Front Propagation Dynamics with Exponentially-Distributed Hopping

We study reaction-diffusion systems where diffusion is by jumps whose sizes are distributed exponentially. We first study the Fisher-like problem of propagation of a front into an unstable state, as typified by the A+B → 2A reaction. We find that the effect of fluctuations is especially pronounced at small hopping rates. Fluctuations are treated heuristically via a density cutoff in the reaction rate. We then consider the case of propagating up a reaction rate gradient. The effect of fluctuations here is pronounced, with the front velocity increasing without limit with increasing bulk particle density. The rate of increase is faster than in the case of a reaction-gradient with nearest-neighbor hopping. We derive analytic expressions for the front velocity dependence on bulk particle density. Computer simulations are performed to confirm the analytical results.     

Surface diffusion of Cr adatoms on Au(111) by quantum tunneling

The low-temperature surface diffusion of isolated Cr adatoms on Au(111) has been determined using nonperturbing x rays. Changes in the x-ray magnetic circular dichroism spectral line shape together with Monte Carlo calculations demonstrate that adatom nucleation proceeds via quantum tunneling diffusion rather than over-barrier hopping for temperatures <40K. The jump rates are shown to be as much as 35 orders of magnitude higher than that expected for thermal over-barrier hopping at 10 K.     

Quantum diffusion of a light particle in the Meissner phase of a superconductor

The influence of a superconducting fermionic environment on quantum diffusion is investigated. Within the framework of a two-state model hopping rates are calculated both for the biased and unbiased case. As for the latter, the jump frequency shows towards lower temperatures an exponential increase caused by the dyingout of quasiparticle excitations. The calculated rates show a much stronger sensitivity on bias than in the normal state. For small bias (compared to the energy gap) they behave non-monotonically: below a certain temperature an exponential decrease is found which leads to a localization of the particle. For large bias the hopping rates are not substantially changed by the onset of superconductivity.     

Influence of interactions on the hopping conductivity of classical particles

We study interaction effects in ionic conductors within Kawasaki's kinetic Ising model. The hopping rates are related to properties of the interaction potential. Numerical results from a continued fraction expansion are presented for a one-dimensional chain. They show that the dynamic conductivity depends considerably on the choice of the rates.     

异质原子在Cu（001）表面扩散的分子动力学模拟

采用分子动力学方法模拟单个增原子Ag,Pd和Cu在Cu（001）表面上的扩散过程.通过对自扩散和异质扩散过程中扩散机制的观察,统计三种不同的增原子在不同温度下的扩散频率,拟合给出扩散势垒和扩散频率的指前因子,并与扩散势垒的静力学计算结果进行比较.结果表明：在800 K以下时,三种增原子均以简单跳跃机制为主扩散,与衬底不互溶的Ag增原子的跳跃频率最大,与衬底互溶的Pd增原子的跳跃频率最小.同质增原子与异质增原子的扩散频率和温度的关系均较好地符合Arrhenius公式,由Arrhenius公式拟合给出的三种不同增原子的扩散势垒与表面结构和增原子表面结合能有关.Pd和Cu增原子从跳跃机制为主向交换机制为主的转换温度分别在825和937 K左右. 关键词： 表面扩散 分子动力学模拟     

Diffusion of particles on a heterogeneous surface: A case of adsorption-induced surface reconstruction

The influence of surface reconstruction on diffusion of particles adsorbed on the surface is investigated in the framework of symmetrical four-position model. The analytical expressions for free energy and diffusion coefficients are obtained assuming the lateral interaction between particles is negligibly small.The critical behavior of the system is described by the Ising spin model. The coverage dependencies of the tracer, jump and chemical diffusion coefficients are calculated for some representative temperatures. The dependencies show clearly strong influence of the surface reconstruction on the thermodynamic and kinetic phenomena: diffusion coefficients become anisotropic on the reconstructed surface. To check the analytical results we have used Monte Carlo simulations of the diffusion on this lattice.     

