Anisotropy of 2PA, 3PA, and Kerr effect in nonpolar ZnO

Anisotropic optical nonlinearity plays an important role in polarization-dependent optoelectronic devices. Taking the advantage of in-plane crystallographic axis, the polarization dependence of third- and fifth-order nonlinearity in nonpolar ZnO has been investigated by z scan. Here, we established the theory model of anisotropic relation of fifth-order nonlinearity in hexagonal wurtzite crystal. Both two-photon absorption (2PA) and three-photon absorption (3PA) coefficients exhibit anisotropic oscillations with a period of 180^◦, and the polarization modulation factor and anisotropy coefficient (r_p, σ) are measured as (2.10, 1.84) for β₂, and (1.66, 1.33) for β₃, respectively. This is the first time, to the best of our knowledge, that the anisotropy of the fifth-order optical nonlinear effect has been characterized and confirmed. It is verified that the self-defocusing effect at 500 nm is isotropy, while the self-focusing effect at 800 nm exhibits significant anisotropy. The maximum value of the nonlinear figure of merit is 5.84 along the [0010] crystalline direction, nearly 1.6 times the minimum value, revealing that ZnO exhibits potential for nonlinear applications containing polarization-related all-optical switching components.