Rational design and construction of chiral-achiral hybrid structures are of great importance to realize the multifunctional complex chiral structures toward emerging technological applications. However, significant challenges remain due to the lack of fine control over the heterostructure. Here, we have developed a general bottom-up synthetic strategy for the site-selective growth of Cu nanodomains on intrinsically chiral Au nanocrystals. Chiral AuCu heterostructures with three distinct architectures were achieved by controlling the overgrowth of Cu nanodomains in a site-specific manner. The geometry-dependent plasmonic chirality of the heterostructures was demonstrated experimentally by circular dichroism spectroscopy and theoretically through finite-difference time-domain simulations. The site-specific geometric control of chiral AuCu heterostructures was also extended to employ anisotropic chiral Au nanoplates and nanorods as the building blocks. By virtue of the galvanic replacement reactions between metal ions and Cu atoms, chiral heterostructures with increasing architectural complexity and compositional diversity can be further achieved. The current work not only opens up a promising strategy to synthesize complex chiral hybrid nanostructures but also provides an important knowledge framework that guides the rational design of multifunctional chiral hybrid nanostructures toward chiroptical applications.
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