Generalized Fluctuation-dissipation Theorem Research Articles

Generalized fluctuation-dissipation theorem for non-Markovian reaction networks.

Intracellular biochemical networks often display large fluctuations in the molecule numbers or the concentrations of reactive species, making molecular approaches necessary for system descriptions. For Markovian reaction networks, the fluctuation-dissipation theorem (FDT) has been well established and extensively used in fast evaluation of fluctuations in reactive species. For non-Markovian reaction networks, however, the similar FDT has not been established so far. Here, we present a generalized FDT (gFDT) for a large class of non-Markovian reaction networks where general intrinsic-event waiting-time distributions account for the effect of intrinsic noise and general stochastic reaction delays represent the impact of extrinsic noise from environmental perturbations. The starting point is a generalized chemical master equation (gCME), which describes the probabilistic behavior of an equivalent Markovian reaction network and identifies the structure of the original non-Markovian reaction network in terms of stoichiometries and effective transition rates (extensions of common reaction propensity functions). From this formulation follows directly the solution of the linear noise approximation of the stationary gCME for all the components in the non-Markovian reaction network. While the gFDT can quickly trace noisy sources in non-Markovian reaction networks, example analysis verifies its effectiveness.

Quantum fluctuation-dissipation theorem far from equilibrium

Fluctuations associated with relaxations in far-from-equilibrium regime is of fundamental interest for a large variety of systems within broad scales. Recent advances in techniques such as spectroscopy have generated the possibility for measuring the fluctuations of the mesoscopic systems in connection to the relaxation processes when driving the underlying quantum systems far from equilibrium. We present a general nonequilibrium Fluctuation-Dissipation Theorem (FDT) for quantum Markovian processes where the detailed-balance condition is violated. Apart from the fluctuations, the relaxation involves extra correlation that is governed by the quantum curl flux emerged in the far-from-equilibrium regime. Such a contribution vanishes for the thermal equilibrium, so that the conventional FDT is recovered. We finally apply the nonequilibrium FDT to the molecular junctions, elaborating the detailed-balance-breaking effects on the optical transmission spectrum. Our results have the advantage of and exceed the scope of the fluctuation-dissipation relation in the perturbative and near equilibrium regimes, and is of broad interest for the study of quantum thermodynamics.ation in the perturbative and near equilibrium regimes, and is of broad interest for the study of quantum thermodynamics.

Violation of generalized fluctuation-dissipation theorem in biological limit cycle oscillators with state-dependent internal drives: Applications to hair cell oscillations

The spontaneously oscillating hair bundle of sensory cells in the inner ear is an example of a stochastic, nonlinear oscillator driven by internal active processes. Moreover, this internal activity is adaptive -- its power input depends on the current state of the system. We study fluctuation dissipation relations in such adaptively-driven, nonequilibrium limit-cycle oscillators. We observe the expected violation of the well-known, equilibrium fluctuation-dissipation theorem (FDT), and verify the existence of a generalized fluctuation-dissipation theorem (GFDT) in the non-adaptively driven model of the hair cell oscillator. This generalized fluctuation theorem requires the system to be analyzed in the co-moving frame associated with the mean limit cycle of the stochastic oscillator. We then demonstrate, via numerical simulations and analytic calculations, that the adaptively-driven dynamical hair cell model violates both the FDT and the GFDT. We go on to show, using stochastic, finite-state, dynamical models, that such a feedback-controlled drive in stochastic limit cycle oscillators generically violates both the FDT and GFDT. We propose that one may in fact use the breakdown of the GFDT as a tool to more broadly look for and quantify the effect of adaptive, feedback mechanisms associated with driven (nonequilibrium) biological dynamics.

Eyring equation and fluctuation-dissipation far away from equilibrium.

Understanding and managing the influence that either external forces or non-equilibrated environments may have on chemical processes is essential for the current and future development of theoretical chemistry. One of the central questions to solve is how to generalize the transition state theory in order to make it applicable in far from equilibrium situations. In this sense, here we propose a way to generalize Eyring's equation based on the definition of an effective thermal energy (temperature) emerging from the coupling of both fast and slow dynamic variables analyzed within the generalized Langevin dynamics scheme. This coupling makes the energy distribution of the fast degrees of freedom not equilibrate because they have been enslaved to the dynamics of the corresponding slow degrees. However, the introduction of the effective thermal energy enables us to restore an effective adiabatic separation of timescales leading to a renormalization of the generalized fluctuation-dissipation theorem. Hence, this procedure opens the possibility to deal with systems far away from equilibrium. A significant consequence of our results is that Eyring's equation is generalized to treat systems under the influence of strong external forces.

