Self-organized patterning through the dynamic segregation of DNA and silica nanoparticles.

Exotic pattern formation as a result of drying of an aqueous solution containing DNA and silica nanoparticles is reported. The pattern due to segregation was found to critically depend on the relative ratio of nanoparticles and DNA, as revealed by polarization microscopy, scanning electron microscopy, and fluorescence microscopy. The blurred radial pattern that is usually observed in the drying of a colloidal solution was shown to be vividly sharpened in the presence of DNA. Uniquely curved, crescent-shaped micrometer-scale domains are generated in regions that are rich in nanoparticles. The characteristic segregated patterns observed in the present study are interpreted in terms of a large aspect ratio between the persistence length (∼ 50 nm) and the diameter (∼ 2 nm) of double-stranded DNA, and the relatively small silica nanoparticles (radius: 5 nm).

Colloidal structure and stability of DNA/polycations polyplexes investigated by small angle scattering.

Polyplexes of short DNA-fragments (300 b.p., 100 nm) with tailor-made amine-based polycations of different architectures (linear and hyperbranched) were investigated in buffer solution as a function of the mixing ratio with DNA. The resulting dispersed polyplexes were characterized using small-angle neutron and X-ray scattering (SANS, SAXS) as well as cryo-TEM with respect to their mesoscopic structure and their colloidal stability. The linear polyimines form rather compact structures that have a high tendency for precipitation. In contrast, the hyperbranched polycation with enzymatic-labile pentaethylenehexamine arms (PEHA) yields polyplexes colloidally stable for months. Here the polycation coating of DNA results in a homogeneous dispersion based on a fractal network with low structural organization at low polycation amount. With increasing polycation, bundles of tens of aligned DNA rods appear that are interconnected in a fractal network with a typical correlation distance on the order of 100 nm, the average length of the DNA used. With higher organization comes a decrease in stability. The 3D network built by these beams can still exhibit some stability as long as the material concentration is large enough, but the structure collapses upon dilution. SAXS shows that the complexation does not affect the local DNA structure. Interestingly, the structural findings on the DNA polyplexes apparently correlate with the transfection efficiency of corresponding siRNA complexes. In general, these finding not only show systematic trends for the colloid stability, but may allow for rational approaches to design effective transfection carriers.