Abstract
Comprehensive SummaryCompounds with magnetic bistability is highly attractive for the construction of switches, thermal sensors, information‐storage media and memory devices. Herein, we report a crystalline fullerene radical anion salt [Na(THF)5]C60 (1), obtained by the reduction of C60 with Na in solution, which exhibits magnetic bistability accompanied with one magnetostructural transition, giving low temperature (LT), high temperature (HT) phases and a metastable phase. Fullerene radical anions (C60•‐) in the structure were found arranged into a three‐dimensional close‐packed honeycomb subnetwork with hollow channels occupied by complex cations [Na(THF)5]+ as spacers. The magnetic bistability is attributed to structural transitions as the LT−IT phase transition was associated with the orientational disorder of fullerene anions and the distortion of the complex cations [Na(THF)5]+ in the 3D packing of fullerene anions.
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