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In this study, we demonstrate the dependence of atmospheric dust size on the near-infrared spectra of ten L dwarfs, and constrain the sizes of dust grains in each L dwarf atmosphere. In previous studies, by comparing observed and modeled spectra, it was suggested that the deviations of their spectral shapes from theoretical prediction are general characteristics. Here, we focus on the dust size in brown dwarf atmospheres to understand the observed spectra. We confirm that changing the dust size changes the temperature-pressure structure of the atmosphere, with the shape of the spectrum changing accordingly. At the wavelength at which dust is the main absorber of radiation (the dust-dominated regime), a large dust opacity combined with a medium grain size, e.g., 0.1 $\mu$m, results in a low photospheric temperature, and thus a small flux. Conversely, for the wavelength at which gas absorption is dominant (the gas-dominated regime), a large dust opacity modifies the temperature-pressure structure, resulting in a high photospheric temperature, which corresponds to large flux emissions. Taking into account the size effect, we compare the model spectral fluxes in the wavelength range 1-5 $\mu$m with the observational ones to constrain the main dust size in the atmosphere of each of the ten L dwarfs observed with AKARI and SpeX or CGS4. Ultimately, we reveal that the observed data are reproduced with higher fidelity by models based on a medium dust size of 0.1-3.0 $\mu$m for six of these L dwarfs; therefore, we suggest that such atmospheric dust sizes apply to the majority of L dwarfs., Comment: 43 pages, 11 figures, 3 tables, Accepted for publication in ApJ

The abundant forms in which the major elements in the universe exist have been determined from numerous astronomical observations and meteoritic analyses. Iron (Fe) is an exception, in that only depletion of gaseous Fe has been detected in the interstellar medium, suggesting that Fe is condensed into a solid, possibly the astronomically invisible metal. To determine the primary form of Fe, we replicated the formation of Fe grains in gaseous ejecta of evolved stars by means of microgravity experiments. We found that the sticking probability for formation of Fe grains is extremely small; only several atoms will stick per hundred thousand collisions, so that homogeneous nucleation of metallic Fe grains is highly ineffective, even in the Fe-rich ejecta of Type Ia supernovae. This implies that most Fe is locked up as grains of Fe compounds or as impurities accreted onto other grains in the interstellar medium.

We revisit classical nucleation theory (CNT) for the homogeneous bubble nucleation rate and improve the classical formula using a new prefactor in the nucleation rate. Most of the previous theoretical studies have used the constant prefactor determined by the bubble growth due to the evaporation process from the bubble surface. However, the growth of bubbles is also regulated by the thermal conduction, the viscosity, and the inertia of liquid motion. These effects can decrease the prefactor significantly, especially when the liquid pressure is much smaller than the equilibrium one. The deviation in the nucleation rate between the improved formula and the CNT can be as large as several orders of magnitude. Our improved, accurate prefactor and recent advances in molecular dynamics simulations and laboratory experiments for argon bubble nucleation enable us to precisely constrain the free energy barrier for bubble nucleation. Assuming the correction to the CNT free energy is of the functional form suggested by Tolman, the precise evaluations of the free energy barriers suggest the Tolman length is $\simeq 0.3 \sigma$ independently of the temperature for argon bubble nucleation, where $\sigma$ is the unit length of the Lenard-Jones potential. With this Tolman correction and our new prefactor one gets accurate bubble nucleation rate predictions in the parameter range probed by current experiments and molecular dynamics simulations., Comment: 10pages, 6figures, Accepted for publication in Physical Review E

We present results from direct, large-scale molecular dynamics (MD) simulations of homogeneous bubble (liquid-to-vapor) nucleation. The simulations contain half a billion Lennard-Jones (LJ) 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 (NVE) 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 events will occur are not above the average temperature, and no correlation of temperature fluctuations with subsequent bubble formation is seen., Comment: 15 pages, 13 figures. Submitted to PRE. Simulation movies available at http://www.ics.uzh.ch/~diemand/movies/

