DNA functionalized gold nanoparticles (NPs) exhibit unique properties that are highly useful in chemistry, materials science, and medicine. We explain key properties of these NPs and compare them to linear nucleic acids. In particular, we describe the design of superlattices by using the high selectivity of DNA recognition “imprinted” in the functionalized NPs. We use molecular dynamics simulations to analyze dynamic aspects of the assembly process and to identify the essential ingredients for a successful assembly of NP superlattices through DNA hybridization.

A scale-accurate coarse-grained model faithfully captures the relevant contributions to the kinetics of the DNA hybridization process and is able to recover all experimentally reported to date binary superlattices. With multi-scale modeling we show assembly into superlattices with a specific crystal habit, providing a nanoscale analogue to the crystallization behavior exhibited by conventional atomic crystals.