Critical-Thickness-Governed Assembly of Nonamphiphilic Molecular Monolayers at the Air–Water Interface for Layer-by-Layer Optoelectronic Architectures

, and coronene, with monolayer thicknesses of 1.3, 0.6, and 0.9 nm, respectively. The resulting monolayers adopt a glassy state that enables transfer and sequential layer-by-layer stacking with centimeter-scale uniformity. Their amorphous nature preserves strong photoluminescence and, combined with molecular-level control over donor-acceptor interfaces, allows precise tuning of charge retention dynamics essential for optoelectronic applications. This work provides experimental evidence that the air-water interface can be utilized to manipulate nonamphiphilic molecules with monolayer precision, thereby enabling bottom-up nanoarchitectonics of functional thin films using molecular building blocks not limited to conventional surface-active species.