Comprehensive Anisotropic Linear Optical Properties of Weyl Semimetals, TaAs and NbAs

Since the experimental discovery of Weyl semimetals, they have attracted significant attention owing to their unique band structure and the chirality of their Weyl points. TaAs and NbAs are two of the earliest identified Weyl semimetals that possess broken inversion symmetry. Linear and nonlinear optics have been employed as tools to probe the Weyl physics in these crystals. Although some literature exists on their linear optical properties, a comprehensive study of its complete anisotropic dielectric function is presently missing. Here, we use eigen-cut crystals to fully determine the complete anisotropic dielectric functions of TaAs and NbAs by combining spectroscopic ellipsometry and density functional theory (DFT). Parameterized Lorentz oscillators are reported from 1.2-6 eV (experiment) and 0-6 eV (DFT). Strong resonances are found below 1 eV, which originate from Ta (5d) to Ta (5d) and As (4p) to Ta (5d) transitions. Given the popular laser wavelengths of 0.7, 1.55, and 3.1 eV, optical transitions near these energies are examined. The contribution of the band structure in the proximity of the Weyl cones to the total linear dielectric function is quantified relative to the contribution from the rest of the Brillouin zone. This analysis shows that the Weyl points contribution to the total dielectric function is highly anisotropic and rises below 0.5 eV; however, these contributions are negligible above 1 eV.