Crystal nucleation rate isotherms in Lennard-Jones liquids

Байдаков, В. Г.; Tipeev, Azat O.; Bobrov, Konstantin S.; Ionov, G.V.

doi:10.1063/1.3439585

Cited by 47 publications

(43 citation statements)

References 30 publications

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“…(2), we obtain where we used i = (4π/3)a 3 n, h = 0.58ε [42], T 0.5ε/k, T m = 0.69ε/k [38], and n = 0.92σ −3 [29]. The diffusion coefficient of the liquid at T 0.5ε/k obtained in [44] was approximately 0.01, which is smaller than our calculated value. This indicates that molecules in small droplets were more diffusive than in the bulk liquid due to the surface effect of the finite boundary and lower density than the bulk liquid [32].…”

Section: Crystal Growthcontrasting

confidence: 49%

Analyzing multistep homogeneous nucleation in vapor-to-solid transitions using molecular dynamics simulations

et al. 2017

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In this paper, we present multistep homogeneous nucleations in vapor-to-solid transitions as revealed by molecular dynamics simulations on Lennard-Jones molecules, where liquidlike clusters are created and crystallized. During a long, direct NV E (constant volume, energy, and number of molecules) involving the integration of (1.9-15) × 10 6 molecules in up to 200 million steps (=4.3 μs), crystallization in many large, supercooled nanoclusters is observed once the liquid clusters grow to a certain size (∼800 molecules for the case of T 0.5ε/k). In the simulations, we discovered an interesting process associated with crystallization: the solid clusters lost 2-5 % of their mass during crystallization at low temperatures below their melting temperatures. Although the crystallized clusters were heated by latent heat, they were stabilized by cooling due to evaporation. The clusters crystallized quickly and completely except at surface layers. However, they did not have stable crystal structures, rather they had metastable structures such as icosahedral, decahedral, face-centered-cubic-rich (fcc-rich), and hexagonal-close-packed-rich (hcp-rich). Several kinds of cluster structures coexisted in the same size range of ∼1000-5000 molecules. Our results imply that multistep nucleation is a common first stage of condensation from vapor to solid.

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Section: Crystal Growthcontrasting

confidence: 49%

Analyzing multistep homogeneous nucleation in vapor-to-solid transitions using molecular dynamics simulations

et al. 2017

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“…Studies of crystal nucleation in bulk LJ liquid report values of γ = 0.28 to 0.30 for T = 0.43 and 0.45, respectively [50], and these compare favourably with the surface tension of a flat interface at the same T [53]. Using our estimates for the parameters other than γ, namely, ∆H = 0.58N p , A = 7.6, f 0 = 1.3 × 10 7 , C = 6.2, and the literature values of T m = 0.618 [50] and γ = 0.3 [50], we obtain B = 2.0 and λ = 8.6 × 10 8 .…”

Section: Surface Tensionmentioning

confidence: 63%

Crystallization of Lennard-Jones nanodroplets: From near melting to deeply supercooled

Malek

Morrow

Saika‐Voivod

2015

The Journal of Chemical Physics

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We carry out molecular dynamics (MD) and Monte Carlo (MC) simulations to characterize nucleation in liquid clusters of 600 Lennard-Jones particles over a broad range of temperatures. We use the formalism of mean first-passage times to determine the rate and find that Classical Nucleation Theory (CNT) predicts the rate quite well, even when employing simple modelling of crystallite shape, chemical potential, surface tension and particle attachment rate, down to the temperature where the droplet loses metastability and crystallization proceeds through growth-limited nucleation in an unequilibrated liquid. Below this crossover temperature, the nucleation rate is still predicted when MC simulations are used to directly calculate quantities required by CNT. Discrepancy in critical embryo sizes obtained from MD and MC arises when twinned structures with five-fold symmetry provide a competing free energy pathway out of the critical region. We find that crystallization begins with hcp-fcc stacked precritical nuclei and differentiation to various end structures occurs when these embryos become critical. We confirm that using the largest embryo in the system as a reaction coordinate is useful in determining the onset of growth-limited nucleation and show that it gives the same free energy barriers as the full cluster size distribution once the proper reference state is identified. We find that the bulk melting temperature controls the rate, even though the solid-liquid coexistence temperature for the droplet is significantly lower. The value of surface tension that renders close agreement between CNT and direct rate determination is significantly lower than what is expected for the bulk system.

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“…(6) in temperature is determined by the range from T* = 0.35 to 2, in pressure from the melting line to the boundary of spontaneous crystallization, which is determined in Ref. [33]. …”

Section: Results and Discussion Of Calculations Of The Self-diffusionmentioning

confidence: 99%

The self-diffusion coefficient in stable and metastable states of the Lennard–Jones fluid

Байдаков¹,

Проценко²,

Kozlova³

2011

Fluid Phase Equilibria

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Crystal nucleation rate isotherms in Lennard-Jones liquids

Cited by 47 publications

References 30 publications

Analyzing multistep homogeneous nucleation in vapor-to-solid transitions using molecular dynamics simulations

Analyzing multistep homogeneous nucleation in vapor-to-solid transitions using molecular dynamics simulations

Crystallization of Lennard-Jones nanodroplets: From near melting to deeply supercooled

The self-diffusion coefficient in stable and metastable states of the Lennard–Jones fluid

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