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

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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.