High-field ESR measurements of the soft ferromagnetic [TDAE]C-60 above
T-c are presented. The ESR spectra are asymmetric already at elevated
temperatures and reflect the symmetry of the unit cell. The data are
critically put in the context to the results of other groups. It will
be shown that in contrast to all previous publications the TDAE cation
s are an essential ingredient for the magnetism of this fullerene char
ge transfer complex. The spins in this complex are localized at higher
temperatures, but are more and more delocalized by spin exchange inte
ractions towards T-c. None of the results gives an indication that [TD
AE]C-60 is an itinerant molecular ferromagnet. The exchange path inclu
des the TDAE cations. That means, a strong exchange coupling between C
-60 and TDAE prevails. Thus, no unplausible cancellation mechanism for
the TDAE radical cation spins, as discussed extensively in the litera
ture, must be considered.