Plasmonically enhanced mid-IR light source based on tunable spectrally and directionally selective thermal emission from nanopatterned graphene

We present a proof of concept for a spectrally selective thermal mid-IR source based on nanopatterned graphene (NPG) with a typical mobility of CVD-grown graphene (up to 3000 hbox {cm}^2,hbox {V}^{-1},hbox {s}^{-1}), ensuring scalability to large areas. For that, we solve the electrostatic problem of a conducting hyperboloid with an elliptical wormhole in the presence of an in-plane electric field. The localized surface plasmons (LSPs) on the NPG sheet, partially hybridized with graphene phonons and surface phonons of the neighboring materials, allow for the control and tuning of the thermal emission spectrum in the wavelength regime from lambda =3 to 12 upmum by adjusting the size of and distance between the circular holes in a hexagonal or square lattice structure. Most importantly, the LSPs along with an optical cavity increase the emittance of graphene from about 2.3% for pristine graphene to 80% for NPG, thereby outperforming state-of-the-art pristine graphene light sources operating in the near-infrared by at least a factor of 100. According to our COMSOL calculations, a maximum emission power per area of 11times 10^3 W/hbox {m}^2 at T=2000 K for a bias voltage of V=23 V is achieved by controlling the temperature of the hot electrons through the Joule heating. By generalizing Planck’s theory to any grey body and deriving the completely general nonlocal fluctuation-dissipation theorem with nonlocal response of surface plasmons in the random phase approximation, we show that the coherence length of the graphene plasmons and the thermally emitted photons can be as large as 13 upmum and 150 upmum, respectively, providing the opportunity to create phased arrays made of nanoantennas represented by the holes in NPG. The spatial phase variation of the coherence allows for beamsteering of the thermal emission in the range between 12^circ and 80^circ by tuning the Fermi energy between E_F=1.0 eV and E_F=0.25 eV through the gate voltage. Our analysis of the nonlocal hydrodynamic response leads to the conjecture that the diffusion length and viscosity in graphene are frequency-dependent. Using finite-difference time domain calculations, coupled mode theory, and RPA, we develop the model of a mid-IR light source based on NPG, which will pave the way to graphene-based optical mid-IR communication, mid-IR color displays, mid-IR spectroscopy, and virus detection.

Electron Induced Massive Dynamics of Magnetic Domain Walls.

We study the dynamics of domain walls (DWs) in a metallic, ferromagnetic nanowire, focusing on inertial effects on the DW due to interaction with a conduction electron bath. We develop a Keldysh collective coordinate technique to describe the effect of conduction electrons on rigid magnetic structures. The effective Lagrangian and Langevin equations of motion for a DW are derived microscopically, including the full response kernel which is nonlocal in time. The DW dynamics is described by two collective degrees of freedom: position and tilt-angle. The coupled Langevin equations therefore involve two correlated noise sources, leading to a generalized fluctuation-dissipation theorem (FDT). The DW response kernel due to electrons contains two parts: one related to dissipation via FDT, and another reactive part. We prove that the latter term leads to a mass for both degrees of freedom, even though the intrinsic bare mass is zero. The electron-induced mass is present even in a clean system without pinning or specifically engineered potentials. The resulting equations of motion contain rich dynamical solutions and point toward a way to control domain wall motion in metals via the electronic system properties. We discuss two observable consequences of the mass, hysteresis in the DW dynamics and resonant response to ac current.

Fluctuations out of equilibrium.

A generalized fluctuation-dissipation theorem involving slowly varying parameters is presented. Application of the Langevin method, the method of moments and of a multiscale technique reveal that not only dissipation but also dispersive contributions determine the spectral functions of fluctuations in arbitrary statistical systems. The non-Joule dispersive contribution is characterized by a novel non-local effect due to the additional phase shift between the force and the response of the system. This phase shift occurs as a result of parametric control to the system. The general formalism is illustrated by concrete examples and applications.This article is part of the theme issue 'Dissipative structures in matter out of equilibrium: from chemistry, photonics and biology (part 2)'.

Out-of-time-order fluctuation-dissipation theorem

We prove a generalized fluctuation-dissipation theorem for a certain class of out-of-time-ordered correlators (OTOCs) with a modified statistical average, which we call bipartite OTOCs, for general quantum systems in thermal equilibrium. The difference between the bipartite and physical OTOCs defined by the usual statistical average is quantified by a measure of quantum fluctuations known as the Wigner-Yanase skew information. Within this difference, the theorem describes a universal relation between chaotic behavior in quantum systems and a nonlinear-response function that involves a time-reversed process. We show that the theorem can be generalized to higher-order n-partite OTOCs as well as in the form of generalized covariance.

