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.

Free volume theory explains the unusual behavior of viscosity in a non-confluent tissue during morphogenesis.

A recent experiment on zebrafish blastoderm morphogenesis showed that the viscosity (η) of a non-confluent embryonic tissue grows sharply until a critical cell packing fraction (ϕS). The increase in η up to ϕS is similar to the behavior observed in several glass-forming materials, which suggests that the cell dynamics is sluggish or glass-like. Surprisingly, η is a constant above ϕS. To determine the mechanism of this unusual dependence of η on ϕ, we performed extensive simulations using an agent-based model of a dense non-confluent two-dimensional tissue. We show that polydispersity in the cell size, and the propensity of the cells to deform, results in the saturation of the available free area per cell beyond a critical packing fraction. Saturation in the free space not only explains the viscosity plateau above ϕS but also provides a relationship between equilibrium geometrical packing to the dramatic increase in the relaxation dynamics.

Fluctuation-Dissipation Relation in a Nonequilibrium Quantum Fluid.

There is no simple fluctuation-dissipation theorem (FDT) for nonequilibrium systems. We show that for a fluid in a nonequilibrium steady state (NESS) characterized by a constant temperature gradient there is a generalized FDT that relates commutator correlation functions to the bilinear response of products of observables. This allows for experimental probes of the long-range correlations in such a system, quantum or classical, via response experiments. We also show that the correlations are not tied to thermal fluctuations but are intrinsic to the NESS and reflect a generalized rigidity.

Nonhydrodynamic initial conditions are not soon forgotten.

Solutions to hydrodynamic equations, which are used for a vast variety of physical problems, are assumed to be specified by boundary conditions and initial conditions on the hydrodynamic variables only. Initial values of other variables are assumed to be irrelevant for a hydrodynamic description. We show that this assumption is not correct because of the existence of long-time-tail effects that are ubiquitous in systems governed by hydrodynamic equations. We illustrate this breakdown of a hydrodynamic description by means of the simple example of diffusion in a disordered electron system.

Rigidity and Superfast Signal Propagation in Fluids and Solids in Non-Equilibrium Steady States.

In the 1980s, it was theoretically predicted that correlations of various observables in a fluid in a non-equilibrium steady state (NESS) are extraordinarily long-ranged, extending, in a well-defined sense, over the size of the system. This is to be contrasted with correlations in an equilibrium fluid, whose range is typically just a few particle diameters. These NESS correlations were later confirmed by numerous experimental studies. Unlike long-ranged correlations at critical points, these correlations are generic in the sense that they exist for any temperature as long as the system is in a NESS. In equilibrium systems, generic long-ranged correlations are caused by spontaneously broken continuous symmetries and are associated with a generalized rigidity, which in turn leads to a new propagating excitation or mode. For example, in a solid, spatial rigidity leads to transverse sound waves, while, in a superfluid, phase rigidity leads to temperature waves known as second sound at finite temperatures and phonons at zero temperature. More generally, long-ranged spatial correlations imply rigidity irrespective of their physical origin. This implies that a fluid in a NESS should also display a type of rigidity and related anomalous transport behavior. Here we show that this is indeed the case. For the particular case of a simple fluid in a constant temperature gradient, the anomalous transport behavior takes the form of a super-diffusive spread of a constant-pressure temperature perturbation. We also discuss the case of an elastic solid, where we predict a spread that is faster than ballistic.

Random First Order Transition Theory for Glassy Dynamics in a Single Condensed Polymer.

The number of compact structures of a single condensed polymer (SCP), with similar free energies, grows exponentially with the degree of polymerization. In analogy with structural glasses (SGs), we expect that at low temperatures chain relaxation should occur by activated transitions between the compact metastable states. By evolving the states of the SCP, linearly coupled to a reference state, we show that, below a dynamical transition temperature (T_{d}), the SCP is trapped in a metastable state leading to slow dynamics. At a lower temperature, T_{K}≠0, the configurational entropy vanishes, resulting in a thermodynamic random first order ideal glass transition. The relaxation time obeys the Vogel-Fulcher-Tamman law, diverging at T=T_{0}≈T_{K}. These findings, accord well with the random first order transition theory, establishing that SCP and SG exhibit similar universal characteristics.

