DNA-Guided Plasmonic Helix with Switchable Chirality

Abstract

The ability to dynamically tune the self-assembled structures of nanoparticles is of significant interest in the fields of chemistry and material studies. However, it continues to be challenging to dynamically tune the chiral superstructures of nanoparticles and actively switch the chiral optical properties thereof. Here, we dynamically controlled a gold nanorod 3D chiral plasmonic superstructure (a stair helix with a pinwheel end view) templated by a DNA origami supramolecular polymer, using DNA-toehold-mediated conformational change in the DNA template. The gold nanorod chiral plasmonic helix was controllably reconfigured between a tightly folded state (with a small inter-rod angle) and an extended state (with a wide inter-rod angle) of the same handedness, or between two mirror-image-like structures of opposite handedness. As a result, the chiral plasmonic properties of the gold nanorod helix superstructures, in terms of the circular dichroism amplitude, peak response frequency, and signature of chirality, were actively switched upon the DNA-guided structural reconfiguration. We envision that the strategy demonstrated here will boost the advancement of reconfigurable chiral materials with increased complexity for active light control applications through rational molecular design and predictable self-assembly procedures.

Create Nanoscale Patterns with DNA Origami

“…D) DNA‐guided self‐assembly and reconfiguration of the AuNR plasmonic helix. Reproduced with permission . Copyright 2018, American Chemical Society.…”

“…The transduction of conformational change resulted in a shift in the plasmonic resonance peak (Figure C). In a more complex plasmonic superstructure, Lan et al reported a reconfigurable plasmonic helix showing switchable chirality (Figure D) . The plasmonic helix consists of many AuNRs in chiral order templated by DNA origami.…”

Dynamic Modulation of Supramolecular Chirality Driven by Factors from Internal to External Levels

“…Supramolecular co‐assemblies, based on intermolecular interactions of building blocks with diverse chemical structures and physical functions synergistically organized into supramolecular aggregates, offer a facile way to tailor supramolecular chirality with switchable stimuli responses . Achiral additives also play an important role in the dynamic modulation of chirality in co‐assemblies.…”

“…Dynamic modulation on the intermolecular level Supramolecular co-assemblies, based on intermolecular interactions of buildingb locks with diverse chemical structures and physicalf unctions synergistically organized into supramolec-ular aggregates, offer af acile way to tailor supramolecular chirality with switchable stimuli responses. [23] Achirala dditives also play an important role in the dynamic modulation of chirality in co-assemblies.I n2 016, Feng et al used phenylalanine-based enantiomersa sb uildingu nits to construct supramolecular chiral nanostructures. [24] Twoa chiral bis(pyridinyl) derivatives with different chemical structures wereu sed to regulate the chirality of the nanostructures.…”

Stress‐Induced 3D Chiral Fractal Metasurface for Enhanced and Stabilized Broadband Near‐Field Optical Chirality

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State-of-the-art fabrication methods for 3D chiral nanostructures or metasurfaces include focused ion/electron beam deposition, [40][41][42][43][44] multistep electron beam lithography, [45] direct laser writing, [21,46] glancing angle deposition, [47,48] and chemical synthesis with the assistance of chiral templates [49][50][51] or circularly polarized illumination. [52] However, these methods are typically complex with multiple fabrication steps involved.

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