Non-equilibrium relaxation and aging in the dynamics of a dipolar fluid quenched towards the glass transition

Peredo-Ortiz, Ricardo; Zubieta, Rico, Pablo F.; Cortés-Morales, Ernesto C.; Pérez-Ángel, Gabriel; Voigtmann, Thomas; Medina‐Noyola, Magdaleno; Elizondo-Aguilera, Luis Fernando

doi:10.1088/1361-648x/ac3b75

Cited by 8 publications

(7 citation statements)

References 74 publications

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“…A detailed characterization of this system has been provided recently in the context of the NE-SCGLE theory. 62 Here, we only bring together some of the most important elements in the context of our present discussion.…”

Section: The Tnm Model For Systems With Rotational-translational Dyna...mentioning

confidence: 99%

“…63 and 64 in terms of a set of equations describing the non-equilibrium evolution of the structural and dynamical properties of a system represented by Eq. ( 27) and has been systematically employed 62 to understand the dynamically arrested states already detected in extensive molecular dynamics (MD) simulations of this model. 65,66 We summarize the relevant ingredients of the non-spherical version of the NE-SCGLE theory in the Appendix.…”

Section: A Non-spherical Ne-scgle Theorymentioning

confidence: 99%

“…From symmetry considerations and within well-defined approximations, 62 only a finite subset of its isotropic and homogeneous diagonal components, denoted as S lm (k, t) ≡ S lm:lm (k, −k, t), are involved in the central NE-SCGLE, which reads 64…”

Section: A Non-spherical Ne-scgle Theorymentioning

confidence: 99%

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“Inner clocks” of glass-forming liquids

Peredo-Ortiz

Noyola

Voigtmann

et al. 2022

The Journal of Chemical Physics

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Providing a physically sound explanation of aging phenomena in non-equilibrium amorphous materialsis a challenging problem in modern statistical thermodynamics. The slow evolution of physical propertiesafter quenches of control parameters is empirically well interpreted via the concept of material time (orinternal clock), based on the Tool-Narayanaswamy-Moynihan (TNM) model. Yet, the fundamental reasonsof its striking success remain unclear. We propose a microscopic rationale behind the material time onthe basis of the linear laws of irreversible thermodynamics and its extension that treats the correspondingkinetic coefficients as state functions of a slowly evolving material state. Our interpretation is based onthe recognition that the same mathematical structure governs both the Tool model and the recently devel-oped non-equilibrium extension of the self-consistent generalized Langevin equation theory (NE-SCGLE),guided by the universal principles of Onsager's theory of irreversible processes. This identification opensthe way for a generalization of the material-time concept to aging systems where several relaxation modeswith very different equilibration processes must be considered, and partially frozen glasses manifest theappearance of partial ergodicity breaking, and hence materials with multiple very distinct inner clocks.

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Section: The Tnm Model For Systems With Rotational-translational Dyna...mentioning

confidence: 99%

Section: A Non-spherical Ne-scgle Theorymentioning

confidence: 99%

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“Inner clocks” of glass-forming liquids

Peredo-Ortiz

Noyola

Voigtmann

et al. 2022

The Journal of Chemical Physics

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“…Essentially, it partially decouples the evolution of the correlation functions from that of the underlying static response functions. The resulting theory tests favorably against both simulation [28,29,44] and experimental data [45][46][47].…”

mentioning

confidence: 97%

“…The initial state before the quench is S(k; 0) = S i (k), and S f (k) characterizes the quenched-to final state. Equation (1) essentially is a formalized extension of the empirical Tool-Narayanaswamy model of physical aging [53]. Equation (1) already predicts universal scaling laws for the aging dynamics to be encoded in the equilibrium dynamics: since the glass transition is a dynamical phenomenon, in its vicinity the static structure functions remain regular, and we can linearize S(k; t w ) for small control-parameter distances ε(t w ) to the transition.…”

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From sub-aging to hyper-aging in structural glasses

Elizondo-Aguilera¹,

Rizzo²,

Voigtmann³

2022

Preprint

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We demonstrate non-equilibrium scaling laws for the aging dynamics in glass formers that emerge from combining a recent application of Onsager's theory of irreversible processes with the equilibrium scaling laws of glassy dynamics. Different scaling regimes are predicted for the evolution of the system's structural relaxation time τ with age (waiting time tw), depending on the depth of the quench from the liquid into the glass: simple aging (τ ∼ tw) applies for quenches close to the critical point of mode-coupling theory (MCT) and implies sub-aging (τ ≈ t δ w with δ < 1) as a broad crossover for quenches to nearly-arrested equilibrium states; hyper-aging (or super-aging, τ ∼ t δ w with δ > 1) emerges for quenches deep into the glass. The latter is cut off by non-mean-field fluctuations that we account for within a recent extension of MCT, the stochastic β-relaxation theory (SBR). We exemplify the scaling laws by a schematic model that allows to quantitatively fit recent simulation results for density-quenched hard-sphere-like particles.

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Structural relaxation, dynamical arrest, and aging in soft-sphere liquids

Mendoza-Méndez

Peredo-Ortiz

Lázaro-Lázaro

et al. 2022

The Journal of Chemical Physics

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We investigate the structural relaxation of a soft-sphere liquid quenched isochorically (φ = 0.7) and instantaneously to different temperatures Tf above and below the glass transition. For this, we combine extensive Brownian dynamics simulations and theoretical calculations based on the non-equilibrium self-consistent generalized Langevin equation (NE-SCGLE) theory. The response of the liquid to a quench generally consists of a sub-linear increase of the α-relaxation time with system's age. Approaching the ideal glass-transition temperature from above (Tf > Ta ) sub-aging appears as a transient process describing a broad equilibration crossover for quenches to nearly arrested states. This allows us to empirically determine an equilibration timescale t eq(Tf) that becomes increasingly longer as Tf approaches Ta . For quenches inside the glass (Tf less than or equal to Ta) the growth rate of the structural relaxation time becomes progressively larger as Tf decreases and, unlike the equilibration scenario, τα remains evolving within the whole observation time-window. These features are consistently found in theory and simulations with remarkable semi-quantitative agreement, and coincide with those revealed in a previous and complementary study [Phys. Rev. 96, 022608 (2017)] that considered a sequence of quenches with fixed final temperature Tf = 0 but increasing φ towards the hard-sphere dynamical arrest volume fraction φ a HS = 0.582. The NESCGLE analysis, however, unveils various fundamental aspects of the glass transition, involving the abrupt passage from the ordinary equilibration scenario to the persistent aging effects that are characteristic of glass-forming liquids.

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Non-equilibrium relaxation and aging in the dynamics of a dipolar fluid quenched towards the glass transition

Cited by 8 publications

References 74 publications

“Inner clocks” of glass-forming liquids

“Inner clocks” of glass-forming liquids

From sub-aging to hyper-aging in structural glasses

Structural relaxation, dynamical arrest, and aging in soft-sphere liquids

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