Femtosecond Laser-Induced Anisotropic Structure and Nonlinear Optical Response of Yttria-Stabilized Zirconia Single Crystals with Different Planes

Nonlinear optical properties have been extensively studied due to their promising nonlinear effects and various applications. With ultrashort duration and ultrahigh intensity, a femtosecond laser can fabricate various superior-quality micro-/nanostructures to improve the nonlinearity of materials, which are promising for stable and high-performance nonlinear devices. In this contribution, yttria-stabilized zirconia (YSZ) with fs laser-induced micro-/nanostructures is demonstrated to exhibit unique anisotropic light–material interaction and nonlinear optical response on [100], [110], and [111] planes. Time-resolved reflectivity of YSZ after fs laser excitation is investigated by a pump–probe experiment, which is consistent with simulations through the plasma model combined with a two-temperature model. These results indicate two early ablation mechanisms: Coulomb explosion and melting. Anisotropic crack structures are formed due to thermal stress, which is always ignored in fs laser fabrication and is verified by Raman mapping and analysis of slip systems on different crystal planes. Through the z-scan measurement, the nonlinear absorption (NLA) of crack structures is effectively improved, and a nearly 18 times enhancement of the NLA coefficient is acquired in [100] samples, while a 2 times enhancement in [110] and [111] samples. Such great enhancement of NLA is mainly due to the abundant presence of crack structures and the increase of fs laser-induced oxygen vacancies in [100] YSZ. These results provide a potential way of utilizing fs laser to improve the nonlinearity for the technological development in nonlinear devices.