Nonequilibrium Steady State Research Articles

Lindblad dynamics from spatio-temporal correlation functions in nonintegrable spin- 1/2 chains with different boundary conditions

We investigate the Lindblad equation in the context of boundary-driven magnetization transport in spin-1/2 chains. Our central question is whether the nonequilibrium steady state of the open system, including its buildup in time, can be described on the basis of the dynamics in the closed system. To this end, we rely on a previous study [Heitmann , ], in which a description in terms of spatio-temporal correlation functions was suggested in the case of weak driving and small system-bath coupling. Because this work focused on integrable systems and periodic boundary conditions, we here extend the analysis in three directions: (1) We consider nonintegrable systems, (2) we take into account open boundary conditions and other bath-coupling geometries, and (3) we provide a comparison to time-evolving block decimation. While we find that nonintegrability plays a minor role, the choice of the specific boundary conditions can be crucial due to potentially nondecaying edge modes. Our large-scale numerical simulations suggest that a description based on closed-system correlation functions is a useful alternative to already existing state-of-the-art approaches. Published by the American Physical Society 2024

Tailoring bistability in optical tweezers with vortex beams and spherical aberration

We demonstrate a bistable optical trap by tightly focusing a vortex laser beam. The optical potential has the form of a Mexican hat with an additional minimum at the center. The bistable trapping corresponds to a nonequilibrium steady state, where the microsphere continually hops, due to thermal activation, between an axial equilibrium state and an orbital state driven by the optical torque. We develop a theoretical model for the optical force field, based entirely on experimentally accessible parameters, combining a Debye-type nonparaxial description of the focused vortex beam with Mie scattering by the microsphere. The theoretical prediction that the microsphere and the annular laser focal spot should have comparable sizes is confirmed experimentally by taking different values for the topological charge of the vortex beam. Spherical aberration introduced by refraction at the interface between the glass slide and the sample is considered and allows us to finetune between axial, bistable, and orbital states as the sample is shifted with respect to the objective focal plane. We find overall agreement between theory and experiment for a rather broad range of topological charges. Our results open the way for applications in stochastic thermodynamics, as they establish a control parameter—the height of the objective focal plane with respect to the glass slide—that allows us to shape the optical force field in real time and in a controllable way. Published by the American Physical Society 2024

Variance sum rule: proofs and solvable models

We derive, in more general conditions, a recently introduced variance sum rule (VSR) (Di Terlizzi et al 2024 Science 383 971) involving variances of displacement and force impulse for overdamped Langevin systems in a nonequilibrium steady state (NESS). This formula allows visualising the effect of nonequilibrium as a deviation of the sum of variances from normal diffusion 2Dt, with D the diffusion constant and t the time. From the VSR, we also derive formulas for the entropy production rate σ that, differently from previous results, involve second-order time derivatives of position correlation functions. This novel feature gives a criterion for discriminating strong nonequilibrium regimes without measuring forces. We then apply and discuss our results to three analytically solved models: a stochastic switching trap, a Brownian vortex, and a Brownian gyrator. Finally, we compare the advantages and limitations of known and novel formulas for σ in an overdamped NESS.

Modeling the Effect of Sulfur Composition in Dispersed Systems Involving Organosulfur Compounds

