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HighlightsDue to the Se composition and thickness gradient within single MoS 2(1− x ) Se 2 x   domains, the bandgap of MoS 2(1− x ) Se 2 x   is gradually tuned from 1.83 to 1.73 eV.    The homojunction phototransistors at zero bias 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 .    The biased devices yield a champion photoresponsivity of 191.5 A W −1 , a specific detectivity up to ~ 10 12  Jones, and a photoconductive gain of 10 6 –10 7 .Electronic supplementary material  The online version of this article (10.1007/s40820-019-0361-2) contains supplementary material, which is available to authorized users.

Spatially Bandgap-Graded MoS2(1−x)Se2x Homojunctions for Self-Powered Visible–Near-Infrared Phototransistors