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Morphometric Approach to Many-Body Correlations in Hard Spheres
Joshua F Robinson1, Francesco Turci1, Roland Roth2
1H. H. Wills Physics Laboratory, University of Bristol, Bristol BS8 1TL, United Kingdom.
Physical Review Letters
|March 2, 2019
Summary
We developed a new method to model the thermodynamics of local structures in hard sphere liquids. This approach accurately predicts free energies and dynamical barriers, revealing insights into liquid and supercooled states.
Area of Science:
- Thermodynamics
- Statistical Mechanics
- Computational Physics
Background:
- Understanding the thermodynamic properties of dense liquids is crucial.
- Hard sphere models provide a fundamental basis for liquid theory.
- Local structural arrangements significantly influence macroscopic properties.
Purpose of the Study:
- To develop a novel method for modeling the thermodynamics of local structures in hard sphere liquids.
- To accurately calculate free energies and predict dynamical barriers.
- To explore the free energy landscape at high volume fractions.
Main Methods:
- Morphometric calculation of n-body correlations.
- Modeling thermodynamics of local structures at arbitrary volume fractions.
- Quantitative comparison with molecular dynamics simulations.
Main Results:
- Excellent agreement between calculated and simulated free energies across liquid and supercooled regimes.
- Discovery of bimodality in the density of states: fivefold symmetric structures are lower in free energy than fourfold.
- Prediction of a dynamical barrier scaling linearly with the compressibility factor.
Conclusions:
- The morphometric method accurately models liquid and supercooled hard sphere systems.
- Local structure symmetry dictates free energy, with fivefold symmetry being more stable.
- This technique offers a new way to study free energy landscapes in dynamically inaccessible regimes.
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