Equilibrium Correlation Functions Research Articles

Quantum correlation functions through tensor network path integral.

Tensor networks have historically proven to be of great utility in providing compressed representations of wave functions that can be used for the calculation of eigenstates. Recently, it has been shown that a variety of these networks can be leveraged to make real time non-equilibrium simulations of dynamics involving the Feynman-Vernon influence functional more efficient. In this work, a tensor network is developed for non-perturbatively calculating the equilibrium correlation function for open quantum systems using the path integral methodology. These correlation functions are of fundamental importance in calculations of rates of reactions, simulations of response functions and susceptibilities, spectra of systems, etc. The influence of the solvent on the quantum system is incorporated through an influence functional, whose unconventional structure motivates the design of a new optimal matrix product-like operator that can be applied to the so-called path amplitude matrix product state. This complex-time tensor network path integral approach provides an exceptionally efficient representation of the path integral, enabling simulations for larger systems strongly interacting with baths and at lower temperatures out to longer time. The derivation, design, and implementation of this method are discussed along with a wide range of illustrations ranging from rate theory and symmetrized spin correlation functions to simulation of response of the Fenna-Matthews-Olson complex to light.

Active and passive microrheology with large tracers in hard colloids.

The dynamics of a tracer particle in a bath of quasi-hard colloidal spheres is studied by Langevin dynamics simulations and mode coupling theory (MCT); the tracer radius is varied from equal to up to seven times larger than the bath particles radius. In the simulations, two cases are considered: freely diffusing tracer (passive microrheology) and tracer pulled with a constant force (active microrheology). Both cases are connected by linear response theory for all tracer sizes. It links both the stationary and transient regimes of the pulled tracer (for low forces) with the equilibrium correlation functions; the velocity of the pulled tracer and its displacement are obtained from the velocity auto-correlation function and the mean squared displacement, respectively. The MCT calculations give insight into the physical mechanisms: At short times, the tracer rattles in its cage of neighbours, with the frequency increasing linearly with the tracer radius asymptotically. The long-time tracer diffusion coefficient from passive microrheology, which agrees with the inverse friction coefficient from the active case, arises from the transport of transverse momentum around the tracer. It can be described with the Brinkman equation for the transverse flow field obtained in extension of MCT, but cannot be recovered from the MCT kernel coupling to densities only. The dynamics of the bath particles is also studied; for the unforced tracer the dynamics is unaffected. When the tracer is pulled, the velocity field in the bath follows the prediction of the Brinkman model, but different from the case of a Newtonian fluid.

Inertial dynamics and equilibrium correlation functions of magnetization at short times

The method of moments is developed and employed to analyze the equilibrium correlation functions of the magnetization of ferromagnetic nanoparticles in the case of inertial magnetization dynamics. The method is based on the Taylor series expansion of the correlation functions and the estimation of the expansion coefficients. This method significantly reduces the complexity of analysis of equilibrium correlation functions. Analytical expressions are derived for the first three coefficients for the longitudinal and transverse correlation functions for the uniaxial magnetocrystalline anisotropy of ferromagnetic nanoparticles with a longitudinal magnetic field. The limiting cases of very strong and negligibly weak external longitudinal fields are considered. The Gordon sum rule for inertial magnetization dynamics is discussed. In addition, we show that finite analytic series can be used as a simple and satisfactory approximation for the numerical calculation of correlation functions at short times.

Kinetic coefficient for ice–water interface from simulated non-equilibrium relaxation at coexistence

In the theory of solidification, the kinetic coefficient multiplies the local supercooling to give the solid-liquid interface velocity. The same coefficient should drive interface migration at the coexistence temperature in proportion to a curvature force. This work computes the ice-water kinetic coefficient from molecular simulations starting from a sinusoidal ice-water interface at the coexistence temperature. We apply this method to the basal and prismatic ice planes and compare results to previous estimates from equilibrium correlation functions and simulations at controlled supercooling.