Probing non-thermal density fluctuations in the one-dimensional Bose gas

Quantum integrable models display a rich variety of non-thermal excited states with unusual properties. The most common way to probe them is by performing a quantum quench, i.e., by letting a many-body initial state unitarily evolve with an integrable Hamiltonian. At late times these systems are locally described by a generalized Gibbs ensemble with as many effective temperatures as their local conserved quantities. The experimental measurement of this macroscopic number of temperatures remains elusive. Here we show that they can be obtained for the Bose gas in one spatial dimension by probing the dynamical structure factor of the system after the quench and by employing a generalized fluctuation-dissipation theorem that we provide. Our procedure allows us to completely reconstruct the stationary state of a quantum integrable system from state-of-the-art experimental observations.

Fluctuation relations between hierarchical kinetically equivalent networks with Arrhenius-type transitions and their roles in systems and structural biology.

The legality of using simple kinetic schemes to determine the stochastic properties of a complex system depends on whether the fluctuations generated from hierarchical equivalent schemes are consistent with one another. To analyze this consistency, we perform lumping processes on the stochastic differential equations and the generalized fluctuation-dissipation theorem and apply them to networks with the frequently encountered Arrhenius-type transition rates. The explicit Langevin force derived from those networks enables us to calculate the state fluctuations caused by the intrinsic and extrinsic noises on the free energy surface and deduce their relations between kinetically equivalent networks. In addition to its applicability to wide classes of network related systems, such as those in structural and systems biology, the result sheds light on the fluctuation relations for general physical variables in Keizer's canonical theory.

Generalized fluctuation-dissipation theorem as a test of the Markovianity of a system

We study how well a generalized fluctuation-dissipation theorem (GFDT) is suited to test whether a stochastic system is not Markovian. To this end, we simulate a stochastic non-equilibrium model of the mechanosensory hair bundle from the inner ear organ and analyze its spontaneous activity and response to external stimulation. We demonstrate that this two-dimensional Markovian system indeed obeys the GFDT, as long as i) the averaging ensemble is sufficiently large and ii) finite-size effects in estimating the conjugated variable and its susceptibility can be neglected. Furthermore, we test the GFDT also by looking only at a one-dimensional projection of the system, the experimentally accessible position variable. This reduced system is certainly non-Markovian and the GFDT is somewhat violated but not as drastically as for the equilibrium fluctuation-dissipation theorem. We explore suitable measures to quantify the violation of the theorem and demonstrate that for a set of limited experimental data it might be difficult to decide whether the system is Markovian or not.

Generalized Fluctuation-Dissipation Theorem Applied to Active Hair Bundles

Generalized Fluctuation-Dissipation Theorem Applied to Active Hair Bundles

Finite-dimensional colored fluctuation-dissipation theorem for spin systems

When nano-magnets are coupled to random external sources, their magnetization becomes a random variable, whose properties are defined by an induced probability density, that can be reconstructed from its moments, using the Langevin equation, for mapping the noise to the dynamical degrees of freedom. When the spin dynamics is discretized in time, a general fluctuation-dissipation theorem, valid for non-Markovian noise, can be established, even when zero modes are present. We discuss the subtleties that arise, when Gilbert damping is present and the mapping between noise and spin degrees of freedom is non–linear.

Determining the continuous family of quantum Fisher information from linear-response theory

The quantum Fisher information represents the continuous family of metrics on the space of quantum states and places the fundamental limit on the accuracy of quantum state estimation. We show that the entire family of the quantum Fisher information can be determined from linear response theory through generalized covariances. We derive the generalized fluctuation-dissipation theorem that relates the linear response function to generalized covariances and hence allows us to determine the quantum Fisher information from linear response functions, which is experimentally measurable quantities. As an application, we examine the skew information, which is one of the quantum Fisher information, of a harmonic oscillator in thermal equilibrium, and show that the equality of the skew information-based uncertainty relation holds.

