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Register a new userRelationship between A-site Cation and Magnetic Structure in 3d-5d-4f Double Perovskite Iridates Ln2NiIrO6 (Ln=La, Pr, Nd)
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We report a comprehensive investigation of Ln2NiIrO6 (Ln = La, Pr, Nd) using thermodynamic and transport properties, neutron powder diffraction, resonant inelastic x-ray scattering, and density functional theory (DFT) calculations to investigate the role of A-site cations on the magnetic interactions in this family of hybrid 3d-5d-4f compositions. Magnetic structure determination using neutron diffraction reveals antiferromagnetism for La2NiIrO6, a collinear ferrimagnetic Ni/Ir state that is driven to long range antiferromagnetism upon the onset of Nd ordering in Nd2NiIrO6, and a non-collinear ferrimagnetic Ni/Ir sublattice interpenetrated by a ferromagnetic Pr lattice for Pr2NiIrO6. For Pr2NiIrO6 heat capacity results reveal the presence of two independent magnetic sublattices and transport resistivity indicates insulating behavior and a conduction pathway that is thermally mediated. First principles DFT calculation elucidates the existence of the two independent magnetic sublattices within Pr2NiIrO6 and offers insight into the behavior in La2NiIrO6 and Nd2NiIrO6. Resonant inelastic x-ray scattering is consistent with spin-orbit coupling splitting the t2g manifold of octahedral Ir4+ into a Jeff = 1/2 and Jeff = 3/2 state for all members of the series considered.
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In this work, we report on the synthesis and magnetic properties of a series of double perovskites Ln$_2$ZnIrO$_6$ with Ln = Nd, Sm, Eu & Gd. These compounds present new examples of the rare case of double perovskites (general formula A$_2$BBO$_6$) with a magnetic 4f -ion on the A-site in combination with the strongly spin-orbit coupled 5d-transition metal ion Ir$^{4+}$ on the B-sublattice. We discuss the impact of different rare earths on the macroscopic magnetic properties. Gd$_2$ZnIrO$_6$ and Eu$_2$ZnIrO$_6$ show weak canted antiferromagnetic order below T$_N$ = 23 K and T$_N$ = 12 K, respectively. Sm$_2$ZnIrO$_6$ orders antiferromagnetically at T$_N$ = 13 K. Nd$_2$ZnIrO$_6$ exhibits complex magnetic properties with strong field dependence ranging from a two-step behavior at H = 0.01 T to an antiferromagnetic ground state at intermediate external fields and a spin-flop phase at H$geq$4 T, which suggests complex interplay between Nd$^{3+}$ and Ir$^{4+}$ . To further shed light on this magnetic interaction, the magnetic structure of Nd$_2$ZnIrO$_6$s ground state is examined via neutron powder diffraction.
Magnetic structures and the relationship between spin and charge-orbital orderings of an A-site ordered double-perovskite manganite SmBaMn2O6, an anticipated multiferroic material, were investigated by means of neutron diffraction. The spin arrangement in MnO2 planes perpendicular to the c axis is revealed to be the same as that in the A-site disordered half-doped manganites CE-type but the stacking pattern is found to be different displaying a unique twofold period. The temperature dependence of the superlattice magnetic and nuclear reflections clarifies that the antiferromagnetic spin ordering occurs at a temperature slightly lower than the temperature at which a rearrangement of the charge-orbital orderings occurs. The result evidences that the rearrangement leads the spin ordering. The intensities of the magnetic reflections are found to change across Tf = 10 K, suggesting a spin-flop by 90 [deg.] while keeping the Mn spin ordering pattern unchanged.
We have synthesized a series of the Ruddlesden-Popper nickelate solid solution Ln4-xLnxNi3O10 (Ln and Ln = La, Pr and Nd; x = 0, 1, 2 and 3) via the citrate precursor method at different reacting atmospheres. Both the electronic-transport and magnetization measurements on these samples show well-defined phase transitions at temperatures between 135 K and 165 K. These transition temperatures, the room-temperature resistivities, as well as the changes of the Pauli-paramagnetic susceptibilities at the respective phase transitions, strongly correlate with the Goldschmidt tolerance factor t, irrespective of the combination of the magnetic rare-earth ions with unmagnetic La3+. We conclude that these changes of the electronic properties are mostly related to the distortion of the NiO6 octahedra at the phase transition which is strongly correlated with the tolerance factor t, but are rather insensitive to the magnetism of the rare-earth ions Ln3+ and Ln3+.
Developing good performance and low-cost oxygen permeable membranes for CO2 capture based on the oxy-fuel concept is greatly desirable but challenging. Despite tremendous efforts in exploring new CO2-stable dual-phase membranes, its presence is however still far from meeting the industrial requirements. Here we report a series of new Ca-containing CO2-resistant oxygen transporting membranes with composition 60wt.%Ce0.9Ln0.1O2-40wt.%Ln0.6Ca0.4FeO3(CLnO-LnCFO; Ln = La, Pr, Nd, Sm) synthesized via a Pechini one-pot method. Our results indicate all investigated compounds are composed of perovskite and fluorite phases, while the perovskite phases in the CNO-NCFO and CSO-SCFO membranes after sintering generates Ca-rich and Ca-less two kinds of grains with different morphologies, where the Ca-less small perovskite grains block the transport of oxygen ions and eventually result in poor oxygen permeability. Among our investigated CLnO-LnCFO membranes, CPO-PCFO exhibits the highest oxygen permeability and excellent CO2 stability, which were mainly associated with the improvement in crystal symmetry, non-negligible electronic conductivity of fluorite phase and the enhancement in electronic conductivity of perovskite. Our results establish Ca-containing oxides as candidate material platforms for membrane engineering devices that combine CO2 capture and oxygen separation.
A review of our investigations on single crystals of LnFeAsO1-xFx (Ln=La, Pr, Nd, Sm, Gd) and Ba1-xRbxFe2As2 is presented. A high pressure technique has been applied for the growth of LnFeAsO1-xFx crystals, while Ba1-xRbxFe2As2 crystals were grown using quartz ampoule method. Single crystals were used for electrical transport, structure, magnetic torque and spectroscopic studies. Investigations of the crystal structure confirmed high structural perfection and show less than full occupation of the (O, F) position in superconducting LnFeAsO1-xFx crystals. Resistivity measurements on LnFeAsO1-xFx crystals show a significant broadening of the transition in high magnetic fields, whereas the resistive transition in Ba1 xRbxFe2As2 simply shifts to lower temperature. Critical current density for both compounds is relatively high and exceeds 2x109 A/m2 at 15 K in 7 T. The anisotropy of magnetic penetration depth, measured on LnFeAsO1-xFx crystals by torque magnetometry is temperature dependent and apparently larger than the anisotropy of the upper critical field. Ba1-xRbxFe2As2 crystals are electronically significantly less anisotropic. Point-Contact Andreev-Reflection spectroscopy indicates the existence of two energy gaps in LnFeAsO1-xFx. Scanning Tunneling Spectroscopy reveals in addition to a superconducting gap, also some feature at high energy (~20 meV).
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