Non-covalent interaction controlled 2D organic semiconductor films: Molecular self-assembly, electronic and optical properties, and electronic devices

The establishment of electronic and opto-electronic products relying on organic semiconductors (OSCs) has been intensely explored over the past few decades due to their great competitiveness in large area, low cost, flexible, wearable and implantable devices. Many of these products already entered our daily lives, such as organic light-emitting diodes-based displays, portable organic solar cells and organic field-effect transistors. The device performance of OSC devices are determined by the supramolecular organization (orientation, morphology) as well as the supramolecular organization dependent energy level alignment at various interfaces (organic/electrode, organic/dielectric, organic/organic). This review focuses on the impact of non-covalent interaction on the molecular self-assembly of organic thin films, their electronic and optical properties, as well as the device performance. Beginning with the growth of multiple OSCs on substrates with different interfacial interaction strengths (metals, insulators, semiconductors), the critical roles of molecule-substrate and intermolecular interactions in determining the thin film organization have been demonstrated. Several non-covalent interactions that contribute to the energy levels of organic materials in solid phase are summarized, mainly including the induction contributions, electrostatic interactions, band dispersions and interface dipoles. The excitonic coupling in specific aggregations of organic molecules and the corresponded effect on their optical properties are also discussed. Finally, the influences of weak intermolecular interactions on the device performance are presented.