Abstract
High-frequency (f = 190 GHz) electron paramagnetic resonance (EPR) at magnetic fields up to 12 T and Q-band (f = 34.1 GHz) EPR were performed on single crystals of the molecular wheel CsFe(8). In this molecule, eight Fe(III) ions, which are coupled by nearest-neighbor antiferromagnetic (AF) Heisenberg exchange interactions, form a nearly perfect ring. The angle-dependent EPR data allow for the accurate determination of the spin Hamiltonian parameters of the lowest spin multiplets with S ≤ 4. Furthermore, the data can be well reproduced by a dimer model with a uniaxial anisotropy term, with only two free parameters J and D. A fit to the dimer model yields J = -15(2) cm(-1) and D = -0.3940(8) cm(-1). A rhombic anisotropy term is found to be negligibly small, E = 0.000(2) cm(-1). The results are in excellent agreement with previous inelastic neutron scattering and high-field torque measurements. They confirm that the CsFe(8) molecule is an excellent experimental model of an AF Heisenberg ring. These findings are also important within the scope of further investigations on this molecule such as the exploration of recently observed magnetoelastic instabilities.
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