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Journal of Chemical Physics / Volume 124 / Issue 1 / ARTICLES / Condensed Phase Dynamics, Structure, and Thermodynamics: Spectroscopy, Reactions, and Relaxation

J. Chem. Phys. 124, 014508 (2006); http://dx.doi.org/10.1063/1.2147262 (5 pages)

Electron spin relaxation of N@C60 in CS2

John J. L. Morton1, Alexei M. Tyryshkin2, Arzhang Ardavan3, Kyriakos Porfyrakis4, S. A. Lyon2, and G. Andrew D. Briggs4

1Department of Materials, Oxford University, Oxford OX1 3PH, United Kingdom and Clarendon Laboratory, Department of Physics, Oxford University, Oxford OX1 3PU, United Kingdom
2Department of Electrical Engineering, Princeton University, Princeton, New Jersey 08544
3Clarendon Laboratory, Department of Physics, Oxford University, Oxford OX1 3PU, United Kingdom
4Department of Materials, Oxford University, Oxford OX1 3PH, United Kingdom

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(Received 25 October 2005; accepted 9 November 2005; published online 6 January 2006)

We examine the temperature dependence of the electron spin 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 spins in liquid solution, and is the mechanism postulated in the literature for these systems. Instead, we find an 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 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 170 K.

© 2006 American Institute of Physics

Article Outline

  1. INTRODUCTION
  2. MATERIALS AND METHODS
  3. RELAXATION OF N@C60 IN CS2
    1. ZFS fluctuations
    2. Orbach relaxation process
  4. RELAXATION OF N@C70 IN CS2
  5. CONCLUSIONS

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KEYWORDS and PACS

Keywords

fullerenes, paramagnetic resonance, caesium

PACS

  • 76.30.-v

    Electron paramagnetic resonance and relaxation

  • 61.48.-c

    Structure of fullerenes and related hollow and planar molecular structures

ARTICLE DATA

Digital Object Identifier
http://dx.doi.org/10.1063/1.2147262

PUBLICATION DATA

ISSN

0021-9606 (print)  
1089-7690 (online)

Publisher

$abstract.society.value is a Member of CrossRef American Institute of Physics

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    References

    J. J. L. Morton, A. M. Tyryshkin, A. Ardavan, K. Porfyrakis, S. A. Lyon, and G. A. D. Briggs, J. Chem. Phys. 122, 174504 (2005)JCPSA6000122000017174504000001.

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    J. J. L. Morton, A. M. Tyryshkin, A. Ardavan, K. Porfyrakis, S. A. Lyon, and G. A. D. Briggs, Phys. Rev. Lett. 95, 200501 (2005).

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