Second-order nonlinear piezo-optic properties of single crystal lithium niobate thin films

Stress plays a crucial role in thin films and layered systems, and thus significantly influences the material's electrical, mechanical and (nonlinear) optical responses. Despite lithium niobate's wide applicability as a nonlinear optical material, the impact of mechanical stress on its nonlinear optical properties is not well characterized. In this work, we systematically study both experimentally and theoretically, the nonlinear optical responses of thin film lithium niobate (TFLN) single crystals. Compressive and tensile stress is applied in our experiment using a piezodriven strain cell. We then record the second-harmonic-generated (SHG) response in back-reflection geometry, and compare these results to theoretical modeling using density functional theory (DFT). Both methods consistently reveal that uniaxial stress induces changes of the nonlinear optical susceptibility of certain tensor elements on the order of up to 1 pm/(V GPa). The exact value depends on the tensor element that is addressed in our SHG analysis, on the crystal orientation, and also whether using compressive or tensile stresses. Furthermore, a lowering of the crystal symmetry when applying stress along the <a:math xmlns:a="http://www.w3.org/1998/Math/MathML"><a:mi>x</a:mi></a:math> or <b:math xmlns:b="http://www.w3.org/1998/Math/MathML"><b:mi>y</b:mi></b:math> crystallographic axes is observed by the appearance of new nonlinear optical tensor elements within the strained crystals.