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    Crystalline water intercalation into the Kitaev honeycomb cobaltate Na2Co2TeO6

    Masaaki Ito1, Yuya Haraguchi1,*, Teruki Motohashi2, Miwa Saito2, Satoshi Ogawa2, Takashi Ikuta3, and Hiroko Aruga Katori1

    • *Contact author: chiyuya3@go.tuat.ac.jp

    Phys. Rev. Materials 9, 094402 – Published 2 September, 2025

    DOI: https://doi.org/10.1103/nyd3-dt8j

    Abstract

    We herein report the successful intercalation of water molecules into the layered honeycomb lattice of Na2Co2TeO6, a Kitaev-candidate compound, to obtain the hydrated phase Na2Co2TeO6·yH2O (y≈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 TN≈17.2 K, accompanied by a discernible weak ferromagnetic component. The application of moderate magnetic fields induces a spin-flop reorientation at μ0H≈5.7 T. The λ-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 2Rln2 magnetic entropy expected for two Jeff=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.

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