A Mononuclear Transition Metal Single-Molecule Magnet in a Nuclear Spin-Free Ligand Environment

The high-spin pseudotetrahedral complex [Co­(C3S5)2]2– exhibits slow magnetic relaxation in the absence of an applied dc magnetic field, one of a small number of mononuclear complexes to display this property. Fits to low-temperature magnetization data indicate that this single-molecule magnet possesses a very large and negative axial zero-field splitting and small rhombicity. The presence of single-molecule magnet behavior in a zero-nuclear spin ligand field offers the opportunity to investigate the potential for this molecule to be a qubit, the smallest unit of a quantum information processing (QIP) system. However, simulations of electron paramagnetic resonance (EPR) spectra and the absence of EPR spectra demonstrate that this molecule is unsuitable as a qubit due to the same factors that promote single molecule magnet behavior. We discuss the influence of rhombic and axial zero-field splitting on QIP applications and the implications for future molecular qubit syntheses.