We obtain an exact Green-Kubo type linear response result for the heat current in an open system. The result is derived for classical Hamiltonian systems coupled to heat baths. Both lattice models and fluid systems are studied and several commonly used implementations of heat baths, stochastic as well as deterministic, are considered. The results are valid in arbitrary dimensions and for any system sizes. Our results are useful for obtaining the linear response transport properties of mesoscopic systems. Also we point out that for systems with anomalous heat transport, as is the case in low-dimensional systems, the use of the standard Green-Kubo formula is problematic and the open system formula should be used.
Currently, the most common method to calculate transport properties for materials under extreme conditions is based on the phenomenological Kubo-Greenwood method. The results of an inquiry into the justification and context of that model are summarized here. Specifically, the basis for its connection to equilibrium DFT and the assumption of static ions are discussed briefly.
We show that vertex corrections to the quasi-harmonic Green-Kubo theory of heat transport in insulators naturally lead to a generalisation of the expression for the conductivity that could be derived from the linearized Boltzmann equation, when the effects of the full scattering matrix are accounted for. Our results, which are obtained from the Mori-Zwanzig memory-function formalism, provide a fully ab initio derivation of the linearized Boltzmann transport equation and establish a connection between two recently proposed unified approaches to heat transport in insulating crystals and glasses.
We study the friction coefficient of a macroscopic sphere in a viscous fluid at low Reynolds number. First, Kirkwood's formula for the friction coefficient is reviewed on the basis of the Hamiltonian description of particle systems. According to this formula, the friction coefficient is expressed in terms of the stress correlation on the surface of the macroscopic sphere. Then, with the aid of large deviation theory, we relate the surface stress correlation to the stress correlation in the bulk of the fluid, where the latter is characterized by the viscosity in the Green-Kubo formula. By combi…
Fluctuation relations without microscopic time reversality: Generalized Green-Kubo relation and integral fluctuation theorem for uniformly sheared granular systems
Near equilibrium, Green-Kubo relations provide microscopic expressions for macroscopic transport coefficients in terms of equilibrium correlation functions. At their core, they are based on the intimate relationship between response and fluctuations as embodied by the equilibrium fluctuation-dissipation theorem, a connection generically broken far from equilibrium. In this work, we identify a class of perturbations whose response around far-from-equilibrium steady states is linked to steady-state correlation functions via an equilibrium-like fluctuation-response equality. We then utilize this …
Active fluids, which are driven at the microscale by non-conservative forces, are known to exhibit novel transport phenomena due to the breaking of time reversal symmetry. Recently, Epstein and Mandadapu [arXiv:1907.10041] obtained Green-Kubo relations for the full set of viscous coefficients governing isotropic chiral active fluids, including the so-called odd viscosity, invoking Onsager's regression hypothesis for the decay of fluctuations in active non-equilibrium steady states. In this Communication, we test these Green-Kubo relations using molecular dynamics simulations of a canonical mod…
We have developed a Green-Kubo relation that enables accurate calculations of friction at solid-liquid interfaces directly from equilibrium molecular dynamics (MD) simulations and that provides a pathway to bypass the time-scale limitations of typical nonequilibrium MD simulations. The theory has been validated for a number of different interfaces and it is demonstrated that the liquid-solid slip is an intrinsic property of an interface. Because of the high numerical efficiency of our method, it can be used in the design of interfaces for applications in aqueous environments, such as nano- and…
By combining confocal microscopy and Stress Assessment from Local Structural Anisotropy (SALSA), we directly measure stresses in 3D quiescent colloidal liquids. Our non-invasive and non-perturbative method allows us to measure forces $\lesssim$ 50 fN with a small and tunable probing volume, enabling us to resolve the stress fluctuations arising from particle thermal motions. We use the Green-Kubo relation to relate these measured stress fluctuations to the bulk Brownian viscosity at different volume fractions and comparing against simulations and conventional rheometry measurements. We demonst…
In recent years it was shown both theoretically and experimentally that in certain systems exhibiting anomalous diffusion the time and ensemble average mean squared displacement are remarkably different. The ensemble average diffusivity is obtained from a scaling Green-Kubo relation, which connects the scale invariant non-stationary velocity correlation function with the transport coefficient. Here we obtain the relation between time averaged diffusivity, usually recorded in single particle tracking experiments, and the underlying scale invariant velocity correlation function. The time average…
