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Molecular functionalization of nanoparticles and metallic substrates can beused to tune their properties for specific applications. However,polycrystalline substrates and nanoparticles exhibit surface planes withdistinct crystallographic orientations. Therefore, the development of reliablestrategies for molecular functionalization requires knowledge of the role ofthe surface plane orientation in the growth kinetics, structure, and propertiesof the molecular layer. Here, we apply a multiscale analysis to investigate theself-assembly of 4,4'-biphenyl-dicarboxylic acid (BDA) on Ag(111) andcritically discuss the difference to Ag(100). Whereas the structural motifs forintact and fully deprotonated BDA are similar on both surfaces, theintermediate phases comprising partially deprotonated BDA differ in thestructure and chemical composition. A real-time view of the phasetransformations enables us to present a generalized picture of the phasetransformations between the self-assembled molecular phases on the surfaces andunderline important features such as the phase stabilization of the chemicalcomposition and the mechanism of the related burst transformation. Theinfluence of the substrate orientation on the structure of molecular layers andphase transformations provides the necessary background for developingfunctionalization strategies of the substrates displaying multiple surfaceplanes and kinetic models for the growth near thermodynamic equilibrium.

The Role of Phase Stabilization and Surface Orientation in 4,4'-Biphenyl-Dicarboxylic Acid Self-Assembly and Transformation on Silver Substrates