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HighlightsA self-powered α-In 2 Se 3 /3R MoS 2  heterojunction is successfully developed and shows strong photo response to the visible and near infrared light.    The heterojunction photodetector delivers an ultrahigh photoresponsivity of 2.9 × 10 3  A W −1  and a substantial specific detectivity of 6.2 × 10 10  Jones under a compressive strain of − 0.26%.    This work demonstrates that the transport of photo generated carriers is clearly modulated by mechanical stimuli through the piezo-phototronic effect at the heterojunction interface.Supplementary material  The online version contains supplementary material available at (10.1007/s40820-020-00584-1) contains supplementary material, which is available to authorized users.

Strain-Modulated Photoelectric Responses from a Flexible α-In2Se3/3R MoS2 Heterojunction