Light‐Responsive Dynamic DNA‐Origami‐Based Plasmonic Assemblies

DNA nanotechnology offers a versatile toolbox for precise spatial and temporal manipulation of matter on the nanoscale. However, rendering DNA‐based systems responsive to light has remained challenging. Herein, we describe the remote manipulation of native (non‐photoresponsive) chiral plasmonic molecules (CPMs) using light. Our strategy is based on the use of a photoresponsive medium comprising a merocyanine‐based photoacid. Upon exposure to visible light, the medium decreases its pH, inducing the formation of DNA triplex links, leading to a spatial reconfiguration of the CPMs. The process can be reversed simply by turning the light off and it can be repeated for multiple cycles. The degree of the overall chirality change in an ensemble of CPMs depends on the CPM fraction undergoing reconfiguration, which, remarkably, depends on and can be tuned by the intensity of incident light. Such a dynamic, remotely controlled system could aid in further advancing DNA‐based devices and nanomaterials. The spatial configuration and optical properties of non‐photoresponsive DNA‐origami‐based plasmonic assemblies can be controlled with light using a photoresponsive medium. Upon exposure to visible light, the medium's pH decreases, inducing the formation of DNA triplex links in the plasmonic assemblies, leading to their spatial reconfiguration, which can be reversed by turning the light off.