We solve numerically the equations of nonlinear fluctuating hydrodynamics (NFH) for the supercooled liquid. The time correlation of the density fluctuations in equilibrium obtained here shows quantitative agreement with molecular dynamics(MD) simulation data. We demonstrate numerically that the 1/rho nonlinearity in the NFH equations of motion is essential in restoring the ergodic behavior in the liquid. Under nonequilibrium conditions the time correlation functions relax in a manner similar to that observed in the molecular dynamics simulations in binary mixtures. The waiting time t_w dependence of the non-equilibrium response function follows a Modified Kohlrausch-Williams-Watts(MKWW) form similar to the behavior seen in dielectric relaxation data.
We generalize the mode-coupling theory of supercooled fluids to systems under stationary shear flow. Our starting point is the generalized fluctuating hydrodynamic equations with a convection term. The method is applied to a two dimensional colloidal suspension. The shear rate dependence of the intermediate scattering function and shear viscosity is analyzed. The results show a drastic reduction of the structural relaxation time due to shear and strong shear thinning behavior of the viscosity which are in qualitative agreement with recent simulations. The microscopic theory with minimal assump…
Despite its appeal, real and simulated glass forming systems do not undergo an ergodic-nonergodic (ENE) transition. We reconsider whether the fluctuating nonlinear hydrodynamics (FNH) model for this system, introduced by us in 1986, supports an ENE transition. Using nonperturbative arguments, with no reference to the hydrodynamic regime, we show that the FNH model does not support an ENE transition. Our results support the findings in the original paper. Assertions in the literature questioning the validity of the original work are shown to be in error.
We investigate hydrodynamic noise in a dilute granular gas during the homogeneous cooling state, by means of a proper application of the Direct Simulation Monte Carlo (DSMC) algorithm. The DSMC includes a source of randomization which is not present in Molecular Dynamics (MD) for inelastic hard disks. Notwithstanding this difference, a fair quantitative agreement is found, including a violation of the fluctuation-dissipation relation for the noise amplitude of the same order observed in MD. This study suggests that deterministic collision dynamics is not an essential ingredient to reproduce, u…
Nanoscale Protein Diffusion in Supercooled Cryoprotectant Solutions
Stockholm University（斯德哥尔摩大学）；Universität Tübingen（蒂宾根大学）；Universität Siegen（锡根大学）；TU Dortmund（多特蒙德工业大学）；The University of Osaka（大阪大学）；Institute for Molecular Science（分子科学研究所）；The Graduate University for Advanced Studies (SOKENDAI)（高级研究院）
Kinetic and hydrodynamic theories are widely employed for describing the collective behaviour of active matter systems. At the fluctuating level, these have been obtained from explicit coarse-graining procedures in the limit where each particle interacts weakly with many others, so that the total forces and torques exerted on each of them is of order unity at all times. Such limit is however not relevant for dilute systems that mostly interact via alignment; there, collisions are rare and make the self-propulsion direction to change abruptly. We derive a fluctuating kinetic theory, and the cor…
A field theoretical method for the fluctuating hydrodynamics with preserving fluctuation-dissipation relations (FDR) is reformulated. It is shown that the long time behavior within the first-loop order perturbation under the assumption that the correlations include the momentum decay fast enough, is equivalent to that for the standard mode-coupling theory.
