ABSTRACT
By quantum-chemical calculations, here, we ascertain the intrinsic electronic and conducting properties of molecular material prototypes for graphene-based nanostructures, and how these properties evolve as a function of their size with an increased dimensionality (from quasi-one dimensional in the case of isolated nanoribbons to three-dimensional arrangements when they self-organize in common samples). As it is expected in regular devices architectures, whether they are purely organic thin lms allowing for the diffusive transport of the charge carrier upon its injection from an external source, or electrode-molecule(s)–electrode nanojunctions targeted to study charge transport in the coherent regime, the relative positions of the interacting molecules can signicantly alter the conclusions found for an isolated molecule. Since the supramolecular ordering of the organic layers is intimately related to the existing noncovalent interactions driving the specic mode of packing, we also investigate how to efciently incorporate these effects into state-of-the-art calculations without giving up the computational cost-effectiveness that allow the tackling of longer and more complicated systems. Thus, owing to a clear understanding of structure-property relationships for isolated and packed molecules in both regimes, we can conrm two-dimensional nanographene-based materials as promising candidates for organic and molecular electronics.