Fragile-to-strong crossover, growing length scales, and dynamic heterogeneity in Wigner glasses.

Colloidal particles, which are ubiquitous, have become ideal testing grounds for the structural glass transition theories. In these systems glassy behavior arises as the density of the particles is increased. Thus, soft colloidal particles with varying degree of softness capture diverse glass-forming properties, observed normally in molecular glasses. Brownian dynamics simulations for a binary mixture of micron-sized charged colloidal suspensions show that tuning the softness of the interaction potential, achievable by changing the monovalent salt concentration results in a continuous transition from fragile to strong behavior. Remarkably, this is found in a system where the well characterized interaction potential between the colloidal particles is isotropic. We also show that the predictions of the random first-order transition (RFOT) theory quantitatively describes the universal features such as the growing correlation length, ξ∼(ϕ_{K}/ϕ-1)^{-ν} with ν=2/3 where ϕ_{K}, the analog of the Kauzmann temperature, depends on the salt concentration. As anticipated by the RFOT predictions, we establish a causal relationship between the growing correlation length and a steep increase in the relaxation time and dynamic heterogeneity as the system is compressed. The broad range of fragility observed in Wigner glasses is used to draw analogies with molecular and polymer glasses. The large variations in the fragility are normally found only when the temperature dependence of the viscosity is examined for a large class of diverse glass-forming materials. In sharp contrast, this is vividly illustrated in a single system that can be experimentally probed. Our work also shows that the RFOT predictions are accurate in describing the dynamics over the entire density range, regardless of the fragility of the glasses.

Ferromagnetic Quantum Critical Point in Noncentrosymmetric Systems.

Ferromagnetic quantum criticality in clean metals has proven elusive due to fermionic soft modes that drive the transition first order. We show that noncentrosymmetric metals with a strong spin-orbit interaction provide a promising class of materials for realizing a ferromagnetic quantum critical point in clean systems. The spin-orbit interaction renders massive the soft modes that interfere with quantum criticality in most materials, while the absence of spatial inversion symmetry precludes the existence of new classes of soft modes that could have the same effect.

Transition to turbulence in driven active matter.

A Lorenz-like model was set up recently to study the hydrodynamic instabilities in a driven active matter system. This Lorenz model differs from the standard one in that all three equations contain nonlinear terms. The additional nonlinear term comes from the active matter contribution to the stress tensor. In this work, we investigate the nonlinear properties of this Lorenz model both analytically and numerically. The significant feature of the model is the passage to chaos through a complete set of period-doubling bifurcations above the Hopf point for Schmidt numbers above a critical value. Interestingly enough, at these Schmidt numbers a strange attractor and stable fixed points coexist beyond the homoclinic point. At the Hopf point, the strange attractor disappears leaving a high-period periodic orbit. This periodic state becomes the expected limit cycle through a set of bifurcations and then undergoes a sequence of period-doubling bifurcations leading to the formation of a strange attractor. This is the first situation where a Lorenz-like model has shown a set of consecutive period-doubling bifurcations in a physically relevant transition to turbulence.

Nonequilibrium Casimir pressures in liquids under shear.

In stationary nonequilibrium states coupling between hydrodynamic modes causes thermal fluctuations to become long ranged inducing nonequilibrium Casimir pressures. Here we consider nonequilibrium Casimir pressures induced in liquids by a velocity gradient. Specifically, we have obtained explicit expressions for the magnitude of the shear-induced pressure enhancements in a liquid layer between two horizontal plates that complete and correct results previously presented in the literature. In contrast to nonequilibrium Casimir pressures induced by a temperature or concentration gradient, we find that in shear nonequilibrium contributions from short-range fluctuations are no longer negligible. In addition, it is noted that currently available computer simulations of model fluids in shear observe effects from molecular correlations at nanoscales that have a different physical origin and do not probe shear-induced pressures resulting from coupling of long-wavelength hydrodynamic modes. Even more importantly, we find that in actual experimental conditions, shear-induced pressure enhancements are caused by viscous heating and not by thermal velocity fluctuations. Hence, isothermal computer simulations are irrelevant for the interpretation of experimental shear-induced pressure enhancements.

