Abstract: Local strain engineering and structural modification of 2D materials furnish benevolent control over their optoelectronic properties and provide an exciting approach to tune light–matter interaction in layered materials. Application of strain at the nanoscale is typically obtained through permanently deformed nanostructures such as nanowrinkles, which yield large band gap modulation, photoluminescence enhancement, and surface potential. Ultrathin transition metal dichalcogenides (TMDs) have been greatly analyzed for such purposes. Herein, we extend strain-induced nanoengineering to an emerging 2D material, CuInP2S6 (CIPS), and visualize extraordinary control over nonlinear light–matter interaction. Wrinkle nanostructures exhibit ∼160-fold enhancement in second harmonic generation (SHG) compared to unstrained regions, which is additionally influenced by a change in the dielectric environment. The SHG enhancement was significantly modulated by the percentage of applied strain which was numerically estimated. Furthermore, polarization-dependent SHG revealed quenching and enhancement in the parallel and perpendicular directions, respectively, due to the direction of the compressive vector. Our work provides an important advancement in controlling optoelectronic properties beyond TMDs for imminent applications in flexible electronics.

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