Anisotropic Third Harmonic Generation in Two-Dimensional Tin Sulfide

Abstract: The in-plane anisotropic properties of two-dimensional (2D) group IV monochalcogenides provide an additional degree of freedom which can be used in future optoelectronic devices. Here, it is shown that the third harmonic generation (THG) signal produced by ultrathin tin (II) sulfide (SnS) is in-plane anisotropic with respect to the incident linear polarization of the laser field. We fit the experimental polarization-resolved THG (P-THG) measurements with a nonlinear optics model, which accounts for the orthorhombic crystal structure of 2D SnS. We calculate the relative magnitudes of the {chi}^3 tensor components by recording and simultaneously fitting both orthogonal components of the P-THG intensity. Furthermore, we introduce a THG anisotropy ratio, whose calculated values compare the total THG intensity when the excitation linear polarization is along the armchair crystallographic direction with the case when it is along the zigzag direction. Our results provide quantitative information on the anisotropic nature of the THG process in SnS, paving the way to a better understanding of anisotropic nonlinear light-matter interactions, and the development of polarization-sensitive nonlinear optical devices.