Minimum free-energy path of homogenous nucleation from the phase-field equation

Iwamatsu, Masao

doi:10.1063/1.3158471

Cited by 19 publications

(23 citation statements)

References 33 publications

(82 reference statements)

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“…Its solution is exactly the same as found by Chan for NG on a plane [36][37][38] (6) shows that the evolution of nuclei's sizes is influenced by the underlying geometry through the geodesic curvature k g . Note that for a planar geometry k g (R)1/R gives the classical growth rate for NG on a plane.…”

Section: Modelsupporting

confidence: 69%

“…In a curved surface the differential of area is d 2 r ffiffi ffi g p dx 1 dx 2 ffiffi ffi g p so the first term in the free energy represents the contribution from a local homogeneous situation, where f c ð Þ is the local free-energy areal density of a phase with an order parameter c. For a two-phase system this term takes the typical double-well form [36][37][38] , with two local minima corresponding to the initial c ¼ 0 ð Þ and final c ¼ 1 ð Þ phases, separated by a local free-energy barrier. This can be written phenomenologically as:…”

Section: Modelmentioning

confidence: 99%

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Phase nucleation in curved space

et al. 2015

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Nucleation and growth is the dominant relaxation mechanism driving first-order phase transitions. In two-dimensional flat systems, nucleation has been applied to a wide range of problems in physics, chemistry and biology. Here we study nucleation and growth of two-dimensional phases lying on curved surfaces and show that curvature modifies both critical sizes of nuclei and paths towards the equilibrium phase. In curved space, nucleation and growth becomes inherently inhomogeneous and critical nuclei form faster on regions of positive Gaussian curvature. Substrates of varying shape display complex energy landscapes with several geometry-induced local minima, where initially propagating nuclei become stabilized and trapped by the underlying curvature.

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Section: Modelsupporting

confidence: 69%

Section: Modelmentioning

confidence: 99%

Phase nucleation in curved space

et al. 2015

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“…Therefore the vapor to solid nucleation rate J SV will be approximately given by Eq. (26) and will be characterized by two nucleation rates J LV and J SL . Our simple capillarity theory cannot include such a kinetic effect as ours is based on the quasi-equilibrium thermodynamics and cannot include kinetic effect.…”

Section: Resultsmentioning

confidence: 99%

Free-energy landscape of nucleation with an intermediate metastable phase studied using capillarity approximation

Iwamatsu

2011

The Journal of Chemical Physics

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Capillarity approximation is used to study the free-energy landscape of nucleation when an intermediate metastable phase exists. The critical nucleus that corresponds to the saddle point of the free-energy landscape as well as the whole free-energy landscape can be studied using this capillarity approximation, and various scenarios of nucleation and growth can be elucidated. In this study, we consider a model in which a stable solid phase nucleates within a metastable vapor phase when an intermediate metastable liquid phase exists. We predict that a composite critical nucleus that consists of a solid core and a liquid wetting layer as well as pure liquid and pure solid critical nuclei can exist depending not only on the supersaturation of the liquid phase relative to that of the vapor phase but also on the wetting behavior of the liquid surrounding the solid. The existence of liquid critical nucleus indicates that the phase transformation from metastable vapor to stable solid occurs via the intermediate metastable liquid phase, which is quite similar to the scenario of nucleation observed in proteins and colloidal systems. By studying the minimum-free-energy path on the free-energy landscape, we can study the evolution of the composition of solid and liquid within nuclei which is not limited to the critical nucleus.

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“…That the CNT underestimates the free energy barrier for nucleation in single component uids has also been pointed out by previous theoretical studies. [33][34][35] To understand this behavior, we note that at the early stage of bubble formation, change in the density prole from the metastable parent phase is quite small (see the density proles in Fig. 6(a)-(f)), resulting in a small difference in the grand potential density difference in the volume contribution.…”

Section: Nucleation Above T Cmentioning

confidence: 99%

Bubble nucleation in polymer–CO2 mixtures

Cristancho

Costeux

et al. 2013

Soft Matter

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We combine density-functional theory with the string method to calculate the minimum free energy path of bubble nucleation in two polymer-CO 2 mixture systems, poly(methyl methacrylate) (PMMA)-CO 2 and polystyrene (PS)-CO 2 . Nucleation is initiated by saturating the polymer liquid with high pressure CO 2 and subsequently reducing the pressure to ambient condition. Below a critical temperature (T c ), we find that there is a discontinuous drop in the nucleation barrier as a function of increased initial CO 2 pressure (P 0 ), as a result of an underlying metastable transition from a CO 2 -rich-vapor phase to a CO 2 -rich-liquid phase. The nucleation barrier is generally higher for PS-CO 2 than for PMMA-CO 2 under the same temperature and pressure conditions, and both higher temperature and higher initial pressure are required to lower the nucleation barrier for PS-CO 2 to experimentally relevant ranges. Classical nucleation theory completely fails to capture the structural features of the bubble nucleus and severely underestimates the nucleation barrier.

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Minimum free-energy path of homogenous nucleation from the phase-field equation

Cited by 19 publications

References 33 publications

Phase nucleation in curved space

Phase nucleation in curved space

Free-energy landscape of nucleation with an intermediate metastable phase studied using capillarity approximation

Bubble nucleation in polymer–CO2 mixtures

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