Publications
Electrochemical Detection of Single Molecules in Nanogap Electrode Fluidic Devices
The purpose of this project was to gain a fundamental understanding of molecular diffusion in nanogap electrodes and the diffusive behavior of single molecules undergoing electron transfer. Electrochemical methods for single molecule detection have remained elusive due to the vanishingly small currents involved in single molecule electron transfer. Electrochemical detection of single molecules undergoing redox cycling would enable detection of single enzymes, proteins, and DNA strands resulting in new and improved ultrasensitive sensing devices impacting Detection At The Limits research challenge (DATL), supporting needs in DHS and DoD. We attempted to integrate orthogonal validation techniques, Total Internal Reflection Fluorescence Microscopy (TIRF), and molecular simulation to clarify (1) the mechanism leading to current build up due to redox cycling and (2) diffusion and adsorption of single molecules undergoing redox reactions. While creation of nanogap electrodes with transparent windows was ultimately successful in this project (along with TIRF demonstration of single molecule imaging), time and methods constraints did not allow final electrochemical measurements to be coupled for simultaneous interrogation.