Development of Open and Closed Shell Multifunctional Materials for Magnetic, Conductive and Optical Applications

世界范围内对能源日益增长的需求不仅推动了对替代(非化石)燃料来源的探索，也推动了对能源和信息采集、转移和处理的新技术的探索。在后晶体管数字时代，新的电子和光学设备需要相对于传统的硅基系统具有更高的性能；它们必须更小、更轻、更高效。鉴于这些需求，有机材料作为新的电子、光学和磁性材料的基础材料具有很大的吸引力。最近的诺贝尔化学奖(2000年)和诺贝尔物理学奖(2010年)因在导电有机物方面的开创性工作而获奖，反映了近年来取得的兴趣和进展。对于继续这些技术进步至关重要的是具有量身定做特性的设计的新材料。这一努力激发了工业和学术环境中的研究，代表了本研究提案的基本动机，该研究提案涉及设计和开发用于分子电子的新型多功能材料。*我们的目标是通过对几个广受关注的领域作出新颖的创新贡献来解决这项任务。具体的研究方向是：*1.杂环自由基：这里我们的重点是双重的；我们试图揭示支配可分离的中性自由基的基本反应性，并将这些应用于领先的材料应用。我们将建立合成方法来制备各种新的查尔卡基和多自由基，并将它们应用到导电、磁性或光学器件中。这项工作将对开壳化合物的合成、结构和性质产生新的和有影响的化学见解，以开发具有改变分子电子学材料设计所需的多样性和特殊性能的创新材料。*2.配体设计和配位化学：利用我们在杂环材料方面的专业知识，我们将挖掘查尔卡基作为配体的巨大潜力。我们将制备多齿配体，并开发轻质、致密的材料，使金属离子可以通过配体进行交流。这项工作将解决影响合成方法学的关键因素，这些因素将影响作为配体的多功能、未被探索的Chalcazyls家族，并为多金属配合物/聚合物/网络的有趣的物理性质提供新的见解。*3.共价有机框架(COF)：在这个新的研究方向，我们将开发基于自由基的COF。这项高风险的工作有望使我们的研究更上一层楼，为寻求高性能共轭聚合物提供新的战略和方向，为从有机电子和能量存储到气体分离和存储等领域的创新铺平道路。

Increasing worldwide demand for energy is driving not only the search for alternative (non-fossil) fuel sources, but also the exploration of new technologies for harvesting, transferring and processing energy and information. In the post-transistor digital age, new electronic and optical devices are required to have improved performance relative to conventional silicon-based systems; they must be smaller, lighter and more efficient. In light of these demands, the case for organic materials as building blocks for new electronic, optical and magnetic materials holds much appeal. Recent Nobel Prizes in Chemistry (2000) and Physics (2010), awarded for groundbreaking work in conductive organics, reflect both the interest and progress that has been made in recent years. Essential to the continuation of these technological advancements are new materials by design with tailor made properties. This endeavour, which inspires research in industrial and academic settings, represents the underlying motivation for the present research proposal involving the design and development of new multifunctional materials for molecular electronics. ******We aim to address this task by making novel innovative contributions to several areas of broad interest. Specific research directions are:******1. Heterocyclic Radicals: Here our focus is twofold; we seek to uncover the fundamental reactivity that governs isolable neutral radicals, and to deploy these within leading materials applications. We will establish the synthetic methodology to prepare a variety of new chalcazyl radicals and polyradicals, and implement them into conductive, magnetic or optical devices. This work will produce novel and impactful chemical insight into the synthesis, structure and properties of open-shell compounds in order to develop innovative materials that have the diversity and exceptional properties required to transform materials design for molecular electronics.******2. Ligand Design & Coordination Chemistry: Exploiting our expertise in heteroaromatic materials, we will tap into the enormous potential of chalcazyls as ligands. We will prepare polydentate ligands, and develop lightweight, densely packed materials in which the metal ions can communicate through the ligand. This work will address key factors that affect the synthetic methodology of the spectacularly versatile, underexplored family of chalcazyls as ligands, and provide novel insight into the intriguing physical properties of multi-metallic complexes/polymers/networks.******3. Covalent Organic Frameworks (COFs): In this new research direction, we will develop radical-based COFs. This high-risk work promises to take our research to the next level, providing a new strategy and direction in the quest for high-performance-conjugated polymers that can pave the way for innovations in fields from organic electronics and energy storage to gas separation and storage.