Spin-liquid-like state in a spin-1/2 square-lattice antiferromagnet perovskite induced by d¹⁰ – d⁰ cation mixing

A quantum spin liquid state has long been predicted to arise in spin-1/2 Heisenberg square-lattice antiferromagnets at the boundary region between Néel (nearest-neighbor interaction dominates) and columnar (next-nearest-neighbor interaction dominates) antiferromagnetic order. However, there are no known compounds in this region. Here we use d¹⁰ – d⁰ cation mixing to tune the magnetic interactions on the square lattice while simultaneously introducing disorder. We find spin-liquid-like behavior in the double perovskite Sr₂Cu(Te_0.5W_0.5)O₆, where the isostructural end phases Sr₂CuTeO₆ and Sr₂CuWO₆ are Néel and columnar type antiferromagnets, respectively. We show that magnetism in Sr₂Cu(Te_0.5W_0.5)O₆ is entirely dynamic down to 19 mK. Additionally, we observe at low temperatures for Sr₂Cu(Te_0.5W_0.5)O₆ - similar to several spin liquid candidates—a plateau in muon spin relaxation rate and a strong T-linear dependence in specific heat. Our observations for Sr₂Cu(Te_0.5W_0.5)O₆ highlight the role of disorder in addition to magnetic frustration in spin liquid physics.