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The organization of nano-objects on macroscopic surfaces is a key challenge for the technological improvement and implementation of nanotechnologies. For achieving operational functions, it is required to assemble nano-objects as controllable building blocks in highly ordered superstructures. Herein, we demonstrate the growth and self-organization of metallic nanowires on surfaces into hexagonal superlattices with tunable characteristic lengths depending of the stabilizing surfactants employed. Starting from a reacting mixture containing a Pt(111) substrate, a Co organometallic precursor, an amine, and an acid dissolved in a solvent, we quantify the structural evolution of superlattices of vertical single-crystalline Co nanowires on Pt, using a combined analysis of small angle neutron scattering, transmission, and scanning electron microscopies. We show the concerted steps of a spontaneous growth and self-organization of the nanowires into two-dimensional (2D) hexagonal lattice on Pt, at intervals starting from a few hours of reaction to a highly ordered superlattice at longer times. Furthermore, it is shown that apart from long-chain acid and long-chain aliphatic amine pairs used as stabilizers, the combination of a long-chain aliphatic and a short-chain aromatic ligand in the synthesis can also be employed for the nanowire superlattices development. Interestingly, the possibility to employ different pairs allows quantitative modulation of the nanowire arrays, such as the interwire distance and the packing fraction.
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