Journal
PHYSICAL REVIEW B
Volume 79, Issue 13, Pages -Publisher
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevB.79.134419
Keywords
ab initio calculations; antiferromagnetic materials; canted spin arrangements; exchange interactions (electron); Heisenberg model; magnetic anisotropy; magnetic moments; magnetic susceptibility; molecular magnetism; weak ferromagnetism
Funding
- NE-MAGMANET [FP6-NMP3-CT-2005-515767]
- Seventh Framework Programme of EC [FP7-PIEF-GA-2008-220498]
- German DFG [SPP1137]
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We investigate theoretically and experimentally the static magnetic properties of single crystals of the molecular-based single-chain magnet of formula [Dy(hfac)(3)NIT(C6H4OPh)](infinity) comprising alternating Dy3+ and organic radicals. The magnetic molar susceptibility chi(M) displays a strong angular variation for sample rotations around two directions perpendicular to the chain axis. A peculiar inversion between maxima and minima in the angular dependence of chi(M) occurs on increasing temperature. Using information regarding the monomeric building block as well as an ab initio estimation of the magnetic anisotropy of the Dy3+ 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 Dy3+ ions dominate, despite the large Dy-Dy separation, over the nearest-neighbor interactions between the radicals and the Dy3+ ions. Measurements of the field dependence of the magnetization, both along and perpendicularly to the chain, and of the angular dependence of chi(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 noncollinear 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-earth-based molecular chains.
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