New Redox-Active Organic pi-Conjugated Building Blocks for Functional Nanoscale Materials and Devices

有机pi共轭材料的快速发展导致了能量存储和转换、有源显示、化学和生物传感以及纳米电子器件和光子器件等前沿技术的巨大进步。有机材料的优势在于其易于通过化学修饰来定制的性质，以及材料加工和器件制造的低成本。在我们最近由NSERC发现基金资助的研究中，在设计和合成各种具有氧化还原活性的共轭分子和相关的大分子体系方面取得了重大突破。这些材料为我们提供了多才多艺的分子“积木”来制备新的纳米材料和组装先进的分子器件。 在这项建议中，我们的目标是在我们已有的知识和专业知识的基础上，通过“合理的分子设计”战略，进一步推动这些新材料的技术开发。在实验方面，这项研究将首先进行先进的有机合成，以生产具有明确分子结构、可控制的电子和氧化还原性质以及对外部刺激的可编程响应的功能材料。利用各种现代合成方法，我们将制备具有氧化还原活性的四硫富瓦烯(TTF)衍生物、PI共轭聚合物(CP)和官能化多芳烃(PAHs)。这些化合物将作为功能构建块来生成具有微/介观有序性、增强的光电子性能和可控的超分子行为的纳米材料或器件。将通过最先进的表征方法以及理论建模(例如从头算和密度泛函理论计算)系统地研究将要开发的新材料的性质，以便更深入地了解基本的结构-性质关系。总体而言，拟议的研究不仅将为基础科学提供变革性的知识，还将为有机半导体、选择性吸附材料、高效化学/生物传感器和其他相关领域的应用提供创新的概念和方法。该计划本质上是多学科的，将巩固与其他研究人员在国家和国际层面的广泛合作。在HQP培训方面，这一建议的实施将为培养众多本科生和研究生创造一个坚实的平台，使他们能够在加拿大高科技劳动力队伍中担任高要求的角色。

The rapid development of organic pi-conjugated materials has led to great advancement in cutting-edge technologies, such as energy storage and conversion, active displays, chemical and biological sensing, as well as nanoscale electronic and photonic devices. The advantages of organic materials lie in their easily tailored properties through chemical modifications and the low costs for material processing and device fabrication. In our recent research supported by NSERC Discovery Grant, significant breakthroughs have been made in the design and synthesis of a variety of redox-active conjugated molecules and relevant macromolecuar systems. These materials have thus offered us versatile molecular “building blocks” to prepare novel nanoscale materials and to assemble advanced molecular devices. In this proposal, we aim to further the technological development of these new materials through a “rational molecular design” strategy, based upon our established knowledge and expertise. Experimentally, the research will first embark on advanced organic synthesis to produce functional materials with well-defined molecular structures, controllable electronic and redox properties, and programmable responsiveness to external stimuli. Using various modern synthetic methodologies, we will prepare redox-active tetrathiafulvalene (TTF) derivatives, pi-conjugated polymers (CPs), and functionalized polyaromatic hydrocarbons (PAHs). These compounds will serve as functional building blocks to generate nanoscale materials or devices featuring micro/mesoscopic ordering, enhanced optoelectronic performances, and controllable supramolecular behavior. The properties of the new materials to be developed will be systematically investigated by state-of-the-art characterization methods, along with theoretical modeling (e.g., ab initio and density functional theory calculations) in order to gain deeper insight into the fundamental structure-property relationships. Overall the proposed research is expected to not only contribute transformative knowledge to fundamental science, but also deliver innovative concepts and methodologies for applications in organic semiconductors, selective sorption materials, efficient chemo-/biosensors, and other related fields. This program is multidisciplinary in nature and will consolidate extensive collaborations with other researchers on both national and international levels. In terms of HQP training, implementation of this proposal will create a solid platform for training numerous undergraduate and graduate students, enabling them to fill high-demand roles in the high-tech workforces in Canada.