Nonequilibrium statistical mechanical formulation for grain growth

A nonequilibrium statistical mechanical theory for grain growth is presented in this paper. The fluctuation of grain growth is determined from the self similarity of grain size distribution. The grain size distribution scaled by the averaged size is derived under the condition that the volume of specimen is strictly conserved. The growth law of grain is also derived. The scaled grain size distribution are compared with the associating lognormal distribution which is usually used in the analysis of the experimental results. It has been found that the theoretical results is in good agreement with experimental results.     

Improved isotope separation in laser dissociation of trifluoromethyl halides: Scavenging of CF3 with HI

The efficiency of¹³C isotope separation by multiphoton dissociation using a CO₂ laser has been shown to increase by ∼33% upon addition of small amounts of HI to the starting mixture. The reason for this increase is that the CF₃ radicals are scavenged by HI more rapidly than they recombine with free iodine atoms to reform the starting material. For Torr and for 0.5J/cm² roughly 65% of the CF₃ and I radicals reform the starting material in the absence of HI. The results of this study indicate that at −80°C the rate constants for CF₃+CF₃→C₂F₆ and CF₃+I→CF₃I are about equal and are roughly 8 times higher than that for CF₃+HI→CF₃H+I.     

Rotational-coherence molecular laser isotope separation

We have proposed a laser isotope separation method, utilizing rotational coherence of a simple molecule. In the scheme, photoexcited molecules are isotopically separated by difference of rotational period between them. To illustrate this method, two-pulse photodissociation of mixed ⁷⁹Br₂/⁸¹Br₂ isotopes has been investigated theoretically. The photodissociation probabilities of ⁷⁹Br₂ and ⁸¹Br₂ have been calculated as functions of time delay between the photoexcitation and dissociation laser pulses. We have demonstrated that isotope enrichment factor of ⁷⁹Br relative to ⁸¹Br can be changed from 0.34 to 1.8, by simply changing the time delay only by 0.2 ns. Additionally, we have shown that this method is effective for heavy isotopes, based on mass dependence of the isotope enrichment factor.     

Effect of flow pattern in a supersonic nozzle reactor on product branching ratio for UV photolysis of UF6/CH4 mixtures

The product branching ratio was studied in relation to the radical scrambling mechanism of laser isotope separation of uranium. A mixture of UF₆/CH₄/Ar was irradiated either using a low-intensity cw-UV source (high-pressure Hg lamp, 250 nm 400 nm) or using high-intensity pulsed UV lasers (4th-harmonic YAG laser at 266 nm or KrF laser at 248 nm) in a supersonic nozzle reactor. While the latter gave a higher C₂H₆/CH₃F ratio in the photoproduct than the former, the C₂H₆/CH₃F branching ratio was found to disagree with the results reported in a static cell experiment. This anomaly in the results obtained using a supersonic nozzle reactor was well represented by a model proposed in this study which assumed no mixing before a shock wave zone and sufficient mixing after it, leading to complete suppression of radical recombination.     

Enskog’s kinetic theory of dense gases for chemically reacting binary mixtures, II: Light scattering and sound propagation

Enskog’s kinetic theory for a symmetric moderately dense reaction A+A?B+B is used to determine Fick’s and Fourier’s law. The transport coefficients of diffusion, thermal-diffusion rate and thermal conductivity are represented graphically for endothermic and exothermic reactions and are analyzed as a function of the activation energy and of the density of the mixture. The Onsager reciprocity relations are numerically investigated and verified. The problems related to sound propagation and light scattering are investigated for such a mixture and it is shown that the influence of chemical reactions on phase velocity, attenuation coefficient and light scattering spectra is more pronounced for rarefied gases although there is a considerable change in these quantities as the mixture becomes denser.     

Dissociative attachment of an electron to a molecule: kinetic theory

Test particles interact with a medium by means of a bimolecular reversible chemical reaction. Two species are assumed to be much more numerous so that they are distributed according to fixed distributions: Maxwellians and Dirac's deltas. Equilibrium and its stability are investigated in the first case. For the second case, a system is constructed, in view of an approximate solution.     

