Biopolymer-mediated analyte detection via photoluminescence modulation of single-walled carbon nanotubes

Single-walled carbon nanotubes (SWNT) have unique photo-physical properties which, through the work in this dissertation, are investigated and harnessed to produce optical sensors with unique capabilities. Early studies of the modulation of SWNT optical properties???both photoluminescence and resonance Raman scattering???demonstrate their tunable nature. Solution dispersed SWNT are sorted by length and the photoluminescence quantum yield is shown to increase nonlinearly with length, suggesting that SWNT ends quench the exciton. The change in Raman scattering cross section and resonant window is mapped as a function of SWNT aggregation, as well as sonochemical effects on photoluminescence. Nanotube photoluminescence and scattering are then detected, via imaging and spectrometry, from within live murine macrophage cells, and shown to be extremely resilient, demonstrating the potential of nanotube-based molecular probes and biosensors. The work culminates in several major findings in optical sensing. We show that a nanotube-ds(GT)15 DNA complex can detect genotoxic analytes by solvatochromism, and measure this from within live cells and tissues in real-time. We find that such optical signals can be multiplexed, resulting in analyte fingerprinting, and a bioanalyte can be detected at the single-molecule level stochastic operation of such sensors. These concepts are employed to detect, identify, and measure bioanalytes, such as reactive oxygen species, as well as explosives, such as TNT and RDX, with single-molecule sensitivity