Background:: Organosulfur compounds within petroleum have far-reaching consequences for the refining industry, combustion of petroleum products, and environmental quality. They induce corrosion in refining equipment, hamper the efficient burning of petroleum products, and contribute to environmental degradation. In high-density asphalt crudes, these compounds are predominantly concentrated within asphaltenes. However, crude oils with extremely high sulfur content, may be distributed across the four constituent families defined by the SARA analysis of crude oil composition. These compounds, characterized by differing polarities, can trigger the formation of a dispersed phase, whose destabilization results in tube clogging issues. Methods:: The research problem focuses on understanding how sulfur composition affects the formation of a dispersed phase in low-polarity organic dispersion media for sulfur-containing hydrocarbons. It is investigated because the presence of sulfur in crude oil significantly affects the behavior of dispersed phases, which can result in operational and environmental quality issues to comprehensively assess the impact of sulfur composition on the dynamics and stability of this dispersed phase, we introduce a mesoscopic model based on the master equation. This model considers the molecular structure of system components and their molecular properties, established through computational quantum chemistry and statistical thermodynamics tools Results:: While our research focuses on a two-phase system, our theoretical insights suggest that increased sulfur content escalates the likelihood of destabilizing the dispersed phase. This adverse effect can be mitigated by incorporating additives capable of reducing the polarizability of the dispersion medium. The novelty lies in the development of a stochastic model to predict the dynamics of dispersed phase formation in sulfur-containing hydrocarbons. This model considers molecular interactions and stochastic processes, offering insights into the influence of sulfur composition on phase behavior. Conclusion:: A stochastic model, based on molecular structure, predicts accelerated formation with increased sulfur concentration, reaching non-equilibrium steady states. Limitations include ad hoc transition probabilities and the exclusion of factors like density and viscosity. Real crudes, with complex compositions, may exhibit different behavior. The presence of sulfur in the dispersion medium enhances the stability of the dispersed system. Our work sheds light on the intricate interplay between sulfur content and the performance of petroleum systems, offering potential solutions to mitigate these issues. Quantitative results include accelerated dispersed phase formation with increased sulfur concentration. Qualitatively, molecular interactions and stochastic processes were explored, highlighting sulfur's impact on phase dynamics.

Thermodynamic work of partial resetting

Partial resetting, whereby a state variable x(t) is reset at random times to a value ax(t) , 0⩽a⩽1 , generalizes conventional resetting by introducing the resetting strength a as a parameter. Partial resetting generates a broad family of non-equilibrium steady states (NESS) that interpolates between the conventional NESS at strong resetting (a = 0) and a Gaussian distribution at weak resetting (a → 1). Here such resetting processes are studied from a thermodynamic perspective, and the mean cost associated with maintaining such NESS are derived. The resetting phase of the dynamics is implemented by a resetting potential Φ(x) that mediates the resets in finite time. By working in an ensemble of trajectories with a fixed number of resets, we study both the steady-state properties of the propagator and its moments. The thermodynamic work needed to sustain the resulting NESS is then investigated. We find that different resetting traps can give rise to rates of work with widely different dependencies on the resetting strength a. Surprisingly, in the case of resets mediated by a harmonic trap with otherwise free diffusive motion, the asymptotic rate of work is insensitive to the value of a. For general anharmonic traps, the asymptotic rate of work can be either increasing or decreasing as a function of the strength a, depending on the degree of anharmonicity. Counter to intuition, the rate of work can therefore in some cases increase as the resetting becomes weaker (a→1) although the work vanishes at a = 1. Work in the presence of a background potential is also considered. Numerical simulations confirm our findings.

Thermodynamic Stability Theories of Irreversible Processes and the Fourth Law of Thermodynamics.

Three approaches for determining the thermodynamic stability of irreversible processes are described in generalized formulations. The simplest is the Gibbs-Duhem theory, specialized to irreversible trajectories, which uses the concept of virtual displacement in the reverse direction. Its only drawback is that even a trajectory leading to an explosion is identified as a thermodynamically stable motion. In the second approach, we use a thermodynamic Lyapunov function and its time rate from the Lyapunov thermodynamic stability theory (LTS, previously known as CTTSIP). In doing so, we demonstrate that the second differential of entropy, a frequently used Lyapunov function, is useful only for investigating the stability of equilibrium states. Nonequilibrium steady states do not qualify. Without using explicit perturbation coordinates, we further identify asymptotic thermodynamic stability and thermodynamic stability under constantly acting disturbances of unperturbed trajectories as well as of nonequilibrium steady states. The third approach is also based on the Lyapunov function from LTS, but here we additionally use the rates of perturbation coordinates, based on the Gibbs relations and without using their explicit expressions, to identify not only asymptotic thermodynamic stability but also thermodynamic stability under constantly acting disturbances. Only those trajectories leading to an infinite rate of entropy production (unstable states) are excluded from this conclusion. Finally, we use these findings to formulate the Fourth Law of thermodynamics based on the thermodynamic stability. It is a comprehensive statement covering all nonequilibrium trajectories, close to as well as far from equilibrium. Unlike previous suggested "fourth laws", this one meets the same level of generality that is associated with the original zeroth to third laws. The above is illustrated using the Schlögl reaction with its multiple steady states in certain regions of operation.

