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We present a comprehensive study of single crystals of Na2Co2TeO6, a putativeKitaev honeycomb magnet, focusing on its low-temperature phase behaviors. A newthermal phase transition is identified at 31.0 K, below which the systemdevelops a two-dimensional (2D) long-range magnetic order. This order precedesthe well-known 3D order below 26.7 K, and is likely driven by stronglyanisotropic interactions. Surprisingly, excitations from the 3D order do notsupport the order's commonly accepted "zigzag" nature, and are insteadconsistent with a "triple-q" description. The 3D order exerts a fundamentalfeedback on high-energy excitations that likely involve orbital degrees offreedom, and it remains highly frustrated until a much lower temperature isreached. These findings render Na2Co2TeO6 a spin-orbit entangled frustratedmagnet that hosts very rich physics.

Spin-orbit phase behaviors of Na2Co2TeO6 at low temperatures