From small molecules to complext supramolecular architectures: underlying physical concepts and phenomena

今天，人们普遍认为，自组装和自组织过程是将化学反应的简约性与生命动态系统的复杂性和出现联系起来的主线。解开这些过程不仅可以更好地理解自然界产生具有预定大小、拓扑、立体化学、层次和形状的超分子结构的方法，而且还可以在工程、科学和医学中应用技术。对物质有组织状态的概念化不仅要求对化学反应的深入了解，还需要对嵌入在分子中的以电荷、偶极和其他功能元素的形式嵌入的化学信息的理解，这些信息是将化学信息转化为功能超结构所必需的。为实现这一目标，我们建议调查四个相互关联的项目。第一种是通过设计和化学合成有机小分子来控制自组装玫瑰花结纳米管(RNTS)的内径。第二个主题是利用RNTS制备具有重要催化性能的单分散金属纳米颗粒。第三个主题涉及通过一种新的自组装机制来研究由RNTS衍生的一类新的纳米管。最后，由于RNTS的自我催化和自我复制的特性，我们建议开发一种体外进化策略来选择具有预定义属性的RNTS。这一计划为我的团队和部门建立了一个真正的多学科环境。除了探索有机化学的新方面，参与这个项目的学生还学习超分子工程的艺术。随后的物理有机研究，以表征所产生的组件，诱使他们学习和实践最先进的光谱和成像技术。

It is accepted today that self-assembly and self-organization processes are the thread that connects the reductionism of chemical reactions to the complexity and emergence of a living dynamic system. Unraveling these processes may lead not only to a better understanding of nature's approach to generating supramolecular architectures with predefined size, topology, stereochemistry, hierarchy, and shape, but also to technological applications in engineering, science, and medicine.The conceptualization of an organized state of matter requires in-debt understanding not only of chemical reactivity but also of the chemical information embedded in the molecules in the form of charges, dipoles, and other functional elements necessary to translate chemical information into functional superstructures. Towards this goal we propose to investigate four inter-related projects. The first deals with controlling the inner diameter of self-assembled rosette nanotubes (RNTs) through the design and chemical synthesis of small organic molecules. The second topic consists in utilizing the RNTs to generate monodisperse metallic nanoparticles endowed with important catalytic properties. The third topic deals with the study of a new family of nanotubules derived from the RNTs through a novel self-assembly mechanism. Finally, because of the auto-catalytic and self-replicating properties of the RNTs, we propose to develop an in-vitro evolution strategy for the selection of RNTs with predefined properties.This program has contributed to a truly multidisciplinary environment within my group and department. In addition to exploring new aspects of organic chemistry, the students involved in this program, learn the art of supramolecular engineering. Subsequent physical organic studies to characterize the resulting assemblies entice them to learn and practice state-of-the-art spectroscopic and imaging techniques.