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We study the dynamics of dense three-dimensional systems of active particles for large persistence times τp at constant average self-propulsion force f. These systems are fluid counterparts of previously investigated extremely persistent systems, which in the large persistence time limit relax only on the time scale of τp. We find that many dynamic properties of the systems we study, such as the mean-squared velocity, the self-intermediate scattering function, and the shear-stress correlation function, become τp-independent in the large persistence time limit. In addition, the large τp limits of many dynamic properties, such as the mean-square velocity and the relaxation times of the scattering function, and the shear-stress correlation function, depend on f as power laws with non-trivial exponents. We conjecture that these systems constitute a new class of extremely persistent active systems.
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Sampling the Boltzmann distribution using forces that violate detailed balance can be faster than with the equilibrium evolution, but the acceleration depends on the nature of the nonequilibrium drive and the physical situation. Here, we study the efficiency of forces transverse to energy gradients in dense liquids through a combination of techniques: Brownian dynamics simulations, exact infinite-dimensional calculation, and a mode-coupling approximation. We find that the sampling speedup varies nonmonotonically with temperature, and decreases as the system becomes more glassy. We characterize the interplay between the distance to equilibrium and the efficiency of transverse forces by means of odd transport coefficients.
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Low-frequency vibrational harmonic modes of glasses are frequently used to rationalize their universal low-temperature properties. One well studied feature is the excess low-frequency density of states over the Debye model prediction. Here, we examine the system size dependence of the density of states for two-dimensional glasses. For systems of fewer than 100 particles, the density of states scales with the system size as if all the modes were plane-wave-like. However, for systems greater than 100 particles, we find a different system-size scaling of the cumulative density of states below the first transverse sound mode frequency, which can be derived from the assumption that these modes are quasi-localized. Moreover, for systems greater than 100 particles, we find that the cumulative density of states scales with the frequency as a power law with the exponent that leads to the exponent ß = 3.5 for the density of states. For systems whose sizes were investigated, we do not see a size-dependence of exponent ß.
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This corrects the article DOI: 10.1103/PhysRevLett.127.248001.
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We propose an alternative theory for the relaxation of density fluctuations in glass-forming fluids. We derive an equation of motion for the density correlation function that is local in time and is similar in spirit to the equation of motion for the average non-uniform density profile derived within the dynamic density functional theory. We identify the Franz-Parisi free energy functional as the non-equilibrium free energy for the evolution of the density correlation function. An appearance of a local minimum of this functional leads to a dynamic arrest. Thus, the ergodicity breaking transition predicted by our theory coincides with the dynamic transition of the static approach based on the same non-equilibrium free energy functional.
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Sound attenuation in low-temperature amorphous solids originates from their disordered structure. However, its detailed mechanism is still being debated. Here, we analyze sound attenuation starting directly from the microscopic equations of motion. We derive an exact expression for the zero-temperature sound damping coefficient. We verify that the sound damping coefficients calculated from our expression agree very well with results from independent simulations of sound attenuation. Small wavevector analysis of our expression shows that sound attenuation is primarily determined by the non-affine displacements' contribution to the sound wave propagation coefficient coming from the frequency shell of the sound wave. Our expression involves only quantities that pertain to solids' static configurations. It can be used to evaluate the low-temperature sound damping coefficients without directly simulating sound attenuation.
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Translational dynamics of 2D glass-forming fluids is strongly influenced by soft, long-wavelength fluctuations first recognized by D. Mermin and H. Wagner. As a result of these fluctuations, characteristic features of glassy dynamics, such as plateaus in the mean-squared displacement and the self-intermediate scattering function, are absent in two dimensions. In contrast, Mermin-Wagner fluctuations do not influence orientational relaxation, and well-developed plateaus are observed in orientational correlation functions. It has been suggested that, by monitoring translational motion of particles relative to that of their neighbors, one can recover characteristic features of glassy dynamics and thus disentangle the Mermin-Wagner fluctuations from the 2D glass transition. Here we use molecular dynamics simulations to study viscoelastic relaxation in two and three dimensions. We find different behavior of the dynamic modulus below the onset of slow dynamics (determined by the orientational or cage-relative correlation functions) in two and three dimensions. The dynamic modulus for 2D supercooled fluids is more stretched than for 3D supercooled fluids and does not exhibit a plateau, which implies the absence of glassy viscoelastic relaxation. At lower temperatures, the 2D dynamic modulus starts exhibiting an intermediate time plateau and decays similarly to the 2D dynamic modulus. The differences in the glassy behavior of 2D and 3D glass-forming fluids parallel differences in the ordering scenarios in two and three dimensions.
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Glasses possess more low-frequency vibrational modes than predicted by Debye theory. These excess modes are crucial for the understanding of the low temperature thermal and mechanical properties of glasses, which differ from those of crystalline solids. Recent simulational studies suggest that the density of the excess modes scales with their frequency ω as ω^{4} in two and higher dimensions. Here, we present extensive numerical studies of two-dimensional model glass formers over a large range of glass stabilities. We find that the density of the excess modes follows D_{exc}(ω)â¼ω^{2} up to around the boson peak, regardless of the glass stability. The stability dependence of the overall scale of D_{exc}(ω) correlates with the stability dependence of low-frequency sound attenuation. However, we also find that, in small systems, where the first sound mode is pushed to higher frequencies, at frequencies below the first sound mode, there are excess modes with a system size independent density of states that scales as ω^{3}.
