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Nanoparticle Superlattices through Template-Encoded DNA Dendrimers

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posted on 11.10.2021, 16:35 authored by Ho Fung Cheng, Max E. Distler, Byeongdu Lee, Wenjie Zhou, Steven Weigand, Chad A. Mirkin
The chemical interactions that lead to the emergence of hierarchical structures are often highly complex and difficult to program. Herein, the synthesis of a series of superlattices based upon 30 different structurally reconfigurable DNA dendrimers is reported, each of which presents a well-defined number of single-stranded oligonucleotides (i.e., sticky ends) on its surface. Such building blocks assemble with complementary DNA-functionalized gold nanoparticles (AuNPs) to yield five distinct crystal structures, depending upon choice of dendrimer and defined by phase symmetry. These DNA dendrimers can associate to form micelle-dendrimers, whereby the extent of association can be modulated based upon surfactant concentration and dendrimer length to produce a low-symmetry Ti5Ga4-type phase that has yet to be reported in the field of colloidal crystal engineering. Taken together, colloidal crystals that feature three different types of particle bonding interactionstemplate–dendron, dendrimer–dendrimer, and DNA–modified AuNP-dendrimerare reported, illustrating how sequence-defined recognition and dynamic association can be combined to yield complex hierarchical materials.