Sensing Molecular Adsorption Through Interfacial Electron Scattering in Atom -Scale Junctions

The goal of this work was to fabricate Au atom-scale junctions as the basis for robust, regenerable, nanostructured sensors to use with mass-limited samples for improved protection of health and safety. Atom-scale junctions were formed between two Au thin film electrodes. The inter-electrode gap was lithographically defined, and a microfluidic channel was aligned over the inter-electrode gap. The inter-electrode gap was reduced with electrodeposition, which was terminated at an atom-scale junction by setting a comparator to trigger a relay at a current corresponding to a junction conductance comparable to the conductance quantum. Based on conductance measurements and estimates from SEM images, atom-scale junctions were successfully formed. Lewis bases were introduced to atom-scale junctions, and the resulting alternating current impedance change was measured. For example, the interfacial scattering from chemisorption of 10 mM hexadecanethiol (HDT) on a 2.6 G0 atom-scale junction caused a normalized impedance change of 71% +/- 1%, with a noise level consistent with a population fluctuation of only 1 HDT molecule. To regenerate the device in situ, the junction was broken with a potential sweep and reformed with comparator-terminated electrodeposition. The atom-scale junction capability to measure small numbers of adsorption/desorption events makes a powerful case for pushing the limits of sensitivity for electrical measurements of single molecule events.

Name thesis:degree_name

Ph.D.

Level thesis:degree_level

Dissertation

Discipline thesis:degree_discipline

Chemistry

Grantor

University of Illinois at Urbana-Champaign

Year dc:date

2015

Author dc:creator

• Castle, Patrick James

Contributors dc:contributor

• Bohn, Paul W.

• Chemistry, Analytical

Language dc:language

eng

Identifier

(MiAaPQ)AAI3198938

OAI identifier oai:identifier

oai:www.ideals.illinois.edu:2142/84182