Landau theory for the phase diagram of multiferroic Mn1−x(Fe,Zn,Mg)xWO4

Abstract

We present a theoretical analysis of the temperature-magnetic field-concentration phase diagram of the multiferroic Mn$_{1-x}$M$_{x}$WO$_{4}$ (M=Fe, Zn, Mg), which exhibits three ordered phases, with collinear and non-collinear incommensurate and with a commensurate magnetic order. The middle phase is also ferroelectric. The analysis uses a semi-phenomenological Landau theory, based on a Heisenberg Hamiltonian with a single-ion anisotropy. With a small number of adjustable parameters, the Landau theory gives an excellent fit to all three transition lines, as well as the magnetic and the ferroelectric order parameters. The fit of the magnetic and ferroelectric order parameters is further improved by including the effect of fluctuations near the transitions. We demonstrate the highly frustrated nature of these materials and suggest a simple explanation for the dramatic effects of doping with different magnetic ions at the Mn sites. The model enables an examination of different sets of exchange couplings that were proposed by a number of groups. Small discrepancies are probably a consequence of small errors in the experimental magnetic parameters. In addition, using the Ginzburg criterion we estimate the temperature range in which fluctuations of the order parameters become important.