On the Brownian motion of a massive sphere suspended in a hard-sphere fluid. II. Molecular dynamics estimates of the friction coefficient

The friction coefficient exerted by a hard-sphere fluid on an infinitely massive Brownian sphere is calculated for several size ratios , where and are the diameters of the Brownian and fluid spheres, respectively. The exact microscopic expression derived in part I of this work from kinetic theory is transformed and shown to be proportional to the time integral of the autocorrelation function of the momentum transferred from the fluid to the Brownian sphere during instantaneous collisions. Three different methods are described to extract the friction coefficient from molecular dynamics simulations carried out onfinite systems. The three independent methods lead to estimates of which agree within statisticalerrors (typically 5%). The results are compared to the predictions of Enskog theory and of the hydrodynamic Stokes law. The former breaks down as the size ratio and/or the packing fraction of the fluid increase. Somewhat surprisingly, Stokes' law is found to hold withstick boundary conditions, in the range 1/4.5 explored in the present simulations, with a hydrodynamic diameterd=. The analysis of the moleuclar dynamics data on the basis of Stokes' law withslip boundary conditions is less conclusive, although the right trend is found as / increases.     

Bulk and shear viscosities of a polydisperse hard-sphere fluid

The bulk and shear viscosity expressions for a multicomponent hard-sphere mixture in the Enskog transport theory are generalized to the polydisperse limit. The effect of polydispersity is expressed in terms of correction factors to the monodisperse fluid results. These correction factors have been evaluated for both a log-normal size distribution with the mass-size relation of a power-law form and a log-normal mass distribution with fixed particle size, which is the continuous limit of isotopes.     

On the theory of Brownian motion. I. Interaction between Brownian particles

The molecular theory of the Brownian motion of heavy particles in a homogeneous solvent of light particles is extended to cover the case of interactions between the Brownian particles. This will have physical effects in the concentration dependence of the Brownian particle self-diffusion coefficient. A density expansion for the Brownian particle friction coefficient is derived, and an approximation permitting the first density correction to be calculated is suggested.This work, part of research supported by NSF Grant GP-8497, was done under the tenure of a National Science Foundation Senior Postdoctoral Fellowship, and of a sabbatical leave granted by the University of Oregon.     

周期场中非各态历经布朗运动

将自由状态下呈弹道扩散的非各态历经系统置于周期场中,进而将非各态历经布朗运动分为两类.第一类是阻尼核的Laplace变换的低频为零的系统,当温度远大于势垒高度时,系统平均能量的动能部分依赖粒子的初始速度分布;随温度降低,系统的各态历经性得到恢复.然后将第一类系统的稳定速度变量作为一个内部噪声,再去驱动一个自由布朗粒子,则阻尼核的Laplace变换在零频时为无穷大.结果发现,粒子扩散系数随温度的增加而趋于零,显示一种经典局域化特征,系统的渐进分布依赖于初始坐标分布.这是第二类非各态历经性运动,不能通过外加势而恢复. 关键词： 非各态历经 非Markov布朗运动 扩散系数 噪声谱     

On the theory of Brownian motion. II. Nonuniform systems

An equation of evolution for a heavy particle immersed in a solvent of lighter particles is derived for the case when the system suffers gradients of temperature composition, or velocity. The derivation unifies the theory by applying the same methods which have proved useful in the uniform case. The final equation contains some new terms due to concentration gradients in the solvent, and is applicable to the case when the heavy particles are present at finite concentration and interact with each other.This work, part of research supported by NSF Grant GP-8497, was done under the tenure of a National Science Foundation Senior Postdoctoral Fellowship and a sabbatical leave from the University of Oregon.     

Determination of the friction coefficient via the force autocorrelation function. A molecular dynamics investigation for a dense Lennard-Jones fluid

For a large region of dense fluid states of a Lennard-Jones system, we have calculated the friction coefficient by the force autocorrelation function of a Brownian-type particle by molecular dynamics (MD). The time integral over the force autocorrelation function showed an interesting behavior and the expected plateau value when the mass of the Brownian particle was chosen to be about a factor of 100 larger than the mass of the fluid particle. Sufficient agreement was found for the friction coefficient calculated by this way and that obtained by MD calculations of the self-diffusion coefficient using the common relation between these coefficients. Furthermore, a modified friction coefficient was determined by integration of the force autocorrelation function up to the first maximum. This coefficient can successfully be used to derive a reasonable soft part of the friction coefficient necessary for the Rice-Allnatt approximation for the shear viscosity of simple liquids.     

