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Measuring the Densities of Aqueous Glasses at Cryogenic Temperatures
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Stability of supercooled binary liquid mixtures.

Søren Toxvaerd1, Ulf R Pedersen, Thomas B Schrøder

  • 1Department of Sciences, DNRF Centre Glass and Time, IMFUFA, Roskilde University, P.O. Box 260, DK-4000 Roskilde, Denmark. st@ruc.dk

The Journal of Chemical Physics
|June 18, 2009
PubMed
Summary
This summary is machine-generated.

Supercooled binary mixtures can crystallize, but a new Weeks-Chandler-Andersen potential model prevents crystallization, enabling faster simulations. This research explores the thermodynamic stability and crystallization kinetics of these mixtures.

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Area of Science:

  • Thermodynamics
  • Materials Science
  • Computational Chemistry

Background:

  • Supercooled binary Lennard-Jones mixtures have shown partial crystallization into MgZn(2) or pure fcc crystals in simulations.
  • Understanding the stability and crystallization kinetics of these systems is crucial for materials design and simulation efficiency.

Purpose of the Study:

  • To provide a general thermodynamic and kinetic treatment for the stability of supercooled binary mixtures.
  • To investigate the crystallization behavior of a modified Kob-Andersen binary Lennard-Jones mixture.
  • To propose a new binary mixture less prone to crystallization and faster to simulate.

Main Methods:

  • Molecular dynamics simulations were employed to study the crystallization of binary Lennard-Jones mixtures.
  • A general thermodynamic and kinetic theory was developed, emphasizing the role of negative mixing enthalpy.
  • A new Weeks-Chandler-Andersen type potential was proposed by modifying interactions.

Main Results:

  • The modified Kob-Andersen mixture was observed to form pure fcc crystals of the majority component.
  • Crystallization time for a Kob-Andersen mixture at T=0.40 was estimated to be 5x10^7 time units (approx. 0.1 ms).
  • A new binary Lennard-Jones mixture, free from like-particle attractions, was proposed.

Conclusions:

  • Negative mixing enthalpy is a key factor in the stability of supercooled binary mixtures.
  • The proposed Weeks-Chandler-Andersen type mixture offers a route to faster simulations by avoiding crystallization.
  • This work contributes to understanding and controlling crystallization in binary mixtures for computational efficiency.