ABSTRACT
We report here the direct evidence of the existence of a permanent electric dipole moment in both crystal phases of a fullerene-based magnet--the ferromagnetic α-phase and the antiferromagnetic α'-phase of tetra-kis-(dimethylamino)-ethylene-C60 (TDAE-C60)--as determined by dielectric measurements. We propose that the permanent electric dipole originates from the pairing of a TDAE molecule with surrounding C60 molecules. The two polymorphs exhibit clear differences in their dielectric responses at room temperature and during the freezing process with dynamically fluctuating electric dipole moments, although no difference in their room-temperature structures has been previously observed. This result implies that two polymorphs have different local environment around the molecules. In particular, the ferromagnetism of the α-phase is founded on the homogeneous molecule displacement and orientational ordering. The formation of the different phases with respect to the different rotational states in the Jahn-Teller distorted C60s is also discussed.
ABSTRACT
We have studied the ground state of a fullerene-based magnet, the alpha;{'}-phase tetra-kis-(dimethylamino)-ethylene-C60 (alpha'-TDAE-C(60)), by electron spin resonance and magnetic torque measurements. Below T(N) = 7 K, nonparamagnetic field dependent resonances with a finite excitation gap (1.7 GHz) are observed along the a axis. Strong enhancement in their intensity as temperature is decreased is inconsistent with excitation from a singlet state, which had been proposed for the alpha'-phase ground state. Below T(N), nonquadratic field dependence of the magnetic torque signal is also observed in contrast to quadratic field dependence in the paramagnetic phase. The angle-dependent torque signals below T(N) indicate the existence of an anisotropy of the bulk magnetization. From both experiments, we propose an antiferromagnetic ground state driven by the cooperative orientational ordering of C(60) in the alpha'-TDAE-C(60).
