Abstract

We have studied the magnetic properties and spin-dynamics of the structurally-ordered double perovskite Sr2_2CoOsO6_6. Our neutron diffraction, muon spin relaxation and ac-susceptibility measurements reveal two antiferromagnetic (AFM) phases on cooling from room temperature down to 2 K. In the first AFM phase, with transition temperature TN=108T_{\mathrm{N}}=108 K, cobalt (3d7d^7, S=3/2S=3/2) and osmium (5d2d^2, S=1S=1) moments fluctuate dynamically, while their \textit{average} effective moments undergo long-range order. In the second AFM phase with TN=67T_{\mathrm{N}}=67 K, cobalt moments first become frozen and induce a noncollinear spin-canted AFM state, while dynamically fluctuating osmium moments are later frozen into a randomly canted state at T≈5T\approx 5 K. Our \textit{ab initio} calculations indicate that the effective exchange coupling between cobalt and osmium sites is rather weak, so that cobalt and osmium sublattices exhibit different ground states and spin-dynamics, making Sr2_2CoOsO6_6 distinct from previously reported double-perovskite compounds.

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