Ferrimagnetic Double Perovskites Research Articles

Coexistence of topological Weyl and nodal-ring states in ferromagnetic and ferrimagnetic double perovskites

Magnetic topological quantum materials have attracted great attention due to their exotic topological quantum physics induced by the interplay among crystalology, magnetism, and topology, which is of profound importance to fundamental research and technology applications. However, limited materials are experimentally available, most of whom are realized by magnetic impurity doping or heterostructural constructions. In this work, based on the first-principles calculations, we predict that double perovskite Ba2CdReO6 is an intrinsic ferromagnetic topological semi-half-metal, while the ferrimagnetic double perovskite with space group symmetry Fm-3m, such as Ba2FeMoO6, belongs to a topological half-metal. One pair of Weyl points and fully spin-polarized nodal-ring states are found in the vicinity of the Fermi level in Ba2CdReO6. Its two-dimensional nearly flat drumhead surface states are fully spin-polarized. In Ba2FeMoO6, however, there exist four pairs of Weyl points and two fully spin-polarized nodal-rings near the Fermi level. These topological properties are stable in the presence of spin-orbit coupling. This makes these materials be an appropriate platform for studying the emerging intriguing properties, especially for the applications in spintronics, information technology, and topological superconductivity.

Tuning magnetic coercivity with external pressure in iron-rhenium based ferrimagnetic double perovskites

We studied the effect of physical pressure on the electronic and magnetic properties of ferrimagnetic double perovskites ${A}_{2}{\mathrm{FeReO}}_{6}$ ($A=\mathrm{Ca}$, Ba) using Re ${L}_{2,3}$ edge x-ray absorption spectroscopy and powder diffraction measurements. Volume compression is shown to dramatically increase the magnetic coercivity (${H}_{c}$) in polycrystalline samples of both compounds with $\mathrm{\ensuremath{\Delta}}{H}_{c}/\mathrm{\ensuremath{\Delta}}V\ensuremath{\sim}150$--200 $\mathrm{Oe}/{\AA{}}^{3}$. A nearly eight-fold increase in ${H}_{c}$, from 0.2 to 1.55 T, is obtained in ${\mathrm{Ba}}_{2}{\mathrm{FeReO}}_{6}$ at $P=29$ GPa. While no signs of structural phase transitions are seen in either sample to $\ensuremath{\sim}30$ GPa, the structural data points to a pressure-driven increase in tetragonal distortion of ${\mathrm{ReO}}_{6}$ octahedra. A sizable but pressure-independent Re orbital-to-spin magnetic moment ratio is observed, pointing to the critical role of spin-orbit interactions at Re sites. We present a ${j}_{\mathrm{eff}}$ description of the electronic structure that combines effects of crystal field and spin-orbit coupling on the Re $5{d}^{2}$ orbitals and use this description to provide insight into the pressure-induced enhancement of magnetic anisotropy.

Magnetism in Ca2CoOsO6 and Ca2NiOsO6: Unraveling the Mystery of Superexchange Interactions between 3d and 5d Ions

In order to rationalize and predict the behavior of compounds containing 5d transition metal ions, an understanding of the local moments and superexchange interactions from which their magnetic properties are derived is necessary. The magnetic and electrical properties of the ferrimagnetic double perovskites Ca2CoOsO6 and Ca2NiOsO6 studied here provide critical insight toward that goal. First-principles density functional theory (DFT) calculations indicate, and experimental measurements confirm, that the Os(VI) moments are directed antiparallel to the Co/Ni moments. X-ray magnetic circular dichroism (XMCD) measurements reveal that the orbital moment on osmium has a magnitude that is approximately 30% of the spin moment, and the two contributions oppose each other. Both the size and direction of the orbital moment are confirmed by the DFT calculations. The size of the Os(VI) total moment is predicted to be 0.6–0.7 μB by DFT calculations. The ferrimagnetic ground state is stabilized by strong antiferromagne...

