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Chiral nanostructures of nanoparticle assemblies have attracted tremendous interest for their fascinating functional properties. Herein, through theoretical simulations, it is shown that nanoparticle tethered block copolymers can self‐assemble into hierarchically chiral nanostructures. Twofold helices are formed in the hierarchically chiral nanostructures: the diblock copolymers form helical supercylinders...
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