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Molecules self-assemble on surfaces forming a variety of patterns that depend on the relative strength between the intermolecular and molecule–surface interactions. In this study, the effect of the physisorption/chemisorption interplay on self-assembly is investigated using Monte Carlo simulations. The molecules are modeled as hexagonal tiles capable of assuming two distinct adsorption states, with different diffusion properties, on a hexagonal lattice. The self-assembled structures that emerge by tuning the molecule–surface and molecule–molecule interactions are systematically mapped out to develop understanding of their phase behavior. The resulting phase diagrams will guide the engineering of novel molecules to obtain desired collective structural properties for the development of innovative two-dimensional devices.

Influence of Molecule–Surface and Molecule–Molecule Interactions on Two-Dimensional Patterns Formed by Functionalized Aromatic Molecules