Spin dependence of ferroelectric polarization in the double exchange model for manganites

TL;DR

This paper develops a theoretical framework using the double exchange model and Berry phase theory to analyze how spin configurations influence ferroelectric polarization in manganites, explaining various magnetic and ferroelectric phenomena.

Contribution

The paper introduces a novel approach combining the DE model with Berry phase theory to quantify spin-dependent ferroelectric polarization in multiferroic manganites.

Findings

Polarization depends on magnetic state and spin arrangement.

Large polarization in inhomogeneous magnetic structures like HoMnO3.

Weaker polarization in more homogeneous spin spiral structures like TbMnO3.

Abstract

The double exchange (DE) model is systematically applied for studying the coupling between ferroelectric (FE) and magnetic orders in several prototypical types of multiferroic manganites. The model was constructed for the magnetically active Mn $3d$ bands in the basis of Wannier functions and include the effect of screened on-site Coulomb interactions. The essence of our approach for the FE polarization is to use the Berry phase theory, formulated in terms of occupied Wannier functions, and to evaluate the asymmetric spin-dependent change of these functions in the framework of the DE model. This enables us to quantify the effect of the magnetic symmetry breaking and derive several useful expressions for the electronic polarization ${\bf P}$, depending on the relative directions of spins. The proposed theory is applied to the solution of three major problems: (i) The magnetic-state dependence of ${\bf P}$ in hexagonal manganites; (ii) The microscopic relationship between canted ferromagnetism and ${\bf P}$ in monoclinic BiMnO$_3$; (iii) The origin of FE activity in orthorhombic manganites. We show that for an arbitrary noncollinear magnetic structure, propagating along the orthorhombic $\boldsymbol{b}$ axis and antiferromagnetically coupled $\boldsymbol{c}$, ${\bf P}$ can be obtained by scaling the one of the E-phase with the prefactor depending only on the relative directions of spins and being the measure of the spin inhomogeneity. This picture works equally well for the twofold (HoMnO$_3$) and fourfold (TbMnO$_3$) periodic manganites. The basic difference is that the twofold periodic magnetic structure is strongly inhomogeneous, that leads to large ${\bf P}$. On the contrary, the fourfold periodic magnetic structure can be viewed as a moderately distorted homogeneous spin spiral, which corresponds to weaker ${\bf P}$.