A Dysprosium Complex with Two Quasi-Degenerate Easy Axes.

The synergistic use of synthesis, single crystal X-ray Diffraction, torque and SQUID magnetometry, luminescence, and ab initio calculations is presented here to unambiguously unfold the magnetic anisotropy of an apparently ordinary low-symmetry eight-coordinated DyIII complex. Surprisingly, we found two low-lying states extremely close in energy, both displaying a strong easy axis anisotropy, tilted by ∼90°. Such a result has been rationalized, and its validity was extended upon targeted molecular modifications. These findings open new possibilities for the exploitation of such a kind of magnetic anisotropy in molecular materials.