91 research outputs found

    Magnetic interactions in the S = 1/2 square-lattice antiferromagnets Ba2CuTeO6 and Ba2CuWO6: parent phases of a possible spin liquid

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    The isostructural double perovskites Ba2CuTeO6 and Ba2CuWO6 are shown by theory and experiment to be frustrated square-lattice antiferromagnets with opposing dominant magnetic interactions. This is driven by differences in orbital hybridisation of Te6+ and W6+. A spin-liquid-like ground state is predicted for Ba2Cu(Te1-xWx)O6 solid solution similar to recent observations in Sr2Cu(Te1-xWx)O6

    Tuning the S=1/2S = 1/2 square-lattice antiferromagnet Sr2_2Cu(Te1−x_{1-x}Wx_x)O6_6 from N\'eel order to quantum disorder to columnar order

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    The spin-1/2 square-lattice Heisenberg model is predicted to have a quantum disordered ground state when magnetic frustration is maximized by competing nearest-neighbor J1J_1 and next-nearest-neighbor J2J_2 interactions (J2/J1≈0.5J_2/J_1 \approx 0.5). The double perovskites Sr2_2CuTeO6_6 and Sr2_2CuWO6_6 are isostructural spin-1/2 square-lattice antiferromagnets with N\'eel (J1J_1 dominates) and columnar (J2J_2 dominates) magnetic order, respectively. Here we characterize the full isostructural solid solution series Sr2_2Cu(Te1−x_{1-x}Wx_x)O6_6 (0≤x≤10 \leq x \leq 1) tunable from N\'eel order to quantum disorder to columnar order. A spin-liquid-like ground state was previously observed for the xx = 0.5 phase, but we show that the magnetic order is suppressed below 1.5 K in a much wider region of x≈x \approx 0.1-0.6. This coincides with significant TT-linear terms in the low-temperature specific heat. However, density functional theory calculations predict most of the materials are not in the highly frustrated J2/J1≈0.5J_2/J_1 \approx 0.5 region square-lattice Heisenberg model. Thus, a combination of both magnetic frustration and quenched disorder is the likely origin of the spin-liquid-like state in xx = 0.5.Comment: 20+5 pages, 6+4 figures. Accepted for publication in PR

    Structure, spin correlations and magnetism of the S=1/2S = 1/2 square-lattice antiferromagnet Sr2_2CuTe1−x_{1-x}Wx_xO6_6 (0≤x≤10 \leq x \leq 1)

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    Quantum spin liquids are highly entangled magnetic states with exotic properties. The S=1/2S = 1/2 square-lattice Heisenberg model is one of the foundational models in frustrated magnetism with a predicted, but never observed, quantum spin liquid state. Isostructural double perovskites Sr2_2CuTeO6_6 and Sr2_2CuWO6_6 are physical realizations of this model, but have distinctly different types magnetic order and interactions due to a d10/d0d^{10}/d^0 effect. Long-range magnetic order is suppressed in the solid solution Sr2_2CuTe1−x_{1-x}Wx_xO6_6 in a wide region of x=0.05−0.6x = 0.05-0.6, where the ground state has been proposed to be a disorder-induced spin liquid. Here we show that the spin-liquid-like x=0.2x = 0.2 and x=0.5x = 0.5 samples have distinctly different local spin correlations, which suggests they have different ground states. Furthermore, the previously ignored interlayer coupling between the square-planes is likely to play a role in the suppression of magnetic order on the W-rich side at x≈0.6x \approx 0.6. These results highlight the complex magnetism of Sr2_2CuTe1−x_{1-x}Wx_xO6_6 and hint at a new quantum critical point at x≈0.3x \approx 0.3.Comment: 19+8 pages, 6+8 figure

    Structure, Spin Correlations, and Magnetism of the S = 1/2 Square-Lattice Antiferromagnet Sr2CuTe1-xWxO6 (0 ≤ x ≤ 1)

