Electronic structure and resonant inelastic x-ray scattering in Ta2NiSe5

Abstract: We study the electronic structure of Ta2NiSe5 in its low-temperature semiconducting phase, using resonant inelastic x-ray scattering (RIXS) at the Ta L3 edge. We also investigate the electronic properties of Ta2NiSe5 within the density-functional theory using the generalized gradient approximation in the framework of the fully relativistic spin-polarized Dirac linear muffin-tin orbital band-structure method. While ARPES, dc transport, and optical measurements indicate that Ta2NiSe5 is a small band-gap semiconductor, DFT gives a metallic nonmagnetic solution in Ta2NiSe5 . To obtain the semiconducting ground state in Ta2 NiSe5 we use a self-interaction correction (SIC) procedure by introducing an orbital-dependent potential Vl into the Hamiltonian. We investigate theoretically the x-ray absorption spectroscopy (XAS) and RIXS spectra at the Ni and Ta L3 edges and analyze the spectra in terms of interband transitions. We investigate the RIXS spectra as a function of momentum transfer vector Q and incident photon energy. Because Ta2 NiSe5 possesses only fully occupied (Ni 3d and Se 4p) and completely empty (Ta 5d) shells with the formal valencies Ta5+ (5d0), Ni0 (3d10 ), and Se2- (4p6 ), both the Ni and Ta L3 RIXS spectra belong to a charge transfer type with ligand-to-metal excitations.