Exact Results for a Boundary-Driven Double Spin Chain and Resource-Efficient Remote Entanglement Stabilization

We derive an exact solution for the steady state of a setup where two XX-coupled N-qubit spin chains (with possibly nonuniform couplings) are subject to boundary Rabi drives and common boundary loss generated by a waveguide (either bidirectional or unidirectional). For a wide range of parameters, this system has a pure entangled steady state, providing a means for stabilizing remote multiqubit entanglement without the use of squeezed light. Our solution also provides insights into a single boundary-driven dissipative XX spin chain that maps to an interacting fermionic model. The nonequilibrium steady state exhibits surprising correlation effects, including an emergent pairing of hole excitations that arises from dynamically constrained hopping. Our system could be implemented in a number of experimental platforms, including circuit QED. Published by the American Physical Society 2024

Thermal transport in fullerene-based molecular junctions: molecular dynamics simulations

We investigate phonon thermal transport of fullerene-based single-molecule junctions by employing classical molecular dynamics (MD) simulations. We compute the thermal conductances of C60 fullerene monomers, dimers, and trimers utilizing three distinct MD methods. We observe the equilibration dynamics in one approach, and employ two other nonequilibrium steady state simulation methods. We discuss technical aspects of each simulation technique, and show that their predictions for the thermal conductance agree. Our simulations reveal that while the thermal conductance of fullerene monomer and dimer junctions remains similar, that of trimer junctions experiences a significant reduction. This study could assist in the design of high-performing thermoelectric junctions, where low thermal conductance is desired.

Active particle in one dimension subjected to resetting with memory.

The study of diffusion with preferential returns to places visited in the past has attracted increased attention in recent years. In these highly non-Markov processes, a standard diffusive particle intermittently resets at a given rate to previously visited positions. At each reset, a position to be revisited is randomly chosen with a probability proportional to the accumulated amount of time spent by the particle at that position. These preferential revisits typically generate a very slow diffusion, logarithmic in time, but still with a Gaussian position distribution at late times. Here we consider an active version of this model, where between resets the particle is self-propelled with constant speed and switches direction in one dimension according to a telegraphic noise. Hence there are two sources of non-Markovianity in the problem. We exactly derive the position distribution in Fourier space, as well as the variance of the position at all times. The crossover from the short-time ballistic regime, dominated by activity, to the long-time anomalous logarithmic growth induced by memory is studied. We also analytically derive a large deviation principle for the position, which exhibits a logarithmic time scaling instead of the usual algebraic form. Interestingly, at large distances, the large deviations become independent of time and match the nonequilibrium steady state of a particle under resetting to its starting position only.

Thermodynamic constraints on kinetic perturbations of homogeneous driven diffusions

We analyze the static response to kinetic perturbations of nonequilibrium steady states that can be modeled as diffusions. We demonstrate that kinetic response is purely a nonequilibirum effect, measuring the degree to which the Fluctuation-Dissipation Theorem is violated out of equilibrium. For driven diffusions in a flat landscape, we further demonstrate that such response is constrained by the strength of the nonequilibrium driving via quantitative inequalities.

Fluctuation-response relation as a probe of long-range correlations in nonequilibrium quantum and classical fluids.