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We derive a distribution function for the position of a tagged active particle in a slowly varying in space external potential, in a system of interacting active particles. The tagged particle distribution has the form of the Boltzmann distribution but with an effective temperature that replaces the temperature of the heat bath. We show that the effective temperature that enters the tagged particle distribution is the same as the effective temperature defined through the Einstein relation, i.e., it is equal to the ratio of the self-diffusion and tagged particle mobility coefficients. This result shows that this effective temperature, which is defined through a fluctuation-dissipation ratio, is relevant beyond the linear response regime. We verify our theoretical findings through computer simulations. Our theory fails when an additional large length scale appears in our active system. In the system we simulated, this length scale is associated with long-wavelength density fluctuations that emerge upon approaching motility-induced phase separation.
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The universal anomalous vibrational and thermal properties of amorphous solids are believed to be related to the local variations of the elasticity. Recently it has been shown that the vibrational properties are sensitive to the glass's stability. Here we study the stability dependence of the local elastic constants of a simulated glass former over a broad range of stabilities, from a poorly annealed glass to a glass whose stability is comparable to laboratory exceptionally stable vapor deposited glasses. We show that with increasing stability the glass becomes more uniform as evidenced by a smaller variance of local elastic constants. We find that, according to the definition of local elastic moduli used in this work, the local elastic moduli are not spatially correlated.
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The temperature dependence of the thermal conductivity is linked to the nature of the energy transport at a frequency ω, which is quantified by thermal diffusivity d(ω). Here we study d(ω) for a poorly annealed glass and a highly stable glass prepared using the swap Monte Carlo algorithm. To calculate d(ω), we excite wave packets and find that the energy moves diffusively for high frequencies up to a maximum frequency, beyond which the energy stays localized. At intermediate frequencies, we find a linear increase of the square of the width of the wave packet with time, which allows for a robust calculation of d(ω), but the wave packet is no longer well described by a Gaussian as for high frequencies. In this intermediate regime, there is a transition from a nearly frequency independent thermal diffusivity at high frequencies to d(ω) â¼ ω-4 at low frequencies. For low frequencies the sound waves are responsible for energy transport and the energy moves ballistically. The low frequency behavior can be predicted using sound attenuation coefficients.
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The temperature dependence of the thermal conductivity of amorphous solids is markedly different from that of their crystalline counterparts, but exhibits universal behaviour. Sound attenuation is believed to be related to this universal behaviour. Recent computer simulations demonstrated that in the harmonic approximation sound attenuation Γ obeys quartic, Rayleigh scattering scaling for small wavevectors k and quadratic scaling for wavevectors above the Ioffe-Regel limit. However, simulations and experiments do not provide a clear picture of what to expect at finite temperatures where anharmonic effects become relevant. Here we study sound attenuation at finite temperatures for model glasses of various stability, from unstable glasses that exhibit rapid aging to glasses whose stability is equal to those created in laboratory experiments. We find several scaling laws depending on the temperature and stability of the glass. First, we find the large wavevector quadratic scaling to be unchanged at all temperatures. Second, we find that at small wavevectors Γâ¼k1.5 for an aging glass, but Γâ¼k2 when the glass does not age on the timescale of the calculation. For our most stable glass, we find that Γâ¼k2 at small wavevectors, then a crossover to Rayleigh scattering scaling Γâ¼k4, followed by another crossover to the quadratic scaling at large wavevectors. Our computational observation of this quadratic behavior reconciles simulation, theory and experiment, and will advance the understanding of the temperature dependence of thermal conductivity of glasses.
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Understanding the difference between the universal low-temperature properties of amorphous and crystalline solids requires an explanation for the stronger damping of long-wavelength phonons in amorphous solids. A longstanding sound attenuation scenario, resulting from a combination of experiments, theories, and simulations, leads to a quartic scaling of sound attenuation with the wavevector, which is commonly attributed to the Rayleigh scattering of sound. Modern computer simulations offer conflicting conclusions regarding the validity of this picture. We simulate glasses with an unprecedentedly broad range of stabilities to perform the first microscopic analysis of sound damping in model glass formers across a range of experimentally relevant preparation protocols. We present convincing evidence that quartic scaling is recovered for small wavevectors irrespective of the glass's stability. With increasing stability, the wavevector where the quartic scaling begins increases by approximately a factor of three and the sound attenuation decreases by over an order of magnitude. Our results uncover an intimate connection between glass stability and sound damping.
