We formulate a superexchange theory of insulating double-perovskite compounds such as Sr$_2$FeWO$_6$. An effective spin-orbital Hamiltonian is derived in the strong coupling limit of Hubbard model for d-electrons on Fe and W ions. The relevant degrees of freedom are the spins S=2 and the three-fold orbital degeneracy of Fe$^{2+}$-ions. W-sites are integrated out by means of a fourth-order perturbative expansion. The magnetically and orbitally ordered ground states of the effective Hamiltonia n are discussed as a function of the model parameters. We show that for realistic values of such parameters the ground state is antiferromagnetic, as experimentally observed. The order found is of type-II, consisting of {111} ferromagnetic planes stac ked antiferromagnetically. The orbital order energy scale found is one order of magnitude less than the spi n one.
Sr$_2$CuWO$_6$ is a double perovskite proposed to be at the border between two and three dimensional magnetism, with a square lattice of $S=frac{1}{2}$ Cu$^{2+}$ ions. We have used inelastic neutron scattering to investigate the spin wave excitations of the system, to find out how they evolve as a function of temperature, as well as to obtain information about the magnetic exchange interactions. We observed well defined dispersive spin wave modes at $6$~K, which partially survive above the magnetic ordering temperature, $T_N=24$~K. Linear spin wave theory is used to determine the exchange interactions revealing them to be highly two-dimensional in nature. Density functional theory calculations are presented supporting this experimental finding, which is in contrast to a previous emph{ab-initio} study of the magnetic interactions. Our analysis confirms that not the nearest neighbour, but the next nearest neighbour interactions in the tetragonal $ab$ plane are the strongest. Low incident energy measurements reveal the opening of a $0.6(1)$~meV gap below $T_N$, which suggests the presence of a very weak single ion anisotropy term in the form of an easy axis along $hat{mathbf{a}}$.
We study the magnetic properties of CaFeTi$_2$O$_6$ (CFTO) by high-field magnetization and specific heat measurements. While the magnetic susceptibility data yield a vanishingly small Curie-Weiss temperature, the magnetic moments are not fully polarized in magnetic field up to 60 T, which reveals a large spin exchange energy scale. Yet, the system shows no long range magnetic order but a spin-glass-like state below 5.5 K in zero field, indicating strong magnetic frustration in this system. Applying magnetic field gradually suppresses the spin-glass-like state and gives rise to a potential quantum spin liquid state whose low-temperature specific heat exhibits a $T^{1.6}$ power-law. Crucially, conventional mechanisms for frustration do not apply to this system as it possesses neither apparent geometrical frustration nor exchange frustration. We suggest that the orbital modulation of exchange interaction is likely the source of hidden frustration in CFTO, and its full characterization may open a new route in the quest for quantum spin liquids.
We report the observation of spin glass state in the double perovskite oxide Sr$_{2}$FeCoO$_{6}$ prepared through sol-gel technique. Initial structural studies using x rays reveal that the compound crystallizes in tetragonal $I 4/m$ structure with lattice parameters, $a$ = 5.4609(2) AA and $c$ = 7.7113(7) AA. The temperature dependent powder x ray studies reveal no structural phase transition in the temperature range 10 -- 300 K. However, the unit cell volume shows an anomaly coinciding with the magnetic transition temperature thereby suggesting a close connection between lattice and magnetism. Neutron diffraction studies and subsequent bond valence sums analysis show that in Sr$_{2}$FeCoO$_{6}$, the $B$ site is randomly occupied by Fe and Co in the mixed valence states of Fe$^{3+}$/Fe$^{4+}$ and Co$^{3+}$/Co$^{4+}$. The random occupancy and mixed valence sets the stage for inhomogeneous magnetic exchange interactions and in turn, for the spin glass like state in this double perovskite which is observed as an irreversibility in temperature dependent dc magnetization at $T_fsim$ 75 K. Thermal hysteresis observed in the magnetization profile of Sr$_{2}$FeCoO$_{6}$ is indicative of the mixed magnetic phases present. The dynamic magnetic susceptibility displays characteristic frequency dependence and confirms the spin glass nature of this material. Dynamical scaling analysis of $chi(T)$ yields a critical temperature $T_{ct}$ = 75.14(8) K and an exponent $z u$ = 6.2(2) typical for spin glasses. The signature of presence of mixed magnetic interactions is obtained from the thermal hysteresis in magnetization of Sr$_{2}$FeCoO$_{6}$. Combining the neutron and magnetization results of Sr$_2$FeCoO$_6$, we deduce the spin states of Fe to be in low spin while that of Co to be in low spin and intermediate spin.
Sr$_2$FeOsO$_6$ is an insulating double perovskite compound which undergoes antiferromagnetic transitions at 140 K ($T_{N1}$) and 67 K ($T_{N2}$). To study the underlying electronic and magnetic interactions giving rise to this behavior we have performed inelastic neutron scattering (INS) and resonant inelastic x-ray scattering (RIXS) experiments on polycrystalline samples of Sr$_2$FeOsO$_6$. The INS data reveal that the spectrum of spin excitations remains ungapped below T$_{N1}$, however below T$_{N2}$ a gap of 6.8 meV develops. The RIXS data reveals splitting of the T$_{2g}$ multiplet consistent with that seen in other 5d$^3$ osmium based double perovskites. Together these results suggest that spin-orbit coupling is important for ground state selection in 3d-5d$^3$ double perovskite materials.
We have prepared crystallographically ordered and disorder specimens of the double perovskite, Sr$_2$FeMoO$_6$ and investigated their magnetoresistance behaviour. The extent of ordering between the Fe and Mo sites in the two samples is determined by Rietveld analysis of powder x-ray diffraction patterns and reconfirmed by M{o}ssbauer studies. While the ordered sample exhibits the sharp low-field response, followed by moderate changes in the magnetoresistance at higher fields, the disordered sample is characterised by the absence of the spectacular low-field response. We argue that the low field response depends crucially on the half-metallic ferromagnetism, while the high-field response follows from the overall magnetic nature of the sample, even in absence of the half-metallic state.
S. Di Matteo
,G. Jackeli
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(2003)
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"An effective spin-orbital Hamiltonian for the double perovskite Sr$_2$FeW O$_6$: Derivation of the phase diagram"
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George Jackeli
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