The absence of a simple fluctuation-dissipation theorem is a major obstacle for studying systems that are not in thermodynamic equilibrium. We show that for a fluid in a nonequilibrium steady state characterized by a constant temperature gradient the commutator correlation functions are still related to response functions; however, the relation is to the bilinear response of products of two observables, rather than to a single linear response function as is the case in equilibrium. This modified fluctuation-response relation holds for both quantum and classical systems. It is both motivated and informed by the long-range correlations that exist in such a steady state and allows for probing them via response experiments. This is of particular interest in quantum fluids, where the direct observation of fluctuations by light scattering would be difficult. In classical fluids it is known that the coupling of the temperature gradient to the diffusive shear velocity leads to correlations of various observables, in particular temperature fluctuations, that do not decay as a function of distance, but rather extend over the entire system. We investigate the nature of these correlations in a fermionic quantum fluid and show that the crucial coupling between the temperature gradient and velocity fluctuations is the same as in the classical case. Accordingly, the nature of the long-ranged correlations in the hydrodynamic regime also is the same. However, as one enters the collisionless regime in the low-temperature limit the nature of the velocity fluctuations changes: they become ballistic rather than diffusive. As a result, correlations of the temperature and other observables are still singular in the long-wavelength limit, but the singularity is weaker than in the hydrodynamic regime.

Confined run-and-tumble particles with non-Markovian tumbling statistics.

Confined active particles constitute simple, yet realistic, examples of systems that converge into a nonequilibrium steady state. We investigate a run-and-tumble particle in one spatial dimension, trapped by an external potential, with a given distribution g(t) of waiting times between tumbling events whose mean value is equal to τ. Unless g(t) is an exponential distribution (corresponding to a constant tumbling rate), the process is non-Markovian, which makes the analysis of the model particularly challenging. We use an analytical framework involving effective position-dependent tumbling rates to develop a numerical method that yields the full steady-state distribution (SSD) of the particle's position. The method is very efficient and requires modest computing resources, including in the large-deviation and/or small-τ regime, where the SSD can be related to the the large-deviation function, s(x), via the scaling relation P_{st}(x)∼e^{-s(x)/τ}.

Signatures of quantum phases in a dissipative system.

Lindbladian formalism, as tuned to dissipative and open systems, has been all-pervasive to interpret non-equilibrium steady states of quantum many-body systems. We study the fate of free fermionic and superconducting phases in a dissipative one-dimensional Kitaev model-where the bath acts both as a source and a sink of fermionic particles with different coupling rates. As a function of these two couplings, we investigate the steady state, its entanglement content, and its approach from varying initial states. Interestingly, we find that the steady state phase diagram retains decipherable signatures of ground state critical physics. We also show that early-time fidelity is a useful marker to find a subclass of phase transitions in such situations. Moreover, we show that the survival of critical signatures at late-times, strongly depend on the thermal nature of the steady state. This connection hints at a correspondence between quantum observables and classical magnetism in the steady state of such systems. Our work uncovers interesting connections between dissipative quantum many-body systems, thermalization of a classical spin and many-body quantum critical phenomena.

Coexistence of distinct nonuniform nonequilibrium steady states in Ehrenfest multiurn model on a ring.

The recently proposed Ehrenfest M-urn model with interactions on a ring is considered as a paradigm model which can exhibit a variety of distinct nonequilibrium steady states. Unlike the previous three-urn model on a ring which consists of a uniform steady state and a nonuniform nonequilibrium steady state, it is found that for even M≥4, an additional nonequilibrium steady state can coexist with the original ones. Detailed analysis reveals that this additional nonequilibrium steady state emerged via a pitchfork bifurcation which cannot occur if M is odd. Properties of this nonequilibrium steady state, such as stability, and steady-state flux are derived analytically for the four-urn case. The full phase diagram with the phase boundaries is also derived explicitly. The associated thermodynamic stability is also analyzed, confirming its stability. These theoretical results are also explicitly verified by direct Monte Carlo simulations for the three-urn and four-urn ring models.

Inelastic neutron scattering study of magnon excitation by ultrasound injection in yttrium iron garnet

The magnon excitation by ultrasound injection in Y3Fe5O12 is studied by inelastic neutron scattering. Both longitudinal and transverse ultrasound injections enhanced the inelastic neutron scattering intensity. We analyzed the nonequilibrium magnon steady state using the effective magnon temperature model. The large deviation of the effective magnon temperature from the sample temperature is observed at the ultrasound longitudinal mode along [0, 0, 1] at ∼10 K and [1, 1, 1] at ∼140 K. This dependence suggests that the nonequilibrium steady state can be achieved only by strong spin–lattice coupling in Y3Fe5O12. The spin–lattice coupling exhibits a decrease largely above 100 K, indicating that it could be the main origin of the degradation of longitudinal spin Seebeck effect at the temperature range.

