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Organic molecules show a strong tendency towards polymorphism, as they are typically weakly bound by isotropic Van der Waals forces and electrostatic interactions. In organic thin films, crystalline polymorphs may form which only exist in the vicinity of the substrate and are, therefore, denoted as (metastable) substrate-mediated polymorphs (SMPs). These types of polymorphs are important for conjugated organic molecules which are employed as organic semiconductors in novel opto-electronic devices and where the crystal structure within thin films is crucial for the device performance. Also for pharmaceutical molecules, exploiting substrate-mediated polymorphism is an emerging field of research, in the search for new medical formulations with enhanced properties compared with bulk polymorphs.