93 research outputs found
Effect of Carrier Gas Pressure on Condensation in a Supersonic Nozzle
Supersonic nozzle experiments were performed with a fixed water or ethanol vapor pressure and varying amounts of nitrogen to test the hypothesis that carrier gas pressure affects the onset of condensation. Such an effect might occur if nonisothermal nucleation were important under conditions of excess carrier gas in the atmospheric pressure range, as has been suggested by Ford and Clement [J. Phys. A 22, 4007 (1989)]. Although a small increase was observed in the condensation onset temperature as the stagnation pressure was reduced from 3 to 0.5 atm, these changes cannot be attributed to any nonisothermal effects. The pulsed nozzle experiments also exhibited two interesting anomalies: (1) the density profiles for the water and ethanol mixtures were shifted in opposite directions from the dry N2 profile; (2) a long transient period was required before the nozzle showed good pulse-to-pulse repeatability for condensible vapor mixtures. To theoretically simulate the observed onset behavior, calculations of nucleation and droplet growth in the nozzle were performed that took into account two principal effects of varying the carrier gas pressure: (1) the change in nozzle shape due to boundary layer effects and (2) the variation in the heat capacity of the flowing gas. Energy transfer limitations were neglected in calculating the nucleation rates. The trend of the calculated results matched that of the experimental results very well. Thus, heat capacity and boundary layer effects are sufficient to explain the experimental onset behavior without invoking energy transfer limited nucleation. The conclusions about the rate of nucleation are consistent with those obtained recently using an expansion cloud chamber, but are at odds with results from thermal diffusion cloud chamber measurements
Doppler Shift Anisotropy in Small Angle Neutron Scattering
The two-dimensional patterns in our small angle neutron scattering (SANS) experiments from rapidly moving aerosols are anisotropic. To test the kinematic theory of two-body scattering that describes the anisotropy, we conducted SANS experiments using a constant source of D2O aerosol with droplets moving at ~440 m/s, and varied the neutron velocity from 267 to 800 m/s. The theoretically predicted anisotropy of the laboratory scattering intensities agrees well with the experimental results. Based on an analysis of the scattering intensity in the Guinier region, we also determined the particle velocity. The results are in very good agreement with independent velocity estimates based on supersonic flow measurements
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Trace element emissions. Semi-annual report, October 1994--February 1995
Many trace elements can exist in raw coal gas either in the form of metallic vapors or gaseous compounds which, besides their action on potentially ``very clean`` advanced power generating systems such as fuel cells and gas turbines, can also be detrimental to plant and animal life when released into the atmosphere. Therefore, volatile trace contaminants from coal which can also be toxic must be removed before they become detrimental to both power plant performance/endurance and the environment. Five trace elements were selected in this project based on: abundance in solid coal, volatility during gasification, effects on downstream systems and toxicity to plant and animal life. An understanding was sought in this investigation of the interactions of these five trace elements (and their high temperature species) with the different components in integrated cleanup and power generating systems, as well as the ultimate effects with respect to atmospheric emissions. Utilizing thermodynamic calculations and various experimental techniques, it was determined that a number of trace contaminants that exist in coal may be substantially removed by flyash, and after that by different sorbent systems. High temperature cleanup of contaminants by sorbents such as zinc titanate, primarily to remove sulfur, can also absorb some metallic contaminants such as cadmium and antimony. Further polishing will be required, however, to eliminate trace contaminant species incorporating the elements arsenic, selemium, lead, and mercury
Non-Markovian polymer reaction kinetics
Describing the kinetics of polymer reactions, such as the formation of loops
and hairpins in nucleic acids or polypeptides, is complicated by the structural
dynamics of their chains. Although both intramolecular reactions, such as
cyclization, and intermolecular reactions have been studied extensively, both
experimentally and theoretically, there is to date no exact explicit analytical
treatment of transport-limited polymer reaction kinetics, even in the case of
the simplest (Rouse) model of monomers connected by linear springs. We
introduce a new analytical approach to calculate the mean reaction time of
polymer reactions that encompasses the non-Markovian dynamics of monomer
motion. This requires that the conformational statistics of the polymer at the
very instant of reaction be determined, which provides, as a by-product, new
information on the reaction path. We show that the typical reactive
conformation of the polymer is more extended than the equilibrium conformation,
which leads to reaction times significantly shorter than predicted by the
existing classical Markovian theory.Comment: Main text (7 pages, 5 figures) + Supplemantary Information (13 pages,
2 figures
Mean first-passage times of non-Markovian random walkers in confinement
The first-passage time (FPT), defined as the time a random walker takes to
reach a target point in a confining domain, is a key quantity in the theory of
