Two-Dimensional Molecular Architectonics through Controlled Noncovalent Interactions: Structure, Functional Properties, and Applications

Fabrication of well-defined two-dimensional (2D) architectures employing organic or organic–inorganic hybrid molecular systems through bottom-up methodologies is a challenging task. The scheme of molecular architectonics aids in fabricating tailor-made 2D architectures through the controlled molecular assembly process. In this methodology, the controlled assembly characteristics are bestowed to functional organic cores by equipping them with appropriate biomolecular auxiliaries with inherent molecular recognition properties. The derived functional building blocks seamlessly integrate into two-dimensional macro-, micro-, and nanosheet structures through subtle noncovalent molecular assembly, coassembly, and templated assembly, ultimately showcasing a range of emergent functional properties and applications across various fields such as optoelectronics, catalysis, sensing, self-cleaning, drug delivery, and tissue engineering, among others. In this Perspective, we discuss auxiliary-guided 2D assembly architectures of functional cores through molecular assembly, coassembly, hierarchical assembly, tweezer-sandwich-inclusion (TIS) assembly, templated assembly, chiral assembly, complex dynamical assembly, self-sorted assembly, and the breath figure technique (BFT)-type assembly. The resulting tailor-made 2D architectures exhibit optoelectronic, conducting, chiro-optical, mechanical, sensor, host–guest recognition, and superhydrophobic properties.