Critical assessment of the equilibrium melting-based, energy distribution theory of supercooled liquids and application to jammed systems

Weingartner, Nicholas B.; Pueblo, Chris; Kelton, K. F.; Nussinov, Zohar

doi:10.48550/arxiv.1512.04565

Cited by 5 publications

(17 citation statements)

References 73 publications

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“…Similar trends (made evident in Fig. 9) are also visible at temperatures above the (typically) higher temperature crossover temperature [38,[42][43][44][45]. The astute reader may note from these figures that for water, at extremely high temperatures, some of these trends are reversed.…”

Section: Usually At Far Higher Temperatures As Well)supporting

confidence: 72%

“…(In the Appendix, in Fig. 8, we present the same data for temperatures larger than a, typically, higher temperature associated with earlier fits [38,[42][43][44][45].) Similarly, in Fig.…”

Section: Hallmarks Of Deviations From Simple Activated Dynamics In Eq...mentioning

confidence: 64%

“…( 8) for all temperatures above the liquidus temperature as well as the scaling temperature discussed in the Introduction. ) The determination of a crossover temperature [38,[42][43][44][45]. Similar to the analysis in [38] for other metallic liquids (and glass formers in particular), we compare viscosity data of Zr 80 Pt 20 to the Arrhenius form of Eq.…”

Section: The Studied Liquids and General Aspects Of The Data Analysismentioning

confidence: 92%

“…9 of the Appendix we display the derivative of Eq. (10) for temperatures > , larger than the posited crossover temperature of earlier approaches [38,[42][43][44][45]. )…”

Section: Hallmarks Of Deviations From Simple Activated Dynamics In Eq...mentioning

confidence: 98%

“…( 5) is assumed. These tests will enable us to comment on the high temperature limits of various well known fits to the viscosity of glass forming liquids, e.g., [38,[42][43][44][45]. Various notable works advanced and tested various (kinematic) viscosity fits, e.g., [46].…”

Section: Introductionmentioning

confidence: 99%

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Deviations from Arrhenius dynamics in high temperature liquids, a possible collapse, and a viscosity bound

Xue¹,

Nogueira²,

Kelton³

et al. 2021

Preprint

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Liquids realize a highly complex state of matter in which strong competing kinetic and interaction effects come to life. As such, liquids are, generally, more challenging to understand than either gases or solids. In weakly interacting gases, the kinetic effects dominate. By contrast, low temperature solids typically feature far smaller fluctuations about their ground state. Notwithstanding their complexity, with the exception of quantum fluids (e.g., superfluid Helium) and supercooled liquids (including glasses), various aspects of common liquid dynamics such as their dynamic viscosity are often assumed to be given by rather simple, Arrhenius-type, activated forms with nearly constant (i.e., temperature independent) energy barriers. In this work, we analyze experimentally measured viscosities of numerous liquids far above their equilibrium melting temperature to see how well this assumption fares. We find marked deviations from simple activated dynamics. Even far above their equilibrium melting temperatures, as the temperature drops, the viscosity of these liquids increases more strongly than predicted by activated dynamics dominated by a single uniform energy barrier. For metallic fluids, the scale of the prefactor in the Arrhenius form for the viscosity is consistent with that given by the product ( ℎ) with the number density and ℎ Planck's constant. More generally, in all fluids (whether metallic or non-metallic), ( ℎ) constitutes a lower bound on the viscosity. We find that a scaling of the temperature axis (complementing that of the viscosity) leads to a partial collapse of the temperature dependent viscosities of different fluids; such a scaling allows for a functional dependence of the viscosity on temperature that includes yet is far more general than activated Arrhenius form alone. We speculate on relations between non-Arrhenius dynamics and thermodynamic observables.

