Abstract
DNA-functionalized Au nanoparticles (AuNPs) have been intensively exploited as programmable atom equivalents (PAEs) for the self-assembly of molecule-like structures. However, it remains challenging to build hierarchical PAE assemblies via discrete DNA bonds at different levels. Here, we report a strategy to program DNA bond length and bond energy on PAEs using DNA encoders carrying consecutive adenines (polyA). On AuNPs, we built three types of DNA motifs with different topologic configurations, which can form bonds for PAE self-assembly. By small-angle X-ray scattering (SAXS) analysis, we found that the bond length and flexibility between the coupled PAEs can be tuned by programming the bond structure. We also found that these bonds show different bond energies and thus differ, depending on their topologic configuration, leading to different PAE assembly efficiencies. We demonstrated that the bonds at different levels can be arranged in different directions on one nanoparticle, leading to asymmetric PAEs that allow ionic strength-controlled hierarchical assembly of multiparticle structures. This programmable bonding system may provide a new route for building complex plasmonic superstructures.
Highlights
In nature, atoms and molecules react with each other via interactions at different levels, which allow bottom-up self-assembly of complex hierarchical biological structures[1,2,3,4,5,6,7]
According to previous studies[35,36,37], the polyA domain has a high affinity for Au, and can be absorbed on the Au nanoparticles (AuNPs) surface
Encoder III is a partially double-stranded structure with two polyA domains, a 20-bp ds stem and a 20-nt sticky end for bonding (Fig. 1a). We propose that these different topological configurations can lead to different bond lengths and bond energies
Summary
Atoms and molecules react with each other via interactions at different levels, which allow bottom-up self-assembly of complex hierarchical biological structures[1,2,3,4,5,6,7]. Au nanoparticles (AuNPs) decorated with DNAs have been intensively explored as programmable atom equivalents (PAEs) for the self-assembly of crystal-like[12,13,14,15,16,17,18,19,20,21,22,23] or molecule-like structures[24,25,26,27,28,29,30,31,32,33,34]. In our previous study[35,36,37], we developed a series of single-stranded
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