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The electronic behavior of polymerized fullerite structures, ranging fromone-dimensional to three-dimensional polymers, was studied using densityfunctional theory. The bandgap across these structures decreases with the riseof sp3-carbon content until metallic behavior is observed. A further increaseinduces a reopening of the bandgap, revealing a reentrant semiconductingbehavior in this class of materials. This behavior is understood in terms ofthe new electronic states originated by polymeric bonding and the effect of thevolume reduction on the dispersion of sp2-states. This study highlights thefullerite polymers as a magnificent platform to tune electronic properties.

Reentrant semiconducting behavior in polymerized fullerite structures with increasing sp3-carbon content