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Section: Usually At Far Higher Temperatures As Well)supporting

confidence: 72%

“…(In the Appendix, in Fig. 8, we present the same data for temperatures larger than a, typically, higher temperature associated with earlier fits [38,[42][43][44][45].) Similarly, in Fig.…”

Section: Hallmarks Of Deviations From Simple Activated Dynamics In Eq...mentioning

confidence: 64%

Section: The Studied Liquids and General Aspects Of The Data Analysismentioning

confidence: 92%

“…9 of the Appendix we display the derivative of Eq. (10) for temperatures > , larger than the posited crossover temperature of earlier approaches [38,[42][43][44][45]. )…”

Section: Hallmarks Of Deviations From Simple Activated Dynamics In Eq...mentioning

confidence: 98%

Section: Introductionmentioning

confidence: 99%

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Deviations from Arrhenius dynamics in high temperature liquids, a possible collapse, and a viscosity bound

Xue¹,

Nogueira²,

Kelton³

et al. 2021

Preprint

Self Cite

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A one parameter fit for glassy dynamics as a quantum corollary of the liquid to solid transition

Nussinov

2017

Philosophical Magazine

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We apply microcanonical ensemble considerations to suggest that, whenever it may thermalize, a general disorder-free many-body Hamiltonian of a typical atomic system has solid-like eigenstates at low energies and fluid-type (and gaseous, plasma) eigenstates associated with energy densities exceeding those present in the melting (and, respectively, higher energy) transition(s). In particular, the lowest energy density at which the eigenstates of such a clean many body atomic system undergo a non-analytic change is that of the melting (or freezing) transition. We invoke this observation to analyze the evolution of a liquid upon supercooling (i.e., cooling rapidly enough to avoid solidification below the freezing temperature). Expanding the wavefunction of a supercooled liquid in the complete eigenbasis of the many-body Hamiltonian, only the higher energy liquid-type eigenstates contribute significantly to measurable hydrodynamic relaxations (e.g., those probed by viscosity) while static thermodynamic observables become weighted averages over both solid-and liquid-type eigenstates. Consequently, when extrapolated to low temperatures, hydrodynamic relaxation times of deeply supercooled liquids (i.e., glasses) may seem to diverge at nearly the same temperature at which the extrapolated entropy of the supercooled liquid becomes that of the solid. In this formal quantum framework, the increasingly sluggish (and spatially heterogeneous) dynamics in supercooled liquids as their temperature is lowered stems from the existence of the single non-analytic change of the eigenstates of the clean many-body Hamiltonian at the equilibrium melting transition present in low energy solid-type eigenstates. We derive a single (possibly computable) dimensionless parameter fit to the viscosity and suggest other testable predictions of our approach.

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Kinetic and structural fragility—a correlation between structures and dynamics in metallic liquids and glasses

Kelton

2016

J. Phys.: Condens. Matter

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The liquid phase remains poorly understood. In many cases, the densities of liquids and their crystallized solid phases are similar, but since they are amorphous they lack the spatial order of the solid. Their dynamical properties change remarkably over a very small temperature range. At high temperatures, near their melting temperature, liquids flow easily under shear. However, only a few hundred degrees lower flow effectively ceases, as the liquid transforms into a solid-like glass. This temperature-dependent dynamical behavior is frequently characterized by the concept of kinetic fragility (or, generally, simply fragility). Fragility is believed to be an important quantity in glass formation, making it of significant practical interest. The microscopic origin of fragility remains unclear, however, making it also of fundamental interest. It is widely (although not uniformly) believed that the dynamical behavior is linked to the atomic structure of the liquid, yet experimental studies show that although the viscosity changes by orders of magnitude with temperature, the structural change is barely perceptible. In this article the concept of fragility is discussed, building to a discussion of recent results in metallic glass-forming liquids that demonstrate the presumed connection between structural and dynamical changes. In particular, it becomes possible to define a structural fragility parameter that can be linked with the kinetic fragility.

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Critical assessment of the equilibrium melting-based, energy distribution theory of supercooled liquids and application to jammed systems

Cited by 5 publications

References 73 publications

Deviations from Arrhenius dynamics in high temperature liquids, a possible collapse, and a viscosity bound

Deviations from Arrhenius dynamics in high temperature liquids, a possible collapse, and a viscosity bound

A one parameter fit for glassy dynamics as a quantum corollary of the liquid to solid transition

Kinetic and structural fragility—a correlation between structures and dynamics in metallic liquids and glasses

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