We examine the temperature dependence of the electron spin relaxation times of the molecules N@C 60 and N@C 70 (which comprise atomic nitrogen trapped within a carbon cage) in liquid CS 2 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 spins in liquid solution, and is the mechanism postulated in the literature for these systems. Instead, we find an Arrhenius temperature dependence for N@C 60, indicating the spin relaxation is driven primarily by an Orbach process. For the asymmetric N@C 70 molecule, which has a permanent ZFS, we resolve an additional relaxation mechanism caused by the rapid reorientation of its ZFS. We also report the longest coherence time (T 2) ever observed for a molecular electron spin, being 0.25 ms at 170 K.
All Science Journal Classification (ASJC) codes
- Physics and Astronomy(all)
- Physical and Theoretical Chemistry