Solid–liquid–solid process for forming free-standing gold nanowhisker superlattice by interfering femtosecond laser irradiation

One-dimensional nanomaterial superlattices are fundamental components in plasmonics, nanophotonics, and nanoelectronics. Bottom-up techniques such as vapour–liquid–solid (VLS) and chemosynthesis have been used to fabricate the structure but are nonoptimal for controlling alignment and size. Here we report the fabrication of gold nanowhisker superlattice, based on a novel mechanism termed solid–liquid–solid (SLS). An interfering femtosecond laser pulse induces fluid flows of nanosize gold, which is followed by droplets pinching off from them and freezing of a free-standing nanowhisker superlattice fixed on a substrate. The shape is defined by liquid motion and not by crystallographic growth although its structure is polycrystalline. The smallest curvature radius of its vertex was 3.4 nm, which is one-half of the smallest nanorods fabricated by chemosynthesis. SLS process is a superior alternative to sequential bottom-up processes involving catalyst fabrication, bottom-up synthesis, purification, alignment, stabilization, and preservation.