Coupled Transport and Reactions in Low-Dimensional Nanofluidic Structures for Enhanced Chemical Measurements

该项目由化学学部化学测量和成像项目资助，Paul Bohn教授和他在圣母大学的研究小组将寻求利用在尺寸小于100纳米的纳米结构中进行化学反应时出现的新物理现象。特别是，在控制反应物的输送和产物的提取的条件下，将化学反应限制在这些小体积内，预计将大大提高分子传感的灵敏度和化学处理的效率。Bohn小组将使用各种沉积和光刻技术制造纳米级反应器容器。反应器结构将允许对其中包含的化学系统进行光学和电学测量。该项目探索了一类新的纳米结构，其中传输与零维、零维和一维、一维结构中的反应性和测量密切相关。具体来说，这些实验通过解决两个广泛的目标，使化学测量与多个顺序反应/操作的耦合成为可能：(1)在一维纳米尺度结构中，电动流动与法拉第电化学的高效耦合；(2)发展高灵敏度（单分子）光谱电化学来表征0-D纳米结构中的单电子转移事件。人们正在开发新的纳米结构，将电动流动与非均相电子转移结合起来，并获得高灵敏度氧化还原循环的新途径，以扩大电化学测量。此外，纳米结构正在被开发，以耦合电子转移事件和光发射的调制，从而提供了在单个分子中的单个电子转移事件。该项目与一项新型化学测量科学研究生课程的开发相结合，该课程被称为巴黎圣母院分析科学与工程（ASEND），涵盖传统工程和自然科学部门的学科。

This project funded by the Chemical Measurement and Imaging Program of the Division of Chemistry, Professor Paul Bohn and his research group at the University of Notre Dame will seek to exploit new physical phenomena that emerge when chemistry is carried out in nanostructures whose dimensions are less than 100 nanometers. In particular, confining chemical reactions to these small volumes under conditions where the delivery of reactants and the extraction of products is controlled, is expected to yield significant improvements in the sensitivity of molecular sensing and the efficiency of chemical processing. The Bohn group will fabricate nanometer scale reactor vessels using various deposition and lithographic techniques. The reactor structures will allow for both optical and electrical measurements to be made on the chemical systems contained within them. This project explores a new class of nanostructures in which transport is intimately coupled with reactivity and measurement in zero-dimensional, 0-D, and one-dimensional, 1-D, architectures. Specifically, the experiments enable the coupling of chemical measurements with multiple sequential reactions/manipulations by addressing two broad objectives: (1) the high efficiency coupling of electrokinetic flow to Faradaic electrochemistry in 1-D nanoscale architectures; and (2) the development of high sensitivity (single molecule) spectroelectrochemistry to characterize single electron transfer events in 0-D nanostructures. New nanoscale architectures are being developed that couple electrokinetic flow to heterogeneous electron transfer and access new routes to high sensitivity redox cycling to amplify electrochemical measurements. Additionally, nanostructures are being developed to couple electron transfer events to modulation of light emission, thereby providing access to single electron transfer events in single molecules. The project is coupled to the development of a new type of graduate program in chemical measurement sciences, termed Analytical Sciences and Engineering at Notre Dame (ASEND), that spans disciplines across traditional engineering and natural sciences departments.