We derive the fluctuating hydrodynamic equation for the number and momentum densities exactly from the underdamped Langevin equation. This derivation is an extension of the Kawasaki-Dean formula in underdamped case. The steady state probability distribution of the number and momentum densities field can be expressed by the kinetic and potential energies. In the massless limit, the obtained fluctuating hydrodynamic equation reduces to the Kawasaki-Dean equation. Moreover, the derived equation corresponds to the field equation derived from the canonical equation when the friction coefficient is …
Theory and simulation of Brownian colloids suspended in an implicit solvent, with the hydrodynamics of the fluid accounted for by effective interactions between the colloids, are shown to yield a marked and hitherto unobserved discrepancy between the viscosity calculated from the average shear stress under an imposed shear rate in the Stokesian regime and the viscosity extracted by the Green-Kubo formalism from the auto-correlations of thermal stress fluctuations in quiescent equilibrium. We show that agreement between both methods is recovered by accounting for the fluctuating Brownian stress…
We analyze the behavior of supercooled fluids under shear both theoretically and numerically. Theoretically, we generalize the mode-coupling theory of supercooled fluids to systems under stationary shear flow. Our starting point is the set of generalized fluctuating hydrodynamic equations with a convection term. A nonlinear integro-differential equation for the intermediate scattering function is constructed. This theory is applied to a two-dimensional colloidal suspension. The shear rate dependence of the intermediate scattering function and the shear viscosity is analyzed. We have also perfo…
Fluctuating hydrodynamics has been successfully combined with several computational methods to rapidly compute the correlated random velocities of Brownian particles. In the overdamped limit where both particle and fluid inertia are ignored, one must also account for a Brownian drift term in order to successfully update the particle positions. In this paper, we present an efficient computational method for the dynamic simulation of Brownian suspensions with fluctuating hydrodynamics that handles both computations and provides a similar approximation as Stokesian Dynamics for dilute and semidil…
We investigate hydrodynamic fluctuations in a 2D granular fluid excited by a vibrating base and in the presence of gravity, focusing on the transverse velocity modes. Since the system is inhomogeneous, we measure fluctuations in horizontal layers whose width is smaller than the characteristic hydrodynamic lengths: they can be considered as almost-homogeneous subsystems. The large time decay of autocorrelations of modes is exponential and compatible with vorticity diffusion due to shear viscosity, as in equilibrium fluids. The velocity structure factor, which strongly deviates from the equilibr…
The traction on the surface of a spherical active colloid in a thermally fluctuating Stokesian fluid contains passive, active, and Brownian contributions. Here we derive these three parts systematically, by "projecting out" the fluid using the boundary-domain integral representation of slow viscous flow. We find an exact relation between the statistics of the Brownian traction and the thermal forces in the fluid and derive, thereby, fluctuation-dissipation relations for every irreducible tensorial harmonic traction mode. The first two modes give the Brownian force and torque, from which we con…
We present a hybrid computational method for simulating the dynamics of macromolecules in solution which couples a mesoscale solver for the fluctuating hydrodynamics (FH) equations with molecular dynamics to describe the macromolecule. The two models interact through a dissipative Stokesian term first introduced by Ahlrichs and Dünweg [J. Chem. Phys. {\bf 111}, 8225 (1999)]. We show that our method correctly captures the static and dynamical properties of polymer chains as predicted by the Zimm model. In particular, we show that the static conformations are best described when the ratio $\frac…
The dynamics of a single fluid bilayer membrane in an external hydrodynamic flow field is considered. The deterministic equation of motion for the configuration is derived taking into account both viscous dissipation in the surrounding liquid and local incompressibility of the membrane. For quasi-spherical vesicles in shear flow, thermal fluctuations can be incorporated in a Langevin-type equation of motion for the deformation amplitudes. The solution to this equation shows an overdamped oscillatory approach to a stationary tanktreading shape. Inclination angle and ellipiticity of the contour …
Fluctuating entropy production is studied for a set of linearly coupled complex fields. The general result is applied to non-equilibrium fluctuating hydrodynamic equations for coarse-grained fields (density, temperature and velocity), in the framework of model granular fluids. We find that the average entropy production, obtained from the microscopic stochastic description, can be expressed in terms of macroscopic quantities, in analogy with linear non-equilibrium thermodynamics. We consider the specific cases of driven granular fluids with two different kinds of thermostat and the homogeneous…
