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Vapor-liquid-solid (VLS) route and its variants are routinely used forscalable synthesis of semiconducting nanowires yet the fundamental growthprocesses remain unknown. Here, we employ atomic-scale computations based onmodel potentials to study the stability and growth of gold-catalyzed siliconnanowires (SiNWs). Equilibrium studies uncover segregation at the solid-likesurface of the catalyst particle, a liquid AuSi droplet, and a silicon-richdroplet-nanowire interface enveloped by heterogeneous truncating facets.Supersaturation of the droplets leads to rapid 1D growth on the truncatingfacets and much slower nucleation-controlled 2D growth on the main facet.Surface diffusion is suppressed and the excess Si flux occurs through thedroplet bulk which, together with the Si-rich interface and contact line,lowers the nucleation barrier on the main facet. The ensuing step flow ismodified by Au diffusion away from the step edges. Our study highlights keyinterfacial characteristics for morphological and compositional control ofsemiconducting nanowire arrays.

Atomistics of vapor-liquid-solid nanowire growth