Using pulsed EPR techniques, the electron spin relaxation properties o
f nitrogen atoms encapsulated in C-60 have been studied. Because of th
e high symmetry of the cage, most of the conventional relaxation mecha
nisms otherwise affecting electron spins in solution are absent, resul
ting in an exceptional homogeneous ERP linewidth of only 2.5 kHz. Appa
rently, solvent collision-induced deformations of the carbon shell whi
ch modulate the zero-field-splitting sensed by the quartet spin state
of N@C-60 are the dominant spin relaxation mechanism. (C) 1997 Elsevie
r Science B.V.