We measured the nucleation and growth kinetics of solid silicon (Si) from liquid gold-silicon (AuSi) catalyst particles as the Si supersaturation increased, which is the first step of the vapor-liquid-solid growth of nanowires. Quantitative measurements agree well with a kinetic model, providing a unified picture of the growth process. Nucleation is heterogeneous, occurring consistently at the edge of the AuSi droplet, yet it is intrinsic and highly reproducible. We studied the critical supersaturation required for nucleation and found no observable size effects, even for systems down to 12 nanometers in diameter. For applications in nanoscale technology, the reproducibility is essential, heterogeneity promises greater control of nucleation, and the absence of strong size effects simplifies process design.
The phase diagram of a nanoscale system can be substantially different than in the bulk, but quantitative measurements have proven elusive. Here we use in situ microscopy to observe a phase transition in a nanoscale system, together with a simple quantitative model to extract the size effects from these measurements. We expose a Au particle to disilane gas, and observe the transition from a two-phase Au + AuSi system to single-phase AuSi. Size effects are evident in the nonlinear disappearance of the solid Au. Our analysis shows a substantial shift in the liquidus line, and a discontinuous change in the liquid composition at the transition. It also lets us estimate the liquid-solid interfacial free energy.
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