Large Magnetization and Frustration Switching of Magnetoresistance in the Double‐Perovskite Ferrimagnet Mn2FeReO6

AbstractFerrimagnetic A2BB′O6 double perovskites, such as Sr2FeMoO6, are important spin‐polarized conductors. Introducing transition metals at the A‐sites offers new possibilities to increase magnetization and tune magnetoresistance. Herein we report a ferrimagnetic double perovskite, Mn2FeReO6, synthesized at high pressure which has a high Curie temperature of 520 K and magnetizations of up to 5.0 μB which greatly exceed those for other double perovskite ferrimagnets. A novel switching transition is discovered at 75 K where magnetoresistance changes from conventional negative tunneling behavior to large positive values, up to 265 % at 7 T and 20 K. Neutron diffraction shows that the switch is driven by magnetic frustration from antiferromagnetic Mn2+ spin ordering which cants Fe3+ and Re5+ spins and reduces spin‐polarization. Ferrimagnetic double perovskites based on A‐site Mn2+ thus offer new opportunities to enhance magnetization and control magnetoresistance in spintronic materials.

Large magnetization and frustration switching of magnetoresistance in the double-perovskite ferrimagnet Mn2FeReO6.

Ferrimagnetic A2 BB'O6 double perovskites, such as Sr2 FeMoO6 , are important spin-polarized conductors. Introducing transition metals at the A-sites offers new possibilities to increase magnetization and tune magnetoresistance. Herein we report a ferrimagnetic double perovskite, Mn2 FeReO6 , synthesized at high pressure which has a high Curie temperature of 520 K and magnetizations of up to 5.0 μB which greatly exceed those for other double perovskite ferrimagnets. A novel switching transition is discovered at 75 K where magnetoresistance changes from conventional negative tunneling behavior to large positive values, up to 265 % at 7 T and 20 K. Neutron diffraction shows that the switch is driven by magnetic frustration from antiferromagnetic Mn(2+) spin ordering which cants Fe(3+) and Re(5+) spins and reduces spin-polarization. Ferrimagnetic double perovskites based on A-site Mn(2+) thus offer new opportunities to enhance magnetization and control magnetoresistance in spintronic materials.

Structures, chemical states and properties of Sr2Fe1+xMo1−xO6 ceramics sintered in N2

We report that the Fe-rich single-phase Sr2Fe1+xMo1−xO6(x = 1/9, 1/6 and 1/3) ceramics can be synthesized in a N2 stream by the solid-state reaction method, while the usual Sr2FeMo2O6 (i.e. x = 0) can only be synthesized in a H2+Ar stream. X-ray diffraction shows that all ceramics are well crystallized with tetragonal symmetry. X-ray photoelectron spectroscopy results confirm that the chemical states of interior Fe and Mo cations are significantly more complex than those of the surface cations. With the increase in x, the materials change from ferrimagnetic (x = 0, 1/9, 1/6) to spin-glass-like behaviour (x = 1/3) and the magnetism decreases dramatically. The Curie temperature (Tc) and the magnetoresistance (MR) at 10 K with a field of 2 T (Tc, MR) are (400 K, −20.9%), (390 K, −10.3%) and (385 K, −4.5%) for x = 0, 1/9 and x = 1/6, respectively. The results are further analysed by Monte Carlo simulations. Our results show that high-Tc ferrimagnetic double perovskites with good magnetic and transport properties can be obtained conveniently in a N2 stream instead of conventional H2+Ar, which not only provides a safe and low-cost way to synthesize these materials, but may also be helpful in decreasing the oxygen vacancy concentration.

Magnetism in Re-based ferrimagnetic double perovskites

We have investigated spin and orbital magnetic moments of the Re 5d ion in the double perovskites A2FeReO6 (A=Ba, Sr, Ca) by x-ray magnetic circular dichroism (XMCD) at the Re L2, 3 edges. In these ferrimagnetic compounds, an unusually large negative spin and positive orbital magnetic moment at the Re atoms was detected. The presence of a finite spin magnetic moment in a ‘non-magnetic’ double perovskite as observed in the double perovskite Sr2ScReO6 proves that Re has also a small, but finite intrinsic magnetic moment. We further show for the examples of Ba and Ca that the usually neglected alkaline earth ions undoubtedly also contribute to the magnetism in the ferrimagnetic double perovskites.