Kinetics of the diffusion of an impurity atom on a fcc(111) surface

An analytical study of the migration of an embedded impurity atom over a solid surface under the influence of the diffusion of vacancies is performed. The case of small surface coverages of both vacancies and impurity atoms is considered. It is shown that the realization of multiple collisions of a single impurity atom with vacancies imparts a Brownian character to its motion. At long times, the dependence of the mean square displacement on the time differs little from the linear, whereas the spatial density distribution is close to the Gaussian, features that makes it possible to introduce a diffusion coefficient. For the latter, an analytical expression is derived, which differs from the product of the diffusion coefficient of vacancies and their relative concentration only by a numerical factor. The dependence of the diffusion coefficient of an impurity atom on the ratio of the frequency of its jumps to the frequency of jumps of vacancies is analyzed. In the kinetic mode, when the frequency of jump ω of the imurity atom is small, the diffusion coefficient of the impurity depends linearly on ω, whereas in the opposite case, a saturation occur and its dependence on the frequency of jumps of the impurity atom disappears.     

Diffusion of particles over triangular inhomogeneous lattice with two non-equivalent sites

We investigate the diffusion of particles adsorbed on a triangular lattice with deep and shallow sites. It is shown that the character of the particle migration depends substantially on the relative jump rates from the deep and shallow sites. The site inhomogeneity imposes specific correlation betweeen successive jumps: particles perform pairs of slow and fast jumps. General analytical expressions have been derived for the chemical and jump diffusion coefficients. We have calculated coverage dependencies of the diffusion coefficients and some thermodynamic quantities for different lateral interactions between the particles. The analytical data have been compared with the numerical data obtained by kinetic Monte Carlo simulations. The agreement between the results obtained by these quite different approaches is found to be very satisfactory.     

Mott Law as Lower Bound for a Random Walk in a Random Environment

We consider a random walk on the support of an ergodic stationary simple point process on ℝ^d, d≥2, which satisfies a mixing condition w.r.t. the translations or has a strictly positive density uniformly on large enough cubes. Furthermore the point process is furnished with independent random bounded energy marks. The transition rates of the random walk decay exponentially in the jump distances and depend on the energies through a factor of the Boltzmann-type. This is an effective model for the phonon-induced hopping of electrons in disordered solids within the regime of strong Anderson localization. We show that the rescaled random walk converges to a Brownian motion whose diffusion coefficient is bounded below by Mott's law for the variable range hopping conductivity at zero frequency. The proof of the lower bound involves estimates for the supercritical regime of an associated site percolation problem.     

On thermal diffusion of nanoparticles in gases

Thermal diffusion of nanoparticles in gases is studied with the help of the kinetic theory and using the nanoparticle-molecule interaction potential developed earlier by the authors. The dependence of the thermal diffusion coefficient of nanoparticles on their radius, volume concentration, and the temperature of carrier gas is analyzed. The results are compared with the data for gas mixtures.     

Phonon-assisted transition rates I. Optical-phonon-assisted hopping in solids

An extensive calculation of the optical-phonon-assisted transition rates for non-adiabatic electronic hopping motion in a solid is presented. Holstein's Molecular Crystal Model is used as a basis for study and the computation involves no restrictions on either the magnitude of the electron-lattice coupling strength, the temperature, or the difference between the electronic energies of the initial and final sites.

In the strong-coupling small-polaron régime, the jump rates, associated d.c. conductivity, a.c. conductivity, and electric-field dependence of the d.c. conductivity, for a crystal are all calculated. These transport properties manifest qualitatively distinct behaviours corresponding to whether the temperature is above or well below the optical-phonon temperature. In the low-temperature régime the energy-conserving processes which involve the absorption of the minimum amount of vibrational energy provide the dominant contribution to the thermally activated jump rates. At sufficiently high temperatures multiphonon processes dominate the transition rate; the high-temperature jump rates are also activated, albeit with a different activation energy than that which characterizes the low-temperature régime.

