Environmentally Responsive Supramolecular Constructs and Models for Chemical Communication

得克萨斯大学的乔纳森·L·塞斯勒获得了大分子、超分子和纳米化学项目的这一奖项，他正在进行旨在创造能够进行化学通信的新系统的研究。生命系统通过纯粹的化学手段进行交流的能力是独一无二的，如果我们能够模仿这种行为，一系列广泛的新技术可能成为可能。生命系统中的化学交流可以发生在短距离内，这就是脑细胞通过释放和捕获神经递质分子进行交流时发生的情况。或者，这种交流可以发生在很远的距离上，比如当昆虫，甚至一些哺乳动物通过释放信息素进行交流时。虽然这些过程在生物界是众所周知的，但还不可能在人工系统中复制这种类型的交流。在这项工作中，研究人员正在做这项工作，使用他们开发的复杂的实验室方法，以受控的方式完成分子设计和构建。这项工作可能会影响可能的新信息系统的开发。由于这项基础性研究，人工智能和无线通信的新方法可能成为可能。这项工作正在通过培训下一代科学家在尖端实验室技术方面产生进一步广泛的影响，这将使参与这项研究的学生为在广泛的技术挑战领域的工作做好准备。本项目侧重于使用电子丰富和电子贫乏的受体，其特征可以通过改变pH、氧化还原电位和底物结合来调节。特别强调四硫富瓦烯、杯吡咯受体和各种缺电子底物，包括富勒烯衍生物。例如，由阴离子与杯吡咯结合而产生的构象转换被用来引起平衡的变化。这些扰动反过来又会释放出小的化学物质，这些化学物质可以触发其他受体系统的调节，比如那些由低聚吡咯构建的受体系统。包括标准光谱、光化学、基于颜色的反应和固态结晶学在内的一系列技术正被用来表征这个项目中涉及的体系以及由于平衡行为的诱导扰动而引起的特征变化。

With this award from the Macromolecular, Supramolecular and Nanochemistry Program, Jonathan L. Sessler of The University of Texas is carrying out research aimed at creating new systems that can communicate chemically. Living systems are unique in their ability to communicate by purely chemical means and a wide array of new technologies could become possible if we were able to mimic this behavior. Chemical communication in living systems can occur over short distances, which is what happens when brain cells communicate by the release and capture of neurotransmitter molecules. Or, the communication can take place over large distances, such as when insects, or even some mammals, communicate by releasing pheromones. Although these processes are well known in the world of biology, it has not yet been possible to reproduce this type of communication in an artificial system. In this work, the investigators are doing just that, using sophisticated laboratory methods they have developed to accomplish molecular design and construction in a controlled fashion. This work will likely impact the development of possible new information systems. New approaches to artificial intelligence and wireless communication may become possible as a result of this fundamental research. The work is having a further broad impact through the training of the next generation of scientists in cutting-edge laboratory techniques that will prepare the students involved in this research for work in a wide variety of technologically challenging areas.This project focuses on the use of electron rich and electron poor receptors whose features can be modulated via changes in pH, redox potential, and substrate binding. Particular emphasis is being placed on tetrathiafulvalene calixpyrrole receptors and various electron deficient substrates, including fullerene derivatives. Conformational switching, as engendered by anion binding to a calixpyrrole, for instance, is used to induce changes in equilibrium. These perturbations, in turn, serve to release small chemical species that can act as triggers for the modulation of other receptor systems, such as those built from oligopyrroles. A range of techniques, including standard spectroscopies, photochemistry, color-based reactions, and solid state crystallography is being used to characterize the systems involved in this project and the changes in their features due to induced perturbations in equilibrium behavior.