15 research outputs found
Theory of Melting and the Optical Properties of Gold/DNA Nanocomposites
We describe a simple model for the melting and optical properties of a
DNA/gold nanoparticle aggregate. The optical properties at fixed wavelength
change dramatically at the melting transition, which is found to be higher and
narrower in temperature for larger particles, and much sharper than that of an
isolated DNA link. All these features are in agreement with available
experiments. The aggregate is modeled as a cluster of gold nanoparticles on a
periodic lattice connected by DNA bonds, and the extinction coefficient is
computed using the discrete dipole approximation. Melting takes place as an
increasing number of these bonds break with increasing temperature. The melting
temperature corresponds approximately to the bond percolation threshold.Comment: 5 pages, 4 figure. To be published in Phys. Rev.
Structure Formation, Melting, and the Optical Properties of Gold/DNA Nanocomposites: Effects of Relaxation Time
We present a model for structure formation, melting, and optical properties
of gold/DNA nanocomposites. These composites consist of a collection of gold
nanoparticles (of radius 50 nm or less) which are bound together by links made
up of DNA strands. In our structural model, the nanocomposite forms from a
series of Monte Carlo steps, each involving reaction-limited cluster-cluster
aggregation (RLCA) followed by dehybridization of the DNA links. These links
form with a probability which depends on temperature and particle
radius . The final structure depends on the number of monomers (i. e. gold
nanoparticles) , , and the relaxation time. At low temperature, the
model results in an RLCA cluster. But after a long enough relaxation time, the
nanocomposite reduces to a compact, non-fractal cluster. We calculate the
optical properties of the resulting aggregates using the Discrete Dipole
Approximation. Despite the restructuring, the melting transition (as seen in
the extinction coefficient at wavelength 520 nm) remains sharp, and the melting
temperature increases with increasing as found in our previous
percolation model. However, restructuring increases the corresponding link
fraction at melting to a value well above the percolation threshold. Our
calculated extinction cross section agrees qualitatively with experiments on
gold/DNA composites. It also shows a characteristic ``rebound effect,''
resulting from incomplete relaxation, which has also been seen in some
experiments. We discuss briefly how our results relate to a possible sol-gel
transition in these aggregates.Comment: 12 pages, 10 figure