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We have studied the ground state of a fullerene--based magnet, the$\alpha'$--phase tetra--$kis$--(dimethylamino)--ethylene--C$_{60}$($\alpha'$--TDAE--C$_{60}$), by electron spin resonance (ESR) and magnetictorque measurements. Below T$_N=7$ K, non--paramagnetic field dependentresonances with a finite excitation gap (1.7 GHz) are observed along the$a$--axis. Strong enhancement in their intensity as temperature is decreased isinconsistent with excitation from a singlet state, which had been proposed forthe $\alpha'$--phase ground state. Below T$_N$, non--quadratic field dependenceof magnetic torque signal is also observed in contrast to quadratic fielddependence in the paramagnetic phase. The angle--dependent torque signals belowT$_N$ indicate the existence of an anisotropy of the bulk magnetization. Fromboth experiments, we propose an antiferromagnetic ground state driven by thecooperative orientational ordering of C$_{60}$ in the$\alpha'$--TDAE--C$_{60}$.

Antiferromagnetic order driven by the molecular orbital order of C$_{60}$ in $\alpha'$--tetra--$kis$--(dimethylamino)--ethylene--C$_{60}$