Relativistic second-order dissipative hydrodynamics from Zubarev’s non-equilibrium statistical operator

We present a new derivation of relativistic second-order dissipative hydrodynamics for quantum systems using Zubarev’s non-equilibrium statistical-operator formalism. This is achieved by a systematic expansion of the energy–momentum tensor and the charge current to second order in deviations from equilibrium. As a concrete example, we obtain the relaxation equations for the shear-stress tensor, the bulk-viscous pressure, and the charge-diffusion currents required to close the set of equations of motion for relativistic second-order dissipative hydrodynamics. We also identify new transport coefficients which describe the relaxation of dissipative processes to second-order and express them in terms of equilibrium correlation functions, thus establishing new Kubo-type formulas for second-order transport coefficients.

Nonequilibrium Green-Kubo relations for hydrodynamic transport from an equilibrium-like fluctuation-response equality

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 prediction to substantiate linearized hydrodynamic transport equations that describe how spatial inhomogeneities in macroscopic nonequilibrium systems relax. As a consequence, we derive nonequilibrium Green-Kubo relations for the transport coefficients of two types of hydrodynamic variables: local conserved densities and broken-symmetry modes. A byproduct of this work is to provide a theoretical foundation for the validity of Onsager's regression hypothesis around nonequilibrium steady states. Our predictions are analytically and numerically corroborated for two model systems: density diffusion in a fluid of soft, spherical active Brownian particles and phase diffusion in the noisy Kuramoto model on a square lattice.

Dynamical conductivity of warm dense matter from correlation functions with account for interband transitions

Within the generalized linear response theory, the dynamical conductivity of charged particle systems is obtained from equilibrium correlation functions. Using the force–force correlation function approach, interband transitions in addition to phonon interaction and umklapp processes are taken into account for warm dense matter. For solid-density aluminum and copper plasmas, the results are shown for dynamical collision frequency, dynamical conductivity, and opacity as functions of laser frequency accounting for interband absorption. Calculated opacities for aluminum plasmas are compared with results of first-principles density functional theory–molecular dynamic (DFT-MD) simulations and recent experiments. The problem of underestimating the size of opacities by theoretical models in the vicinity of the L edge is discussed.

Revisiting the Mazur bound and the Suzuki equality

Among the few known rigorous results for time-dependent equilibrium correlations, important for understanding transport properties, are the Mazur bound and the Suzuki equality. The Mazur inequality gives a lower bound, on the long-time average of the time-dependent auto-correlation function of observables, in terms of equilibrium correlation functions involving conserved quantities. On the other hand, Suzuki proposes an exact equality for quantum systems. In this paper, we discuss the relation between the two results and in particular, look for the analogue of the Suzuki result for classical systems. This requires us to examine as to what constitutes a complete set of conserved quantities required to saturate the Mazur bound. We present analytic arguments as well as illustrative numerical results from a number of different systems. Our examples include systems with few degrees of freedom as well as many-particle integrable models, both free and interacting.

Fluctuation-dissipation relations far from equilibrium: a case study.

Fluctuation–dissipation relations or “theorems” (FDTs) are fundamental for statistical physics and can be rigorously derived for equilibrium systems. Their applicability to non-equilibrium systems is, however, debated. Here, we simulate an active microrheology experiment, in which a spherical colloid is pulled with a constant external force through a fluid, creating near-equilibrium and far-from-equilibrium systems. We characterize the structural and dynamical properties of these systems, and reconstruct an effective generalized Langevin equation (GLE) for the colloid dynamics. Specifically, we test the validity of two FDTs: The first FDT relates the non-equilibrium response of a system to equilibrium correlation functions, and the second FDT relates the memory friction kernel in the GLE to the stochastic force. We find that the validity of the first FDT depends strongly on the strength of the external driving: it is fulfilled close to equilibrium and breaks down far from it. In contrast, we observe that the second FDT is always fulfilled. We provide a mathematical argument why this generally holds for memory kernels reconstructed from a deterministic Volterra equation for correlation functions, even for non-stationary non-equilibrium systems. Motivated by the Mori–Zwanzig formalism, we therefore suggest to impose an orthogonality constraint on the stochastic force, which is in fact equivalent to the validity of this Volterra equation. Such GLEs automatically satisfy the second FDT and are unique, which is desirable when using GLEs for coarse-grained modeling.