In the complementary weak-coupling régime, the jump rate is characterized by the dominance of those processes which involve the absorption or emission of the minimum number of phonons consistent with the requirements of energy conservation. Once again two distinct temperature domains manifest themselves: a low-temperature, thermally activated, régime and a high-temperature non-activated régime.

Finally, it is shown that, while optical-phonon-assisted transition rates are well defined for a three-dimensional model, divergences will occur for a linear chain (at ω = 0) and for a planar model (at the optical phonon frequency).

The calculations in this article bring together many of the results previously obtained for special cases into a single framework and reveal a number of new considerations. The article is the first of two, the second dealing with acoustic-phonon-assisted hopping.     

Diffusion of particles over strongly anisotropic surface with traps

We investigate surface diffusion in a system of particles adsorbed on a two-dimensional strongly anisotropic lattice. There are two kinds of the lattice sites - ordinary sites and deep traps. Particles adsorbed in the ordinary sites can migrate over the surface, but particles adsorbed in traps are immobile. These particles do not move over the surface and they obstacle also the mobile particles migration (surface defects). Using kinetic Monte Carlo simulations we obtained coverage dependencies of the tracer, jump, and chemical diffusion coefficients. The coefficients are rather sensitive to the defect concentration. Even small admixture of the defects decreases drastically the fast diffusion. The effect is rather specific: strong dependence of the pre-exponential factor on the defect concentration and almost independent activation energy. The defect influence on the slow diffusion is weak. It results in strong decreasing of the surface diffusion anisotropy with the defect concentration. Such unusual behavior of the diffusion coefficients was observed in many experimental investigations of the surface diffusion of lithium, cesium, potassium, and strontium over strongly anisotropic W(1 1 2) and Mo(1 1 2) planes. It was shown that this specific behavior arises exclusively due to the surface anisotropy, and does not depend on the lateral interaction between the particles.     

Indirect RKKY interaction in doped armchair nanotube due to electron phonon interaction effects

We study the Ruderman-Kittle-Kasuya-Yosida (RKKY) interaction in doped armchair nanotube in the presence of gap parameter. The effects of both next nearest neighbor hopping parameter and electron-Holstein phonon on RKKY interaction have been addressed. RKKY interaction as a function of distance between localized moments have been analyzed. In order to calculate the exchange interaction along arbitrary direction between two magnetic moments, we should obtain the transverse static spin susceptibility of armchair graphene nanoribbon in the presence of electron-phonon coupling and gap parameter. The spin susceptibility components are calculated using Green’s function approach for Holstein model Hamiltonian. The effects of electron doping on dependence of exchange interaction on distance between moments are investigated via calculating correlation function of spin density operators. Our results show the influences of next nearest neighbor hopping parameter on the spatial behavior of RKKY interactions are different in the presence of electron phonon coupling.     

THE APPLICATIONS OF NUCLEAR SPIN RELAXATION TO POLYMER DYNAMICS AND INTERMOLECULAR INTERACTIONS

The correlation functions of the side - groups and side ?chains of polymers are obtained for nuclear spin relaxation if the segmental motion of the polymers is described by VJGM model, these functions are derived from unequal two ?side and three -site jump internal rotation, diffusion internal rotation, restricted internal rotation and multiple internal rotation. The corresponding spectral density functions are also given, and these functions are used to interpret the nuclear spin relaxation data of the side-groups of some polymers. The average spectral density functions of side-groups are derived under the magic angle spinning, the correlation times and diffusion coefficients of the side-groups of crosslinked poly (methyl methacry-latcs) and solid poly(vinylbutyral) are obtained by using these average spectral density functions. The multiphase structures of nylon 6, poly (ethylenc glycol) and its complexes are investigated with cross ?polarization and magic angle spinning techniques.Three methods using     

