Strain Engineering of Second-Harmonic Generation and Symmetry Breaking in Few-Layer ε-InSe

ε-phase indium selenide (ε-InSe), a non-centrosymmetric van der Waals layered semiconductor, exhibits broken inversion symmetry in all layer numbers, giving rise to exceptional second-order nonlinear optical responses and holding great promise for nonlinear optoelectronic applications. The dynamic control of the nonlinear efficiency of ε-InSe is crucial for its engineering applications. However, the quantitative manipulation of second-harmonic generation (SHG) intensity and crystal symmetry in few-layer ε-InSe via strain engineering is still lacking. In this work, we systematically investigate the modulation of SHG intensity and angle-resolved SHG patterns in few-layer ε-InSe under uniaxial tensile strain. Using a home-built straining apparatus, we apply controlled tensile strain and measure the strain-dependent SHG responses. The experimental results demonstrate that the SHG intensity of few-layer ε-InSe shows a non-monotonic response to increasing tensile strain, first increasing and then decreasing. Concurrently, the sixfold symmetry of the SHG pattern is broken, confirming the significant strain-induced modulation of the lattice symmetry. This study provides a viable route for the design of flexible and tunable nonlinear optoelectronic devices based on ε-InSe.