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

该项目由化学系化学测量和成像计划资助，圣母大学的保罗·博恩教授和他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时出现的新物理现象。特别是，在反应物的输送和产物的提取受到控制的条件下，将化学反应限制在这些小体积内，有望显著提高分子传感的灵敏度和化学处理的效率。博恩集团将使用各种沉积和光刻技术制造纳米级的反应堆容器。反应堆结构将允许对其中包含的化学系统进行光学和电学测量。这个项目探索了一类新的纳米结构，在这种结构中，传输与零维、0维和一维、一维结构中的反应和测量密切相关。具体地说，这些实验能够将化学测量与多个顺序反应/操作相结合，以解决两个广泛的目标：(1)一维纳米结构中电动流动与法拉第电化学的高效耦合；(2)高灵敏度(单分子)光谱电化学的发展，以表征0-D纳米结构中的单电子转移事件。新的纳米尺度结构正在被开发，它将电动流动耦合到非均相电子转移，并获得高灵敏度氧化还原循环的新途径，以放大电化学测量。此外，正在开发纳米结构以将电子转移事件耦合到光发射的调制，从而提供对单分子中的单电子转移事件的访问。该项目与开发一种新型的化学测量科学研究生项目相结合，该项目被称为圣母大学分析科学和工程(ASEND)，该项目跨越传统工程学和自然科学系的学科。

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.