Reciprocal Control of Hierarchical DNA Origami-Nanoparticle Assemblies*

A major focus in bionanotechnology is interfacing with inorganic materials, such as nanoparticles (NPs), for effective integration and control over emergent functions of composite materials. The structural precision and dynamic capabilities of DNA origami make it ideal to achieve these goals. We present an actuation scheme utilizing NPs as control elements enabling rapid and reversible thermal actuation of DNA origami and higher order assemblies. We demonstrate tunable thermal actuation between open and closed configurations on the timescale of seconds, with evidence that reconfiguration is only limited by heating or cooling rates of the bulk solution. We extend the dynamic capabilities in higher-order assemblies by polymerizing hinges which can achieve micron-scale reconfiguration. Control of NPs at the arrays scale combined with NP based control of hinges at the individual scale serves as a basis for reciprocal control of hierarchical assemblies. We also polymerize hinges side-to-side to create more compact NP arrays, or use a combination of polymerization schemes to assemble expandable 2D NP arrays. These NP-hinge composites serve as a novel basis for creating reconfigurable emergent materials.