“…Structural polymorphism of 2D self-assemblies at the solid/liquid or solid/gas interface has attracted increasing attention in recent years, owing to their potential applications in new material fields, such as OLEDs, , organic photovoltaic cells (OPVs), , and organic field effect transistors (OFETs). , Thus it requires us to gain deep insight into the underlying mechanism behind the formation of specific monolayer morphology to guide the design of optical devices with desirable performance. In general, the outcome of a self-assembled monolayer is determined by a delicate balance of noncovalent intermolecular interactions, including hydrogen bonding, , van der Waals force, , dipole–dipole interaction, , electrostatic force, − and so on. Great efforts have been made by researchers to understand the influence of chemical design of molecular building blocks on the self-assembled structures. − In addition, other factors, such as solute concentration, , nature of solvent, , and temperature, , are also manifested to have great impact on the outcome of the self-assemblies.…”