We report the temperature dependence of the spin dynamics of the octacyanometallates [Mo(CN) _(8) ] ~(3?) and [W(CN) _(8) ] ~(3?) . At 5 K, these complexes display remarkably long spin–lattice relaxation times of 1.05 s, and 0.63 s, respectively. We probe the contributing factors to the spin relaxation and demonstrate the impact of spin–orbit coupling as a handle to tune vibrationally mediated spin–lattice relaxation.
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