Magnetization induced local electric dipoles and multiferroic properties of Ba2CoGe2O7

Abstract

Ba2CoGe2O7, crystallizing in the noncentrosymmetric but nonpolar structure, belongs to a special class of multiferroic materials, whose properties are predetermined by the rotoinversion symmetry. Unlike inversion, the rotoinversion symmetry can be easily destroyed by the magnetization. Moreover, due to specific structural pattern, the magnetic structure of Ba2CoGe2O7 is relatively soft. Altogether, this leads to the rich variety of multiferroic properties, where the magnetic structure can be easily deformed by the magnetic field, inducing the electric polarization in the direction, which depends on the direction of the magnetic field. In this paper, we show that all these properties can be successfully explained on the basis of realistic low-energy model, derived from the first-principles electronic structure calculations for the magnetically active Co 3d bands, and the Berry-phase theory of electric polarization. Particularly, we argue that the magnetization induced electric polarization in Ba2CoGe2O7 is essentially local and expressed via the expectation values of some dipole matrices, calculated in the Wannier basis of the model, and the site-diagonal density matrices of the magnetic Co sites. Thus, the basic aspects of the behavior of Ba2CoGe2O7 can be understood already in the atomic limit, where both magnetic anisotropy and magnetoelectric coupling are specified by density matrix. Then, the macroscopic polarization can be found as a superposition of electric dipoles of the individual Co sites. We discuss the behavior of interatomic magnetic interactions, main contributions to the magnetocrystalline anisotropy and the spin canting, as well as the similarities and differences of the proposed picture from the phenomenological model of spin-dependent p-d hybridization.