Structure, spin correlations and magnetism of the $S=1/2$ square-lattice antiferromagnet Sr${}_2$CuTe${}_{1-x}$W${}_x$O${}_6$ ($0\le x\le 1$)

Abstract

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 Sr${}_2$CuTeO${}_6$ and Sr${}_2$CuWO${}_6$ are physical realizations of this model, but have distinctly different types magnetic order and interactions due to a $d^{10}/d^0$ effect. Long-range magnetic order is suppressed in the solid solution Sr${}_2$CuTe${}_{1-x}$W${}_x$O${}_6$ 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 show that the spin-liquid-like $x=0.2$ and $x=0.5$ 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 $x\approx 0.6$. These results highlight the complex magnetism of Sr${}_2$CuTe${}_{1-x}$W${}_x$O${}_6$ and hint at a new quantum critical point at $x\approx 0.3$.

19+8 pages, 6+8 figures

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