Thermodynamic precision in the nonequilibrium exchange scenario.

We discuss exchange scenario thermodynamic uncertainty relations for the work done on a two-qubit entangled nonequilibrium steady state obtained by coupling the two qubits and putting each of them in weak contact with a thermal bath. In this way we investigate the use of entangled nonequilibrium steady states as end points of thermodynamic cycles. In this framework we prove analytically that for a paradigmatic unitary it is possible to construct an exchange scenario thermodynamic uncertainty relation. However, despite holding in many cases, we also show that such a relation ceases to be valid when considering other suitable unitary quenches. Furthermore, this paradigmatic example allows us to shed light on the role of the entanglement between the two qubits for precise work absorption. By considering the projection of the entangled steady state onto the set of separable states, we provide examples where such projection implies an increase of the relative uncertainty, showing the usefulness of entanglement.

Intermittent random walks under stochastic resetting.

We analyze a one-dimensional intermittent random walk on an unbounded domain in the presence of stochastic resetting. In this process, the walker alternates between local intensive search, diffusion, and rapid ballistic relocations in which it does not react to the target. We demonstrate that Poissonian resetting leads to the existence of a non-equilibrium steady state. We calculate the distribution of the first arrival time to a target along with its mean and show the existence of an optimal reset rate. In particular, we prove that the initial condition of the walker, i.e., either starting diffusely or relocating, can significantly affect the long-time properties of the search process. Moreover, we demonstrate the presence of distinct parameter regimes for the global optimization of the mean first arrival time when ballistic and diffusive movements are in direct competition.

Variance sum rule for entropy production.

Entropy production is the hallmark of nonequilibrium physics, quantifying irreversibility, dissipation, and the efficiency of energy transduction processes. Despite many efforts, its measurement at the nanoscale remains challenging. We introduce a variance sum rule (VSR) for displacement and force variances that permits us to measure the entropy production rate σ in nonequilibrium steady states. We first illustrate it for directly measurable forces, such as an active Brownian particle in an optical trap. We then apply the VSR to flickering experiments in human red blood cells. We find that σ is spatially heterogeneous with a finite correlation length, and its average value agrees with calorimetry measurements. The VSR paves the way to derive σ using force spectroscopy and time-resolved imaging in living and active matter.

Competition between lanes and transient jammed clusters in driven binary mixtures.

We consider mixtures of oppositely driven particles, showing that their nonequilibrium steady states form lanes parallel to the drive, which coexist with transient jammed clusters where particles are temporarily immobilized. We analyze the interplay between these two types of nonequilibrium pattern formation, including their implications for macroscopic demixing perpendicular to the drive. Finite-size scaling analysis indicates that there is no critical driving force associated with demixing, which appears as a crossover in finite systems. We attribute this effect to the disruption of long-ranged order by the transient jammed clusters.

Challenges in molecular dynamics simulations of heat exchange statistics.

We study heat exchange in temperature-biased metal-molecule-metal molecular junctions by employing the molecular dynamics simulator LAMMPS. Generating the nonequilibrium steady state with Langevin thermostats at the boundaries of the junction, we show that the average heat current across a gold-alkanedithiol-gold nanojunction behaves physically, with the thermal conductance value matching the literature. In contrast, the full probability distribution function for heat exchange, as generated by the simulator, violates the fundamental fluctuation symmetry for entropy production. We trace this failure back to the implementation of the thermostats and the expression used to calculate the heat exchange. To rectify this issue and produce the correct statistics, we introduce single-atom thermostats as an alternative to conventional many-atom thermostats. Once averaging heat exchange over the hot and cold thermostats, this approach successfully generates the correct probability distribution function, which we use to study the behavior of both the average heat current and its noise. We further examine the thermodynamic uncertainty relation in the molecular junction and show that it holds, albeit demonstrating nontrivial trends. Our study points to the need to carefully implement nonequilibrium molecular dynamics solvers in atomistic simulation software tools for future investigations of noise phenomena in thermal transport.