Orbital Dependent Phase Control in Ca2-xSrxRuO4

We present first-principles studies on the orbital states of the layered perovskites Ca$_{2-x}$Sr$_x$RuO$_4$. The crossover from antiferromagnetic (AF) Mott insulator for $x < 0.2$ to nearly ferromagnetic (FM) metal at $x=0.5$ is characterized by the systematic change of the $xy$ orbital occupation. For the AF side ($x < 0.2$), we present firm evidence for the $xy$ ferro-orbital ordering. It is found that the degeneracy of $t_{2g}$ (or $e_g$) states is lifted robustly due to the two-dimensional (2D) crystal-structure, even without the Jahn-Teller distortion of RuO$_6$. This effect dominates, and the cooperative occupation of $xy$ orbital is concluded. In contrast to recent proposals, the resulting electronic structure explains well both the observed X-ray absorption spectra and the double peak structure of optical conductivity. For the FM side ($x=0.5$), however, the $xy$ orbital with half filling opens a pseudo-gap in the FM state and contributes to the spin $S$=1/2 moment (rather than $S$=1 for $x$=0.0 case) dominantly, while $yz,zx$ states are itinerant with very small spin polarization, explaining the recent neutron data consistently.Comment: 17 pages, 5 figure

Local Charge Excesses in Metallic Alloys: a Local Field Coherent Potential Approximation Theory

Electronic structure calculations performed on very large supercells have shown that the local charge excesses in metallic alloys are related through simple linear relations to the local electrostatic field resulting from distribution of charges in the whole crystal. By including local external fields in the single site Coherent Potential Approximation theory, we develop a novel theoretical scheme in which the local charge excesses for random alloys can be obtained as the responses to local external fields. Our model maintains all the computational advantages of a single site theory but allows for full charge relaxation at the impurity sites. Through applications to CuPd and CuZn alloys, we find that, as a general rule, non linear charge rearrangements occur at the impurity site as a consequence of the complex phenomena related with the electronic screening of the external potential. This nothwithstanding, we observe that linear relations hold between charge excesses and external potentials, in quantitative agreement with the mentioned supercell calculations, and well beyond the limits of linearity for any other site property.Comment: 11 pages, 1 table, 7 figure

Screened Coulomb interactions in metallic alloys: II Screening beyond the single-site and atomic sphere approximations

A quantitative description of the configurational part of the total energy of metallic alloys with substantial atomic size difference cannot be achieved in the atomic sphere approximation: It needs to be corrected at least for the multipole moment interactions in the Madelung part of the one-electron potential and energy. In the case of a random alloy such interactions can be accounted for only by lifting the atomic sphere and single-site approximations, in order to include the polarization due to local environment effects. Nevertheless a simple parameterization of the screened Coulomb interactions for the ordinary single-site methods, including the generalized perturbation method, is still possible. We obtained such a parameterization for bulk and surface NiPt alloys, which allows one to obtain quantitatively accurate effective interactions in this system.Comment: 24 pages, 2 figure