Evaporation of Lennard-Jones Fluids

Evaporation and condensation at a liquid/vapor interface are ubiquitous interphase mass and energy transfer phenomena that are still not well understood. We have carried out large scale molecular dynamics simulations of Lennard-Jones (LJ) fluids composed of monomers, dimers, or trimers to investigate these processes with molecular detail. For LJ monomers in contact with a vacuum, the evaporation rate is found to be very high with significant evaporative cooling and an accompanying density gradient in the liquid domain near the liquid/vapor interface. Increasing the chain length to just dimers significantly reduces the evaporation rate. We confirm that mechanical equilibrium plays a key role in determining the evaporation rate and the density and temperature profiles across the liquid/vapor interface. The velocity distributions of evaporated molecules and the evaporation and condensation coefficients are measured and compared to the predictions of an existing model based on kinetic theory of gases. Our results indicate that for both monatomic and polyatomic molecules, the evaporation and condensation coefficients are equal when systems are not far from equilibrium and smaller than one, and decrease with increasing temperature. For the same reduced temperature $T/T_c$, where $T_c$ is the critical temperature, these two coefficients are higher for LJ dimers and trimers than for monomers, in contrast to the traditional viewpoint that they are close to unity for monatomic molecules and decrease for polyatomic molecules. Furthermore, data for the two coefficients collapse onto a master curve when plotted against a translational length ratio between the liquid and vapor phase.Comment: revised version, 15 pages, 15 figures, to appear in J. Chem. Phy

Gamow-Teller strength distributions for nuclei in pre-supernova stellar cores

Electron-capture and $\beta$-decay of nuclei in the core of massive stars play an important role in the stages leading to a type II supernova explosion. Nuclei in the f-p shell are particularly important for these reactions in the post Silicon-burning stage of a presupernova star. In this paper, we characterise the energy distribution of the Gamow-Teller Giant Resonance (GTGR) for mid-fp-shell nuclei in terms of a few shape parameters, using data obtained from high energy, forward scattering (p,n) and (n,p) reactions. The energy of the GTGR centroid $E_{GT}$ is further generalised as function of nuclear properties like mass number, isospin and other shell model properties of the nucleus. Since a large fraction of the GT strength lies in the GTGR region, and the GTGR is accessible for weak transitions taking place at energies relevant to the cores of presupernova and collapsing stars, our results are relevant to the study of important $e^-$-capture and $\beta$-decay rates of arbitrary, neutron-rich, f-p shell nuclei in stellar cores. Using the observed GTGR and Isobaric Analog States (IAS) energy systematics we compare the coupling coefficients in the Bohr-Mottelson two particle interaction Hamiltonian for different regions of the Isotope Table.Comment: Revtex, 28 pages +7 figures (PostScript Figures, uuencoded, filename: Sutfigs.uu). If you have difficulty printing the figures, please contact [email protected]. Accepted for publication in Phys. Rev. C, Nov 01, 199

A Study of Activated Processes in Soft Sphere Glass

On the basis of long simulations of a binary mixture of soft spheres just below the glass transition, we make an exploratory study of the activated processes that contribute to the dynamics. We concentrate on statistical measures of the size of the activated processes.Comment: 17 pages, 9 postscript figures with epsf, uses harvmac.te

A discretized integral hydrodynamics

Using an interpolant form for the gradient of a function of position, we write an integral version of the conservation equations for a fluid. In the appropriate limit, these become the usual conservation laws of mass, momentum and energy. We also discuss the special cases of the Navier-Stokes equations for viscous flow and the Fourier law for thermal conduction in the presence of hydrodynamic fluctuations. By means of a discretization procedure, we show how these equations can give rise to the so-called "particle dynamics" of Smoothed Particle Hydrodynamics and Dissipative Particle Dynamics.Comment: 10 pages, RevTex, submitted to Phys. Rev.

Measurement of the Absolute Differential Cross Section for np Elastic Scattering at 194 MeV

A tagged medium-energy neutron beam has been used in a precise measurement of the absolute differential cross section for np back-scattering. The results resolve significant discrepancies within the np database concerning the angular dependence in this regime. The experiment has determined the absolute normalization with 1.5% uncertainty, suitable to verify constraints of supposedly comparable precision that arise from the rest of the database in partial wave analyses. The analysis procedures, especially those associated with evaluation of systematic errors in the experiment, are described in detail so that systematic uncertainties may be included in a reasonable way in subsequent partial wave analysis fits incorporating the present results.Comment: 22 pages, 21 figures, submitted for publication in Physical Review

Effect of bond lifetime on the dynamics of a short-range attractive colloidal system

