DNA-Guided Plasmonic Helix with Switchable Chirality

[Image: see text] 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.