Orientation dependence of phase memory relaxation in the V(IV) ion at high frequencies

Understanding how magnetic relaxation depends on molecular orientation is a fundamental parameter for designing magnetic molecules for application. Herein we report the first use of pulsed high-frequency electron paramagnetic resonance spectroscopy (HFEPR, 120 and 240 GHz) to define the orientation dependence of phase memory relaxation in the S = 1/2 V(IV) complex (n-Bu3NH)(2)[V(C6H4O2)(3)]. We demonstrate a variation of 20% of the phase memory relaxation time (T-m) as a function of the orientation of the [V(C6H4O2)(3)](2-) molecule in the applied magnetic field. Ultimately, this work underlines an important design strategy for molecule-based quantum computing architectures.