Collaborative Research: Supramolecular Materials by Nucleic Acid Block Copolymer Self-Assembly

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Nontechnical: These Collaborative awards by the Biomaterials program in the Division of Materials Research to Duke University (Lead) and North Carolina State University (Nonlead) are cofunded by the Biomedical Engineering program in the Division of Chemical, Bioengineering, Environmental, and Transport Systems (ENG). These awards are for the enzymatic synthesis of long DNA chains and the systematic scientific approaches for exploring their assembly into aggregates (micelles) and networks, and are expected to advance the field of DNA-based materials. The proposed research is transformative because it will provide design rules for the synthesis of multi-functional DNA chains that can self-assemble into morphologies with potential for drug delivery applications. The proposed research will also yield methods and strategies to fabricate oriented DNA nanowire networks over large areas. These polynucleotide networks can be metallized and thus contribute to an essential need in the rapidly growing number of nanoscale devices with applications ranging from flexible electronics to photovoltaics. The proposed projects are also emblematic for a research and training paradigm termed Reverse Engineering Biology (REBio), where students will integrate biological sciences within the engineering paradigm of design to forward engineer new products and processes. Under the REBio paradigm, the PIs are committed to: (i) providing an integrated educational and research training program for undergraduate and graduate students involved with the project; and (ii) increasing public awareness and engagement with some of the scientific concepts underlying the proposed research through hands-on, informal education opportunities for K-12 students and general audiences.Technical: Polyelectrolyte block-co-polymers show rich micellization behavior in solution and hold promise for novel functional materials in nano- and biotechnological applications. To date, however, the synthesis of polynucleotides with high molecular weight, and of oligonucleotide hybrid block-copolymers is still a challenge. Moreover, little is known about the design rules for micellar morphologies formed by block-co-polynucleotides. Despite the astounding successes in the field of DNA nanotechnology, the alignment, patterning and large scale ordering of polynucleotide assemblies on surfaces are still challenging problems that prevent use of these materials in functional devices. The research activities in this interdisciplinary, collaborative research proposal address these shortcomings. The research team will combine theory, experiment and simulations to answer questions in three specific aims: (1) to provide guidelines for synthesis and self-assembly of block-co-polynucleotides into a range of micellar structures in aqueous solutions; (2) to develop fundamental understanding and control over the assembly of functional nucleic acid networks on surfaces and the use of the networks as scaffolds for metallization; and (3) to provide cost-effective access to terminal deoxynucleotidyl Transferase needed for the scale-up of polynucleotide materials synthesis.