We perform molecular dynamics simulations of short-range attractive colloid particles modeled by a narrow (3% of the hard sphere diameter) square well potential of unit depth. We compare the dynamics of systems with the same thermodynamics but different bond lifetimes, by adding to the square well potential a thin barrier at the edge of the attractive well. For permanent bonds, the relaxation time $\tau$ diverges as the packing fraction $\phi$ approaches a threshold related to percolation, while for short-lived bonds, the $\phi$-dependence of $\tau$ is more typical of a glassy system. At intermediate bond lifetimes, the $\phi$-dependence of $\tau$ is driven by percolation at low $\phi$, but then crosses over to glassy behavior at higher $\phi$. We also study the wavevector dependence of the percolation dynamics.Comment: Revised; 9 pages, 9 figure

Generalized Rosenfeld scalings for tracer diffusivities in not-so-simple fluids: Mixtures and soft particles

Rosenfeld [Phys. Rev. A 15, 2545 (1977)] noticed that casting transport coefficients of simple monatomic, equilibrium fluids in specific dimensionless forms makes them approximately single-valued functions of excess entropy. This has predictive value because, while the transport coefficients of dense fluids are difficult to estimate from first principles, excess entropy can often be accurately predicted from liquid-state theory. Here, we use molecular simulations to investigate whether Rosenfeld's observation is a special case of a more general scaling law relating mobility of particles in mixtures to excess entropy. Specifically, we study tracer diffusivities, static structure, and thermodynamic properties of a variety of one- and two-component model fluid systems with either additive or non-additive interactions of the hard-sphere or Gaussian-core form. The results of the simulations demonstrate that the effects of mixture concentration and composition, particle-size asymmetry and additivity, and strength of the interparticle interactions in these fluids are consistent with an empirical scaling law relating the excess entropy to a new dimensionless (generalized Rosenfeld) form of tracer diffusivity, which we introduce here. The dimensionless form of the tracer diffusivity follows from knowledge of the intermolecular potential and the transport / thermodynamic behavior of fluids in the dilute limit. The generalized Rosenfeld scaling requires less information, and provides more accurate predictions, than either Enskog theory or scalings based on the pair-correlation contribution to the excess entropy. As we show, however, it also suffers from some limitations, especially for systems that exhibit significant decoupling of individual component tracer diffusivities.Comment: 15 pages, 10 figure

Measurement of the Absolute np Scattering Differential Cross Section at 194 MeV

We describe a double-scattering experiment with a novel tagged neutron beam to measure differential cross sections for np back-scattering to better than 2% absolute precision. The measurement focuses on angles and energies where the cross section magnitude and angle-dependence constrain the charged pion-nucleon coupling constant, but existing data show serious discrepancies among themselves and with energy-dependent partial wave analyses (PWA). The present results are in good accord with the PWA, but deviate systematically from other recent measurements.Comment: 4 pages, 4 figure

Generalized quantum cumulant dynamics

A means of unifying some semiclassical models of computational chemistry is presented; these include quantized Hamiltonian dynamics, quantal cumulant dynamics, and semiclassical Moyal dynamics (SMD). A general method for creating the infinite hierarchy of operator dynamics in the Heisenberg picture is derived together with a general method for truncation (or closure) of that series, and in addition, we provide a simple link to the phase space methods of SMD. Operator equations of arbitrary order may be created readily, avoiding the tedious algebra identified previously. Truncation is based on a simple recurrence formula which is related to, but avoids the more complex contractions of, Wick's theorem. This generalized method is validated against a number of trial problems considered using the previous methods. We also touch on some of the limitations involved using such methods, noting, in particular, that any truncation will lead to a state which is in some sense unphysical. Finally, we briefly introduce our quantum algebra package QuantAL which provides an automated method for the generation of the required equation set, the initial conditions for all variables from any start, and all the higher order approximations necessary for truncation of the series, at essentially arbitrary order

Using the fractional interaction law to model the impact dynamics in arbitrary form of multiparticle collisions

Using the molecular dynamics method, we examine a discrete deterministic model for the motion of spherical particles in three-dimensional space. The model takes into account multiparticle collisions in arbitrary forms. Using fractional calculus we proposed an expression for the repulsive force, which is the so called fractional interaction law. We then illustrate and discuss how to control (correlate) the energy dissipation and the collisional time for an individual article within multiparticle collisions. In the multiparticle collisions we included the friction mechanism needed for the transition from coupled torsion-sliding friction through rolling friction to static friction. Analysing simple simulations we found that in the strong repulsive state binary collisions dominate. However, within multiparticle collisions weak repulsion is observed to be much stronger. The presented numerical results can be used to realistically model the impact dynamics of an individual particle in a group of colliding particles.Comment: 17 pages, 8 figures, 1 table; In review process of Physical Review