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    Quantum spin liquids are highly entangled magnetic states with exotic properties. The S = 1/2 square-lattice Heisenberg model is one of the foundational models in frustrated magnetism with a predicted, but never observed, quantum spin liquid state. Isostructural double perovskites Sr2CuTeO6 and Sr2CuWO6 are physical realizations of this model but have distinctly different types of magnetic order and interactions due to a d10/d0 effect. Long-range magnetic order is suppressed in the solid solution Sr2CuTe1-xWxO6 in a wide region of x = 0.05-0.6, where the ground state has been proposed to be a disorder-induced spin liquid. Here, we present a comprehensive neutron scattering study of this system. We show using polarized neutron scattering that the spin liquid-like x = 0.2 and x = 0.5 samples have distinctly different local spin correlations, which suggests that they have different ground states. Low-temperature neutron diffraction measurements of the magnetically ordered W-rich samples reveal magnetic phase separation, which suggests that the previously ignored interlayer coupling between the square planes plays a role in the suppression of magnetic order at x ≈ 0.6. These results highlight the complex magnetism of Sr2CuTe1-xWxO6 and hint at a new quantum critical point between 0.2 &lt; x &lt; 0.4.</p

    Structure, spin correlations, and magnetism of the S = 1/2 square-lattice antiferromagnet Sr2CuTe1–xWxO6 (0 ≤ x ≤ 1)

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    Quantum spin liquids are highly entangled magnetic states with exotic properties. The S = 1/2 square-lattice Heisenberg model is one of the foundational models in frustrated magnetism with a predicted, but never observed, quantum spin liquid state. Isostructural double perovskites Sr2CuTeO6 and Sr2CuWO6 are physical realizations of this model but have distinctly different types of magnetic order and interactions due to a d10/d0 effect. Long-range magnetic order is suppressed in the solid solution Sr2CuTe1–xWxO6 in a wide region of x = 0.05–0.6, where the ground state has been proposed to be a disorder-induced spin liquid. Here, we present a comprehensive neutron scattering study of this system. We show using polarized neutron scattering that the spin liquid-like x = 0.2 and x = 0.5 samples have distinctly different local spin correlations, which suggests that they have different ground states. Low-temperature neutron diffraction measurements of the magnetically ordered W-rich samples reveal magnetic phase separation, which suggests that the previously ignored interlayer coupling between the square planes plays a role in the suppression of magnetic order at x ≈ 0.6. These results highlight the complex magnetism of Sr2CuTe1–xWxO6 and hint at a new quantum critical point between 0.2 < x < 0.4

    Conductivity and redox stability of new double perovskite oxide Sr 1.6 K 0.4 Fe 1+ x Mo 1− x O 6− δ (x= 0.2, 0.4, 0.6)

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    A series of new perovskite oxides Sr1.6K0.4Fe1+xMo1−xO6−δ (x = 0.2, 0.4, 0.6) were synthesised by solid state reaction method. Synthesis of Sr1.6K0.4Fe1+xMo1−xO6−δ (x = 0.2, 0.4, 0.6) was achieved above 700 °C in 5 % H2/Ar, albeit with the formation of impurity phases. Phase stability upon redox cycling was only observed for sample Sr1.6K0.4Fe1.4Mo0.6O6−δ. Redox cycling of Sr1.6K0.4Fe1+xMo1−xO6−δ (x = 0.2, 0.4, 0.6) demonstrates a strong dependence on high temperature reduction to achieve high conductivities. After the initial reduction at 1200 °C in 5 %H2/Ar, then re-oxidation in air at 700 °C and further reduction at 700 °C in 5 %H2/Ar, the attained conductivities were between 0.1 and 58.4 % of the initial conductivity after reduction 1200 °C in 5 %H2/Ar depending on the composition. In the investigated new oxides, sample Sr1.6K0.4Fe1.4Mo0.6O6−δ is most redox stable also retains reasonably high electrical conductivity, ~70 S/cm after reduction at 1200 °C and 2–3 S/cm after redox cycling at 700 °C, indicating it is a potential anode for SOFCs
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