Mathematical Formalism of Nonequilibrium Thermodynamics for Nonlinear Chemical Reaction Systems with General Rate Law

This paper studies a mathematical formalism of nonequilibrium thermodynamics for chemical reaction models with $N$ species, $M$ reactions, and general rate law. We establish a mathematical basis for J. W. Gibbs' macroscopic chemical thermodynamics under G. N. Lewis' kinetic law of entire equilibrium (detailed balance in nonlinear chemistry kinetics). In doing so, the equilibrium thermodynamics is then naturally generalized to nonequilibrium settings without detailed balance. The kinetic models are represented by a Markovian jumping process. A generalized macroscopic chemical free energy function and its associated balance equation with nonnegative source and sink are the major discoveries. The proof is based on the large deviation principle of this type of Markov processes. A general fluctuation dissipation theorem for stochastic reaction kinetics is also proved. The mathematical theory illustrates how a novel macroscopic dynamic law can emerges from the mesoscopic kinetics in a multi-scale system.

Topological sigma models & dissipative hydrodynamics

We outline a universal Schwinger-Keldysh effective theory which describes macroscopic thermal fluctuations of a relativistic field theory. The basic ingredients of our construction are three: a doubling of degrees of freedom, an emergent abelian symmetry associated with entropy, and a topological (BRST) supersymmetry imposing fluctuationdissipation theorem. We illustrate these ideas for a non-linear viscous fluid, and demonstrate that the resulting effective action obeys a generalized fluctuation-dissipation theorem, which guarantees a local form of the second law.

Electromagnetic fluctuations in magnetized plasmas II: Extension of the theory for parallel wave vectors

Starting from the recently derived general expressions for the electromagnetic fluctuation spectra (electric and magnetic field) from uncorrelated plasma particles in plasmas with an uniform magnetic field, the case of strictly parallel (k⊥=0) oriented wave vectors with the respect to the uniform magnetic field direction is investigated. To derive fluctuation spectra valid in the entire complex frequency plane, the relevant dispersion functions and form factors are analytically continued to negative values of the imaginary part of the frequency for arbitrary gyrotropic plasma particle distribution functions. The generalized fluctuation-dissipation theorems for non-collective fluctuations in isotropic equal-temperature thermal distribution functions for general complex values of the frequency of the fluctuations with parallel wave vectors are derived.

Generalized fluctuation-dissipation theorem in a soluble out of equilibrium model

In the context of an exactly soluble out of equilibrium (quenched) model, we study an extension of the fluctuation-dissipation relation. This involves a modified differential form of this relation, with an effective temperature which may have an explicit dependence on time scales.

Response Function Theory for Many-Body Systems Away from Equilibrium: Conditions of Ultrafast-Time and Ultrasmall-Space Experimental Resolution

A response function theory and scattering theory applicable to the study of physical properties of systems driven arbitrarily far removed from equilibrium, specialized for dealing with ultrafast processes, and in conditions of space resolution (including the nanometric scale) are presented. The derivation is done in the framework of a Gibbs-style nonequilibrium statistical ensemble formalism. The observable properties are shown to be connected with time- and space-dependent correlation functions out of equilibrium. A generalized fluctuation-dissipation theorem, which relates these correlation functions with generalized susceptibilities, is derived. The method of nonequilibrium-thermodynamic Green functions, which proves useful for calculations, is also presented. Two illustrative applications of the formalism, which study optical responses in ultrafast laser spectroscopy and Raman scattering of electrons in III-N semiconductors (of “blue diodes”) driven away from equilibrium by electric fields of moderate to high intensities, are described.

Nonequilibrium Brownian Motion beyond the Effective Temperature

The condition of thermal equilibrium simplifies the theoretical treatment of fluctuations as found in the celebrated Einstein’s relation between mobility and diffusivity for Brownian motion. Several recent theories relax the hypothesis of thermal equilibrium resulting in at least two main scenarios. With well separated timescales, as in aging glassy systems, equilibrium Fluctuation-Dissipation Theorem applies at each scale with its own “effective” temperature. With mixed timescales, as for example in active or granular fluids or in turbulence, temperature is no more well-defined, the dynamical nature of fluctuations fully emerges and a Generalized Fluctuation-Dissipation Theorem (GFDT) applies. Here, we study experimentally the mixed timescale regime by studying fluctuations and linear response in the Brownian motion of a rotating intruder immersed in a vibro-fluidized granular medium. Increasing the packing fraction, the system is moved from a dilute single-timescale regime toward a denser multiple-timescale stage. Einstein’s relation holds in the former and is violated in the latter. The violation cannot be explained in terms of effective temperatures, while the GFDT is able to impute it to the emergence of a strong coupling between the intruder and the surrounding fluid. Direct experimental measurements confirm the development of spatial correlations in the system when the density is increased.