Phase transitions in fluctuations and their role in two-step nucleation

The Journal of Chemical Physics
Daniella JamesPeter H Poole

Abstract

We consider the thermodynamic behavior of local fluctuations occurring in a stable or metastable bulk phase. For a system with three or more phases, we present a simple analysis based on classical nucleation theory that predicts thermodynamic conditions at which small fluctuations resemble the phase having the lowest surface tension with the surrounding bulk phase, even if this phase does not have a lower chemical potential. We also identify the conditions at which a fluctuation may convert to a different phase as its size increases, referred to here as a "fluctuation phase transition" (FPT). We demonstrate these phenomena in simulations of a two dimensional lattice model by evaluating the free energy surface that describes the thermodynamic properties of a fluctuation as a function of its size and phase composition. We show that a FPT can occur in the fluctuations of either a stable or metastable bulk phase and that the transition is first-order. We also find that the FPT is bracketed by well-defined spinodals, which place limits on the size of fluctuations of distinct phases. Furthermore, when the FPT occurs in a metastable bulk phase, we show that the superposition of the FPT on the nucleation process results in two-step nuc...Continue Reading

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Citations

Jul 10, 2019·Proceedings of the National Academy of Sciences of the United States of America·Sangmin LeeSharon C Glotzer
Sep 6, 2020·Biomolecules·Shakiba NikfarjamTaylor J Woehl
Apr 1, 2019·The Journal of Chemical Physics·Hao JiangAthanassios Z Panagiotopoulos
Feb 17, 2021·The Journal of Chemical Physics·Lara A PatelKatie A Maerzke
Mar 18, 2021·Journal of the American Chemical Society·Atanu K Metya, Valeria Molinero
Apr 17, 2021·Physical Review Letters·Lifen WangXuedong Bai
Apr 24, 2021·Physical Review Letters·Ravi Kumar Reddy Addula, Sudeep N Punnathanam
May 5, 2021·The Journal of Physical Chemistry. B·Abhishek K Sharma, Fernando A Escobedo
Jul 10, 2021·The Journal of Chemical Physics·Dean EatonPeter H Poole

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