On the theory of brownian motion. III. Two-body distribution function

The equation of evolution governing the probability density of a pair of heavy particles in a fluid of lighter particles is derived. The derivation starts from the Liouville equation and proceeds by expansion in the ratio of light to heavy masses, using the technique previously applied successfully to the singlet distribution.This work is part of research supported by NSF Grant GP-8497.     

On the Brownian motion in a double-well potential in the overdamped limit

The Brownian motion of a particle in a double-well potential is considered and the position correlation function (excluding inertial effects) for the potential V(x)=ax²/2+bx⁴/4 is evaluated first by averaging the governing Langevin equation over its realizations. The exact solution is then obtained via matrix continued fractions by using a representation, which symmetrizes the recurrence relations for the observables generated by the averaging procedure leading to convergence of these recurrence relations unlike the previous approaches to the problem. A reliable approximate solution based on the exponential separation of the time scales of the fast intrawell and low overbarrier relaxation processes associated with the bistable potential is also given. It is shown that a knowledge of the three characteristic relaxation times (the integral, effective and the longest relaxation times) of the position correlation function allows one to accurately predict the relaxation behavior of the system in the overdamped limit for all time scales of interest.     

On the calculation of equilibrium time correlation functions in hard-sphere fluids

We discuss in detail techniques that have been used to determine single-particle equilibrium time correlation functions in a hard-sphere fluid on the basis of kinetic theory. The accuracy of various procedures is assessed.On leave from Interuniversitair Reactor Instituut, Delft, The Netherlands.     

Brownian motion and thermophoresis effects on unsteady stagnation point flow of Eyring-Powell nanofluid: a Galerkin approach

This article concerns the analysis of an unsteady stagnation point flow of Eyring-Powell nanofluid over a stretching sheet. The influence of thermophoresis and Brownian motion is also considered in transport equations. The nonlinear ODE set is obtained from the governing nonlinear equations via suitable transformations. The numerical experiments are performed using the Galerkin scheme. A tabular form comparison analysis of outcomes attained via the Galerkin approach and numerical scheme (RK-4) is available to show the credibility of the Galerkin method. The numerical exploration is carried out for various governing parameters, namely, Brownian motion, steadiness, thermophoresis, stretching ratio, velocity slip, concentration slip, thermal slip, and fluid parameters, and Hartmann, Prandtl and Schmidt numbers. The velocity of fluid enhances with an increase in fluid and magnetic parameters for the case of opposing, but the behavior is reversed for assisting cases. The Brownian motion and thermophoresis parameters cause an increase in temperature for both cases (assisting and opposing). The Brownian motion parameter provides a drop-in concentration while an increase is noticed for the thermophoresis parameter. All the outcomes and the behavior of emerging parameters are illustrated graphically. The comparison analysis and graphical plots endorse the appropriateness of the Galerkin method. It is concluded that said method could be extended to other problems of a complex nature.     

布朗运动理论及其在复杂气候系统研究中的应用

文章将从非平衡态统计物理发展和应用的角度,介绍德国科学家哈塞尔曼荣获2021年诺贝尔物理学奖的研究工作——基于布朗运动理论,建立了描述气象(天气)影响气候长期演化的随机气候学模型,并建立了寻求影响气候主因的最优指纹方法,从而能够分辨出人类活动和自然界局部改变对气候这一复杂系统的影响。哈塞尔曼的工作本质上是理论物理在实际复杂系统领域的成功应用,他采用的基础物理方法——布朗运动理论是我国杰出女物理学家王明贞和其导师乌伦贝克在20世纪40年代基于爱因斯坦的工作发展起来的^[1,2]。文章将介绍布朗运动理论的发展及其相关的非平衡统计物理思想的当代发展,以展示哈塞尔曼如何把相关的物理理论巧妙地用于气候长期预测的实际应用研究：(1)建立了快变的局部“气象”变量涨落通过耗散涨落关系影响缓变的整体气候变量的基础理论;(2)通过最优指纹方法,寻找局部“噪音”和外驱动力影响气候演化的关键要素。     

Brownian motion under a time-dependent periodic potential proportional to the square of the position of a particle and classical fluctuation squeezing

A general stationary case of a Brownian particle with a time-dependent periodic potential proportional to the square of the position of the particle is treated. Even though the vigorous change of the time-dependent proportionality coefficient is applied, there are cases where the fluctuation of the particle decreases in contrary to our intuition, which is called classical fluctuation squeezing. We obtain time-average variances analytically for general cases of an arbitrary change in the coefficient and find conditions favorable for classical fluctuation squeezing. We introduce an asymmetric function behaves like trigonometric cosine one and consider its behavior explicitly.     

