Long-wavelength density fluctuations as nucleation precursors

Abstract

Recent theories of nucleation that go beyond Classical Nucleation Theory predict that diffusion-limited nucleation of both liquid droplets and of crystals from a low-density vapor (or weak solution) begins with long-wavelength density fluctuations. This means that in the early stages of nucleation, 'clusters' can have low density but large spatial extent, which is at odds with the classical picture of arbitrarily small clusters of the condensed phase. We present the results of kinetic Monte Carlo simulations using Forward Flux Sampling to show that these predictions are confirmed: namely that on average, nucleation begins in the presence of low-amplitude, but spatially extended density fluctuations thus confirming a significant prediction of the non-classical theory.

References in corpus (10)

• Forward Flux Sampling for rare event simulations
• Simulating rare events in equilibrium or non-equilibrium stochastic systems
• How crystals form: A theory of nucleation pathways
• Core crystallization and pile-up in the cooling sequence of evolving white dwarfs
• Homogeneous Bubble Nucleation driven by local hot spots: a Molecular Dynamics Study
• A dynamical theory of nucleation for colloids and macromolecules
• Mechanism of the Cassie-Wenzel transition via the atomistic and continuum string methods
• A Two-parameter Extension of Classical Nucleation Theory
• Systematically extending classical nucleation theory
• A dynamical theory of homogeneous nucleation for colloids and macromolecules