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We present a theory for the steady-state dynamics of a two-dimensional system of spherically symmetric active Brownian particles. The derivation of the theory consists of two steps. First, we integrate out the self-propulsions and obtain a many-particle evolution equation for the probability distribution of the particles' positions. Second, we use the projection operator technique and a mode-coupling-like factorization approximation to derive an equation of motion for the density correlation function. The nonequilibrium character of the active system manifests itself through the presence of a steady-state correlation function that quantifies spatial correlations of microscopic steady-state currents of the particles. This function determines the dependence of the short-time dynamics on the activity. It also enters into the expression for the memory matrix and thus influences the long-time glassy dynamics.
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Despite the diversity of materials designated as active matter, virtually all active systems undergo a form of dynamic arrest when crowding and activity compete, reminiscent of the dynamic arrest observed in colloidal and molecular fluids undergoing a glass transition. We present a short perspective on recent and ongoing efforts to understand how activity competes with other physical interactions in dense systems. We review recent experimental work on active materials that uncovered both classic signatures of glassy dynamics and intriguing novel phenomena at large density. We discuss a minimal model of self-propelled particles where the competition between interparticle interactions, crowding, and self-propulsion can be studied in great detail. We present more complex models that include some additional, material-specific ingredients. We provide some general perspectives on dense active materials, suggesting directions for future research, in particular, for theoretical work.
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Glasses prepared by vapor depositing molecules onto a properly prepared substrate can have enhanced kinetic stability when compared with glasses prepared by cooling from the liquid state. The enhanced stability is due to the high mobility of particles at the surface, which allows them to find lower energy configurations than for liquid cooled glasses. Here we use molecular dynamics simulations to examine the temperature dependence of the single particle dynamics in the bulk of the film and at the surface of the film. First, we examine the temperature dependence of the self-intermediate scattering functions for particles in the bulk and at the surface. We then examine the temperature dependence of the probability of the logarithm of single particle displacements for bulk and surface particles. Both bulk and surface particle displacements indicate populations of slow and fast particles, i.e., heterogeneous dynamics. We find that the temperature dependence of the surface dynamics mirrors the bulk despite being several orders of magnitude faster.
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The Stokes-Einstein relation (SER) is one of the most robust and widely employed results from the theory of liquids. Yet sizable deviations can be observed for self-solvation, which cannot be explained by the standard hydrodynamic derivation. Here, we revisit the work of Masters and Madden [J. Chem. Phys. 74, 2450-2459 (1981)], who first solved a statistical mechanics model of the SER using the projection operator formalism. By generalizing their analysis to all spatial dimensions and to partially structured solvents, we identify a potential microscopic origin of some of these deviations. We also reproduce the SER-like result from the exact dynamics of infinite-dimensional fluids.
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We propose a simple theory for the dynamics of model glass-forming fluids, which should be solvable using a mean-field-like approach. The theory is based on transparent physical assumptions, which can be tested in computer simulations. The theory predicts an ergodicity-breaking transition that is identical to the so-called dynamic transition predicted within the replica approach. Thus, it can provide the missing dynamic component of the random first order transition framework. In the large-dimensional limit the theory reproduces the result of a recent exact calculation of Maimbourg et al. [Phys. Rev. Lett. 116, 015902 (2016)PRLTAO0031-900710.1103/PhysRevLett.116.015902]. Our approach provides an alternative, physically motivated derivation of this result.
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We study the glassy dynamics taking place in dense assemblies of athermal active particles that are driven solely by a nonequilibrium self-propulsion mechanism. Active forces are modeled as an Ornstein-Uhlenbeck stochastic process, characterized by a persistence time and an effective temperature, and particles interact via a Lennard-Jones potential that yields well-studied glassy behavior in the Brownian limit, which is obtained as the persistence time vanishes. By increasing the persistence time, the system departs more strongly from thermal equilibrium and we provide a comprehensive numerical analysis of the structure and dynamics of the resulting active fluid. Finite persistence times profoundly affect the static structure of the fluid and give rise to nonequilibrium velocity correlations that are absent in thermal systems. Despite these nonequilibrium features, for any value of the persistence time we observe a nonequilibrium glass transition as the effective temperature is decreased. Surprisingly, increasing departure from thermal equilibrium is found to promote (rather than suppress) the glassy dynamics. Overall, our results suggest that with increasing persistence time, microscopic properties of the active fluid change quantitatively, but the general features of the nonequilibrium glassy dynamics observed with decreasing the effective temperature remain qualitatively similar to those of thermal glass-formers.
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We use computer simulations to study the cooling rate dependence of the stability and energetics of model glasses created at constant pressure conditions and compare the results with glasses formed at constant volume conditions. To examine the stability, we determine the time it takes for a glass cooled and reheated at constant pressure to transform back into a liquid, ttrans, and calculate the stability ratio S=ttrans/τα, where τα is the equilibrium relaxation time of the liquid. We find that, for slow enough cooling rates, cooling and reheating at constant pressure results in a larger stability ratio S than for cooling and reheating at constant volume. We also compare the energetics of glasses obtained by cooling while maintaining constant pressure with those of glasses created by cooling from the same state point while maintaining constant volume. We find that cooling at constant pressure results in glasses with lower average potential energy and average inherent structure energy. We note that in model simulations of the vapor deposition process, glasses are created under constant pressure conditions, and thus they should be compared to glasses obtained by constant pressure cooling.