Stepwise surface encoding for high-throughput assembly of nanoclusters

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Abstract
Solution-based syntheses of nanoscale clusters using biomolecules as links between nanoparticles are frequently inefficient and normally produce many different multimers or isomers of clusters. Dimer nanoclusters and Janus nanoclusters have now been designed and produced in high yields using nanoparticles grafted with single-stranded DNA. Self-assembly offers a promising method to organize functional nanoscale objects into two-dimensional (2D) and 3D superstructures for exploiting their collective effects1,2,3. On the other hand, many unique phenomena emerge after arranging a few nanoscale objects into clusters, the so-called artificial molecules4,5,6,7,8,9,10. The strategy of using biomolecular linkers between nanoparticles has proven especially useful for construction of such nanoclusters4,5,6,11,12,13,14,15,16. However, conventional solution-based reactions typically yield a broad population of multimers or isomers of clusters; furthermore, the efficiency of fabrication is often limited4,5,6,11,12,13,14,15,16. Here, we describe a novel high-throughput method for designing and fabricating clusters using DNA-encoded nanoparticles assembled on a solid support in a stepwise manner. This method efficiently imparts particles with anisotropy during their assembly and disassembly at a surface, generating remarkably high yields of well-defined dimer clusters and Janus (two-faced) nanoparticles. The method is scalable and modular, assuring large quantities of clusters of designated sizes and compositions.

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