On the derivation of Smoluchowski equations with corrections in the classical theory of Brownian motion

Differential equations governing the time evolution of distribution functions for Brownian motion in the full phase space were first derived independently by Klein and Kramers. From these so-called Fokker-Planck equations one may derive the reduced differential equations in coordinate space known as Smoluchowski equations. Many such derivations have previously been reported, but these either involved unnecessary assumptions or approximations, or were performed incompletely. We employ an iterative reduction scheme, free of assumptions, and calculate formally exact corrections to the Smoluchowski equations for many-particle systems with and without hydrodynamic interaction, and for a single particle in an external field. In the absence of hydrodynamic interaction, the lowest order corrections have been expressed explicitly in terms of the coordinate space distribution function. An additional application of the method is made to the reduction of the stress tensor used in evaluating the intrinsic viscosity of particles in solution. Most of the present work is based on classical Brownian motion theory, but brief consideration is given in an appendix to some recent developments regarding non-Markovian equations for Brownian motion.Supported by the National Science Foundation.     

Evaluation of the translational and rotational diffusion coefficients of a cubic particle (for the application to Brownian dynamics simulations)

By estimating the force and torque acting on the cube for the two cases of a uniform flow field and a rotational flow field, we have discussed whether or not there is a coupling between the translational and the rotational motion. From the characteristics of the friction coefficients, we may understand that there is no coupling between the translation motion and the rotational motion in the situation of the Reynolds number being sufficiently smaller than unity. In contrast, in the case of a non-slow flow field with the Reynolds number larger than unity, the coupling characteristics of the motion of a cube is certainly recognised and therefore the interaction with the ambient fluid is characterised by a variety of friction coefficients including friction coefficients that relate the forces acting on the cube to the angular velocities of the rotational motion. Hence, the employment of these translational and rotational diffusion coefficients for a cube enables the implementation of Brownian dynamics simulations for a suspension composed of cubic particles in order to analyse the dynamic characteristics of a cubic particle suspension.

Highlights

1. We have considered a flow problem around a cube in order to numerically clarify the characteristics of the translational and rotational friction or diffusion coefficients.

2. In a slow flow field the motion of the cube need only to be characterised by two friction coefficients, i.e. the translational and rotational friction coefficients.

3. In the case of a non-slow flow field, the coupling characteristics between the translational motion and the rotational motion are recognised.

4. Employment of these diffusion coefficients enables the implementation of Brownian dynamics simulations for a suspension composed of cubic particles.

     

Global existence in L1 for the Enskog equation and convergence of the solutions to solutions of the Boltzmann equation

For the Enskog equation in a box an existence theorem is proved for initial data with finite mass, energy, and entropy. Then, by letting the diameter of the molecules go to zero, the weak convergence of solutions of the Enskog equation to solutions of the Boltzmann equation is proved.     

Friction tensor for a pair of Brownian particles: Spurious finite-size effects and molecular dynamics estimates

In this work, we show thatin any finite system, the binary friction tensor for two Brownian particlescannot be directly estimated from an evaluation of the microscopic Green-Kubo formula, involving the time integral of force-force autocorrelation functions. This pitfall is associated with a subtle inversion of the thermodynamic and long-time limits and leads to spurious results for the estimates of the friction matrix based on molecular dynamics simulations. Starting from a careful analysis of the coupled Langevin equations for two interacting Brownian particles, we derive a method to circumvent these effects and extract the binary friction tensor from the correlation function matrix of the instantaneous forces exerted by the bath particles on the fixed Brownian particles, and from the relaxation of the total momentum of the bath in afinite system. The general methodology is applied to the case of two hard or soft Brownian spheres in a bath of light particles. Numerical estimates of the relevant correlation functions and of the resulting self and mutual components of the matrix of friction tensors are obtained by molecular dynamics simulations for various spacings between the Brownian particles. This paper is dedicated to B. Jancovici on the occassion of his 65th birthday.     

Diffusion coefficient for a Brownian particle in a periodic field of force: I. Large friction limit

The diffusion tensor for a Brownian particle in a periodic field of force is studied in the strong damping limit, in which the Smoluchowski equation is valid.A general relation between the diffusion tensor and the Smoluchowski “relaxation operator” is derived; the effect of the periodic force, at least in the simplest situation of diagonal and uniform friction, appears as a dressing of the bare particle mass to an effective tensor mass.From this the explicit form of the diffusion coefficient as a functional of the potential energy in the one-dimensional case is obtained, showing a temperature dependence which deviates at high temperatures from a simple Arrhenius behaviour.Finally, the expression for the mobility of the Brownian particle is derived, and by comparison with the expression for the diffusion coefficient the Einstein relation between diffusion and mobility is proved to be satisfied.