Optical anisotropy offers a heightened degree of flexibility in shaping optical properties and designing cutting-edge devices. Quasi-one-dimensional Ta2NiS5, with giant optical anisotropy, has been used in the development of new lasers and sensors. In this research endeavor, we successfully acquired the complete dielectric tensor of Ta2NiS5, utilizing the advanced technique of Mueller matrix spectroscopic ellipsometry, enabling a rigorous quantitative assessment of its optical anisotropy. The results indicate that Ta2NiS5 demonstrates giant birefringence and dichroism, with Δnmax = 1.54 and Δkmax = 1.80. This pursuit also delves into the fundamental underpinnings of this optical anisotropy, drawing upon a fusion of first-principles calculations and critical points analysis. The anisotropy of Ta2NiS5 arises from differences in optical transitions in different directions and is shown to be due to van Hove singularities without exciton effects. Its giant optical anisotropy is expected to be useful in the design of novel optical devices, and the revelation of the physical mechanism facilitates the modulation of its optical properties.
Keywords: Mueller matrix spectroscopic ellipsometry; Ta2NiS5; critical points analysis; dielectric tensor; optical anisotropy.