Spin canting in a Dy-based Single-Chain Magnet with dominant next-nearest neighbor antiferromagnetic interactions

We investigate theoretically and experimentally the static magnetic properties of single crystals of the molecular-based Single-Chain Magnet (SCM) of formula [Dy(hfac)$_{3}$NIT(C$_{6}$H$_{4}$OPh)]$_{\infty}$ comprising alternating Dy$^{3+}$ and organic radicals. A peculiar inversion between maxima and minima in the angular dependence of the magnetic molar susceptibility $χ_{M}$ occurs on increasing temperature. Using information regarding the monomeric building block as well as an {\it ab initio} estimation of the magnetic anisotropy of the Dy$^{3+}$ ion, this anisotropy-inversion phenomenon can be assigned to weak one-dimensional ferromagnetism along the chain axis. This indicates that antiferromagnetic next-nearest-neighbor interactions between Dy$^{3+}$ ions dominate, despite the large Dy-Dy separation, over the nearest-neighbor interactions between the radicals and the Dy$^{3+}$ ions. Measurements of the field dependence of the magnetization, both along and perpendicularly to the chain, and of the angular dependence of $χ_{M}$ in a strong magnetic field confirm such an interpretation. Transfer matrix simulations of the experimental measurements are performed using a classical one-dimensional spin model with antiferromagnetic Heisenberg exchange interaction and non-collinear uniaxial single-ion anisotropies favoring a canted antiferromagnetic spin arrangement, with a net magnetic moment along the chain axis. The fine agreement obtained with experimental data provides estimates of the Hamiltonian parameters, essential for further study of the dynamics of rare-earths based molecular chains.

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