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Register a new userEffective temperatures from the fluctuation-dissipation measurements in soft glassy materials
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Added by
Sara Jabbari-Farouji
Publication date
2008
fields
Physics
and research's language is
English
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We have investigated the validity of the fluctuation-dissipation theorem (FDT) and the applicability of the concept of effective temperature in a number of non-equilibrium soft glassy materials. Using a combination of passive and active microrheology to measure displacement fluctuations and the mechanical response function of probe particles embedded in the materials, we have directly tested the validity of the FDT. Our results show no violation of the FDT over several decades in frequency (1-10$^4$ Hz) for hard sphere colloidal glasses and colloidal glasses and gels of Laponite. We further extended the bandwidth of our measurements to lower frequencies (down to 0.1 Hz) using video microscopy to measure the displacement fluctuations, again without finding any deviations from the FDT.
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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.
In order to perform numerical simulations of the KPZ equation, in any dimensionality, a spatial discretization scheme must be prescribed. The known fact that the KPZ equation can be obtained as a result of a Hopf--Cole transformation applied to a diffusion equation (with emph{multiplicative} noise) is shown here to strongly restrict the arbitrariness in the choice of spatial discretization schemes. On one hand, the discretization prescriptions for the Laplacian and the nonlinear (KPZ) term cannot be independently chosen. On the other hand, since the discretization is an operation performed on emph{space} and the Hopf--Cole transformation is emph{local} both in space and time, the former should be the same regardless of the field to which it is applied. It is shown that whereas some discretization schemes pass both consistency tests, known examples in the literature do not. The requirement of consistency for the discretization of Lyapunov functionals is argued to be a natural and safe starting point in choosing spatial discretization schemes. We also analyze the relation between real-space and pseudo-spectral discrete representations. In addition we discuss the relevance of the Galilean invariance violation in these consistent discretization schemes, and the alleged conflict of standard discretization with the fluctuation--dissipation theorem, peculiar of 1D.
We present a comprehensive study about the relationship between the way Detailed Balance is broken in non-equilibrium systems and the resulting violations of the Fluctuation-Dissipation Theorem. Starting from stochastic dynamics with both odd and even variables under Time-Reversal, we exploit the relation between entropy production and the breakdown of Detailed Balance to establish general constraints on the non-equilibrium steady-states (NESS), which relate the non-equilibrium character of the dynamics with symmetry properties of the NESS distribution. This provides a direct route to derive extended Fluctuation-Dissipation Relations, expressing the linear response function in terms of NESS correlations. Such framework provides a unified way to understand the departure from equilibrium of active systems and its linear response. We then consider two paradigmatic models of interacting self-propelled particles, namely Active Brownian Particles (ABP) and Active Ornstein-Uhlenbeck Particles (AOUP). We analyze the non-equilibrium character of these systems (also within a Markov and a Chapman-Enskog approximation) and derive extended Fluctuation-Dissipation Relations for them, clarifying which features of these active model systems are genuinely non-equilibrium.
We study the stationary dynamics of an active interacting Brownian particle system. We measure the violations of the fluctuation dissipation theorem, and the corresponding effective temperature, in a locally resolved way. Quite naturally, in the homogeneous phases the diffusive properties and effective temperature are also homogeneous. Instead, in the inhomogeneous phases (close to equilibrium and within the MIPS sector) the particles can be separated in two groups with different diffusion properties and effective temperatures. Notably, at fixed activity strength the effective temperatures in the two phases remain distinct and approximately constant within the MIPS region, with values corresponding to the ones of the whole system at the boundaries of this sector of the phase diagram. We complement the study of the globally averaged properties with the theoretical and numerical characterization of the fluctuation distributions of the single particle diffusion, linear response, and effective temperature in the homogeneous and inhomogeneous phases. We also distinguish the behavior of the (time-delayed) effective temperature from the (instantaneous) kinetic temperature, showing that the former is independent on the friction coefficient.
Soft glassy materials are out of thermodynamic equilibrium and show time dependent slowing down of the relaxation dynamics. Under such situation these materials follow Boltzmann superposition principle only in the effective time domain, wherein time dependent relaxation processes are scaled by a constant relaxation time. In this work we extend effective time framework to successfully demonstrate time - temperature superposition of creep and stress relaxation data of a model soft glassy system comprised of clay suspension. Such superposition is possible when average relaxation time of the material changes with time and temperature without affecting shape of the spectrum. We show that variation in relaxation time as a function of temperature facilitates prediction of long and short time rheological behavior through time - temperature superposition from the experiments carried out over experimentally accessible timescales.
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