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Central hyperfine components of a mixture of N@C 60 (large peak) and N@C 70 shown on an expanded scale. 5(3) ppm. 4. 1. Long range order in N@C60 crystals below 260 K As an example for the applicability of N@C 6o as a local symmetry probe, we studied the first-order phase transition of crystalline C60 at 258 K [22]. 2Pic) high temperature face centered cubic Fm3m to the ordered simple cubic Pa3 phase, as was revealed by X-ray and neutron scattering methods [48, 49] . , the position occupied by the nitrogen atom, is lowered from Th to S6' allowing for a non-vanishing second-rank tensor interaction ofaxial symmetry in the low temperature phase.

However, additional relaxation processes caused by lattice vibrations come into play and limit the relaxation times. The phonons lead to time dependent distortions of the cage and, via the fine structure interaction, to a spin lattice relaxation. Since the fine structure affects the 13121 --7 11/21 and 1/2 --7 -1/2 transitions differently, different relaxation times are expected. However, one should bear in mind that the transition rates are not independent from one another and therefor a clear separation is not possible.

At elevated temperatures, N@C 60 , P@C 60 and N@C 70 become unstable and decay, probably via the escape of the trapped atom from the cage. The decay can be monitored via the EPR intensity in an isochronal annealing experiment [30]. Figure 16 shows the number of N@C 60 in the sampie (derived from the EPR intensity multiplied by the absolute temperature to correct for the Curie dependence) 36 B. PIETZAK ET AL. Table 2. Stable endohedral compounds formed of group V elements and fullerenes. C60 C 70 CS4 Nitrogen Phosphorus N@C60 N@C70 P@C60 Arsenic not stable as a function of the annealing temperature.

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