Static and dynamical structure factors for shear and longitudinal modes of the velocity and density fields are computed for a granular system fluidized by a stochastic bath with friction. Analytical expressions are obtained through fluctuating hydrodynamics and are successfully compared with numerical simulations up to a volume fraction $\sim 50%$. Hydrodynamic noise is the sum of external noise due to the bath and internal one due to collisions. Only the latter is assumed to satisfy the fluctuation-dissipation relation with the average granular temperature. Static velocity structure factors $…
We propose a new formulation of the fluctuating lattice Boltzmann equation that is consistent with both equilibrium statististical mechanics and fluctuating hydrodynamics. The formalism is based on a generalized lattice-gas model, with each velocity direction occupied by many particles. We show that the most probable state of this model corresponds to the usual equilibrium distribution of the lattice Boltzmann equation. Thermal fluctuations about this equilibrium are controlled by the mean number of particles at a lattice site. Stochastic collision rules are described by a Monte Carlo process …
We present a numerical method that consistently implements thermal fluctuations and hydrodynamic interactions to the motion of Brownian particles dispersed in incompressible host fluids. In this method, the thermal fluctuations are introduced as random forces acting on the Brownian particles. The hydrodynamic interactions are introduced by directly resolving the fluid motions with the particle motion as a boundary condition to be satisfied. The validity of the method has been examined carefully by comparing the present numerical results with the fluctuation-dissipation theorem whose analytical…
We study the statistical properties of many Brownian particles under the We study the statistical properties of many Brownian particles under the influence of both a spatially homogeneous driving force and a periodic potential with period $\ell$ in a two-dimensional space. In particular, we focus on two asymptotic cases, $\ell_{\rm int} \ll \ell$ and $\ell_{\rm int} \gg \ell$, where $\ell_{\rm int}$ represents the interaction length between two particles. We derive fluctuating hydrodynamic equations describing the evolution of a coarse-grained density field defined on scales much larger than $…
The dynamics of the fragile glass-forming o-ter-phenyl is investigated by time-resolved transient grating experiment with an heterodyne detection technique in a wide temperature range. We investigated the dynamics processes of this glass-former over more then 6 decades in time with an excellent signal/noise. Acoustic, structural and thermal relaxations have been clearly identify and measured in a time-frequency window not covered by previous spectroscopic investigations. A detailed comparison with the density response function, calculated on the basis of generalized hydrodynamics model, has be…
Many coarse-grained models have been developed for equilibrium studies of lipid bilayer membranes. To achieve in simulations access to length-scales and time-scales difficult to attain in fully atomistic molecular dynamics, these coarse-grained models provide a reduced description of the molecular degrees of freedom and often remove entirely representation of the solvent degrees of freedom. In such implicit-solvent models the solvent contributions are treated through effective interaction terms within an effective potential for the free energy. For investigations of kinetics, Langevin dynamics…
The correlations of the fluctuating stress tensor are calculated in an equilibrium molecular-dynamics simulation of a Lennard--Jones liquid. We define a coarse-grained local stress tensor which can be calculated numerically and which allows for the first time to determine the stress correlation function both in time and in space. Our findings corroborate the assumptions made in fluctuating hydrodynamics as long as the liquid is isotropic, that is in bulk. In the vicinity of a rigid plate, however, the isotropy is restricted, and major modifications must be done with respect to the usual theory…
The mean-square displacement (MSD) is widely utilized to study the dynamical properties of stochastic processes. The time-averaged MSD (TAMSD) provides some information on the dynamics which cannot be extracted from the ensemble-averaged MSD. In particular, the relative standard deviation (RSD) of the TAMSD can be utilized to study the long time relaxation behavior. In this work, we consider a class of Langevin equations which are multiplicatively coupled to time-dependent and fluctuating diffusivities. Various interesting dynamics models such as entangled polymers and supercooled liquids can …
A recently introduced particle-based model for fluid dynamics with continuous velocities is generalized to model immiscible binary mixtures. Excluded volume interactions between the two components are modeled by stochastic multiparticle collisions which depend on the local velocities and densities. Momentum and energy are conserved locally, and entropically driven phase separation occurs for high collision rates. An explicit expression for the equation of state is derived, and the concentration dependence of the bulk free energy is shown to be the same as that of the Widom-Rowlinson model. Ana…
We derive a fluctuating lattice Boltzmann method for the diffusion equation. The derivation removes several shortcomings of previous derivations for fluctuating lattice Boltzmann methods for hydrodynamic systems. The comparative simplicity of this diffusive system highlights the basic features of this first exact derivation of a fluctuating lattice Boltzmann method.
