Abstract
Chiral Au nanocrystals are promising materials for biosensing and therapeutic applications. However, how chirality emerges during their seed-mediated synthesis remains unclear, leading to limited control over morphologies and chiroptical properties. Herein, it is shown that chiral growth can be mediated by orientational order of chiral micelles at Au surfaces. Quantitative 3D electron microscopy and molecular dynamics simulations reveal growth rules for this mechanism and demonstrate that worm-like micelles register with preferential crystal directions at the surface of the seeds to template the growth of hierarchically chiral features. These features have a specific torsion-orientation coupling, which explains how both the molecular chiral inducer and the seed crystal structure can act as stereoselective parameters. These analyses suggest a new role of surfactant assemblies in seed-mediated synthesis, and uncover fundamental aspects of chirality transfer with implications for the rational synthesis of chiral and anisotropic nanostructures.