Monte Carlo simulation of homogeneous binary vapor–liquid nucleation: Mutual enhancement of nucleation in a partially miscible system

Yoo, Soohaeng; Oh, Kwang Jin; Zeng, Xiao Cheng

doi:10.1063/1.1409364

Cited by 18 publications

(15 citation statements)

References 37 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…This results in massive discrepancies between the nucleation rates predicted by CNT and those measured in laboratory experiments [6][7][8][9][10][11][12][13][14][15] and molecular dynamics 13,[16][17][18][19][20][21][22][23][24][25][26] or Monte Carlo simulations. [27][28][29][30][31][32][33][34] More recent nucleation theories have made significant improvements since the introduction of the CNT. Density functional theory (DFT) 35 and the extended modified liquid drop model take into account the extended transition rea) Electronic mail: diemand@physik.uzh.ch; URL: http://www.physik.uzh.ch/~diemand/ gion from liquid to vapor, sometimes referred to as the the "corona," and match MD results far better than the CNT.…”

Section: Introductionmentioning

confidence: 99%

Large scale molecular dynamics simulations of homogeneous nucleation

Diemand

Angélil

Tanaka

et al. 2013

The Journal of Chemical Physics

118

163

View full text Add to dashboard Cite

We present results from large-scale molecular dynamics (MD) simulations of homogeneous vapor-to-liquid nucleation. The simulations contain between 1 × 109 and 8 × 109 Lennard-Jones (LJ) atoms, covering up to 1.2 s (56 × 106 time-steps). They cover a wide range of supersaturation ratios, S = 1.55-104, and temperatures from kT = 0.3 to 1.0 (where is the depth of the LJ potential, and k is the Boltzmann constant). We have resolved nucleation rates as low as 1017 cm-3 s-1 (in the argon system), and critical cluster sizes as large as 100 atoms. Recent argon nucleation experiments probe nucleation rates in an overlapping range, making the first direct comparison between laboratory experiments and molecular dynamics simulations possible: We find very good agreement within the uncertainties, which are mainly due to the extrapolations of argon and LJ saturation curves to very low temperatures. The self-consistent, modified classical nucleation model of Girshick and Chiu [J. Chem. Phys. 93, 1273 (1990)] underestimates the nucleation rates by up to 9 orders of magnitudes at low temperatures, and at kT = 1.0 it overestimates them by up to 105. The predictions from a semi-phenomenological model by Laaksonen et al. [Phys. Rev. E 49, 5517 (1994)] are much closer to our MD results, but still differ by factors of up to 104 in some cases. At low temperatures, the classical theory predicts critical clusters sizes, which match the simulation results (using the first nucleation theorem) quite well, while the semi-phenomenological model slightly underestimates them. At kT = 1.0 , the critical sizes from both models are clearly too small. In our simulations the growth rates per encounter, which are often taken to be unity in nucleation models, lie in a range from 0.05 to 0.24. We devise a new, empirical nucleation model based on free energy functions derived from subcritical cluster abundances, and find that it performs well in estimating nucleation rates. We present results from large-scale molecular dynamics (MD) simulations of homogeneous vapor-toliquid nucleation. The simulations contain between 1 × 10 9 and 8 × 10 9 Lennard-Jones (LJ) atoms, covering up to 1.2 μs (56 × 10 6 time-steps). They cover a wide range of supersaturation ratios, S 1.55-10 4 , and temperatures from kT = 0.3 to 1.0 (where is the depth of the LJ potential, and k is the Boltzmann constant). We have resolved nucleation rates as low as 10 17 cm −3 s −1 (in the argon system), and critical cluster sizes as large as 100 atoms. Recent argon nucleation experiments probe nucleation rates in an overlapping range, making the first direct comparison between laboratory experiments and molecular dynamics simulations possible: We find very good agreement within the uncertainties, which are mainly due to the extrapolations of argon and LJ saturation curves to very low temperatures. The self-consistent, modified classical nucleation model of Girshick and Chiu [J. Chem. Phys. 93, 1273 (1990)] underestimates the nucleation rates by up to 9 orders of magnitudes at l...

show abstract

Section: Introductionmentioning

confidence: 99%

Large scale molecular dynamics simulations of homogeneous nucleation

Diemand

Angélil

Tanaka

et al. 2013

The Journal of Chemical Physics

118

163

View full text Add to dashboard Cite

show abstract

“…The MD and MC simulations also showed that the nucleation rates obtained by MD and MC simulations are significantly different from predictions by the CNT. [19][20][21][22][23][24][25][26][27][28][29][30][31][32][33][34][35][36][37] The nucleation rate is determined by the number density (or the work of formation) of the critical clusters, which are thermodynamically the largest unstable clusters. Although the critical clusters are nano-sized in the parameter range of nucleation experiments, the CNT estimates the work of formation of such small critical clusters, by simply using the surface tension of bulk material.…”

Section: Introductionmentioning

confidence: 99%

Molecular dynamics simulations of nucleation from vapor to solid composed of Lennard-Jones molecules

Tanaka

Yamamoto

et al. 2011

The Journal of Chemical Physics

108

View full text Add to dashboard Cite

We performed molecular dynamics (MD) simulations of nucleation from vapor at temperatures below the triple point for systems consisting of 10 4 -10 5 Lennard-Jones (L-J) type molecules in order to test nucleation theories at relatively low temperatures. Simulations are performed for a wide range of initial supersaturation ratio (S 0 10 − 10 8 ) and temperature (kT = 0.2 − 0.6ε), where ε and k are the depth of the L-J potential and the Boltzmann constant, respectively. Clusters are nucleated as supercooled liquid droplets because of their small size. Crystallization of the supercooled liquid nuclei is observed after their growth slows. The classical nucleation theory (CNT) significantly underestimates the nucleation rates (or the number density of critical clusters) in the low-T region. The semi-phenomenological (SP) model, which corrects the CNT prediction of the formation energy of clusters using the second virial coefficient of a vapor, reproduces the nucleation rate and the cluster size distributions with good accuracy in the low-T region, as well as in the higher-T cases considered in our previous study. The sticking probability of vapor molecules onto the clusters is also obtained in the present MD simulations. Using the obtained values of sticking probability in the SP model, we can further refine the accuracy of the SP model.

show abstract

“…Since the phase behavior of a compressible mixture is much richer than that of a onecomponent fluid, 9 we also expect the nucleation behavior to be complex. [10][11][12][13][14][15][16][17] There is, for instance, the possibility of a competition between a gas-liquid and a fluid-fluid phase separation in a compressible binary mixtures, and an anomalous decrease of the nucleation rate with temperature for certain parameters. 18,19 Understanding bubble nucleation is a key ingredient for controlling processability and materials properties.…”

Section: Introductionmentioning

confidence: 99%