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Register a new userCurvature Dependence of Surface Free Energy of Liquid Drops and Bubbles: A Simulation Study
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We study the excess free energy due to phase coexistence of fluids by Monte Carlo simulations using successive umbrella sampling in finite LxLxL boxes with periodic boundary conditions. Both the vapor-liquid phase coexistence of a simple Lennard-Jones fluid and the coexistence between A-rich and B-rich phases of a symmetric binary (AB) Lennard-Jones mixture are studied, varying the density rho in the simple fluid or the relative concentration x_A of A in the binary mixture, respectively. The character of phase coexistence changes from a spherical droplet (or bubble) of the minority phase (near the coexistence curve) to a cylindrical droplet (or bubble) and finally (in the center of the miscibility gap) to a slab-like configuration of two parallel flat interfaces. Extending the analysis of M. Schrader, P. Virnau, and K. Binder [Phys. Rev. E 79, 061104 (2009)], we extract the surface free energy gamma (R) of both spherical and cylindrical droplets and bubbles in the vapor-liquid case, and present evidence that for R -> Infinity the leading order (Tolman) correction for droplets has sign opposite to the case of bubbles, consistent with the Tolman length being independent on the sign of curvature. For the symmetric binary mixture the expected non-existence of the Tolman length is confirmed. In all cases {and for a range of radii} R relevant for nucleation theory, gamma(R) deviates strongly from gamma (Infinity) which can be accounted for by a term of order gamma(Infinity)/gamma(R)-1 ~ 1/R^2. Our results for the simple Lennard-Jones fluid are also compared to results from density functional theory and we find qualitative agreement in the behavior of gamma(R) as well as in the sign and magnitude of the Tolman length.
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A possibility for the observation of so-called structure resonances (SR) in electrolytes arising due to relative motion of the cluster charged nucleus and its solvation shell is demonstrated. The discussed method considers the resonant contribution of the SR to the frequency dependence of the reflection (transmission) coefficient of the electromagnetic wave interacting with the free electrolyte surface. Of special interest is the observation of SR for multiply charged particles in electrolyte providing direct information on the charge of single cluster. Also important are other not so prominent details of the wave interaction with mobile charged clusters in electrolyte related to the formation and complicated nature of the frequency dependence of the charged cluster associated mass.
We present a detailed study of the heating effects in dielectric measurements carried out on a liquid. Such effects come from the dissipation of the electric power in the liquid and give a contribution to the nonlinear third harmonics susceptibility chi_3 which depends on the frequency and temperature. This study is used to evaluate a possible `spurious contribution to the recently measured nonlinear susceptibility of an archetypical glassforming liquid (Glycerol). Those measurements have been shown to give a direct evaluation of the number of dynamically correlated molecules temperature dependence close to the glass transition temperature T_g~190K (Crauste-Thibierge et al., Phys. Rev. Lett 104,165703(2010)). We show that the heating contribution is totally negligible (i) below 204K at any frequency; (ii) for any temperature at the frequency where the third harmonics response chi_3 is maximum. Besides, this heating contribution does not scale as a function of f/f_{alpha}, with f_{alpha}(T) the relaxation frequency of the liquid. In the high frequency range, when f/f_{alpha} >= 1, we find that the heating contribution is damped because the dipoles cannot follow instantaneously the temperature modulation due to the heating phenomenon. An estimate of the magnitude of this damping is given.
A new mechanism for the passive removal of drop on a horizontal surface is described that does not require pre-fabrication of a surface energy gradient. The method relies upon the preparation of alternate hydrophilic/hydrophobic stripes on a surface. When one side of this surface is exposed to steam, with its other surface convectively cooled with cold water, steam condenses as a continuous film on the hydrophilic stripes but as droplets on the hydrophobic stripes. Coalescence leads to a random motion of the center of mass of the fused drops on the surface, which are readily removed as they reach near the boundary of the hydrophobic and hydrophilic zones thus resulting in a net diffusive flux of the coalesced drops from the hydrophobic to the hydrophilic stripes of the surface. Although an in-situ produced thermal gradient due to differential heat transfer coefficients of the hydrophilic and hydrophobic stripes could provide additional driving force for such a motion, it is, however, not a necessary condition for motion to occur. This method of creating directed motion of drops does not require a pre-existing wettability gradient and may have useful applications in thermal management devices.
Recently 1, we presented a general theory for calculat- ing the strength and properties of colloidal interactions mediated by ligand-receptor bonds (such as those that bind DNA-coated colloids). In this communication, we derive a surprisingly simple analytical form for the inter- action free energy, which was previously obtainable only via a costly numerical thermodynamic integration. As a result, the computational effort to obtain potentials of in- teraction is significantly reduced. Moreover, we can gain insight from this analytic expression for the free energy in limiting cases. In particular, the connection of our general theory to other previous specialised approaches is now made transparent. This important simplification will significantly broaden the scope of our theory.
Surface bubbles have attracted much interest in the past decades. In this article, we propose to explore the lifetime and thinning dynamics of centimetric surface bubbles. We study the impact of the bubbles size as well as that of the atmospheric humidity through a careful control and systematic variation of the relative humidity in the measuring chamber. We first adress the question of the drainage under saturated water vapor conditions and show that a model including both capillary and gravity driven drainage provides the best prediction for this process. Additionally, unprecedented statistics on the bubbles lifetimes confirm experimentally that this parameter is set by evaporation to leading order. We make use of a model based on the overall thinning dynamics of the thin film and assume a rupture thickness of the order 10-100 nm to obtain a good representation of these data. For experiments conducted far from saturation, the convective evaporation of the bath is shown to dominate the overall mass loss in the cap film due to evaporation.
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