Electron doping in the double perovskite LaxA2−xCrWO6 with A=Sr and Ca

The ferrimagnetic double perovskites can have high Curie temperatures TC above 600K. In the system Sr2FeMoO6 (TC≈420K) electron doping by substituting, for example, La3+ for Sr2+ ions leads to a considerable increase in TC. Here we report the same effect for LaxCa2−xCrWO6. This demonstrates that electron doping generically increases TC in the ferrimagnetic double perovskites. However, in the system Sr2CrWO6 (TC≈450K) the preferential formation of LaCrO3 prevents electron doping by La substitution as supported by neutron scattering and x-ray diffraction.

Magnetic moments of W5dinCa2CrWO6andSr2CrWO6double perovskites

We have investigated the magnetic moment of the W ion in the ferrimagnetic double perovskites Sr2CrWO6 and Ca2CrWO6 by X-ray magnetic circular dichroism (XMCD) at the W L(2,3) edges. In both compounds a finite negative spin and positive orbital magnetic moment was detected. The experimental results are in good agreement with band-structure calculations for (Sr/Ca)2CrWO6 using the full-potential linear muffin-tin orbital method. It is remarkable, that the magnetic ordering temperature, TC, is correlated with the magnetic moment at the 'non-magnetic' W atom.

Epitaxial growth of electron doped double perovskites [formula omitted] with [formula omitted] and Ca

Ferrimagnetic double perovskites are interesting for tunnel magnetoresistance (TMR) devices due to their high Curie-temperature and their half-metallicity. Because of the preferential formation of LaCrO 3, the synthesis of bulk samples of electron-doped La x Sr 2 - x CrWO 6 is difficult. However, due to the non-equilibrium growth conditions during pulsed laser deposition (PLD), the material can be grown as high-quality epitaxial film. We report the growth parameters of the compound La x Sr 2 - x CrWO 6 on SrTiO 3 substrates. Using reflection high-energy electron diffraction (RHEED) a layer-by-layer growth over the whole film thickness has been observed. Ca 2CrWO 6 grown on NdGaO 3 has worse crystalline quality and shows paramagnetic behavior.

Dynamical mean-field theory of double perovskite ferrimagnets

The dynamical mean field method is used to analyze the magnetic transition temperature and optical conductivity of a model for the ferrimagnetic double perovskites such as $Sr_2FeMoO_6$. The calculated transition temperatures and optical conductivities are found to depend sensitively on the band structure. For parameters consistent with local spin density approximation band calculations, the computed transition temperatures are lower than observed, and in particular decrease dramatically as band filling is increased, in contradiction to experiment. Band parameters which would increase the transition temperature are identified.

Metallic and nonmetallic double perovskites: A case study ofA2FeReO6(A=Ca, Sr, Ba)

We have investigated the structure and electronic properties of ferrimagnetic double perovskites, A2FeReO6 (A= Ca, Sr, Ba). The A=Ba phase is cubic (Fm3m) and metallic, while the A=Ca phase is monoclinic (P21/n) and nonmetallic. 57Fe Mossbauer spectroscopy shows that iron is present mainly in the high-spin (S=5/2) Fe3+ state in the Ca compound, while it occurs in an intermediate state between high-spin Fe2+ and Fe3+ in the Ba compound. It is argued that a direct Re t2g - Re t2g interaction is the main cause for the metallic character of the Ba compound; the high covalency of Ca-O bonds and the monoclinic distortion (which lifts the degeneracy of t2g states) seem to disrupt the Re-Re interaction in the case of the Ca compound, making it non-metallic for the same electron count.