K$_2$Co$_2$(TeO$_{3}$)$_{3}$ $\cdot$ 2.5 H$_2$O : A mineral-inspired pseudo-honeycomb cobalt dimer antiferromagnet

Abstract

In recent years, magnetically-frustrated triangular and honeycomb lattice cobaltates have seen extensive study in the pursuit of a quantum spin liquid (QSL) state in a real material. In this work, we describe the hydroflux synthesis of K$_2$Co$_2$(TeO$_{3}$)$_{3}$ $\cdot$ 2.5 H$_2$O (KCoTOH), a novel zemannite-type antiferromagnet (AFM) possessing structural elements of both triangular dimer and honeycomb structural motifs. Bulk magnetometry and specific heat data support the onset of long-range AFM order below $T_\text{N}$ = 7.6(1) K, with neutron diffraction and muon spin relaxation ($\mu$SR) measurements placing the majority of the ordered moment within the pseudo-honeycomb plane. We resolve three unique oscillation frequencies from the zero-field $\mu$SR spectra, additionally suggesting a remarkably low level of structural disorder in as-grown KCoTOH crystals. Whereas interactions between dimerized chains of Co$^{2+}$ cations are typically observed to be negligible or ferromagnetic in nature, the largely planar ordering motif observed in KCoTOH is instead stabilized by net antiferromagnetic interactions through bridging tellurite groups. This work highlights the potential of hydroflux synthesis methods in the stabilization of magnetic materials possessing novel and potentially more frustrated lattice geometries.