Mononuclear transition metal complexes demonstrate significant potential in the divergent applications of spintronics and quantum information processing. The facile tunability of these complexes enables structure function correlations for a plethora of relevant magnetic quantities. We present a series of pseudotetrahedral [Co(C3S5)2]2- complexes with varying deviations from D2d symmetry to investigate the influence of structural distortions on spin relaxation dynamics and qubit viability, as tuned by the variable transverse magnetic anisotropy, E. To overcome the traditional challenge of measuring E in species where D ≫ E, we employed a different approach of harnessing ac magnetic susceptibility to probe the emergence of quantum tunneling of magnetization as a proxy for E. Across the range of values for E in the series, we observe magnetic hysteresis for the smallest value of E. The hysteresis disappears with increasing E, concomitant with the appearance of an observable, low frequency (L-band) electron paramagnetic resonance (EPR) signal, indicating the potential to controllably shift the molecule's utilization from classical to quantum information processing applications. The development of design principles for molecular magnet information processing requires separate design principles for classical versus quantum regimes. Here we show for the first time how subtle structural changes can switch the utility of a complex between these two types of applications.
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