stochastic processes. Its importance comes from its crucial role to quantify
the efficiency of processes as varied as diffusion-limited reactions, target
search processes or spreading of diseases. Most methods to determine the FPT
properties in confined domains have been limited to Markovian (memoryless)
processes. However, as soon as the random walker interacts with its
environment, memory effects can not be neglected. Examples of non Markovian
dynamics include single-file diffusion in narrow channels or the motion of a
tracer particle either attached to a polymeric chain or diffusing in simple or
complex fluids such as nematics \cite{turiv2013effect}, dense soft colloids or
viscoelastic solution. Here, we introduce an analytical approach to calculate,
in the limit of a large confining volume, the mean FPT of a Gaussian
non-Markovian random walker to a target point. The non-Markovian features of
the dynamics are encompassed by determining the statistical properties of the
trajectory of the random walker in the future of the first-passage event, which
are shown to govern the FPT kinetics.This analysis is applicable to a broad
range of stochastic processes, possibly correlated at long-times. Our
theoretical predictions are confirmed by numerical simulations for several
examples of non-Markovian processes including the emblematic case of the
Fractional Brownian Motion in one or higher dimensions. These results show, on
the basis of Gaussian processes, the importance of memory effects in
first-passage statistics of non-Markovian random walkers in confinement.Comment: Submitted version. Supplementary Information can be found on the
Nature website :
http://www.nature.com/nature/journal/v534/n7607/full/nature18272.htm
The low-density/high-density liquid phase transition for model globular proteins
The effect of molecule size (excluded volume) and the range of interaction on
the surface tension, phase diagram and nucleation properties of a model
globular protein is investigated using a combinations of Monte Carlo
simulations and finite temperature classical Density Functional Theory
calculations. We use a parametrized potential that can vary smoothly from the
standard Lennard-Jones interaction characteristic of simple fluids, to the ten
Wolde-Frenkel model for the effective interaction of globular proteins in
solution. We find that the large excluded volume characteristic of large
macromolecules such as proteins is the dominant effect in determining the
liquid-vapor surface tension and nucleation properties. The variation of the
range of the potential only appears important in the case of small excluded
volumes such as for simple fluids. The DFT calculations are then used to study
homogeneous nucleation of the high-density phase from the low-density phase
including the nucleation barriers, nucleation pathways and the rate. It is
found that the nucleation barriers are typically only a few and that
the nucleation rates substantially higher than would be predicted by Classical
Nucleation Theory.Comment: To appear in Langmui
Phase space reduction of the one-dimensional Fokker-Planck (Kramers) equation
A pointlike particle of finite mass m, moving in a one-dimensional viscous
environment and biased by a spatially dependent force, is considered. We
present a rigorous mapping of the Fokker-Planck equation, which determines
evolution of the particle density in phase space, onto the spatial coordinate
x. The result is the Smoluchowski equation, valid in the overdamped limit,
m->0, with a series of corrections expanded in powers of m. They are determined
unambiguously within the recurrence mapping procedure. The method and the
results are interpreted on the simplest model with no field and on the damped
harmonic oscillator.Comment: 13 pages, 1 figur
Diffusion in Stationary Flow from Mesoscopic Non-equilibrium Thermodynamics
We analyze the diffusion of a Brownian particle in a fluid under stationary
flow. By using the scheme of non-equilibrium thermodynamics in phase space, we
obtain the Fokker-Planck equation which is compared with others derived from
kinetic theory and projector operator techniques. That equation exhibits
violation of the fluctuation dissipation-theorem. By implementing the
hydrodynamic regime described by the first moments of the non-equilibrium
distribution, we find relaxation equations for the diffusion current and
pressure tensor, allowing us to arrive at a complete description of the system
in the inertial and diffusion regimes. The simplicity and generality of the
method we propose, makes it applicable to more complex situations, often
encountered in problems of soft condensed matter, in which not only one but
more degrees of freedom are coupled to a non-equilibrium bath.Comment: 10 pages, accepted in Phys. Rev.
Diffusion in Stationary Flow from Mesoscopic Non-equilibrium Thermodynamics
We analyze the diffusion of a Brownian particle in a fluid under stationary
flow. By using the scheme of non-equilibrium thermodynamics in phase space, we
obtain the Fokker-Planck equation which is compared with others derived from
kinetic theory and projector operator techniques. That equation exhibits
violation of the fluctuation dissipation-theorem. By implementing the
hydrodynamic regime described by the first moments of the non-equilibrium
distribution, we find relaxation equations for the diffusion current and
pressure tensor, allowing us to arrive at a complete description of the system
in the inertial and diffusion regimes. The simplicity and generality of the
method we propose, makes it applicable to more complex situations, often
encountered in problems of soft condensed matter, in which not only one but
more degrees of freedom are coupled to a non-equilibrium bath.Comment: 10 pages, accepted in Phys. Rev.
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