Structural Effects on the Spin Dynamics of Potential Molecular Qubits
Control of spin–lattice magnetic relaxation is crucial to observe long quantum coherence in spin systems at reasonable temperatures. Such a control is most often extremely difficult to achieve, because of the coexistence of several relaxation mechanisms, that is direct, Raman, and Orbach . These are not always easy to relate to the energy states of the investigated system, because of the contribution to the relaxation of additional spin-phonon coupling phenomena mediated by intramolecular vibrations. In this work, we have investigated the effect of slight changes on the molecular structure of four vanadium(IV)-based potential spin qubits on their spin dynamics, studied by alternate current (AC) susceptometry. The analysis of the magnetic field dependence of the relaxation time correlates well with the low-energy vibrational modes experimentally detected by time-domain THz spectroscopy. This confirms and extends our preliminary observations on the role played by spin-vibration coupling in determining the fine structure of the spin–lattice relaxation time as a function of the magnetic field, for S = 1 / 2 potential spin qubits. This study represents a step forward in the use of low-energy vibrational spectroscopy as a prediction tool for the design of molecular spin qubits with long-lived quantum coherence. Indeed, quantum coherence times of ca. 4.0–6.0 μs in the 4–100 K range are observed for the best performing vanadyl derivatives identified through this multitechnique approach.