

Two-dimensional (2D) layered group-IV monochalcogenides with large surface-to-volume ratio and high surface activity make that their structural and optoelectronic properties are sensitive to air oxidation. Here, we report the utilization of oxidation-induced gradient doping to modulate electronic structures and optoelectronic properties of 2D group-IV monochalcogenides by using SnS nanoplates grown by physical vapor deposition as a model system. By a precise control of oxidation time and temperature, the structural transition from SnS to SnSO could be driven by the layer-by-layer oxygen doping and intercalation. The resulting SnSO with a graded narrowing bandgap exhibits the enhanced optical absorption and photocurrent, leading to the fabricated SnSO photodetector with remarkable photoresponsivity and fast response speed (<64 μs) at a broadband spectrum range of 520-1550 nm. The peak responsivity (7294 A/W) and detectivity (9.54 × 10 Jones) of SnSO device are at least two orders of magnitude larger than those of SnS photodetector. Moreover, its photodetection performance can be competed with state-of-the-art of 2D materials-based photodetectors. This work suggests that the air oxidation could be utilized as an efficient strategy to engineer the electronic and optical properties of SnS and other 2D group-IV monochalcogenides for the development of high-performance broadband photodetectors.