By performing high-resolution EPR and ENDOR experiments on nitrogen atoms e
ncapsulated in C-60, the capability of the quartet spin system to sense sma
ll local fields at the site of the atom is demonstrated. Such symmetry lowe
ring can either be induced by chemical modification of the cage or by a pha
se transition in polycrystalline C-60. Additional line splittings in the EP
R spectrum indicate the presence of a non-vanishing zero-field-splitting Fr
eezing of cage rotation can be observed via the magnetic dipole interaction
with C-13 nuclei of the carbon shell resulting in broadening of ENDOR tran
sitions. Fluctuating magnetic fields originating from additional paramagnet
ic species in solution can also be detected by their influence on the spin
relaxation times. (C) 2000 Elsevier Science Ltd. All rights reserved.