Realization of the Landau definitions of effective Hamiltonian and nonequilibrium free energy in microscopic theory

Equilibrium fluctuations of some set of parameters in the states described by the canonical Gibbs distribution are investigated. In the theory of phase transitions of the second kind, these parameters are components of the order parameter. The microscopic realization of the Landau definition of the effective Hamiltonian of the system for studying the equilibrium fluctuations of the specified system of parameters is discussed in the terms of the probability density of their values. A general formula for this function is obtained and it is expressed through the equilibrium correlation functions of these parameters. An expression for the effective Hamiltonian in terms of deviations of the parameters from their equilibrium values is obtained. The deviations are considered small for conducting the calculations. The possibility of calculating the exact free energy of the system using the found effective Hamiltonian is discussed.
 In the microscopic theory, the implementation of the Landau definition of nonequilibrium thermodynamic potentials introduced in his phenomenological theory of phase transitions of the second kind is investigated. Nonequilibrium states of a fluctuating system described with some sets of parameters are considered. A general formula for nonequilibrium free energy expressed through the correlation functions of these parameters is obtained as for the effective Hamiltonian above. Like the previous case, the free energy expression via parameter deviations from the equilibrium values is obtained and small deviations are considered for calculations. The idea of the identity of the effective Hamiltonian of the system and its nonequilibrium free energy is discussed in connection with the Boltzmann distribution. The Gaussian approximation of both developed formalisms is considered.
 A generalization of the constructed theory for the case of spatially inhomogeneous states and the study of long-wave fluctuations are developed.

Density dynamics in the mass-imbalanced Hubbard chain

We consider two mutually interacting fermionic particle species on a one-dimensional lattice and study how the mass ratio $\eta$ between the two species affects the (equilibration) dynamics of the particles. Focussing on the regime of strong interactions and high temperatures, two well-studied points of reference are given by (i) the case of equal masses ${\eta = 1}$, i.e., the standard Fermi-Hubbard chain, where initial non-equilibrium density distributions are known to decay, and (ii) the case of one particle species being infinitely heavy, ${\eta = 0}$, leading to a localization of the lighter particles in an effective disorder potential. Given these two opposing cases, the dynamics in the case of intermediate mass ratios ${0 < \eta < 1}$ is of particular interest. To this end, we study the real-time dynamics of pure states featuring a sharp initial non-equilibrium density profile. Relying on the concept of dynamical quantum typicality, the resulting non-equilibrium dynamics can be related to equilibrium correlation functions. Summarizing our main results, we observe that diffusive transport occurs for moderate values of the mass imbalance, and manifests itself in a Gaussian spreading of real-space density profiles and an exponential decay of density modes in momentum space. For stronger imbalances, we provide evidence that transport becomes anomalous on intermediate time scales and, in particular, our results are consistent with the absence of strict localization in the long-time limit for any ${\eta > 0}$. Based on our numerical analysis, we provide an estimate for the "lifetime" of the effective localization as a function of $\eta$.

Selected applications of typicality to real-time dynamics of quantum many-body systems

Abstract Loosely speaking, the concept of quantum typicality refers to the fact that a single pure state can imitate the full statistical ensemble. This fact has given rise to a rather simple but remarkably useful numerical approach to simulate the dynamics of quantum many-body systems, called dynamical quantum typicality (DQT). In this paper, we give a brief overview of selected applications of DQT, where particular emphasis is given to questions on transport and thermalization in low-dimensional lattice systems like chains or ladders of interacting spins or fermions. For these systems, we discuss that DQT provides an efficient means to obtain time-dependent equilibrium correlation functions for comparatively large Hilbert-space dimensions and long time scales, allowing the quantitative extraction of transport coefficients within the framework of, e. g., linear response theory (LRT). Furthermore, it is discussed that DQT can also be used to study the far-from-equilibrium dynamics resulting from sudden quench scenarios, where the initial state is a thermal Gibbs state of the pre-quench Hamiltonian. Eventually, we summarize a few combinations of DQT with other approaches such as numerical linked cluster expansions or projection operator techniques. In this way, we demonstrate the versatility of DQT.

