Collaborative Research: Directed Charge Transfer in Metal Containing Peptide Nucleic Acid Assemblies

在这个由化学系大分子、超分子和纳米化学计划资助的项目中，卡内基梅隆大学的Catalina Achim、匹兹堡大学的David WalDeck和杜克大学的David Beratan将开发无机-核酸混合结构，并研究通过这些结构的电荷转移，目标是在长达数十纳米的尺度上指导和控制电荷流动。含有电活性单元的肽核酸(PNA)构建块将与互补核酸(DNA或PNA)一起用作构建块的模板，以自组装和形成预先编程的电活性组件。拟议研究的主要特点是采用通用和模块化的方法，将预定义空间位置的无机或有机电荷转移成分合并到基于核酸的结构支架中。具有互补专业知识(合成、表征和理论)的研究团队将合作定义合成方法，开发预测模型，并量化这些新的电活性超分子结构的结构和功能。这一合作研究计划的更广泛影响来自：(1)为电荷转移创建新的范例，(2)为利用网络基础设施的科学教育创造新的教学工具，以及(3)加强STEM劳动力的多样性的外联活动。这项工作将加强我们对纳米尺寸的超分子结构中电荷转移的基本理解，这种结构模仿了生物系统中存在的类似尺寸的结构。最终，这种工作可能导致一种将电子平台与生物系统相结合的一般方法。

In this project funded by the Macromolecular, Supramolecular and Nanochemistry Program of the Chemistry Division, Catalina Achim of Carnegie Mellon University, David Waldeck of University of Pittsburgh, and David Beratan of Duke University will develop hybrid inorganic-nucleic acid structures and study charge transfer through these structures with the goal to direct and control charge flow on length scales up to tens of nanometers. Peptide nucleic acid (PNA) building blocks that contain electroactive units will be used, together with complementary nucleic acids (DNA or PNA) as a template for the building blocks, to self-assemble and form preprogrammed electroactive assemblies. The key feature of the proposed research is the general and modular approach to incorporate inorganic or organic charge transfer components at predefined spatial locations in a nucleic acid-based structural scaffold. The team of researchers with complementary expertise (synthesis, characterization, and theory) will collaborate to define the synthetic methodologies, to develop the predictive models, and to quantify the structure and the function of these novel electroactive, supramolecular structures. The broader impacts of this collaborative research program originate from: (1) the creation of new paradigms for charge transfer, (2) the creation of new pedagogical tools for science education that make use of cyber-infrastructure, and (3) outreach activities that enhance diversity in the STEM workforce. This work will enhance our fundamental understanding of charge transfer in nano-size, supramolecular structures that mimic similar-size structures present in biological systems. Ultimately such work could lead to a general approach for integrating electronic platforms with biological systems.