Stochastic simulation of heat flow with application to laser–solid interactions

Received: 5 September 1997/Accepted: 8 September 1997     

Simulation of the free molecular flow of vapor for laser isotope separation

Vapor flows from a single channel (tube) and from a set of tubes are simulated in the free molecular motion approximation. The integrated characteristics (the fractions of transmitted, sticking, and reflected particles) and the angular distributions of the flux and flux density of the vapor are obtained. Calculations of the flux of atoms scattered as a result of single collisions in an atomic beam are performed. Zh. Tekh. Fiz. 68, 77–81 (May 1998)     

Carbon molecular sieves from PET for separations involving CH4, CO2, O2 and N2

Carbon molecular sieves (CMS) have been made for the first time from PET textile fibres by carbonisation and pore mouth narrowing using CVD of benzene. The diffusion of O₂, N₂, CO₂ and CH₄ in these materials, and also in the commercial CMS Takeda 3A, was studied. It was found that the best PET based CMS was obtained after 10 min CVD time and had adsorption capacities and rates of diffusion similar to those of the Takeda 3A.     

Implementation of diffuse reflection boundary conditions in a thermal lattice Boltzmann model with flux limiters

We discuss three new implementation versions of diffuse reflection boundary conditions in a thermal lattice Boltzmann model. Their accuracy is investigated in the case of Couette flow by considering the slip regime. The best results are recovered with versions 2 and 3, which rely on outgoing fluxes to express the particle distribution functions in the ghost nodes outside the flow domain. Version 2 is found to be more economical since it involves no interpolation procedure. This version was thereafter used to investigate the temperature profile in Couette flow for various values of Prandtl number, as well as the capability of the thermal LB model to capture the Knudsen minimum in Poiseuille flow.     

Conservative force fields in non-Gaussian statistics

In this Letter, we determine the κ-distribution function for a gas in the presence of an external field of force described by a potential U(r). In the case of a dilute gas, we show that the κ-power law distribution including the potential energy factor term can rigorously be deduced in the framework of kinetic theory with basis on the Vlasov equation. Such a result is significant as a preliminary to the discussion on the role of long range interactions in the Kaniadakis thermostatistics and the underlying kinetic theory.     

Diffusion in a bistable potential

The problem of diffusion of a particle in a bistable potential is studied on the basis of the one-dimensional Smoluchowski equation for the space- and time-dependent probability distribution. The potential is modeled as two parabolic wells separated by a parabolic barrier. For the model potential the Smoluchowski equation is solved exactly by a Laplace transform with respect to time for the initial condition that at time zero the probability distribution is given by a thermal equilibrium distribution in one of the wells. In the limit of a high barrier the rate of transition to the other well is given by an asymptotic result due to Kramers. For a potential barrier of moderate height there are significant corrections to the asymptotic result.     

Molecular dynamics simulation about porous thin-film growth in secondary deposition

The thin film growth has been confirmed to be assembled by an enormous number of clusters in experiments of CVD. Sequence of clusters’ depositions proceeds to form the thin film at short time as gas fluids through surface of substrate. In order to grow condensed thin film using series of cluster deposition, the effect of initial velocity, substrate temperature and density of clusters on property of deposited thin film, especially appearance of nanoscale pores inside thin film must be investigated. In this simulation, three different cluster sizes of 203, 653, 1563 atoms with different velocities (0, 10, 100, 1000 and 3000 m/s) were deposited on a Cu(0 0 1) substrate whose temperatures were set between 300 and 1000 K. Four clusters and one cluster were used in primary deposition and secondary deposition, respectively. We have clarified that adhesion between clusters and substrate is greatly influenced by initial velocity. As a result, the exfoliation pattern of deposited thin film is dependent on initial velocity and different between them. One borderline dividing whole region into porous region and nonporous region are obtained to show the effect of growth conditions on appearance of nanoscale pores inside thin film. Moreover, we have also shown that the likelihood of porous thin film is dependent on the point of impact of a cluster relative to previously deposited clusters.     