We extend recent results on the exact hydrodynamics of a system of diffusive active particles displaying a motility-induced phase separation to account for typical fluctuations of the dynamical fields. By calculating correlation functions exactly in the homogeneous phase, we find that two macroscopic length scales develop in the system. The first is related to the diffusive length of the particles and the other to the collective behavior of the particles. The latter diverges as the critical point is approached. Our results show that the critical behavior of the model in one dimension belongs t…
We study diffusion of colloids on a fluid-fluid interface using particle simulations and fluctuating hydrodynamics. Diffusion on a two-dimensional interface with three-dimensional hydrodynamics is known to be anomalous, with the collective diffusion coefficient diverging like the inverse of the wavenumber. This unusual collective effect arises because of the compressibility of the fluid flow in the plane of the interface, and leads to a nonlinear nonlocal convolution term in the diffusion equation for the ensemble-averaged concentration. We extend the previous hydrodynamic theory to account fo…
Electrolyte solutions play an important role in energy storage devices, whose performance highly relies on the electrokinetic processes at sub-micron scales.\ Although fluctuations and stochastic features become more critical at small scales, the long-range Coulomb interactions pose a particular challenge for both theoretical analysis and simulation of fluid systems with fluctuating hydrodynamic and electrostatic interactions. Here, we present a theoretical framework based on the Landau-Lifshitz theory to derive closed-form expressions of fluctuation correlations in electrolyte solutions, indi…
We study the transport properties of dilute electrolyte solutions on the basis of the fluctuating hydrodynamic equation, which is a set of nonlinear Langevin equations for the ion densities and flow velocity. The nonlinearity of the Langevin equations generally leads to effective kinetic coefficients for the deterministic dynamics of the average ion densities and flow velocity; the effective coefficients generally differ from the counterparts in the Langevin equations and are frequency-dependent. Using the path-integral formalism involving auxiliary fields, we perform systematic perturbation c…
The random first order transition theory of the dynamics of supercooled liquids is extended to treat aging phenomena in nonequilibrium structural glasses. A reformulation of the idea of ``entropic droplets'' in terms of libraries of local energy landscapes is introduced which treats in a uniform way the supercooled liquid (reproducing earlier results) and glassy regimes. The resulting microscopic theory of aging makes contact with the Nayaranaswamy-Moynihan-Tool nonlinear relaxation formalism and the Hodge-Scherer extrapolation of the Adam-Gibbs formula, but deviations from both approaches are…
This paper describes the development and analysis of finite-volume methods for the Landau-Lifshitz Navier-Stokes (LLNS) equations and related stochastic partial differential equations in fluid dynamics. The LLNS equations incorporate thermal fluctuations into macroscopic hydrodynamics by the addition of white-noise fluxes whose magnitudes are set by a fluctuation-dissipation relation. Originally derived for equilibrium fluctuations, the LLNS equations have also been shown to be accurate for non-equilibrium systems. Previous studies of numerical methods for the LLNS equations focused primarily …
We analyze the Lattice Boltzmann method for the simulation of fluctuating hydrodynamics by Adhikari et al. [Europhys. Lett. 71, 473 (2005)] and find that it shows excellent agreement with theory even for small wavelengths as long as a stationary system is considered. This is in contrast to other finite difference and older lattice Boltzmann implementations that show convergence only in the limit of large wavelengths. In particular cross correlators vanish to less than 0.5%. For larger mean velocities, however, Galilean invariance violations manifest themselves through errors of a magnitude sim…
We apply microcanonical ensemble considerations to suggest that, whenever it may thermalize, a general disorder-free many-body Hamiltonian of a typical atomic system has solid-like eigenstates at low energies and fluid-type (and gaseous, plasma) eigenstates associated with energy densities exceeding those present in the melting (and, respectively, higher energy) transition(s). In particular, the lowest energy density at which the eigenstates of such a clean many body atomic system undergo a non-analytic change is that of the melting (or freezing) transition. We invoke this observation to analy…
