Person:

Albertorio, Fernando

We describe experiments and modeling results that reveal and explain the distribution of times that identical double-stranded DNA (dsDNA) molecules take to pass through a voltage-biased solid-state nanopore. We show that the observed spread in this distribution is caused by viscous-drag-induced velocity fluctuations that are correlated with the initial conformation of nanopore-captured molecules. This contribution exceeds that due to diffusional Brownian motion during the passage. Nevertheless, and somewhat counterintuitively, the diffusional Brownian motion determines the fundamental limitations of rapid DNA strand sequencing with a nanopore. We model both diffusional and conformational fluctuations in a Langevin description. It accounts well for passage time variations for DNA molecules of different lengths, and predicts conditions required for low-error-rate nanopore-strand DNA sequencing with nanopores.

We quantify the base dependent interactions between single stranded DNA and single walled carbon nanotubes (SWNTs) in solution. DNA/SWNT hybrids hold the promise of applications ranging from nanoscale electronics and assembly of nanotube based materials, to drug delivery and DNA sequencing. These applications require control over the hybrid assembly and disassembly. Our analytical assay reveals the order of nucleobase binding strengths with SWNTs as G>C>A>T. Furthermore, time dependent fixed temperature experiments that probe the kinetics of the dissociation process provide values for the equilibrium constants and dissociation enthalpies that underlie the microscopic interactions. Quantifying the base dependency of hybrid stability shows how insight into the energetics of the component interactions facilitates control over hybrid assembly and disassembly.

We report experimental escape time distributions of double-stranded DNA molecules initially threaded halfway through a thin solid-state nanopore. We find a universal behavior of the escape time distributions consistent with a one-dimensional first passage formulation notwithstanding the geometry of the experiment and the potential role of complex molecule-liquid-pore interactions. Diffusion constants that depend on the molecule length and pore size are determined. Also discussed are the practical implications of long time diffusive molecule trapping in the nanopore.