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Exotic Magnetism and Spin-Orbit Assisted Mott Insulating State in a $3d-5d$ Double Perovskite

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 Added by Eduardo Granado
 Publication date 2018
  fields Physics
and research's language is English




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The magnetic structure of Ca$_2$MnReO$_6$ double perovskite is investigated by neutron powder diffraction and bulk magnetization, showing dominant non-collinear Mn magnetic moments [$4.35(7)$ $mu_B$] that are orthogonally aligned with the small Re moments [$0.22(4)$ $mu_B$]. $Ab$-initio electronic structure calculations show that the strong spin-orbit coupling for Re $5d$ electrons combined with a relatively modest on-site Coulomb repulsion ($U_{eff}^{Re} gtrsim 0.6$ eV) is sufficient to render this material insulating. This is a rare example of spin-orbit assisted Mott insulator outside the realm of iridates, with remarkable magnetic properties.



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The ability to tune exchange (magnetic) interactions between 3d transition metals in perovskite structures has proven to be a powerful route to discovery of novel properties. Here we demonstrate that the introduction of 3d-5d exchange pathways in double perovskites enables additional tunability, a result of the large spatial extent of 5d wave functions. Using x-ray probes of magnetism and structure at high pressure, we show that compression of Sr2FeOsO6 drives an unexpected continuous change in the sign of Fe-Os exchange interactions and a transition from antiferromagnetic to ferrimagnetic order. We analyze the relevant electron-electron interactions, shedding light into fundamental differences with the more thoroughly studied 3d-3d systems.
135 - W. K. Zhu , J.-C. Tung , W. Tong 2016
Double-perovskite oxides that contain both 3d and 5d transition metal elements have attracted growing interest as they provide a model system to study the interplay of strong electron interaction and large spin-orbit coupling (SOC). Here, we report on experimental and theoretical studies of the magnetic and electronic properties of double-perovskites (La$_{1-x}$Sr$_x$)$_2$CuIrO$_6$ ($x$ = 0.0, 0.1, 0.2, and 0.3). The undoped La$_2$CuIrO$_6$ undergoes a magnetic phase transition from paramagnetism to antiferromagnetism at T$_N$ $sim$ 74 K and exhibits a weak ferromagnetic behavior below $T_C$ $sim$ 52 K. Two-dimensional magnetism that was observed in many other Cu-based double-perovskites is absent in our samples, which may be due to the existence of weak Cu-Ir exchange interaction. First-principle density-functional theory (DFT) calculations show canted antiferromagnetic (AFM) order in both Cu$^{2+}$ and Ir$^{4+}$ sublattices, which gives rise to weak ferromagnetism. Electronic structure calculations suggest that La$_2$CuIrO$_6$ is an SOC-driven Mott insulator with an energy gap of $sim$ 0.3 eV. Sr-doping decreases the magnetic ordering temperatures ($T_N$ and $T_C$) and suppresses the electrical resistivity. The high temperatures resistivity can be fitted using a variable-range-hopping model, consistent with the existence of disorders in these double-pervoskite compounds.
Motivated by the presence of an unquenched orbital angular momentum in CoO, a team at Chalk River, including a recently hired research officer Roger Cowley, performed the first inelastic neutron scattering experiments on the classic Mott insulator [Sakurai $textit{et al.}$ 1968 Phys. Rev. $mathbf{167}$ 510]. Despite identifying magnon modes at the zone boundary, the team was unable to parameterise the low energy magnetic excitation spectrum below $Trm{_{N}}$ using conventional pseudo-bosonic approaches. It would not be for another 40 years that Roger, now at Oxford and motivated by the discovery of the high-$T_{c}$ cuprate superconductors [Bednorz & Muller 1986 Z. Phys. B $mathbf{64}$ 189], would make another attempt at the parameterisation of the magnetic excitation spectrum that had previously alluded him. Upon his return to CoO, Roger found a system embroiled in controversy, with some of its most fundamental parameters still remaining undetermined. Faced with such a formidable task, Roger performed a series of inelastic neutron scattering experiments in the early 2010s on both CoO and a magnetically dilute structural analogue MgO. These experiments would prove instrumental in the determination of both single-ion [Cowley $textit{et al.}$ 2013 Phys. Rev. B $mathbf{88}$ 205117] and cooperative magnetic parameters [Sarte $textit{et al.}$ 2018 Phys. Rev. B $mathbf{98}$ 024415] for CoO. Both these sets of parameters would eventually be used in a spin-orbit exciton model [Sarte $textit{et al.}$ 2019 Phys. Rev. B $mathbf{100}$ 075143], developed by his longtime friend and collaborator Bill Buyers, to successfully parameterise the complex spectrum that both measured at Chalk River almost 50 years prior. The story of CoO is of one that has come full circle, one filled with both spectacular failures and intermittent, yet profound, little victories.
We report the structural transformation of hexagonal Ba3YIr2O9 to a cubic double perovskite form (stable in ambient conditions) under an applied pressure of 8GPa at 1273K. While the ambient pressure (AP) synthesized sample undergoes long-range magnetic ordering at 4K, the high pressure(HP) synthesized sample does not order down to 2K as evidenced from our susceptibility, heat capacity and nuclear magnetic resonance (NMR) measurements. Further, for the HP sample, our heat capacity data have the form gamma*T+beta*T3 in the temperature (T) range of 2-10K with the Sommerfeld coefficient gamma=10mJ/mol-Ir K2. The 89Y NMR shift has no T-dependence in the range of 4-120K and its spin-lattice relaxation rate varies linearly with T in the range of 8-45K (above which it is T-independent). Resistance measurements of both the samples confirm that they are semiconducting. Our data provide evidence for the formation of a 5d based, gapless, quantum spin-liquid (QSL) in the cubic (HP) phase of Ba3YIr2O9. In this picture, the T term in the heat capacity and the linear variation of 89Y 1/T1 arises from excitations out of a spinon Fermi surface. Our findings lend credence to the theoretical suggestion [G. Chen, R. Pereira, and L. Balents, Phys. Rev. B 82, 174440 (2010)] that strong spin-orbit coupling can enhance quantum fluctuations and lead to a QSL state in the double perovskite lattice.
Cation displacements, oxygen octahedral tilts, and magnetism of epitaxial, ferrimagnetic, insulating GdTiO3 films sandwiched between cubic SrTiO3 layers are studied using scanning transmission electron microscopy and magnetization measurements. With decreasing GdTiO3 film thickness, structural (GdFeO3-type) distortions are reduced, concomitant with a reduction in the Curie temperature. Ferromagnetism persists to smaller deviations from the cubic perovskite structure than is the case for the bulk rare earth titanates. The results indicate that the FM ground state is controlled by the narrow bandwidth, exchange and orbital ordering, and only to second order depends on amount of the GdFeO3-type distortion.
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