Magnetic properties of Ca-doped SrRuO3 from full-potential calculations

We have carried out accurate generalized-gradient-corrected fully-relativistic full-potential calculations for Sr_1−xCa_xRuO₃ (x=0, 0.25, 0.5, 0.75, and 1) in para-, ferro-, and A-, C-, and G-type antiferromagnetic configurations. We have performed electronic structure calculations for the experimentally observed orthorhombic structure as well as the hypothetical cubic structure. Our results are analyzed with the help of total, site-, spin-, and orbital-projected density of states. The total-energy studies show that CaRuO₃ stabilizes in the G-type antiferromagnetic state. The octahedral tilting owing to the relatively small radius of Ca²⁺ leads to weak hybridization between Ru 4d and O 2p. This weak hybridization along with exchange splitting causes a pseudogap-like feature close to the Fermi level, which should stabilize G-type antiferromagnetic ordering in CaRuO₃. However, powder neutron diffraction data on CaRuO₃ taken at 8 and do not show any magnetic peaks, implying that CaRuO₃ exhibits a spin-glass-like state with dominant short-range antiferromagnetic interaction. The calculated magnetic ground state of Sr_1−xCa_xRuO₃ is found to be consistent with the experimental findings. We have also calculated optical spectra as well as X-ray and ultra-violet photoemission spectra and Ru and O K-edge X-ray absorption spectra for G-type CaRuO₃ and found good agreement with available experimental spectra.