All- and one-particle distribution functions at nonequilibrium steady state under thermal gradient.

We provide a concrete expression for the phase-space distribution function at nonequilibrium steady state under a constant thermal gradient, which is a typical system of the nonequilibrium molecular dynamics simulation of heat conduction. First, the phase-space distribution function of all particles in a local volume is formulated. Our formulation explicitly takes into account the entropy production due to the change in equilibrium thermodynamic variables in addition to the traditional entropy production described by the spatial gradients and fluxes of equilibrium thermodynamic variables. This treatment is necessary to explain the nonequilibrium response of a quantity that has no equilibrium correlation with mass and heat fluxes and is essential to correctly deduce one-particle distribution functions from the all-particle one. From the all-particle distribution function, we derive the Green-Kubo relations that express the one-particle distribution functions of density and velocity in terms of equilibrium correlation functions and verify these expressions using the molecular dynamics simulation of a Lennard-Jones liquid. These nonequilibrium one-particle distribution functions are sufficiently tractable for practical use, such as for the analytical evaluation of the nonequilibrium average of physical quantities.

Auxiliary master equation approach within stochastic wave functions: Application to the interacting resonant level model.

We present further developments of the auxiliary master equation approach (AMEA), a numerical method to simulate many-body quantum systems in as well as out of equilibrium and apply it to the interacting resonant level model to benchmark the new developments. In particular, our results are obtained by employing the stochastic wave functions method to solve the auxiliary open quantum system arising within AMEA. This development allows us to reach extremely low wall times for the calculation of correlation functions with respect to previous implementations of AMEA. An additional significant improvement is obtained by extrapolating a series of results obtained by increasing the number of auxiliary bath sites, N_{B}, used within the auxiliary open quantum system formally to the limit of N_{B}→∞. Results for the current-voltage characteristics and for equilibrium correlation functions are compared with the one obtained by exact and matrix-product states-based approaches. Further, we complement this benchmark by the presentation of spectral functions for higher temperatures where we find different behaviors around zero frequency depending on the hybridization strength.

Entanglement dynamics at flat surfaces: Investigations using multi-chain molecular dynamics and a single-chain slip-spring model.

The dynamics of an entangled polymer melt confined in a channel by parallel plates is investigated by Molecular Dynamics (MD) simulations of a detailed, multi-chain model. A primitive path analysis predicts that the density of entanglements remains approximately constant throughout the gap and drops to lower values only in the immediate vicinity of the surface. Based on these observations, we propose a coarse-grained, single-chain slip-spring model with a uniform density of slip-spring anchors and slip-links. The slip-spring model is compared to the Kremer-Grest MD bead-spring model via equilibrium correlation functions of chain orientations. Reasonably good agreement between the single-chain model and the detailed multi-chain model is obtained for chain relaxation dynamics, both away from the surface and for chains whose center of mass positions are at a distance from the surface that is less than the bulk chain radius of gyration, without introducing any additional model parameters. Our results suggest that there is no considerable drop in topological interactions for chains in the vicinity of a single flat surface. We infer from the slip-spring model that the experimental plateau modulus of a confined polymer melt may be different to a corresponding unconfined system even if there is no drop in topological interactions for the confined case.

Relation between far-from-equilibrium dynamics and equilibrium correlation functions for binary operators

