Spiral ground state against ferroelectricity in the frustrated magnet BiMnFe2O6

The spiral magnetic structure and underlying spin lattice of BiMnFe2O6 are investigated by low-temperature neutron powder diffraction and density functional theory band structure calculations. In spite of the random distribution of the Mn3+ and Fe3+ cations, this compound undergoes a transition into an incommensurate antiferromagnetically ordered state below TN ~ 220 K. The magnetic structure is characterized by the propagation vector k=[0,beta,0] with beta ~ 0.14 and the P22_12_11'(0 \beta 0)0s0s magnetic superspace symmetry. It comprises antiferromagnetic helixes propagating along the b-axis. The magnetic moments lie in the ac plane and rotate about pi*(1+beta) ~ 204.8 deg angle between the adjacent magnetic atoms along b. The spiral magnetic structure arises from the peculiar frustrated arrangement of exchange couplings in the ab plane. The antiferromagnetic coupling along the c-axis leads to the cancellation of electric polarization, and results in the lack of ferroelectricity in BiMnFe2O6.Comment: 11 pages, 8 figures, 8 table

Magnetic and electric properties of double-perovskites and estimation of their Curie temperatures by ab initio calculations

First principles electronic structure calculations have been carried out on ordered double perovskites Sr_2B'B"O_6 (for B' = Cr or Fe and B" 4d and 5d transition metal elements) with increasing number of valence electrons at the B-sites, and on Ba_2MnReO_6 as well as Ba_2FeMoO_6. The Curie temperatures are estimated ab initio from the electronic structures obtained with the local spin-density functional approximation, full-potential generalized gradient approximation and/or the LDA+U method (U - Hubbard parameter). Frozen spin-spirals are used to model the excited states needed to evaluate the spherical approximation for the Curie temperatures. In cases, where the induced moments on the oxygen was found to be large, the determination of the Curie temperature is improved by additional exchange functions between the oxygen atoms and between oxygen and B' and B" atoms. A pronounced systematics can be found among the experimental and/or calculated Curie temperatures and the total valence electrons of the transition metal elements.Comment: 8 pages, 11 figures. Submitted to the Physical Review

Antiferromagnetic structure and electronic properties of BaCr2As2 and BaCrFeAs2

The chromium arsenides BaCr2As2 and BaCrFeAs2 with ThCr2Si2 type structure (space group I4/mmm; also adopted by '122' iron arsenide superconductors) have been suggested as mother compounds for possible new superconductors. DFT-based calculations of the electronic structure evidence metallic antiferromagnetic ground states for both compounds. By powder neutron diffraction we confirm for BaCr2As2 a robust ordering in the antiferromagnetic G-type structure at T_N = 580 K with mu_Cr = 1.9 mu_B at T = 2K. Anomalies in the lattice parameters point to magneto-structural coupling effects. In BaCrFeAs2 the Cr and Fe atoms randomly occupy the transition-metal site and G-type order is found below 265 K with mu_Cr/Fe = 1.1 mu_B. 57Fe Moessbauer spectroscopy demonstrates that only a small ordered moment is associated with the Fe atoms, in agreement with electronic structure calculations with mu_Fe ~ 0. The temperature dependence of the hyperfine field does not follow that of the total moments. Both compounds are metallic but show large enhancements of the linear specific heat coefficient gamma with respect to the band structure values. The metallic state and the electrical transport in BaCrFeAs2 is dominated by the atomic disorder of Cr and Fe and partial magnetic disorder of Fe. Our results indicate that Neel-type order is unfavorable for the Fe moments and thus it is destabilized with increasing iron content.Comment: 14 pages, 14 figures, submitted to Physical Review

Micromagnetic and Magnetoresistance Studies of Ferromagnetic La\u3csub\u3e0.83\u3c/sub\u3eSr\u3csub\u3e0.13\u3c/sub\u3eMnO\u3csub\u3e2.98\u3c/sub\u3e Crystals

