No Arabic abstract
We present a comprehensive study on the magnetic structure, dynamics, and phase evolution in the single-phase double perovskite $La_2CoMnO_6$. The mixed valence state due to oxygen deficiency is verified by X-ray photoelectron spectroscopy, and confirms a double ferromagnetic transition observed in DC magnetization. Neutron diffraction reveals that the magnetic structure is dominated by long-range ferromagnetic ordering, which is further corroborated by a critical exponents analysis of the paramagnetic to ferromagnetic phase transition. An analysis of the magnetization dynamics by means of linear and nonlinear ac magnetic susceptibilities marks the presence of two distinct cluster glass-like states that emerge at low temperatures. The isothermal entropy change as a function of temperature and magnetic field (H) is exploited to investigate the mechanism of stabilization of the magnetic phases across the H-T phase diagram. In the regime of the phase diagram where thermal energy is sufficiently low, regions of competing interactions due to local disorder become stabilized and display glass-like dynamics. The freezing mechanism of clusters is illustrated using a unique probe of transverse susceptibility that isolates the effects of the local anisotropy of the spin clusters. The results are summarized in a new H-T phase diagram of $La_2CoMnO_6$ revealed for the first time from these data.
The structural and magnetic properties of the face-centered cubic double perovskite Ba2MnWO6 were investigated using neutron powder diffraction, DC-magnetometry, muon spin relaxation and inelastic neutron scattering. Ba2MnWO6 undergoes Type II long-range antiferromagnetic ordering at a Neel temperature of 8(1) K with a frustration index, f = 8. Inelastic neutron scattering was used to identify the magnetic coupling constants J1 and J2, which were found to equal -0.080 meV and -0.076 meV respectively. This indicated that both of the magnetic coupling constants were antiferromagnetic with similar magnitudes, which is in contrast to other known 3d metal double perovskites Ba2MWO6. Above the Neel temperature, muon spin relaxation measurements and inelastic neutron scattering techniques identify a short-range correlated magnetic state that is similar to that observed in the archetypical face-centered cubic lattice antiferromagnet MnO.
Recent theoretical studies [Chen et al., Phys. Rev. B 82, 174440 (2010), Ishizuka et al., Phys. Rev. B 90, 184422 (2014)] for the magnetic Mott insulator Ba2NaOsO6 have proposed a low-temperature order parameter that breaks lattice rotational symmetry without breaking time reversal symmetry leading to a nematic phase just above magnetic ordering temperature. We present high-resolution calorimetric and magnetization data of the same Ba2NaOsO6 single crystal and show evidence for a weakly field-dependent phase transition occurring at a temperature of Ts ~ 9.5K, above the magnetic ordering temperature of Tc ~ 7.5K. This transition appears as a broadened step in the low-field temperature dependence of the specific heat. The evolution of the phase boundary with applied magnetic field suggests that this phase coincides with the phase of broken local point symmetry seen in high field NMR experiments [Lu et al., Nat. Comm. 8 14407 (2017)]. Furthermore, the magnetic field dependence of the specific heat provides clear indications for magnetic correlations persisting at temperatures between Tc and Ts where long-range magnetic order is absent giving support for the existence of the proposed nematic phase.
The double-perovskite A$_2$BBO$_6$ with heavy transition metal ions on the ordered B sites is an important family of compounds to study the interplay between electron correlation and spin-orbit coupling (SOC). Here we prepared high-quality Sr$_2$MgReO$_6$ powder and single-crystal samples and performed non-resonant and resonant synchrotron x-ray diffraction experiments to investigate its magnetic ground state. By combining the magnetic susceptibility and heat capacity measurements, we conclude that Sr$_2$MgReO$_6$ exhibits a layered antiferromagnetic (AF) order at temperatures below $sim$ 55 K with a propagation vector q = (001), which contrasts the previously suspected spin glass state. Our works clarify the magnetic order in Sr$_2$MgReO$_6$ and demonstrate it as a candidate system to look for magnetic octupolar orders and exotic spin dynamics.
Oxide double perovskites wherein octahedra formed by both 3d elements and sp-based heavy elements give rise to unconventional magnetic ordering and correlated quantum phenomena crucial for futuristic applications. Here, by carrying out experimental and first principles investigations, we present the electronic structure and magnetic phases of Ba2MnTeO6, where Mn^2+ ions with S = 5/2 spins constitute a perfect triangular lattice. The magnetic susceptibility reveals a large Curie- Weiss temperature -152 K suggesting the presence of strong antiferromagnetic interactions between Mn^2+ moments in the spin lattice. A phase transition at 20 K is revealed by magnetic susceptibility and specific heat which is attributed to the presence of a sizeable inter-plane interactions. Below the transition temperature, the specific heat data show antiferromagnetic magnon excitations with a gap of 1.4 K. Furthermore, muon spin-relaxation reveals the presence of static internal fields in the ordered state and provides strong evidence of short-range spin correlations for T > TN. The DFT+U calculations and spin-dimer analysis infer that Heisenberg interactions govern the inter and intra-layer spin-frustrations in this perovskite. The inter and intra-layer exchange interactions are of comparable strengths (J1 = 4.6 K, J2 = 0.92 J1). However, a weak third nearest-neighbor ferromagnetic inter-layer interaction exists (J3=-0.04 J1) due to double-exchange interaction via the linear path Mn-O-Te-O-Mn. The combined effect of J2 and J3 interactions stabilizes a three dimensional long-range magnetic ordering in this frustrated magnet.
Ca2-xLaxFeMoO6 double perovskite with La concentration x = 0 to 0.6 was synthesized using solid state sintering route. The standard techniques of XRD, SEM and EDX were applied to characterize the material. Crystal structure of the samples was stabilized in monoclinic phase with space group P2I/n and lattice expansion was indicated with the increase of x. The increase of La concentration gradually suppressed the coexisting minor secondary phase in the material and simultaneously, EDX results indicated the accommodation of more Mo atoms in the crystal structure. A significant modification in the surface morphology of the material was noted from adhesive type surface for x = 0 to brittle type surface with more grain boundary contributions for La doped samples. We understand a significant change in magnetic properties (appearance of cluster glass component, reduction of magnetic moment and indication of higher TC) and in electrical properties (reduction of metallic character) in terms of enhanced internal disorder in the material, introduced due to La doping in double perovskite structure.