Giant Casimir Nonequilibrium Forces Drive Coil to Globule Transition in Polymers.

We develop a theory to probe the effect of nonequilibrium fluctuation-induced forces on the size of a polymer confined between two horizontal, thermally conductive plates subject to a constant temperature gradient, ∇ T. We assume that (a) the solvent is good and (b) the distance between the plates is large so that in the absence of a thermal gradient the polymer is a coil, whose size scales with the number of monomers as Nν, with ν ≈ 0.6. We find that above a critical temperature gradient, ∇ Tc ≈ N-5/4, a favorable attractive monomer-monomer interaction due to the giant Casimir force (GCF) overcomes the chain conformational entropy, resulting in a coil-globule transition. Our predictions can be verified using light-scattering experiments with polymers, such as polystyrene or polyisoprene in organic solvents in which the GCF is attractive.

Work probability distribution for a ferromagnet with long-ranged and short-ranged correlations.

Work fluctuations and work probability distributions are fundamentally different in systems with short-ranged versus long-ranged correlations. Specifically, in systems with long-ranged correlations the work distribution is extraordinarily broad compared to systems with short-ranged correlations. This difference profoundly affects the possible applicability of fluctuation theorems like the Jarzynski fluctuation theorem. The Heisenberg ferromagnet, well below its Curie temperature, is a system with long-ranged correlations in very low magnetic fields due to the presence of Goldstone modes. As the magnetic field is increased the correlations gradually become short ranged. Hence, such a ferromagnet is an ideal system for elucidating the changes of the work probability distribution as one goes from a domain with long-ranged correlations to a domain with short-ranged correlations by tuning the magnetic field. A quantitative analysis of this crossover behavior of the work probability distribution and the associated fluctuations is presented.

Contrasting Work Fluctuations and Distributions in Systems with Short-Range and Long-Range Correlations.

It is shown that the work fluctuations and work distribution functions are fundamentally different in systems with short-range versus long-range correlations. The two cases considered with long-range correlations are magnetic work fluctuations in an equilibrium isotropic ferromagnet and work fluctuations in a nonequilibrium fluid with a temperature gradient. The long-range correlations in the former case are due to equilibrium Goldstone modes, while in the latter they are due to generic nonequilibrium effects. The magnetic case is of particular interest, since an external magnetic field can be used to tune the system from one with long-range correlations to one with only short-range correlations. It is shown that in systems with long-range correlations the work distribution is extraordinarily broad compared to systems with only short-range correlations. Surprisingly, these results imply that fluctuation theorems such as the Jarzynski fluctuation theorem are more useful in systems with long-range correlations than in systems with short-range correlations.

Quantum Triple Point and Quantum Critical End Points in Metallic Magnets.

In low-temperature metallic magnets, ferromagnetic (FM) and antiferromagnetic (AFM) orders can exist, adjacent to one another or concurrently, in the phase diagram of a single system. We show that universal quantum effects qualitatively alter the known phase diagrams for classical magnets. They shrink the region of concurrent FM and AFM order, change various transitions from second to first order, and, in the presence of a magnetic field, lead to either a quantum triple point where the FM, AFM, and paramagnetic phases all coexist or a quantum critical end point.

Scaling Theory of a Compressibility-Driven Metal-Insulator Transition in a Two-Dimensional Electron Fluid.

