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This investigation reports on anisotropy in the magnetic interaction, lattice-orbital coupling and degree of phonon softening in single crystal Ni 3 TeO 6  (NTO) using temperature- and polarization-dependent X-ray absorption spectroscopic techniques. The magnetic field-cooled and zero-field-cooled measurements and temperature-dependent Ni  L  3,2 -edge X-ray magnetic circular dichroism spectra of NTO reveal a weak Ni-Ni ferromagnetic interaction close to ~60 K ( T  SO : temperature of the onset of spin ordering) with a net alignment of Ni spins (the uncompensated components of the Ni moments) along the crystallographic  c -axis, which is absent from the  ab -plane. Below the Néel temperature,  T  N ~ 52 K, NTO is stable in the antiferromagnetic state with its spin axis parallel to the  c -axis. The Ni  L  3,2 -edge X-ray linear dichroism results indicate that above  T  SO , the Ni 3 d e  g  electrons preferentially occupy the out-of-plane 3 d  3z  2  −r  2  orbitals and switch to the in-plane 3 d  x  2  −y  2  orbitals below  T  SO . The inherent distortion of the NiO 6  octahedra and anisotropic nearest-neighbor Ni-O bond lengths between the  c -axis and the  ab -plane of NTO, followed by anomalous Debye-Waller factors and orbital-lattice in conjunction with spin-phonon couplings, stabilize the occupied out-of-plane (3 d  3z  2  −r  2 ) and in-plane (3 d  x  2  −y  2 ) Ni  e  g  orbitals above and below  T  SO , respectively.

Anisotropy in the magnetic interaction and lattice-orbital coupling of single crystal Ni3TeO6