Ab initio predictions of graphite-like phase with anomalous grain boundaries and flexoelectricity from collapsed...

Although large-radius carbon nanotubes (CNTs) are now available in macroscopic quantities, little is known about their condensed phase. Large-scale density functional theory calculations predict a low energy phase in which the same-diameter "dog-bone" collapsed CNTs form a graphite-like phase with complex, anomalous grain boundaries (GBs). The excess GB volume does not prevent the strong van der Waals coupling of the flattened CNT sides into AB stacking. The associated GB energetics is dominated by the van der Waals energy penalty and high curvature bending of the loop CNT edges, which exhibit reactivity and flexoelectricity. The large density and superior mechanical rigidity of the proposed microstructural organization as well as the GB flexoelectricity are desirable properties for developing ultra-strong composites based on large-radius CNTs.