Quasi two dimensional magnetic structure of the triclinic double perovskite Ca$_2$CuWO$_6$

Abstract

We present the antiferromagnetic ground state of the triclinic double perovskite Ca$_2$CuWO$_6$solved by neutron powder diffraction, and analyze it in direct comparison with tetragonal Sr$_2$CuWO$_6$. Below $T_\mathrm{N} \simeq 32$ K, the magnetic Bragg reflections of Ca$_2$CuWO$_6$ are indexed by the commensurate propagation vector $\mathbf{k}=(\tfrac{1}{2},\tfrac{1}{2},0)$ in its native $P\bar{1}$ cell. Rietveld refinement yields a collinear structure with equal-magnitude, antiparallel moments on the crystallographically inequivalent Cu1 and Cu2 sites and an ordered moment of $0.66(3)~\mu_{\mathrm B}$ per Cu at 1.5 K. A direct comparison with Sr$_2$CuWO$_6$ is obscured by different crystallographic settings and orientations of the cooperative Jahn-Teller elongation axes. Hence, we introduce a common crystallographic supercell through which effects of symmetry lowering from tetragonal to triclinic in the double perovskite are explored: Apparently different magnetic propagation vectors map onto the same supercell wave vector, revealing a common magnetic structure stabilized by tungsten-mediated, second-neighbor interactions. Mean field calculations further show that tetragonal symmetry preserves the degeneracy of four magnetic $\mathbf{k}$-domains in Sr$_2$CuWO$_6$, whereas the triclinic splitting of symmetry-related exchange pathways in Ca$_2$CuWO$_6$, most strongly within the Cu2 network, selects a single $\mathbf{k}$-domain. These results establish the magnetic ground state of Ca$_2$CuWO$_6$ and show how symmetry breaking selects a given ordered state without changing the underlying magnetic motif of the Sr analogue.