DNA Programmable Self-Assembly of Planar, Thin-Layered Chiral Nanoparticle Superstructures with Complex Two-Dimensional Patterns

Abstract

Planar, thin-layered chiral plasmonic superstructures with complex two-dimensional (2D) patterns, namely, double-layered binary stars (bi-stars) and pinwheels, were realized through DNA programmable 2D supramolecular self-assembly of gold nanorods (AuNRs). The chirality of the chiral superstructures was defined by a finite number of AuNR pairs as enantiomeric motifs, and their sizes (∼240 nm) were precisely defined by the underlying DNA template. These planar, thin-layered chiral nanoparticle superstructures exhibited prescribed shapes and sizes at the dried state on the substrate surface and are characteristic of giant anisotropy of chiroptical responses, with enhanced g-factors from the axial incident excitation as compared to the in-plane excitation. This work will inspire possibilities for the construction of 2D chiral materials, for example, chiral metasurfaces, for the on-chip manipulation of chiral light-matter interactions via programmable self-assembly of nanoparticles.

DNA-Assembled Chiral Satellite-Core Nanoparticle Superstructures: Two-State Chiral Interactions from Dynamic and Static Conformations

“…We employed our previously published fabrication method for planar chiral plasmonic nanostructures. 21 As shown in Figure 2a, we first extended DNA single strands at specific positions on a triangular DNA origami, 40 which could capture and precisely locate AuNRs decorated with the complementary DNA strands at the desired positions. These monomers were then patterned into S-type or D-type spirals via the 2D connection of the DNA triangle sheets into a hexagonal shape.…”

“…Understanding the chiral light–matter interactions of chiral substances is of paramount importance in photonics, − catalysis, − biology, − etc. − By mimicking naturally existing chiral substances, chiral metasurfaces, sterometamaterials, colloidal groupings of nanoparticles were largely fabricated via top-down − or bottom-up − approaches. In contrast to these heavily developed 2D and 3D products, the well-defined integration of planar chiral colloidal superstructures with nanocomponents that vary in size, shape, or composition in the third dimension is scarce so far.…”

DNA-mediated dynamic plasmonic nanostructures: assembly, actuation, optical properties, and biological applications

“…24,30,137,166 By exploiting the programmability and scalability of DNA selfassembly, colloidal nanoparticles have been assembled into various LH or RH plasmonic structures. 30,[167][168][169][170][171] Organizing anisotropic nanoparticles such as AuNRs into asymmetric nanoassemblies, enhanced chirality can be generated compared to isotropic NP nanostructures due to the high dissymmetry factor and strong plasmon antenna effect. 169,172 As an example of utilizing AuNR dimers as dynamic plasmonic structures with chiroplasmonic activities, Liu's group demonstrated an active plasmonic nanoassembly, in which the AuNRs can perform directional, progressive and reverse nanoscale rows on 2D or 3D DNA origami after adding corresponding blocking and removal strands (Fig.…”

A Review on Self-Assembled Colloidal Nanoparticle Clusters, Patterns and Films: Emerging Synthesis Techniques and Applications

“…Still, for certain niche applications, DNA-directed assembly can still be promising in view of the state-of-the-art. Reprinted with permission [55] © 2021, American Chemical Society. (b) Nano-gearsets by the selfassembly of two Au nanoparticles by cross-linking in between two concentric DNA origami nanorings.…”

“…Figure 4. (a) Self-assembly of Au nanorods into deterministic patterns on DNA hexamer origamis.Reprinted with permission[55] © 2021, American Chemical Society. (b) Nano-gearsets by the selfassembly of two Au nanoparticles by cross-linking in between two concentric DNA origami nanorings [52].…”