Post‐Lattice‐Match Growth of Corrugated Gold Nanoplates for Enhanced Plasmonics and Catalysis

ABSTRACT Precise engineering of surface topography in noble metal nanocrystals is pivotal for advanced applications but remains challenging due to the thermodynamic preference for epitaxial, layer‐by‐layer (Frank‐van der Merwe) growth on lattice‐matched seeds. Here, we report a kinetic‐mediated strategy that disrupts this paradigm, enabling the post‐lattice‐match synthesis of corrugated gold nanoplates with programmable roughness. By introducing trace shape‐mediators (e.g., Pd 2+ ), we create a reduction kinetics disparity that directs sequential deposition, intentionally breaking epitaxial ordering and inducing a Stranski–Krastanov‐like island growth mode under mild, one‐pot conditions. The resulting nanostructures feature a high density of plasmonic hotspots, leading to exceptional surface‐enhanced Raman spectroscopy sensitivity with a detection limit down to 10 −7 m for molecules such as crystal violet. Furthermore, these corrugated surfaces exhibit enhanced CO Faraday efficiency in electrocatalytic CO 2 reduction. This work establishes a general approach to transcending thermodynamic constraints in nanocrystal growth, offering a versatile platform for designing functional nanomaterials with customized surface architectures.