38 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
Density functional study of Au (n=2-20) clusters: lowest-energy structures and electronic properties
We have investigated the lowest-energy structures and electronic properties
of the Au(n=2-20) clusters based on density functional theory (DFT) with
local density approximation. The small Au clusters adopt planar structures
up to n=6. Tabular cage structures are preferred in the range of n=10-14 and a
structural transition from tabular cage-like structure to compact
near-spherical structure is found around n=15. The most stable configurations
obtained for Au and Au clusters are amorphous instead of
icosahedral or fcc-like, while the electronic density of states sensitively
depend on the cluster geometry. Dramatic odd-even alternative behaviors are
obtained in the relative stability, HOMO-LUMO gaps and ionization potentials of
gold clusters. The size evolution of electronic properties is discussed and the
theoretical ionization potentials of Au clusters compare well with
experiments.Comment: 6 pages, 7 figure
Computer-aided design of nano-filter construction using DNA self-assembly
Computer-aided design plays a fundamental role in both top-down and bottom-up nano-system fabrication. This paper presents a bottom-up nano-filter patterning process based on DNA self-assembly. In this study we designed a new method to construct fully designed nano-filters with the pores between 5 nm and 9 nm in diameter. Our calculations illustrated that by constructing such a nano-filter we would be able to separate many molecules
The sequence-specific cellular uptake of spherical nucleic acid nanoparticle conjugates
The sequence-dependent cellular uptake of spherical nucleic acid nanoparticle conjugates (SNAs) is investigated. This process occurs by interaction with class A scavenger receptors (SR-A) and caveolae-mediated endocytosis. It is known that linear poly(guanine) (poly G) is a natural ligand for SR-A, and it has been proposed that interaction of poly G with SR-A is dependent on the formation of G-quadruplexes. Since G-rich oligonucleotides are known to interact strongly with SR-A, it is hypothesized that SNAs with higher G contents would be able to enter cells in larger amounts than SNAs composed of other nucleotides, and as such, cellular internalization of SNAs is measured as a function of constituent oligonucleotide sequence. Indeed, SNAs with enriched G content show the highest cellular uptake. Using this hypothesis, a small molecule (camptothecin) is chemically conjugated with SNAs to create drug-SNA conjugates and it is observed that poly G SNAs deliver the most camptothecin to cells and have the highest cytotoxicity in cancer cells. Our data elucidate important design considerations for enhancing the intracellular delivery of spherical nucleic acids
Multivesicular assemblies as real-world testbeds for embryogenic evolutionary systems
Embryogenic evolution emulates in silico cell-like entities to get more powerful methods for complex evolutionary tasks. As simulations have to abstract from the biological model, implicit information hidden in its physics is lost. Here, we propose to use cell-like entities as a real-world in vitro testbed. In analogy to evolutionary robotics, where solutions evolved in simulations may be tested in real-world on macroscale, the proposed vesicular testbed would do the same for the embryogenic evolutionary tasks on mesoscale. As a first step towards a vesicular testbed emulating growth, cell division, and cell differentiation, we present a modified vesicle production method, providing custom-tailored chemical cargo, and present a novel self-assembly procedure to provide vesicle aggregates of programmable composition
Towards tailored communication networks in assemblies of artificial cells
Living Technology is researching novel IT making strong use of programmable chemical systems. These chemical systems shall finally converge to artificial cells resulting in evolvable complex information systems. We focus on procedural manageability and information processing capabilities of such information systems. Here, we present a novel resource-saving formation, processing, and examination procedure to generate and handle single compartments representing preliminary stages of artificial cells. Its potential is exemplified by testing the influence of different glycerophospholipids on the stability of the compartments. We discuss how the procedure could be used both in evolutionary optimization of self-assembling amphiphilic systems and in engineering tailored communication networks enabling life-like information processing in multicompartment aggregates of programmable composition and spatial configuration