Abstract
AbstractDNA 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.
Highlights
DNA nanotechnology offers a versatile toolbox for precise spatial and temporal manipulation of matter on the nanoscale
DNA nanotechnology utilizes the specificity and programmability of Watson–Crick base pairing for assembling DNA molecules into complex structures.[1]
The pH-responsive triplex locks were incorporated into chiral plasmonic molecules (CPMs) consisting of two gold nanorods (AuNRs) assembled on reconfigurable DNA origami templates (Figure 1 C)
Summary
DNA nanotechnology offers a versatile toolbox for precise spatial and temporal manipulation of matter on the nanoscale. Protons dissociated from MCH+ can protonate the cytosine bases in the ssDNA part of the lock, which leads to triplex formation and closure of the lock through sequence-specific parallel Hoogsteen interactions.[44,46] The pH-responsive triplex locks were incorporated into CPMs consisting of two gold nanorods (AuNRs) assembled on reconfigurable DNA origami templates (Figure 1 C). CPMs with 40 % TAT locks exhibited a strong dependence of chiroptical responses on pH in a range between 5.5 and 7 (Figure 2 B).
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