C-13 hyperfine coupling constants of the MuC(60) radical have been mea
sured by muon level-crossing spectroscopy, using a dilute solution of
99% enriched C-13(60) in decalin. The signs as well as the magnitudes
of the hyperfine constants were determined. The results range from 52.
6 to -25.4 MHz and support those calculations which predict an extende
d distribution of unpaired electron spin density in radical adducts of
fullerenes. The hyperfine constants are consistent with published ele
ctron spin resonance results for (CD3)(3)CC60, but contradict a recent
report for HC60, where a considerably smaller value is reported for t
he largest splitting.