Pressure-induced structural, electronic, and magnetic effects in BiFeO3

We present a first-principles study of multiferroic BiFeO3 at high pressures. Our work reveals the main structural (change in Bi's coordination and loss of ferroelectricity), electronic (spin crossover and metallization), and magnetic (loss of order) effects favored by compression and how they are connected. Our results are consistent with the striking manifold transition observed experimentally by Gavriliuk et al. [Phys. Rev. B 77, 155112 (2008)] and provide an explanation for it.Comment: 4 pages with 4 figures embedded. More information at http://www.icmab.es/dmmis/leem/jorg

Pressure dependence of the Curie temperature in Ni2MnSn Heusler alloy: A first-principles study

The pressure dependence of electronic structure, exchange interactions and Curie temperature in ferromagnetic Heusler alloy Ni2MnSn has been studied theoretically within the framework of the density-functional theory. The calculation of the exchange parameters is based on the frozen--magnon approach. The Curie temperature, Tc, is calculated within the mean-field approximation by solving the matrix equation for a multi-sublattice system. In agrement with experiment the Curie temperature increased from 362K at ambient pressure to 396 at 12 GPa. Extending the variation of the lattice parameter beyond the range studied experimentally we obtained non-monotonous pressure dependence of the Curie temperature and metamagnetic transition. We relate the theoretical dependence of Tc on the lattice constant to the corresponding dependence predicted by the empirical interaction curve. The Mn-Ni atomic interchange observed experimentally is simulated to study its influence on the Curie temperature.Comment: 8 pages, 8 figure

Magnetoelectric Effect and Spontaneous Polarization in HoFe3_3(BO3_3)4_4 and Ho0.5_{0.5}Nd0.5_{0.5}Fe3_3(BO3_3)4_4

The thermodynamic, magnetic, dielectric, and magnetoelectric properties of HoFe$_3$(BO$_3$)$_4$ and Ho$_{0.5}$Nd$_{0.5}$Fe$_3$(BO$_3$)$_4$ are investigated. Both compounds show a second order Ne\'{e}l transition above 30 K and a first order spin reorientation transition below 10 K. HoFe$_3$(BO$_3$)$_4$ develops a spontaneous electrical polarization below the Ne\'{e}l temperature (T$_N$) which is diminished in external magnetic fields. No magnetoelectric effect could be observed in HoFe$_3$(BO$_3$)$_4$. In contrast, the solid solution Ho$_{0.5}$Nd$_{0.5}$Fe$_3$(BO$_3$)$_4$ exhibits both, a spontaneous polarization below T$_N$ and a magnetoelectric effect at higher fields that extends to high temperatures. The superposition of spontaneous polarization, induced by the internal magnetic field in the ordered state, and the magnetoelectric polarizations due to the external field results in a complex behavior of the total polarization measured as a function of temperature and field.Comment: 12 pages, 15 figure

Role of the conduction electrons in mediating exchange interactions in Heusler alloys

Because of large spatial separation of the Mn atoms in Heusler alloys the Mn 3d states belonging to different atoms do not overlap considerably. Therefore an indirect exchange interaction between Mn atoms should play a crucial role in the ferromagnetism of the systems. To study the nature of the ferromagnetism of various Mn-based semi- and full-Heusler alloys we perform a systematic first-principles calculation of the exchange interactions in these materials. The calculation of the exchange parameters is based on the frozen-magnon approach. The calculations show that the magnetism of the Mn-based Heusler alloys depends strongly on the number of conduction electrons, their spin polarization and the position of the unoccupied Mn 3d states with respect to the Fermi level. Various magnetic phases are obtained depending on the combination of these characteristics. The Anderson's s-d model is used to perform a qualitative analysis of the obtained results. The conditions leading to diverse magnetic behavior are identified. If the spin polarization of the conduction electrons at the Fermi energy is large and the unoccupied Mn 3d states lie well above the Fermi level, an RKKY-type ferromagnetic interaction is dominating. On the other hand, the contribution of the antiferromagnetic superexchange becomes important if unoccupied Mn 3d states lie close to the Fermi energy. The resulting magnetic behavior depends on the competition of these two exchange mechanisms. The calculational results are in good correlation with the conclusions made on the basis of the Anderson s-d model which provides useful framework for the analysis of the results of first-principles calculations and helps to formulate the conditions for high Curie temperature.Comment: 16 pages, 9 figures, 2 table

