Inherent Structure Entropy of Supercooled Liquids

Sciortino, Francesco; Kob, Walter; Tartaglia, P.

doi:10.1103/physrevlett.83.3214

Cited by 441 publications

(583 citation statements)

References 40 publications

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“…Since this relation is proposed to be valid in the limit of low T , it is a useful relation for studying the properties of a deeply supercooled liquid. Notably, several recent works showed that this prediction is obeyed at low T for binary LennardJones liquids [47,48,49]. This observation provided a physical basis for extrapolating U (and thermodynamic properties derived from it) to T near T g , and so made possible determination of the Kauzmann temperature for this system.…”

Section: Introductionmentioning

confidence: 96%

Computer simulations of liquid silica: Equation of state and liquid–liquid phase transition

Saika‐Voivod¹,

Sciortino²,

Poole³

2000

Phys. Rev. E

243

231

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We conduct extensive molecular dynamics computer simulations of two models for liquid silica [the model of Woodcock, Angell and Cheeseman, J. Phys. Chem. 65, 1565Chem. 65, (1976; and that of van Beest, Kramer and van Santen, Phys. Rev. Lett. 64, 1955, (1990)] to determine their thermodynamic properties at low temperature T across a wide density range. We find for both models a wide range of states in which isochores of the potential energy U are a linear function of T 3/5 , as recently proposed for simple liquids [Rosenfeld and P. Tarazona, Mol. Phys. 95, 141 (1998)]. We exploit this behavior to fit an accurate equation of state to our thermodynamic data. Extrapolation of this equation of state to low T predicts the occurrence of a liquid-liquid phase transition for both models. We conduct simulations in the region of the predicted phase transition, and confirm its existence by direct observation of phase separating droplets of atoms with distinct local density and coordination environments.

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Section: Introductionmentioning

confidence: 96%

Computer simulations of liquid silica: Equation of state and liquid–liquid phase transition

Saika‐Voivod¹,

Sciortino²,

Poole³

2000

Phys. Rev. E

243

231

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“…43,44 For solids and certain fluid states, the system can be assumed to spend the majority of its time in one of the local minima, only occasionally making excursions over the saddles separating the minima. Based on these ideas, as applied in previous work on supercooled liquids and glasses, 45,46 a direct computational approach for measuring the total ͑classical͒ free energy of a defect cluster has been developed; a brief discussion of the method is provided here and further details are given in Ref. 38.…”

Section: Computational Framework For Single Cluster Thermodynamicmentioning

confidence: 99%

Detailed microscopic analysis of self-interstitial aggregation in silicon. II. Thermodynamic analysis of single clusters

2010

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We analyze results generated by large-scale molecular-dynamics simulations of self-interstitial clusters in crystalline silicon using a recently developed computational method for probing the thermodynamics of defects in solids. In this approach, the potential-energy landscape is sampled with lengthy moleculardynamics simulations and repeated energy minimizations in order to build distribution functions that quantitatively describe the formation thermodynamics of a particular defect cluster. Using this method, a comprehensive picture for interstitial aggregation is proposed. In particular, we find that both vibrational and configuration entropic factors play important roles in determining self-interstitial cluster morphology. In addition to the expected role of temperature, we also find that applied (hydrostatic) pressure and the commensurate lattice strain greatly influence the resulting aggregation pathways. Interestingly, the effect of pressure appears to manifest not by altering the thermodynamics of individual defect configurations but rather by changing the overall energy landscape associated with the defect. These effects appear to be general and are predicted using multiple, well-tested, empirical interatomic potentials for silicon. Our results suggest that internal stress environments within a silicon wafer (e.g., created by ion implantation) could have profound effects on the observed selfinterstitial cluster morphology. We analyze results generated by large-scale molecular-dynamics simulations of self-interstitial clusters in crystalline silicon using a recently developed computational method for probing the thermodynamics of defects in solids. In this approach, the potential-energy landscape is sampled with lengthy molecular-dynamics simulations and repeated energy minimizations in order to build distribution functions that quantitatively describe the formation thermodynamics of a particular defect cluster. Using this method, a comprehensive picture for interstitial aggregation is proposed. In particular, we find that both vibrational and configuration entropic factors play important roles in determining self-interstitial cluster morphology. In addition to the expected role of temperature, we also find that applied ͑hydrostatic͒ pressure and the commensurate lattice strain greatly influence the resulting aggregation pathways. Interestingly, the effect of pressure appears to manifest not by altering the thermodynamics of individual defect configurations but rather by changing the overall energy landscape associated with the defect. These effects appear to be general and are predicted using multiple, well-tested, empirical interatomic potentials for silicon. Our results suggest that internal stress environments within a silicon wafer ͑e.g., created by ion implantation͒ could have profound effects on the observed selfinterstitial cluster morphology. Disciplines Biochemical and Biomolecular Engineering | Chemical Engineering | Engineering

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“…Qualitatively, one may say that TLS probe the PEL on a very local scale whereas for the understanding of the glass transition much larger regions of the PEL are relevant. Here we would like to mention that in recent years computer simulations succeeded in extracting many important features of the PEL of supercooled liquids [26,27,28,29,30,31,32,33,34].…”

Section: Introductionmentioning

confidence: 99%

Local properties of the potential-energy landscape of a model glass: Understanding the low-temperature anomalies

Reinisch

Heuer

2004

Phys. Rev. B

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Though the existence of two-level systems (TLS) is widely accepted to explain low temperature anomalies in the sound absorption, heat capacity, thermal conductivity and other quantities, an exact description of their microscopic nature is still lacking. We performed computer simulations for a binary Lennard-Jones system, using a newly developed algorithm to locate double-well potentials (DWP) and thus two-level systems on a systematic basis. We show that the intrinsic limitations of computer simulations like finite time and finite size problems do not hamper this analysis. We discuss how the DWP are embedded in the total potential energy landscape. It turns out that most DWP are connected to the dynamics of the smaller particles and that these DWP are rather localized. However, DWP related to the larger particles are more collective.

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Inherent Structure Entropy of Supercooled Liquids

Cited by 441 publications

References 40 publications

Computer simulations of liquid silica: Equation of state and liquid–liquid phase transition

Computer simulations of liquid silica: Equation of state and liquid–liquid phase transition

Detailed microscopic analysis of self-interstitial aggregation in silicon. II. Thermodynamic analysis of single clusters

Local properties of the potential-energy landscape of a model glass: Understanding the low-temperature anomalies

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