Crystalline water intercalation into the Kitaev honeycomb cobaltate Na$_2$Co$_2$TeO$_6$

Abstract

We herein report the successful intercalation of water molecules into the layered honeycomb lattice of Na$_2$Co$_2$TeO$_6$, a Kitaev-candidate compound, to obtain the hydrated phase Na$_2$Co$_2$TeO$_6$$\cdot$$y$H$_2$O ($y \sim$ 2.4). Fourier transform infrared spectroscopy, thermogravimetric analysis, differential scanning calorimetry, and Rietveld refinements indicate that crystalline water resides between the cobalt-based honeycomb layers. This insertion of neutral molecules significantly alters the crystal structure, increasing the interlayer spacing and modifying the local bonding environment. Magnetization measurements reveal an antiferromagnetic transition at $T_N \sim 17.2$ K, accompanied by a discernible weak ferromagnetic component. The application of moderate magnetic fields induces a spin-flop reorientation at $\mu_0H \sim 5.7$ T. The $\lambda$-type anomaly and long-range order persist up to 9 T, showing the reconfiguration of the ground state as opposed to its suppression. Heat-capacity analysis reveals the full $2R\ln2$ magnetic entropy expected for two $J_{\rm eff} = 1/2$ moments per formula unit, confirming the pseudospin description. These findings demonstrate that water intercalation is a robust strategy for tuning the magnetic properties of honeycomb lattice materials. Overall, this study highlights neutral-molecule insertion as a promising route toward the discovery and engineering of quantum magnets based on layered transition metal oxides.