Thin film deposition on weakly interacting substrates exhibits a unique growth mode characterized by initially strong island formation and rapidly increasing roughness, which reaches a maximum and subsequently decreases as the film returns to a smooth morphology. Here we show this rough-to-smooth growth mode experimentally for two molecular systems with substantially different geometries, namely, the effectively spherical buckminsterfullerene (${\mathrm{C}}_{60}$) and the disk-like 1,4,5,8,9,11-hexaazatriphenylenehexacarbonitrile. This growth mode is explained by a geometrical model that captures the basic mechanisms of multilayer island growth, island coalescence, and formation of a continuous film. Additionally, kinetic Monte Carlo simulations with minimal ingredients demonstrate that this mode generally occurs for weakly interacting substrates, providing quantitative estimates of parameters that characterize adsorbate-adsorbate and adsorbate-substrate interactions. Both the model and simulations accurately describe the experimental data and highlight the generic nature of the phenomenon, independently of the details of the interactions and the molecular flux, which opens up a path for controlling nanoscale film roughness.

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• Adsorption
• Growth
• Island
• Nucleation on surfaces
• Roughness
• Surfaces
• Thin films
• Atomic force microscopy
• Crystallography
• Film deposition
• Grazing-incidence X-ray diffraction
• Grazing-incidence small-angle x-ray scattering
• Monte Carlo methods
• X-ray reflectivity