Raymond Angélil

Large scale molecular dynamics simulations of homogeneous nucleation.

We present results from large-scale molecular dynamics (MD) simulations of homogeneous vapor-to-liquid 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 1.0ε (where ε 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 low temperatures, and at kT = 1.0ε it overestimates them by up to 10(5). 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 10(4) 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 = 1.0ε, 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.

Properties of liquid clusters in large-scale molecular dynamics nucleation simulations

We have performed large-scale Lennard-Jones molecular dynamics simulations of homogeneous vapor-to-liquid nucleation, with 10(9) atoms. This large number allows us to resolve extremely low nucleation rates, and also provides excellent statistics for cluster properties over a wide range of cluster sizes. The nucleation rates, cluster growth rates, and size distributions are presented in Diemand et al. [J. Chem. Phys. 139, 74309 (2013)], while this paper analyses the properties of the clusters. We explore the cluster temperatures, density profiles, potential energies, and shapes. A thorough understanding of the properties of the clusters is crucial to the formulation of nucleation models. Significant latent heat is retained by stable clusters, by as much as ΔkT = 0.1ε for clusters with size i = 100. We find that the clusters deviate remarkably from spherical-with ellipsoidal axis ratios for critical cluster sizes typically within b/c = 0.7 ± 0.05 and a/c = 0.5 ± 0.05. We examine cluster spin angular momentum, and find that it plays a negligible role in the cluster dynamics. The interfaces of large, stable clusters are thinner than planar equilibrium interfaces by 10%-30%. At the critical cluster size, the cluster central densities are between 5% and 30% lower than the bulk liquid expectations. These lower densities imply larger-than-expected surface areas, which increase the energy cost to form a surface, which lowers nucleation rates.

Direct simulations of homogeneous bubble nucleation: Agreement with classical nucleation theory and no local hot spots

We present results from direct, large-scale molecular dynamics simulations of homogeneous bubble (liquid-to-vapor) nucleation. The simulations contain half a billion Lennard-Jones atoms and cover up to 56 million time steps. The unprecedented size of the simulated volumes allows us to resolve the nucleation and growth of many bubbles per run in simple direct micro-canonical simulations while the ambient pressure and temperature remain almost perfectly constant. We find bubble nucleation rates which are lower than in most of the previous, smaller simulations. It is widely believed that classical nucleation theory (CNT) generally underestimates bubble nucleation rates by very large factors. However, our measured rates are within two orders of magnitude of CNT predictions; only at very low temperatures does CNT underestimate the nucleation rate significantly. Introducing a small, positive Tolman length leads to very good agreement at all temperatures, as found in our recent vapor-to-liquid nucleation simulations. The critical bubbles sizes derived with the nucleation theorem agree well with the CNT predictions at all temperatures. Local hot spots reported in the literature are not seen: Regions where a bubble nucleation event will occur are not above the average temperature, and no correlation of temperature fluctuations with subsequent bubble formation is seen.

Testing scalar-tensor theories and parametrized post-Newtonian parameters in Earth orbit

We compute the PPN parameters

Clocks around Sgr A

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Homogeneous SPC/E water nucleation in large molecular dynamics simulations.

and

GALACTIC-CENTER S STARS AS A PROSPECTIVE TEST OF THE EINSTEIN EQUIVALENCE PRINCIPLE

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Spacecraft Clocks and Relativity: Prospects for Future Satellite Missions

for general scalar-tensor theories in the Einstein frame, which we compare to the existing PPN formulation in the Jordan frame for alternative theories of gravity. This computation is important for scalar-tensor theories that are expressed in the Einstein frame, such as chameleon and symmetron theories, which can incorporate hiding mechanisms that predict environment-dependent PPN parameters. We introduce a general formalism for scalar-tensor theories and constrain it using the limit on

Bubble evolution and properties in homogeneous nucleation simulations

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Molecular dynamics simulations of bubble nucleation in dark matter detectors

given by the Cassini experiment. In particular we discuss massive Brans-Dicke scalar fields for extended sources. Next, using a recently proposed Earth satellite experiment, in which atomic clocks are used for spacecraft tracking, we compute the observable perturbations in the redshift induced by PPN parameters deviating from their general relativistic values. Our estimates suggest that