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Controlling the self-assembly of surface-adsorbed molecules intonanostructures requires understanding physical mechanisms that act acrossmultiple length and time scales. By combining scanning tunneling microscopywith hierarchical ab initio and statistical mechanical modeling of1,4-substituted benzenediamine (BDA) molecules adsorbed on a gold (111)surface, we demonstrate that apparently simple nanostructures are selected by asubtle competition of thermodynamics and dynamics. Of the collection ofpossible BDA nanostructures mechanically stabilized by hydrogen bonding, theinterplay of intermolecular forces, surface modulation, and assembly dynamicsselect at low temperature a particular subset: low free energy oriented linearchains of monomers, and high free energy branched chains.

Competing thermodynamic and dynamic factors select molecular assemblies on a gold surface