Synthesizing Complex Conjugated Molecular Materials

刺激响应性有机化合物和电活性有机化合物分别是材料和设备制造技术发展的组成部分。尽管目前人们对这些领域感兴趣，但我们对它们的基础知识仍然存在重大差距，这继续推动着分子工程的研究。拟议的研究计划有两个流派，涉及合成小的、高度功能化的分子：一个致力于解决有机电子学中的问题，另一个致力于控制开关动力学和解决响应性分子的多态开关。对有机器件操作的更好理解导致了越来越高效的共轭聚合物(CP)和小分子/低聚物的生产，用作有机电子器件的组件。尽管我们的知识在不断增加，但有机设备的有效性仍然很低。有机电子学的进步将在很大程度上依赖于获得分子单元的能力，这些分子单元可以组合在一起，对生产高效材料所需的物理和电子特征进行编程。然而，当前的大多数CP和小分子设计依赖于令人惊讶的有限的分子构建块。拟议的研究计划侧重于设计和合成一系列高度官能化和可调的分子单元，这些单元将用于研究具有扩展的圆周率共轭的新型体系，并生产更好的有机材料用于器件应用。分子开关被广泛用于制造复杂的分子和结构。虽然已知许多双稳态开关，但其中只有少数是可合成的，足以用于所需的材料应用范围。其结果是，几乎所有调节材料结构和功能的尝试都局限于少数可用的可切换基序。这些开关大多是双稳的，在两个稳定状态之间相互转换。另一方面，多稳态开关是非常罕见的，但由于它们能够精确地访问许多分子取向，以及它们在信息存储等领域的应用，因此是理想的。拟议的研究计划侧重于开发新的和未被充分探索的反应功能。它们将与更传统的分子开关相结合，创造出具有新开关基元的多稳定分子开关。具体目标包括确定如何合成必然是复杂的分子；如何使用正交刺激来最大限度地控制分子运动；以及如何在不同状态之间进行高产率转换。最终，探索这些目标将使我们能够实现我们的长期目标，即构建具有远程可调活动的光响应传感器，并构建下一代分子机器。

Stimuli-responsive and electroactive organic compounds are integral to technological developments in materials and device manufacturing, respectively. Despite the current interest in these areas, significant gaps remain in our fundamental knowledge about them, which continue to drive research in molecular engineering. The proposed research program has two streams involving the synthesis of small, highly functionalized molecules: one dedicated to solving problems in organic electronics, and the other to controlling switching dynamics and addressing multi-state switching in responsive molecules.A better understanding of organic device operation has led to the production of increasingly efficient conjugated polymers (CPs) and small molecules/oligomers for use as components of organic electronic devices. Despite our increasing knowledge, the effectiveness of organic devices is still low. Advances in organic electronics will rely heavily on the ability to access molecular units that can be combined to program the physical and electronic features required to produce an efficient material. However, the majority of current CP and small molecule designs rely on a surprisingly limited range of molecular building blocks. The proposed research program focuses on the design and synthesis of a range of highly functionalizable and tunable molecular units that will be used to investigate novel systems with extended pi-conjugation, and to produce better organic materials for device applications. Molecular switches are used extensively to create complex molecules and architectures. While a number of bistable switches are known, only a few of these are synthetically accessible enough to be useful for the desired range of materials applications. The result is that virtually all attempts to regulate structure and function in materials are limited to a small number of available switchable motifs. Most of these switches are bistable, interconverting between two stable states. Multi-stable switches, on the other hand, are very rare, but are desirable for their ability to precisely access a number of molecular orientations, and for their applications in fields such as information storage. The proposed research plan focuses on the development of new and underexplored responsive functionalities. They will be utilized in combination with more traditional molecular switches to create multi-stable molecular switches with novel switching motifs. Specific objectives include determining how to synthesize what are necessarily complex molecules; how to use orthogonal stimuli to maximize control over molecular movements; and how to transform between different states in high yields. Ultimately, exploring these objectives will allow us to fulfill our long-term goals of building light responsive sensors with remote tunable activity, and constructing the next generation of molecular machines.