Spin Dynamics and Low Energy Vibrations: Insights from Vanadyl-Based Potential Molecular Qubits

Here we report the
investigation of the magnetization dynamics
of a vanadyl complex with diethyldithiocarbamate (Et2dtc–) ligands, namely [VO­(Et2dtc)2] (1), in both solid-state and frozen solution. This
showed an anomalous and unprecedentedly observed field dependence
of the relaxation time, which was modeled with three contributions
to the relaxation mechanism. The temperature dependence of the weight
of the two processes dominating at low fields was found to well correlate
with the low energy vibrations as determined by THz spectroscopy.
This detailed experimental comparative study represents a fundamental
step to understand the spin dynamics of potential molecular quantum
bits, and enriches the guidelines to design molecule-based systems
with enhanced quantum coherence.