Precisely Shaped, Uniformly Formed Gold Nanocubes with Ultrahigh Reproducibility in Single-Particle Scattering and Surface-Enhanced Raman Scattering

Synthesizing plasmonic nanostructures in an ultraprecise manner is of paramount importance because the nanometer-scale structural details can significantly affect their plasmonic properties. Au nanocubes (AuNCs) have been a highly promising, heavily studied nanostructure with high potential in various fields, but an ultraprecise synthesis from 10 to 100 nm in size over a large number of AuNCs has not been well established. Precisely structured AuNC-based studies for a highly reproducible, quantitative plasmonic signal generation [e.g., quantitative surface-enhanced Raman scattering (SERS)] are needed for reliable use and exploration in the beneficial properties of AuNCs. Here, we developed a strategy for AuNC synthesis with the desired size and shape, ranging from 17 to 78 nm particularly with highly controlled corner sharpness, by precisely controlling the growth rate of different facets and AuNC-specific flocculation which enabled ultrahigh yields (similar to 98-99%). Importantly, the precisely shaped AuNCs can scatter light in a spectrally reproducible manner, and the SERS enhancement factors (EFs) for the AuNC dimers are very narrowly distributed (the EFs of 72 nm sharp-cornered cube dimers have a distribution within 1 order of magnitude). Our results pave the paths to ultrahigh yield synthesis of metal nanocubes with a precise size and shape and offer single-particle-level spectral controllability and reproducibility over a large number of particles.