Giant Light Emission Enhancement in Strain-Engineered InSe/MS₂ (M = Mo or W) van der Waals Heterostructures

Two-dimensional (2D) heterostructures (HSs) offer unlimited possibilities for playing with layer number, order, and twist angle. The realization of high-performance optoelectronic devices, however, requires the achievement of specific band alignments, <i>k</i>-space matching between conduction and valence band extrema, and efficient charge transfer between the constituent layers. Fine-tuning mechanisms to design ideal HSs are lacking. Here, we show that layer-selective strain engineering can be exploited as an extra degree of freedom to tailor the band alignment and optical properties of 2D HSs. To that end, strain is selectively applied to MS₂ (M = Mo or W) monolayers in InSe/MS₂ HSs, triggering a giant photoluminescence enhancement of the highly tunable but weakly emitting InSe of up to >2 orders of magnitude. Resonant excitation measurements, supported by first-principles calculations, provide evidence of a strain-activated charge transfer from the MS₂ monolayers toward InSe. The huge emission enhancement of InSe widens its range of applications for optoelectronics.