Multi-Wavelength Photopolymerization of Stable Poly(Catecholamines)-DNA Origami Nanostructures

Orthogonality is pivotal yet chemically challenging in the bottom-up synthesis of multicomponent nanostructures. Here, we leverage the fidelity of the DNA origami technique to install a multi wavelength responsive photopolymerization system with nanometer resolution. By precisely immobilizing various photosensitizers on the origami template, which are only activated at their respective peak wavelength, we can control sequential polymerization processes. In particular, the triggered photosensitizers generate reactive oxygen species that in turn initiate the polymerization of the catecholamines dopamine and norepinephrine. We imprint polymeric layers at designated positions on DNA origami, which modifies the polyanionic nature of the DNA objects, thus, promoting their uptake into living cells while preserving their integrity. Our herein proposed methodology provides a rapid platform to access complex 3D nanostructures by customizing material and biological interfaces.