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Van der Waals (vdW) materials have recently attracted significant interest in the context of orientation-dependent linear and nonlinear optical properties. Recently, arsenic trisulfide (As₂S₃) or orpiment is identified as a new vdW layered material having anisotropic vibrational and optomechanical responses due to the reduced in-plane crystal symmetry, but its nonlinear optical response is still not well understood yet. Herein, the anisotropic third-harmonic generation (THG) response of mechanically exfoliated As₂S₃thin flakes is reported. The polarization-dependent evolution of THG emission from butterfly-shaped pattern to four-lobe pattern is comprehensively explored. Moreover, the third-order nonlinear susceptibility of As₂S₃crystal is extracted by analyzing the thickness-dependent THG emission. We anticipate that the discussed results will not only update the existing understanding on the nonlinear light-matter interaction in anisotropic vdW materials, but also promote future applications in integrated photonic circuits, on-chip nonlinear signal processing, and polarization-sensitive optical devices. 

Naturally occurring layered mineral livingstonite is identified as a new type of van der Waals (vdW) heterostructure based 2D material, consisting of two commensurately modulated alternating layers of HgSb₂S₄and Sb₂S₄. The heterostructures of livingstonite crystal are prepared as thin flakes via mechanical exfoliation method. The prepared livingstonite crystals are further investigated in the context of vibrational, linear, and nonlinear optical properties, including anisotropic Raman scattering, wavelength-dependent linear dichroism (LD) transition effect, birefringence, and anisotropic third-harmonic generation (THG). Owing to the monoclinic crystal structure, livingstonite crystals exhibit strong anisotropic vibrational and optical responses. In contrast to conventional vdW heterostructures, the anomalous LD transition effect and the evolution of butterfly-shaped THG emission pattern in livingstonite crystals are demonstrated. Furthermore, the third-order nonlinear susceptibility is estimated for livingstonite crystal using the thickness-dependent THG emission response. Overall, the discussed outcomes establish livingstonite as a new type of naturally grown vdW heterostructure based 2D material and offer insights in tailoring linear and nonlinear light-matter interactions in such vdW heterostructures, which may find further relevance in polarized optical applications and on-chip integrated photonic circuits.