Abstract
We have investigated the low-temperature magnetic state of face-centered-cubic (fcc) ${\mathrm{Cs}}_{3}{\mathrm{C}}_{60}$, a Mott insulator and the first molecular analog of a geometrically frustrated Heisenberg fcc antiferromagnet with $S=1/2$ spins. Specific heat studies reveal the presence of both long-range antiferromagnetic ordering and a magnetically disordered state below ${T}_{N}=2.2$ K, which is in agreement with local probe experiments. These results together with the strongly suppressed ${T}_{N}$ are unexpected for conventional atom-based fcc antiferromagnets, implying that the fulleride molecular degrees of freedom give rise to the unique magnetic ground state.
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