表面Cu原子间相互作用对Cu(001)表面跳跃扩散行为的影响

采用嵌入原子方法的原子间相互作用势，利用准静态分子动力学模拟研究了Cu原子在Cu(001)表面吸附所导致的基体晶格畸变以及对其附近的另一个吸附原子自扩散行为的影响.研究结果表明，吸附原子的存在可以导致多达10层的Cu基体晶格产生畸变.两个吸附原子所产生的晶格畸变应力场之间的相互作用，可以导致吸附原子运动活性的增加.通过比较同一路径上往返跳跃扩散势垒的差异发现，在原子间相互作用势的有效距离之外，两个吸附原子的扩散行为可以认为是存在晶格畸变应力场相互作用的两个独立吸附原子的扩散；在原子间相互作用势的有效距离之 关键词： 表面吸附原子 晶格畸变 表面二聚体 扩散     

Diffusion and correlation in a coherent representation

Using a Fock-space formalism for the Master equation and introducing the density operator we present an unified method to derive kinetic equations for hopping processes with and without exclusion on a lattice. The corresponding Liouvillians are written in terms of Fermi or Bose operators, respectively. Although the Liouvillians are different the averaged particle numbers obey the same diffusion equation. Differences appear in the correlation functions only. The Master equation can be transformed into a differential equation in a coherent state representation. Using the algebraic properties of Grassmann numbers we are able to find the exact statonary solution for diffusion with exclusion. The conductivity can be derived in the bosonic and the fermionic case. The results are in accordance with those obtained with different other methods.     

Velocity and diffusion constant of a periodic one-dimensional hopping model

The velocity and the diffusion constant are obtained for a periodic onedimensional hopping model of arbitrary periodN. These two quantities are expressed as explicit functions of all the hopping rates. The velocity and the diffusion constant of random systems are calculated by taking the limit N→Β. One finds by varying the distribution of hopping rates that the diffusion constant and the velocity are singular at different points. Lastly, several possible applications are proposed.     

Effect of electric field on diffusion in disordered materials

The effect of electric field on diffusion of charge carriers in disordered materials is studied by Monte Carlo computer simulations and analytical calculations. It is shown how an electric field enhances the diffusion coefficient in the hopping transport mode. The enhancement essentially depends on the temperature and on the energy scale of the disorder potential. It is shown that in one‐dimensional hopping the diffusion coefficient depends linearly on the electric field, while for hopping in three dimensions the dependence is quadratic.     

Reaction-diffusion processes in the “adsorbate-substrate” system

We obtain a chain of quantum kinetic reaction-diffusion-type equations for “adsorbate-substrate” system taking into account the coupling of a light particle with a metallic surface, the adsorbate surface diffusion by the tunnelling mechanism and the occurrence of bimolecular chemical reactions. We calculate the temperature dependence of the kinetic kernels related to the diffusion coefficients and the reaction rates. It is shown that one can alter the temperature dependence of the reaction rates by changing the “adsorbate-substrate” coupling. It is also shown that the mean field terms contribute to the activation energies of the reaction rates, while their contribution to the activation energies of the diffusion coefficients vanishes.     

The motion of light interstitials in metals: Recent experiments

Recent theoretical considerations suggest, that at low temperatures the transport properties of light interstitials in metals are dominated by the interaction with the conduction electrons. After briefly surveying the state of the theory, experimental examples for the low and high temperature cases are presented. We begin with the low T regime and display first neutron scattering experiments on H trapped at O-impurities in Nb where a coherent tunneling state is observed. Its dependence on temperature and its properties in normal and superconducting Nb are discussed. Thereafter muon diffusion results in Al are examined. In Al, muon diffusion is observed via diffusion limited trapping and local properties of the impurity as well as long range diffusion are playing a role. Using a large variety of impurities it was possible to evaluate the diffusion coefficient over a large T-range. Muon motion in Al at accessible temperatures falls entirely in the hopping regime and constitutes an example for the high T regime of the theory.