“…The field of organic electronics has attracted large attention during the last decades because of its promising perspective for the fabrication of flexible thin-film devices. − Compared with covalently bound inorganic semiconductors, organic semiconductors (OSCs) are only weakly bound, which results in small sublimation enthalpies and low barriers for diffusion processes, , hence making the preparation of ordered (possibly crystalline) thin films and heterostructures challenging. , Owing to the shape anisotropy of the molecular entities, the optoelectronic properties of OSC solids are also rather anisotropic and further depend on the molecular and crystalline orientation , as well as on the adopted packing motifs (e.g., polymorphs), − which adds another complexity to the task of producing ordered OSC films for optoelectronic applications. OSC films on metal or insulator substrates often grow in a Stranski–Krastanov mode and exhibit a notable dewetting and island formation which originates from the structural mismatch between the first monolayer (i.e., wetting layer) and the OSC bulk crystal structure. , In addition, many OSCs exhibit a kinetic roughening upon thin-film deposition, which is attributed to the Ehrlich–Schwöbel barriers at terrace edges or grain boundaries, − and aggravates the preparation of smooth OSC films. Such growth instabilities are critical issues because discontinuity and defect-induced trap states significantly reduce the resulting charge carrier mobility in organic thin-film devices. , Besides such device requirements, the fabrication of smooth and crystalline films of homogeneous thickness is also of great interest for more fundamental studies such as time-resolved studies of photoexcitations in OSC films because it enables to obtain thickness-dependent transfer dynamics toward metallic electrodes. , …”