The Green-Kubo theory of thermal transport has long be considered incompatible with modern simulation methods based on electronic-structure theory, because it is based on such concepts as energy density and current, which are ill-defined at the quantum-mechanical level. Besides, experience with classical simulations indicates that the estimate of heat-transport coefficients requires analysing molecular trajectories that are more than one order of magnitude longer than deemed feasible using ab initio molecular dynamics. In this paper we report on recent theoretical advances that are allowing on…
We address the question of whether transport coefficients obtained from a unitary closed system setting, i.e., the standard equilibrium Green-Kubo formula, are the same as the ones obtained from a weakly driven nonequilibrium steady-state calculation. We first derive a nonequilibrium Kubo-like expression for the steady-state diffusion constant expressed as a time-integral of either a current or a conserved density nonequilibrium correlation function. This expression has certain advantages over the equilibrium Green-Kubo formula, but is not clear if it gives the same value of the diffusion cons…
The closely related Green-Kubo and Helfand moment approaches are applied to obtain the thermal conductivity tensor of $β$-1,3,5,7-tetranitro-1,3,5,7-tetrazoctane ($β$-HMX) at $T=300$ K and $P=1$ atm from equilibrium molecular dynamics (MD) simulations. Direct application of the Green-Kubo formula exhibits slow convergence of the integrated thermal conductivity values even for long (120 ns) simulation times. To partially mitigate this slow convergence we developed a numerical procedure that involves filtering of the MD-calculated heat current. The filtering is accomplished by physically justifi…
Nature of energy transport around a critical point is studied in the Creutz cellular automaton. Fourier heat law is confirmed to hold in this model by a direct measurement of heat flow under a temperature gradient. The thermal conductivity is carefully investigated near the phase transition by the use of the Kubo formula. As the result, the thermal conductivity is found to take a finite value at the critical point contrary to some previous works. Equal-time correlation of the heat flow is also analyzed by a mean-field type approximation to investigate the temperature dependence of thermal cond…
Diffusive transport is characterized by a diffusivity tensor which may, in general, contain both a symmetric and an antisymmetric component. Although the latter is often neglected, we derive Green-Kubo relations showing it to be a general characteristic of random motion breaking time-reversal and parity symmetries, as encountered in chiral active matter. In analogy with the odd viscosity appearing in chiral active fluids, we term this component the odd diffusivity. We show how odd diffusivity emerges in a chiral random walk model, and demonstrate the applicability of the Green-Kubo relations t…
Recent studies have revealed that the symmetry of interparticle potential plays an important role in one-dimensional heat conduction problem. Here we demonstrate that by stretching or compressing the Fermi-Pasta-Ulam-\b{eta} lattice, one can control the symmetry of the potential, and thus manipulate the decaying behavior of the heat current autocorrelation function (HCAF). In fact, stretching or compressing induces a fast decaying stage (FDS) during which the HCAF decays faster than power-law manners or in a power law manner but faster than ~t -1. The time range as well as the decay amplitude …
We provide a stochastic fractional diffusion equation description of energy transport through a finite one-dimensional chain of harmonic oscillators with stochastic momentum exchange and connected to Langevian type heat baths at the boundaries. By establishing an unambiguous finite domain representation of the associated fractional operator, we show that this equation can correctly reproduce equilibrium properties like Green-Kubo formula as well as non-equilibrium properties like the steady state temperature and current. In addition, this equation provides the exact time evolution of the tempe…
The standard equilibrium Green-Kubo and nonequilibrium molecular dynamics (MD) methods for computing thermal transport coefficients in solids typically require relatively long simulation times and large system sizes. To this end, we revisit here the homogeneous nonequilibrium MD method by Evans [Phys. Lett. A \textbf{91}, 457 (1982)] and generalize it to many-body potentials that are required for more realistic materials modeling. We also propose a method for obtaining spectral conductivity and phonon mean free path from the simulation data. This spectral decomposition method does not require …
In the hydrodynamic regime, the evolution of a stochastic lattice gas with symmetric hopping rules is described by a diffusion equation with density-dependent diffusion coefficient encapsulating all microscopic details of the dynamics. This diffusion coefficient is, in principle, determined by a Green-Kubo formula. In practice, even when the equilibrium properties of a lattice gas are analytically known, the diffusion coefficient cannot be computed except when a lattice gas additionally satisfies the gradient condition. We develop a procedure to systematically obtain analytical approximations …