Recent very large molecular dynamics simulations of homogeneous nucleation with $(1-8) \cdot 10^9$ Lennard-Jones atoms [Diemand et al. J. Chem. Phys. {\bf 139}, 074309 (2013)] allow us to accurately determine the formation free energy of clusters over a wide range of cluster sizes. This is now possible because such large simulations allow for very precise measurements of the cluster size distribution in the steady state nucleation regime. The peaks of the free energy curves give critical cluster sizes, which agree well with independent estimates based on the nucleation theorem. Using these results, we derive an analytical formula and a new scaling relation for nucleation rates: $\ln J' / \eta$ is scaled by $\ln S / \eta$, where the supersaturation ratio is $S$, $\eta$ is the dimensionless surface energy, and $J'$ is a dimensionless nucleation rate. This relation can be derived using the free energy of cluster formation at equilibrium which corresponds to the surface energy required to form the vapor-liquid interface. At low temperatures (below the triple point), we find that the surface energy divided by that of the classical nucleation theory does not depend on temperature, which leads to the scaling relation and implies a constant, positive Tolman length equal to half of the mean inter-particle separation in the liquid phase., Comment: 7 figures

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. {\bf 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 $\Delta kT = 0.1 \epsilon$ 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 $b/c = 0.7\pm 0.05$ and $a/c = 0.5 \pm 0.05$. 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 thiner than planar equilibrium interfaces by $10-30\%$. At the critical cluster size, the cluster central densities are between $5-30\%$ 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., Comment: 16 pages, 19 figures, accepted for publication in J. Chem. Phys

We performed molecular dynamics (MD) simulations of the nucleation of water vapor in order to test nucleation theories. Simulations were performed for a wide range of supersaturation ratios (S = 3-25) and water temperatures (Tw=300-390K). We obtained the nucleation rates and the formation free energies of a subcritical cluster from the cluster size distribution. The classical nucleation theory (CNT) and the modified classical nucleation theory (MCNT) overestimate the nucleation rates in all cases. The semi-phenomenological (SP) model, which corrects the MCNT prediction using the second virial coefficient of a vapor, reproduces the formation free energy of a cluster with the size < 20 to within 10 % and the nucleation rate and cluster size distributions to within one order of magnitude. The sticking probability of the vapor molecules to the clusters was also determined from the growth rates of the clusters. The sticking probability rapidly increases with the supersaturation ratio S, which is similar to the Lennard-Jones system., Comment: 11 pages, 11 figures, 2 tables

We present results from large-scale molecular dynamics (MD) simulations of homogeneous vapor-to-liquid nucleation. The simulations contain between one and eight billion Lennard-Jones (LJ) atoms, covering up to 1.2 {\mu}s (56 million time-steps). They cover a wide range of supersaturation ratios, S=1.55 to 10^4, and temperatures from kT = 0.3 to 1.0 {\epsilon} (where {\epsilon} is the depth of the LJ potential, and k 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 = 1.0 {\epsilon} 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 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 {\epsilon} the critical sizes from both models are clearly too small. (abridged), Comment: 17 pages, 17 figures, to appear in J. Chem. Phys. Fixed some typos, matches version in print

We construct a theoretical model for low-temperature crystallization of amorphous silicate grains induced by exothermic chemical reactions. As a first step, the model is applied to the annealing experiments, in which the samples are (1) amorphous silicate grains and (2) amorphous silicate grains covered with an amorphous carbon layer. We derive the activation energies of crystallization for amorphous silicate and amorphous carbon from the analysis of the experiments. Furthermore, we apply the model to the experiment of low-temperature crystallization of amorphous silicate core covered with an amorphous carbon layer containing reactive molecules. We clarify the conditions of low-temperature crystallization due to exothermic chemical reactions. Next, we formulate the crystallization conditions so as to be applicable to astrophysical environments. We show that the present crystallization mechanism is characterized by two quantities: the stored energy density Q in a grain and the duration of the chemical reactions \tau . The crystallization conditions are given by Q > Q_{min} and \tau < \tau _{cool} regardless of details of the reactions and grain structure, where \tau _{cool} is the cooling timescale of the grains heated by exothermic reactions, and Q_{min} is minimum stored energy density determined by the activation energy of crystallization. Our results suggest that silicate crystallization occurs in wider astrophysical conditions than hitherto considered., Comment: 9 figures, accepted for publication in Astrophysical J