![]() Analyses of numerous reported epitaxial molecular films reveal that coincidence is quite common even though, based on overlayer–substrate interface energies alone, not as energetically favorable as commensurism. In the case of molecular overlayers, the mismatch of overlayer and substrate symmetries commonly leads to coincident epitaxy in which some of the overlayer lattice points do not reside on substrate lattice points. The different modes of epitaxy can be organized hierarchically to reflect the balance of overlayer–substrate and molecule–molecule energies. A much-needed grammar of epitaxy is presented that classifies the various modes of epitaxy according to transformation matrices that relate the overlayer lattice to the substrate lattice. This review describes the role of epitaxy in molecular organization on crystalline substrates. The recent emergence of molecular films as candidates for functional electronic materials has prompted numerous investigations of the underlying mechanisms responsible for their structure and formation.
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