Electron spin relaxation of N@C 60 in CS 2

John J.L. Morton, Alexei M. Tyryshkin, Arzhang Ardavan, Kyriakos Porfyrakis, S. A. Lyon, G. Andrew, D. Briggs

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Abstract

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.

Original languageEnglish (US)
Article number014508
JournalJournal of Chemical Physics
Volume124
Issue number1
DOIs
StatePublished - Apr 10 2006

All Science Journal Classification (ASJC) codes

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

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    Morton, J. J. L., Tyryshkin, A. M., Ardavan, A., Porfyrakis, K., Lyon, S. A., Andrew, G., & Briggs, D. (2006). Electron spin relaxation of N@C 60 in CS 2 Journal of Chemical Physics, 124(1), [014508]. https://doi.org/10.1063/1.2147262