Material-Specific Investigations of Correlated Electron Systems

We present the results of numerical studies for selected materials with strongly correlated electrons using a combination of the local-density approximation and dynamical mean-field theory (DMFT). For the solution of the DMFT equations a continuous-time quantum Monte-Carlo algorithm was employed. All simulations were performed on the supercomputer HLRB II at the Leibniz Rechenzentrum in Munich. Specifically we have analyzed the pressure induced metal-insulator transitions in Fe2O3 and NiS2, the charge susceptibility of the fluctuating-valence elemental metal Yb, and the spectral properties of a covalent band-insulator model which includes local electronic correlations.Comment: 14 pages, 7 figures, to appear in "High Performance Computing in Science and Engineering, Garching 2009" (Springer

Pressure-Induced Electronic Spin Transition of Iron in Magnesiow?stite-(Mg,Fe)O

An electronic transition of iron in magnesiowuestite has been studied with synchrotron Moessbauer and X-ray emission spectroscopies under high pressures. Synchrotron Moessbauer studies show that the quadrupole splitting disappears and the isomer shift drops significantly across the spin-paring transition of iron in (Mg{sub 0.75},Fe{sub 0.25})O between 62 and 70 GPa, whereas X-ray emission spectroscopy of the Fe-K{sub {beta}} fluorescence lines in dilute (Mg{sub 0.95},Fe{sub 0.05})O also confirms that a high-spin to low-spin transition occurs between 46 GPa and 55 GPa. Based upon current results and percolation theory, we reexamine the high-pressure phase diagram of (Mg,Fe)O and find that iron-iron exchange interaction plays an important role in stabilizing the high-spin state of iron in FeO-rich (Mg,Fe)O

Magnetoelectric ordering of BiFeO3 from the perspective of crystal chemistry

In this paper we examine the role of crystal chemistry factors in creating conditions for formation of magnetoelectric ordering in BiFeO3. It is generally accepted that the main reason of the ferroelectric distortion in BiFeO3 is concerned with a stereochemical activity of the Bi lone pair. However, the lone pair is stereochemically active in the paraelectric orthorhombic beta-phase as well. We demonstrate that a crucial role in emerging of phase transitions of the metal-insulator, paraelectric-ferroelectric and magnetic disorder-order types belongs to the change of the degree of the lone pair stereochemical activity - its consecutive increase with the temperature decrease. Using the structural data, we calculated the sign and strength of magnetic couplings in BiFeO3 in the range from 945 C down to 25 C and found the couplings, which undergo the antiferromagnetic-ferromagnetic transition with the temperature decrease and give rise to the antiferromagnetic ordering and its delay in regard to temperature, as compared to the ferroelectric ordering. We discuss the reasons of emerging of the spatially modulated spin structure and its suppression by doping with La3+.Comment: 18 pages, 5 figures, 3 table

Anomalous high-temperature superconductivity in YH6_6

Pressure-stabilized hydrides are a new rapidly growing class of high-temperature superconductors which is believed to be described within the conventional phonon-mediated mechanism of coupling. Here we report the synthesis of yttrium hexahydride Im3m-YH$_6$ that demonstrates the superconducting transition with T$_c$ = 224 K at 166 GPa, much lower than the theoretically predicted (>270 K). The measured upper critical magnetic field B$_c$$_2$(0) of YH$_6$ was found to be 116-158 T, which is 2-2.5 times larger than the calculated value. A pronounced shift of T$_c$ in yttrium deuteride YD$_6$ with the isotope coefficient 0.4 supports the phonon-assisted superconductivity. Current-voltage measurements showed that the critical current I$_c$ and its density J$_c$ may exceed 1.75 A and 3500 A/mm$^2$ at 0 K, respectively, which is comparable with the parameters of commercial superconductors, such as NbTi and YBCO. The superconducting density functional theory (SCDFT) and anharmonic calculations suggest unusually large impact of the Coulomb repulsion in this compound. The results indicate notable departures of the superconducting properties of the discovered YH$_6$ from the conventional Migdal-Eliashberg and Bardeen-Cooper-Schrieffer theories.Comment: arXiv admin note: text overlap with arXiv:1902.1020