Anisotropic Second-Harmonic Generation From Monocrystalline Gold Flakes

Noble metals with well-defined crystallographic orientation constitute an appealing class of materials for controlling light-matter interactions on the nanoscale. Nonlinear optical processes, being particularly sensitive to anisotropy, are a natural and versatile probe of crystallinity in nano-optical devices. Here we study the nonlinear optical response of monocrystalline gold flakes, revealing a polarization dependence in second-harmonic generation from the {111} surface that is markedly absent in polycrystalline films. Our findings confirm that second-harmonic microscopy is a robust and non-destructive method for probing the crystallographic orientation of gold, and can serve as a guideline for enhancing nonlinear response in plasmonic systems.