A Chemo‐Mechanically Coupled DNA Origami Clamp Capable of Generating Robust Compression Forces

Abstract DNA nanostructures have been utilized to study biological mechanical processes and construct artificial nanosystems. Many application scenarios necessitate nanodevices able to robustly generate large single molecular forces. However, most existing dynamic DNA nanostructures are triggered by probabilistic hybridization reactions between spatially separated DNA strands, which only non‐deterministically generate relatively small compression forces (≈0.4 piconewtons (pN)). Here, an intercalator‐triggered dynamic DNA origami nanostructure is developed, where large amounts of local binding reactions between intercalators and the nanostructure collectively lead to the robust generation of relatively large compression forces (≈11.2 pN). Biomolecular loads with different stiffnesses, 3, 4, and 6‐helix DNA bundles are efficiently bent by the compression forces. This work provides a robust and powerful force‐generation tool for building highly chemo‐mechanically coupled molecular machines in synthetic nanosystems.