Origin of ferroelectricity in the multiferroic barium fluorides BaMF4

We present a first principles study of the series of multiferroic barium fluorides with the composition BaMF4, where M is Mn, Fe, Co, or Ni. We discuss trends in the structural, electronic, and magnetic properties, and we show that the ferroelectricity in these systems results from the "freezing in" of a single unstable polar phonon mode. In contrast to the case of the standard perovskite ferroelectrics, this structural distortion is not accompanied by charge transfer between cations and anions. Thus, the ferroelectric instability in the multiferroic barium fluorides arises solely due to size effects and the special geometrical constraints of the underlying crystal structure.Comment: 8 pages, 6 figures, 3 table

Observation of Substitutional Site Preference in a Quasicrystal and Implication on Local Structure

A combination of magnetic susceptibility and Mössbauer measurements on quasicrystalline i-Al74Mn20-xFexSi6 (0.02≤x≤7.5) establishes that Mn atoms in i-Al74Mn20Si6 occupy two distinct classes of sites, and that Fe substitutes for only one of them. The two classes are distinguished by the possession or otherwise of a localized magnetic moment. The data are consistent with a structure of interconnecting Mackay icosahedra (MI) in which localized moments are possessed only by Mn atoms adjacent to broken MI connections. The implied connectivity of the resulting MI network is close to that anticipated for a packing of MI on a three-dimensional Penrose-tile lattice

Towards a microscopic theory of toroidal moments in bulk periodic crystals

We present a theoretical analysis of magnetic toroidal moments in periodic systems, in the limit in which the toroidal moments are caused by a time and space reversal symmetry breaking arrangement of localized magnetic dipole moments. We summarize the basic definitions for finite systems and address the question of how to generalize these definitions to the bulk periodic case. We define the toroidization as the toroidal moment per unit cell volume, and we show that periodic boundary conditions lead to a multivaluedness of the toroidization, which suggests that only differences in toroidization are meaningful observable quantities. Our analysis bears strong analogy to the modern theory of electric polarization in bulk periodic systems, but we also point out some important differences between the two cases. We then discuss the instructive example of a one-dimensional chain of magnetic moments, and we show how to properly calculate changes of the toroidization for this system. Finally, we evaluate and discuss the toroidization (in the local dipole limit) of four important example materials: BaNiF_4, LiCoPO_4, GaFeO_3, and BiFeO_3.Comment: replaced with final (published) version, which includes some changes in the text to improve the clarity of presentatio