Hierarchical assemblies in supramolecular comb polymers and discotic mesophases with mixed ligands

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This award is funded by the Macromolecular, Supramolecular and Nanochemistry Program in the Division of Chemistry. Professors Chinedum Osuji and Corey O'Hern of Yale University are supported to conduct a combined theoretical and experimental research project. The objective is to shed light on how different chemical species (atoms, molecules, ions) assemble into supramolecular functional structures. In addition to advancing fundamental knowledge, this research also provides a way to design and create new materials with useful properties. Specifically, the research aims to develop new semiconducting molecular assemblies that can be used in organic electronic devices. Supramolecular assembly is responsible for the highly optimized structures and functions of many biological macromolecules in nature. A broad variety of useful man-made materials can also be produced using supramolecular assembly, ranging from semiconductors for photovoltaics to chemical sensors and self-healing polymers. This project is supporting interdisciplinary training of graduate students and is focused on broadening participation in science through outreach to elementary, middle and high school students, and the implementation of a specially designed summer research program for high school science teachers. This project is focused on supramolecular assembly in systems in which a single species displays multiple binding sites at each of which the species can interact non-covalently with a single ligand, and in which there is more than one type of ligand present. The overarching goal of this work is to systematically elucidate self-assembly in such mixed-ligand supramolecular systems, specifically in comb polymers and discotic mesophases. The research involves a tight integration of experimental and computational efforts to understand assembly and to design novel mesophases. The specific objectives are: 1) Quantitative assessment of binding energetics and thermophysical properties; 2) Systematic experimental exploration of the structure of supramolecular assemblies in comb polymers and discotic mesophases with mixed ligands; 3) Development of coarse-grained potentials and systematic computational exploration of the structure of supramolecular assemblies in comb polymers and discotic mesophases with mixed ligands; 4) Computationally informed rational design and characterization of donor-acceptor discotic mesophases. The impact of this project originates in its development of new fundamental knowledge regarding the role of mixed ligands on supramolecular assembly, and the coherent combination of experimental and computational efforts to enable the design of new supramolecular materials.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.