Anisotropic Third Harmonic Generation in 2D Tin Sulfide

Abstract The in‐plane anisotropic properties of 2D group IV monochalcogenides offer an additional degree of freedom which can be advantageous in optoelectronic applications. Here, it is demonstrated that the third harmonic generation (THG) produced by ultrathin tin (II) sulfide (SnS) is in‐plane anisotropic with respect to the direction of the excitation linear polarization. The polarization‐resolved THG (P‐THG) measurements are described with a nonlinear optics model, which accounts for the orthorhombic crystal structure of the 2D SnS. The relative magnitudes of the χ⁽³⁾ tensor components are calculated by recording and simultaneously fitting two orthogonal polarization components of the P‐THG signals. Furthermore, the “THG anisotropy ratio” is introduced, which compares the THG intensity produced when the excitation linear polarization is along the armchair crystallographic direction, with the case when it is along the zigzag direction. The experimental findings provide quantitative information on the anisotropic nature of the THG process in various SnS flakes. Nonlinear anisotropic 2D materials can be used in future optoelectronic devices, where anisotropic polarization sensitivity is required. Having an optical tool that quantitatively probes the effect of the in‐plane anisotropy among different 2D materials, could be of considerable importance for evaluating the performance of such materials and devices.