Molecular assembly has been explored from various hierarchical structures with diverse functions and application. Pioneering efforts from modern soft-matter chemistry are now discovering rich libraries of combination of the chemical functionalities and mesoatomic building structures. The observation of unique arrays and alignments assembled by new ordered structures facilitates the study of corresponding structure-property relationships and the development of functional materials. In the past two decades, the fascinating sphere-packing Frank-Kasper (FK) phases have come to us as an intriguing molecular assembly. Well-studied self-assembling soft-matter systems include small-molecular components of dendrons, surfactants, liquid crystals, and block copolymers. Among those candidates, the dendrons show the modular structures that can pack into ordered structures with complex 2D and 3D geometries, enabling potential applications in the fields of molecular electronics, catalysts, porous materials, drug delivery, and bio-mimetic systems. In this study, we design and present a strategy to create the FK phases from simple second-generation (G2) dendrons possessing different apex functionalities (Xs) that modulate core interactions among the apex groups. The dendrons of G2-X were synthesized by a convergent method and post-functionalized at terminal X to have CONH2, CH2OH, and CH2NH2 which are in decreasing order of core interactions (or H-bonding). With a versatile modular platform of G2-X, we seek to answer a question about how enthalpic and entropic contributions affect dendron assemblies. In-situ small-angle X-ray scattering (SAXS) and FT-IR spectroscopy are measured to trace temperature-dependent assembly phases with respect to the core interactions.

Apex-dependent mesoscale crystals from second-generation dendron assembly

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ACS Fall 2022

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