Landau Analysis of the Symmetry of the Magnetic Structure and Magnetoelectric Interaction in Multiferroics

This paper presents a detailed instruction manual for constructing the Landau expansion for magnetoelectric coupling in incommensurate ferroelectric magnets, including Ni3V2O8, TbMnO3, MnWO4, TbMn2O5, YMn2O5, CuFeO2, and RbFe(MO4)2. The first step is to describe the magnetic ordering in terms of symmetry adapted coordinates which serve as complex-valued magnetic order parameters whose transformation properties are displayed. In so doing, we use the previously proposed technique to exploit inversion symmetry, since this symmetry has seemingly been universally overlooked. Inversion symmetry severely reduces the number of fitting parameters needed to describe the spin structure, usually by fixing the relative phases of the complex fitting parameters. By introducing order parameters of known symmetry to describe the magnetic ordering, we are able to construct the trilinear magnetoelectric interaction which couples incommensurate magnetic order to the uniform polarization, and thereby we treat many of the multiferroic systems so far investigated. In most cases, the symmetry of the magnetoelectric interaction determines the direction of the magnetically induced spontaneous polarization. We use the Landau description of the magnetoelectric phase transition to discuss the qualitative behavior of various susceptibilities near the phase transition. The consequences of symmetry for optical properties such as polarization induced mixing of Raman and infrared phonons and electromagnons are analyzed. The implication of this theory for microscopic models is discussed.