Title

Single wall carbon nanotubes: Separation and applications to biosensors

Date of Completion

January 2007

Keywords

Chemistry, Analytical|Chemistry, Physical|Engineering, Materials Science

Degree

Ph.D.

Abstract

Single wall carbon nanotubes uniquely exhibit one-dimensional quantum confined properties by being either semiconducting (sem-) or metallic (met-) depending on their atomic arrangements. The stochastic nature of SWNT growth renders met-:sem- ratio being 1:2 and diameter range being distributed in 0.4-2nm with a close-packed bundle configuration. For many high-performance devices using SWNTs, acquiring well-separated and/or isolated single-diameter, metallicity and/or chirality nanotubes is greatly in demand. Recently, the bulk separation and/or enrichment of single wall carbon nanotubes (SWNTs) according to type (or otherwise termed "metallicity") and diameter (dt) has become possible. This thesis presents a route to probe mechanisms in diameter and metallicity dependent separation of SWNTs. A systematic analysis tool, that enables the quantitative examination of resonance Raman spectra, is established from nanotube samples that have been separated according to metallicity and d t via an octadecylamine mediated protocol. This protocol uses the relative changes in the integrated intensities of the radial-breathing mode region for the quantitative evaluation. By further establishing the physicochemical properties of charge-stabilized SWNT dispersions in polar aprotic media (i.e. N,N-dimethylformide) a more detailed description of the underlying separation mechanism is given. Here, I use resonance Raman spectroscopy (RRS) as a tool to probe SWNT redox chemistry. The Gibbs free energy, modeled by calculating the charge-loss from the (n,m)-dependent integrated density of states across the corresponding jump in the redox potential, is utilized to support the separation mechanism. Additionally, the evaluation of SWNT forest platforms for amperometric protein immunoassays is presented. Horseradish peroxidase is used as the label and the sensing signals are acquired from electrochemical reduction of hydrogen peroxide. Specific studies on human serum albumin and prostate specific antigen detection are explained. Signal amplification strategies are introduced by using redox mediator, enzyme, and enzyme-decorated carbon nanotubes.^