Magnetic force microscopy (MFM) and atomic force microscopy (AFM) were used to investigate the surface topography and micromagnetic structure of La0.83Sr0.13MnO2.98 single crystals with colossal magnetoresistance (CMR). The crystals were grown by fused salt electrolysis and characterized by chemical analysis, X-ray diffraction, magnetic and transport measurements. The crystals are rhombohedral (R 3 c). Magnetic and transport measurements indicate that the ferromagnetic ordering at 310 K is associated with an insulator-metal transition at the same temperature. A maximum negative magnetoresistance (-62 %) is observed at 290 K in an applied magnetic field of 5 T. The magnetoresistance increases in magnitude sharply (1.8 %), comparing to the rest of the change, with increasing magnetic field up to 20 G, and then it increases slowly with increasing field. MFM and AFM were used to study the (110) surface as well as a number of unspecified surfaces. Surface topography of an as-grown crystal exhibits well-developed surface corrugations due to extensive twinning. The corrugation angle at twin boundaries can be related to the unit cell parameters, surface and twinning planes. Magnetic force microscopy images show that magnetic domain boundaries are pinned to the crystallographic twins; a small number of unpinned boundaries are observed. The statistical analysis of domain boundary angle distribution is consistent with cubic magnetocrystalline anisotropy with easy axis along [100] directions for this material. Unusual magnetization behavior in the vicinity of topological defects on the surface is also reported. MFM contrast was found to disappear above the ferromagnetic Curie temperature; after cooling a new magnetic structure comprised of Bloch walls of opposite chiralities developed

Pressure-induced magnetic collapse and metallization of TlFe1.6Se2\mathrm{TlF}{\mathrm{e}}_{1.6}\mathrm{S}{\mathrm{e}}_{2}

The crystal structure, magnetic ordering, and electrical resistivity of TlFe1.6Se2 were studied at high pressures. Below ~7 GPa, TlFe1.6Se2 is an antiferromagnetically ordered semiconductor with a ThCr2Si2-type structure. The insulator-to-metal transformation observed at a pressure of ~ 7 GPa is accompanied by a loss of magnetic ordering and an isostructural phase transition. In the pressure range ~ 7.5 - 11 GPa a remarkable downturn in resistivity, which resembles a superconducting transition, is observed below 15 K. We discuss this feature as the possible onset of superconductivity originating from a phase separation in a small fraction of the sample in the vicinity of the magnetic transition.Comment: 12 pages, 5 figure

Crystal Growth and Unusual Electronic Transport Properties of Some Reduced Molybdenum Oxides with Bi-Octahedral Mo10 Clusters

Single crystals of AM05O3 (A = Ca, Sr, La-Gd), suitable for electrical conductivity measurements have been grown by high temperature and fused salt electrolytic techniques. The structures of all of these compounds are dominated by the presence of bi-octahedral clusters of Mo atoms joined together parallel to the monoclinic a axis, forming infinite chains. Temperature dependent electrical resistivity measurements on AMo5Og (A = La, Ce, Pr, Nd, Sm) show anomalous metal-semiconductor transitions near 180 and 30 K. The resistivities of the Eu and Gd analogues are different, in that the former is semiconducting while the latter shows a weak anomaly ~ 110 K. The Ca and Sr analogues are also semiconducting in the range 20-300 K. The electrical conductivity of these phases appears to be closely related to the inter-cluster separation and the number of metal-cluster electrons. The magnetic susceptibility of these compounds show no anomalies at the temperatures corresponding to the transitions seen in their electrical resistivities. The magnetic susceptibility of LaMosOg shows a small decrease in the !y (dy/dT) vs T plot in the vicinity of ~ 150 K

Designing Polar and Magnetic Oxides: Zn2FeTaO6 - in Search of Multiferroics

Polar oxides are technically of great interest but difficult to prepare. Our recent discoveries predicted that polar oxides can be synthesized in the corundum-derivative A2BB′O6 family with unusually small cations at the A-site and a d0 electron configuration ion at B′-site. When magnetic transition-metal ions are incorporated more interesting polar magnetic oxides can form. In this work we experimentally verified this prediction and prepared LiNbO3 (LN)-type polar magnetic Zn2FeTaO6 via high pressure and temperature synthesis. The crystal structure analysis indicates highly distorted ZnO6 and (Fe/Ta)O6 octahedra, and an estimated spontaneous polarization (PS) of ∼50 μC/cm2 along the c-axis was obtained from point charge model calculations. Zn2Fe3+Ta5+O6 has a lower magnetic transition temperature (TN ∼ 22 K) than the Mn2FeTaO6 analogue but is less conductive. The dielectric and polarization measurements indicate a potentially switchable component