Effects of crystal structure and on-site Coulomb interactions on the electronic and magnetic structure of A2Mo2O7 (A = Y, Gd, and Nd) pyrochlores -: art. no. 174406

Being motivated by recent experimental studies, we investigate magnetic structures of the Mo pyrochlores A(2)Mo(2)O(7) (A=Y, Nd, and Gd) and their impact on the electronic properties. The latter are closely related with the behavior of twelve Mo(t(2g)) bands, located near the Fermi level and well separated from the rest of the spectrum. We use a mean-field Hartree-Fock approach, which combines fine details of the electronic structure for these bands, extracted from the conventional calculations in the local-density approximation, the spin-orbit interaction, and the on-site Coulomb interactions among the Mo(4d) electrons, treated in the most general rotationally invariant form. The Coulomb repulsion U plays a very important role in the problem, and the semi-empirical value Usimilar to1.5-2.5 eV accounts simultaneously for the metal-insulator (MI) transition, the ferromagnetic (FM)-spin-glass (SG) transition, and for the observed enhancement of the anomalous Hall effect (AHE). The MI transition is mainly controlled by U. The magnetic structure at the metallic side is nearly collinear FM, due to the double exchange mechanism. The transition into the insulating state is accompanied by the large canting of spin and orbital magnetic moments. The sign of exchange interactions in the insulating state is controlled by the Mo-Mo distances. Smaller distances favor the antiferromagnetic coupling, which predetermines the SG behavior in the frustrated pyrochlore lattice. A large AHE is expected in the nearly collinear FM state, near the point of MI transition, and is related with the unquenched orbital magnetization at the Mo sites. We also predict a large magneto-optical effect in the same FM compounds.