Light‐Responsive Dynamic DNA‐Origami‐Based Plasmonic Assemblies

Abstract

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.

Revealing the chirality origin and homochirality crystallization of Ag14 nanocluster at the molecular level

“…Chirality is ubiquitous in (supra)molecular structures, such as DNA in living organisms and natural products in plants, which plays a pivotal role in biological activity, catalysis, medicines, and a variety of other applications 1 , 2 . Although the enantioselective preparation and separation of chiral small molecules induced by chiral reagents have been well established, the realization of this process with achiral reagents still faces great challenges, especially for these higher-order motifs such as nanoclusters, nanoparticles, and supramolecules 3 – 14 .…”

Double‐ to Single‐Strand Transition Induces Forces and Motion in DNA Origami Nanostructures

“…Notably, several approaches have been developed to increase the response speed of dynamic DNA devices. On the other hand, external stimuli such as light, [ 35,36 ] temperature, [ 37 ] ions, [ 11,23 ] pH, [ 38–40 ] and electric fields [ 21,41 ] often enable much faster operation up to an increase in speed by many orders of magnitude. [ 41 ] For example, Karna et al.…”

Azobenzene‐Based Photomechanical Biomaterials

“…Stimuli‐responsive biomaterials are a class of materials that exhibit smart behavior: their physicochemical properties respond to changes in the external environment, such as light, temperature, ultrasound, electricity, magnetic field, and pH. [ 1–11 ] These tailorable systems have promising biomedical applications in the fields of drug delivery, [ 12–16 ] sensors, [ 17,18 ] artificial muscles, [ 19–24 ] actuators, [ 25–28 ] and tissue engineering. [ 29–31 ] Among these materials, light‐responsive biomaterials are an emerging class of materials promising for biomedical applications.…”