We present a scaling description of a metal-insulator transition in two-dimensional electron systems that is driven by a vanishing compressibility rather than a vanishing diffusion coefficient. A small set of basic assumptions leads to a consistent theoretical framework that is compatible with existing transport and compressibility measurements, and allows us to make predictions for other observables. We also discuss connections between these ideas and other theories of transitions to an incompressible quantum fluid.

Work, work fluctuations, and the work distribution in a thermal nonequilibrium steady state.

Long-ranged correlations generically exist in nonequilibrium fluid systems. In the case of a nonequilibrium steady state caused by a temperature gradient, the correlations are especially long-ranged and strong. The anomalous light scattering predicted to exist in these systems is well-confirmed by numerous experiments. Recently, the Casimir force or pressure due to these fluctuations or correlations has been discussed in great detail. In this paper, the notion of a Casimir work is introduced, and an alternative way to measure the nonequilibrium Casimir force is suggested. In particular, the nonequilibrium Casimir force is related to nonequilibrium heat, and not, as in equilibrium, to a volume derivative of an average energy. The nonequilibrium work fluctuations are determined and shown to be very anomalous compared to equilibrium work fluctuations. The nonequilibrium work distribution is also computed, and it is contrasted with work distributions in systems with short-range correlations. Again, there is a striking difference in the two cases. Formal theories of work and work distributions in nonequilibrium steady states are not explicit enough to illustrate any of these interesting features.

Nonequilibrium fluctuation-induced Casimir pressures in liquid mixtures.

In this article we derive expressions for Casimir-like pressures induced by nonequilibrium concentration fluctuations in liquid mixtures. The results are then applied to liquid mixtures in which the concentration gradient results from a temperature gradient through the Soret effect. A comparison is made between the pressures induced by nonequilibrium concentration fluctuations in liquid mixtures and those induced by nonequilibrium temperature fluctuations in one-component fluids. Some suggestions for experimental verification procedures are also presented.

Physical origin of nonequilibrium fluctuation-induced forces in fluids.

Long-range thermal fluctuations appear in fluids in nonequilibrium states leading to fluctuation-induced Casimir-like forces. Two distinct mechanisms have been identified for the origin of the long-range nonequilibrium fluctuations in fluids subjected to a temperature or concentration gradient. One is a coupling between the heat or mass-diffusion mode with a viscous mode in fluids subjected to a temperature or concentration gradient. Another one is the spatial inhomogeneity of thermal noise in the presence of a gradient. We show that in fluids fluctuation-induced forces arising from mode coupling are several orders of magnitude larger than those from inhomogeneous noise.

Nonequilibrium is different.

Nonequilibrium and equilibrium fluid systems differ due to the existence of long-range correlations in nonequilibrium that are not present in equilibrium, except at critical points. Here we examine fluctuations of the temperature, of the pressure tensor, and of the heat current in a fluid maintained in a nonequilibrium stationary state (NESS) with a fixed temperature gradient, a system in which the nonequilibrium correlations are especially long-ranged. For this particular NESS, our results show that (i) the mean-squared fluctuations in nonequilibrium differ markedly in their system-size scaling compared to their equilibrium counterparts, and (ii) there are large, nonlocal correlations of the normal stress in this NESS. These terms provide important corrections to the fluctuating normal stress in linearized Landau-Lifshitz fluctuating hydrodynamics.

Non-equilibrium concentration fluctuations in binary liquids with realistic boundary conditions.

Because of the spatially long-ranged nature of spontaneous fluctuations in thermal non-equilibrium systems, they are affected by boundary conditions for the fluctuating hydrodynamic variables. In this paper we consider a liquid mixture between two rigid and impervious plates with a stationary concentration gradient resulting from a temperature gradient through the Soret effect. For liquid mixtures with large Lewis and Schmidt numbers, we are able to obtain explicit analytical expressions for the intensity of the non-equilibrium concentration fluctuations as a function of the frequency ω and the wave number q of the fluctuations. In addition we elucidate the spatial dependence of the intensity of the non-equilibrium fluctuations responsible for a non-equilibrium Casimir effect.