  We examine the temperature dependence of the relaxation times of the
molecules N@C60 and N@C70 (which comprise atomic nitrogen trapped within a
carbon cage) in liquid CS2 solution. The results are inconsistent with the
fluctuating zero field splitting (ZFS) mechanism, which is commonly invoked to
explain electron spin relaxation for S > 1/2 spins in liquid solution, and is
the mechanism postulated in the literature for these systems. Instead, we find
a clear Arrhenius temperature dependence for N@C60, indicating the spin
relaxation is driven primarily by an Orbach process. For the asymmetric N@C70
molecule, which has a permanent non-zero ZFS, we resolve an additional
relaxation mechanism caused by the rapid reorientation of its ZFS. We also
report the longest coherence time (T2) ever observed for a molecular electron
spin, being 0.25 ms at 170K.
