Molecular quartet states, generated by photoexcitation of chromophore-radical conjugates, have been shown to exhibit attractive properties for applications in the field of molecular spintronics. Many of these applications, such as quantum sensing, require a coherent manipulation of the spin system, implying the need to control the quartet state spin coherence properties. By examining the influence of structural and matrix-related factors, we demonstrate a correlation between the coherence decay of the photogenerated quartet state and that of the tethered stable radical, paving the way for a rational design of photogenerated molecular three-spin systems with optimized coherence properties.
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