Linear response theory (LRT) is one of the main approaches to the dynamics of quantum many-body systems. However, this approach has limitations and requires, e.g., that the initial state is (i) mixed and (ii) close to equilibrium. In this paper, we discuss these limitations and study the nonequilibrium dynamics for a certain class of properly prepared initial states. Specifically, we consider thermal states of the quantum system in the presence of an additional static force which, however, become nonequilibrium states when this static force is eventually removed. While for weak forces the relaxation dynamics is well captured by LRT, much less is known in the case of strong forces, i.e., initial states far away from equilibrium. Summarizing our main results, we unveil that, for high temperatures, the nonequilibrium dynamics of so-called binary operators is always generated by an equilibrium correlation function. In particular, this statement holds true for states in the far-from-equilibrium limit, i.e., outside the linear response regime. In addition, we confirm our analytical results by numerically studying the dynamics of local fermionic occupation numbers and local energy densities in the spin-1/2 Heisenberg chain. Remarkably, these simulations also provide evidence that our results qualitatively apply in a more general setting, e.g., in the anisotropic XXZ model where the local energy is a non-binary operator, as well as for a wider range of temperature. Furthermore, exploiting the concept of quantum typicality, all of our findings are not restricted to mixed states, but are valid for pure initial states as well.

Landau effective Hamiltonian and its application to magnetic systems

The Landau definition of the effective Hamiltonian (of the nonequilibrium free energy) is realized in a microscopic theory. According to Landau remark, the consideration is based on classical statistical mechanics. In his approach nonequilibrium states coinciding with equilibrium fluctuations are taken into account (the Onsager principle). The definition leads to the exact fulfillment of the Boltzmann principle written in the form with the complete free energy. The considered system is assumed to consist of two subsystems. The first subsystem is an equilibrium one. The second subsystem is a nonequilibrium one and its state is described by quantities that are considered as order parameters. The effective Hamiltonian is calculated near equilibrium in the form of a series in powers of deviations of the order parameters from their equilibrium values. The coefficients of the series are expressed through equilibrium correlation functions of the order parameters. In the final approximation correlations of six and more order parameters are neglected and correlations of four parameters are assumed to be small that leads to the corresponding perturbation theory. The developed theory is compared with the phenomenological Landau theory of phase transitions of the second kind. The obtained results are concretized for paramagnetic-ferromagnetic system. The consideration is restricted by paramagnetic phase.

Kubo formulas for thermodynamic transport coefficients

Uncharged relativistic fluids in 3+1 dimensions have three independent thermodynamic transport coefficients at second order in the derivative expansion. Fluids with a single global U(1) current have nine, out of which seven are parity preserving. We derive the Kubo formulas for all nine thermodynamic transport coefficients in terms of equilibrium correlation functions of the energy-momentum tensor and the current. All parity-preserving coefficients can be expressed in terms of two-point functions in flat space without external sources, while the parity-violating coefficients require three-point functions. We use the Kubo formulas to compute the thermodynamic coefficients in several examples of free field theories.

Relativistic Dissipative Fluid Dynamics from the Non-Equilibrium Statistical Operator

We present a new derivation of second-order relativistic dissipative fluid dynamics for quantum systems using Zubarev’s formalism for the non-equilibrium statistical operator. In particular, we discuss the shear-stress tensor to second order in gradients and argue that the relaxation terms for the dissipative quantities arise from memory effects contained in the statistical operator. We also identify new transport coefficients which describe the relaxation of dissipative processes to second order and express them in terms of equilibrium correlation functions, thus establishing Kubo-type formulae for the second-order transport coefficients.

Energy Current Cumulants in One-Dimensional Systems in Equilibrium.

A recent theory based on fluctuating hydrodynamics predicts that one-dimensional interacting systems with particle, momentum, and energy conservation exhibit anomalous transport that falls into two main universality classes. The classification is based on behavior of equilibrium dynamical correlations of the conserved quantities. One class is characterized by sound modes with Kardar-Parisi-Zhang scaling, while the second class has diffusive sound modes. The heat mode follows Lévy statistics, with different exponents for the two classes. Here we consider heat current fluctuations in two specific systems, which are expected to be in the above two universality classes, namely, a hard particle gas with Hamiltonian dynamics and a harmonic chain with momentum conserving stochastic dynamics. Numerical simulations show completely different system-size dependence of current cumulants in these two systems. We explain this numerical observation using a phenomenological model of Lévy walkers with inputs from fluctuating hydrodynamics. This consistently explains the system-size dependence of heat current fluctuations. For the latter system, we derive the cumulant-generating function from a more microscopic theory, which also gives the same system-size dependence of cumulants.