Abstract

The $B$-site ordered double perovskites ${\mathrm{Sr}}_{2}\mathrm{Cu}({\mathrm{Te}}_{1\ensuremath{-}x}{\mathrm{W}}_{x}){\mathrm{O}}_{6}$ provide an excellent arena for investigating exotic phases expected for the ${J}_{1}\text{\ensuremath{-}}{J}_{2}$ square-lattice Heisenberg antiferromagnet. Here, combining magnetic susceptibility and specific-heat measurements with electron spin resonance (ESR) and muon spin rotation/relaxation $(\ensuremath{\mu}\mathrm{SR})$ techniques, we explore a spin-liquid-like state in the vicinity of the N\'eel critical end point $(x=0.05--0.1)$. The specific heat and the ESR and muon relaxation rates give evidence for an energy hierarchy of low-energy excitations, reminiscent of randomness-induced singlet states. In addition, the weak transverse $\ensuremath{\mu}\mathrm{SR}$ data show a fraction of frozen magnetic moments in the random-singlet background. The origin of a random-singlet-like state near the phase boundary is discussed in terms of concomitant exchange randomness and local strain generated by the ${\mathrm{W}}^{6+}\text{\ensuremath{-}}\mathrm{for}\text{\ensuremath{-}}{\mathrm{Te}}^{6+}$ substitution.

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