Transitions between wells and escape by diffusion in a one-dimensional potential landscape

The time-dependence of the occupation probabilities of neighboring wells due to diffusion in one dimension is formulated in terms of a set of generalized rate equations describing transitions between neighboring wells and escape across a final barrier. The equations contain rate coefficients, memory coefficients, and a long-time coefficient characterizing the amplitude of long-time decay. On a more microscopic level the stochastic process is described by a Smoluchowski equation for the one-dimensional probability distribution. A numerical procedure is presented which allows calculation of the transport coefficients in the set of generalized rate equations on the basis of the Smoluchowski equation.     

Studies of the collision frequency of ideal gas particles with the surfaces of the objects created using the ballistic deposition technique

This paper is a continuation of our studies of the collision frequency of ideal gas particles with the rough/fractal surfaces. Here, we applied a more realistic surface growth model, i.e. ballistic deposition for creation of fractal objects. We found that the collision frequency with irregular surfaces is the linear function of pressure and this frequency per unit pressure is quite a complicated function of the surface fractal dimension as well as the diameter of colliding particle. The collision frequency with rough surfaces cannot be exactly described by the analytical formula called the Langmuir-Hertz equation. However, we have stated that the deviations of the true collision frequency from the Langmuir-Hertz prediction are not huge and in typical catalytic studies the error introduced by replacing the true frequency by the Langmuir-Hertz prediction can be safely neglected. We have also studied the probability of finding on the surface an atom which has been hit a certain number of times by a gas particle. This probability reveals an interesting behaviour for small gas particles, i.e. it perfectly correlates with the number of directions from which the surface atom is accessible from the gas phase. We have also estimated the evolution of the adsorption energy distribution with the increasing fractal dimension of the surface in the ballistic deposition.     

Mixture of ultracold lithium and cesium atoms in an optical dipole trap

We present the first simultaneous trapping of two different ultracold atomic species in a conservative trap. Lithium and cesium atoms are stored in an optical dipole trap formed by the focus of a CO₂ laser. Techniques for loading both species of atoms are discussed and observations of elastic and inelastic collisions between the two species are presented. A model for sympathetic cooling of two species with strongly different mass in the presence of slow evaporation is developed. From the observed Cs-induced evaporation of Li atoms we estimate a cross-section for cold elastic Li-Cs collisions. Received: 1 August 2001 / Published online: 23 November 2001     

Efficient laser isotope separation of 13C using novel linear multi-pass cavity

¹³C isotope has been separated in the form of enriched product C₂F₄ by selective multi-photon dissociation (MPD) of Freon-22 (CHClF₂) using the 9P(26) laser line of a transversely excited atmospheric CO₂ laser. The non-linearity factor, γ, that determines the dependence of the yield of ¹³C isotope on the fluence (J/cm²) has been determined for various laser rotational lines (9P(20)–9P(26)) and the advantage of a lower γ in the case of 9P(26) is highlighted for macroscopic production of ¹³C isotope. It is also shown that a higher value of the optimum fluence at 9P(26) not only results in a higher enrichment efficiency but in a relatively lower value of γ also. The laser pulse energy is efficiently utilized for selective MPD of Freon-22 by focusing the pulse energy repeatedly with the help of a novel linear multi-pass cavity (LMPC). The novelty of this optical arrangement lies in its ability to maintain the laser fluence around an optimum value for a desired enrichment of ¹³C in the product. This also ensures a higher quantity of enriched product because of the higher reaction volume. The advantage of the LMPC over the conventionally used Herriott multi-pass cell has also been presented. The gain in reaction volume in the present optical cavity having 20 passes with a constant fluence in each pass is as high as 12. Isotope-selective MPD of Freon in a LMPC with constant fluence in each pass showed a distinct advantage in energy utilization to separate ¹³C isotope over the gradually reducing fluence case.This revised version was published online in August 2005 with a corrected cover date.     

On-line computer controlled cw dye laser spectrometer for laser isotope separation

An on-line cw dye laser multichannel spectrometer is described, which can be controlled by FORTRAN. Automatic tuning of a dye laser to the wavelength of maximum excitation selectivity for photochemical isotope separation is achieved. Applying the system to the selective photoaddition of iodine chloride ICl to acetylene, an enrichment factor of³⁷Cl in the photoproduct C₂H₂ICl of β=100±5 was obtained. Both stable chlorine isotopes can be enriched to more than 97% purity in a single step, starting from natural samples in both cases.