Magnetic and Thermodynamic Computations for Supramolecular Assemblies between a Cr(III) and Fe(III) Single-Ion Magnet and an Fe(II) Spin-Crossover Complex

Experimental results on two supramolecular complexes
in which a
CrIII or FeIII d-orbital single-ion magnet center
is embedded between a pair of FeII spin-crossover moieties
make those two complexes interesting as possible candidates for use
in quantum information technologies. We report detailed computational
results for their structure and electronic properties and use the
resulting data to parametrize a spin Hamiltonian that facilitates
comparison with experimental results and their interpretation. Consistent
with experimental results on decoherence in [Fe(ox)3]@[Fe2L3]+, we find it to be easy-plane type
while the [Cr(ox)3]@[Fe2L3]+ system is easy-axis type.