Spatially Bandgap-Graded MoS(2(1−x))Se(2x) Homojunctions for Self-Powered Visible–Near-Infrared Phototransistors

Ternary transition metal dichalcogenide alloys with spatially graded bandgaps are an emerging class of two-dimensional materials with unique features, which opens up new potential for device applications. Here, visible–near-infrared and self-powered phototransistors based on spatially bandgap-graded MoS(2(1−x))Se(2x) alloys, synthesized by a simple and controllable chemical solution deposition method, are reported. The graded bandgaps, arising from the spatial grading of Se composition and thickness within a single domain, are tuned from 1.83 to 1.73 eV, leading to the formation of a homojunction with a built-in electric field. Consequently, a strong and sensitive gate-modulated photovoltaic effect is demonstrated, enabling the homojunction phototransistors at zero bias to deliver a photoresponsivity of 311 mA W(−1), a specific detectivity up to ~ 10(11) Jones, and an on/off ratio up to ~ 10(4). Remarkably, when illuminated by the lights ranging from 405 to 808 nm, the biased devices yield a champion photoresponsivity of 191.5 A W(−1), a specific detectivity up to ~ 10(12) Jones, a photoconductive gain of 10(6)–10(7), and a photoresponsive time in the order of ~ 50 ms. These results provide a simple and competitive solution to the bandgap engineering of two-dimensional materials for device applications without the need for p–n junctions. [Image: see text] ELECTRONIC SUPPLEMENTARY MATERIAL: The online version of this article (10.1007/s40820-019-0361-2) contains supplementary material, which is available to authorized users.