Potential energy surface of monatomic liquids

Sjostrom, Travis; De Lorenzi-Venneri, Giulia; Wallace, Duane C.

doi:10.1103/physrevb.98.054201

Potential energy surface of monatomic liquids

Journal Article · Thu Aug 09 00:00:00 EDT 2018 · Physical Review. B

DOI:https://doi.org/10.1103/physrevb.98.054201· OSTI ID:1659169

^[1]; De Lorenzi-Venneri, Giulia ^[1]; Wallace, Duane C. ^[1]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

In the last decade, significant progress has been made in the many-body Hamiltonian formulation of liquid dynamics theory. Earlier analysis of experimental data for a wide variety of elemental liquids had provided the reliable but qualitative description of the atomic motion: vibrations in a representative 3N -dimensional potential energy valley, plus transits, in which atoms cross the intersections between these valleys. Recent comparisons of first-principles theory with experiment for several elemental liquids at melt revealed a highly accurate and versatile theory. In the present work, we report on an extensive quench study of the entire condensed-matter structure-energy distribution for a metallic Na MD system. With these results, all that was learned from experimental data is confirmed, refined in detail, and made more accurate. Here, we show the entire structure-energy distribution, composed of widespread symmetrics and higher lying randoms, we show the increasing dominance of the randoms as N increases, until the symmetrics vanish completely, and we show the random distribution continue its spectacular narrowing as N continues to increase. This behavior certifies our early assignment of the random distribution to the liquid phase and our prediction of macroscopic uniformity of the random structures. Procedures are discussed to identify and calibrate a single random structure to represent the liquid, and the role of the structure energy in liquid thermodynamics is described. A comparison with other liquid dynamics theories is observed in the Introduction, and the relation to the equation-of-state program is noted in the Conclusion.

View Accepted Manuscript (DOE)

Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: 89233218CNA000001; AC52-06NA25396

OSTI ID:: 1659169

Alternate ID(s):: OSTI ID: 1463766

Report Number(s):: LA-UR--18-25275

Journal Information:: Physical Review. B, Journal Name: Physical Review. B Journal Issue: 5 Vol. 98; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

References (32)

Electron-ion pseudopotentials in metals Ashcroft, N. W. Physics Letters, Vol. 23, Issue 1 https://doi.org/10.1016/0031-9163(66)90251-4	journal	October 1966
Non-perturbative treatment of strongly-interacting fields: Insights from liquid theory Trachenko, K.; Brazhkin, V. V. Annals of Physics, Vol. 347 https://doi.org/10.1016/j.aop.2014.04.025	journal	August 2014
Modified Van der Waals equation and law of corresponding states Zhong, Wei; Xiao, Changming; Zhu, Yongkai Physica A: Statistical Mechanics and its Applications, Vol. 471 https://doi.org/10.1016/j.physa.2016.12.029	journal	April 2017
The phonon theory of liquid thermodynamics Bolmatov, D.; Brazhkin, V. V.; Trachenko, K. Scientific Reports, Vol. 2, Issue 1 https://doi.org/10.1038/srep00421	journal	May 2012
A high‐density fluid‐perturbation theory based on an inverse 12th‐power hard‐sphere reference system Ross, Marvin The Journal of Chemical Physics, Vol. 71, Issue 4 https://doi.org/10.1063/1.438501	journal	August 1979
Perturbation theory and the thermodynamic properties of fluids. I. General theory Kerley, Gerald I. The Journal of Chemical Physics, Vol. 73, Issue 1 https://doi.org/10.1063/1.439842	journal	July 1980
Perturbation theory and the thermodynamic properties of fluids. III. Inverse‐power and 6–12 potentials Kerley, Gerald I. The Journal of Chemical Physics, Vol. 73, Issue 1 https://doi.org/10.1063/1.439844	journal	July 1980
Perturbation theory and the thermodynamic properties of fluids. II. The CRIS model Kerley, Gerald I. The Journal of Chemical Physics, Vol. 73, Issue 1 https://doi.org/10.1063/1.439898	journal	July 1980
Melting at high Pressures Stishov, Sergei M. Soviet Physics Uspekhi, Vol. 11, Issue 6 https://doi.org/10.1070/PU1969v011n06ABEH003777	journal	June 1969
Liquid state theories and critical phenomena Parola, Alberto; Reatto, Luciano Advances in Physics, Vol. 44, Issue 3 https://doi.org/10.1080/00018739500101536	journal	June 1995
A generic model for the ionic contribution to the equation of state Johnson, J. D. High Pressure Research, Vol. 6, Issue 5 https://doi.org/10.1080/08957959108203212	journal	December 1991
Collective modes and thermodynamics of the liquid state Trachenko, K.; Brazhkin, V. V. Reports on Progress in Physics, Vol. 79, Issue 1 https://doi.org/10.1088/0034-4885/79/1/016502	journal	December 2015
Fitting of a multiphase equation of state with swarm intelligence Cox, G. A.; Christie, M. A. Journal of Physics: Condensed Matter, Vol. 27, Issue 40 https://doi.org/10.1088/0953-8984/27/40/405201	journal	September 2015
Atomic motion from the mean square displacement in a monatomic liquid Wallace, Duane C.; De Lorenzi-Venneri, Giulia; Chisolm, Eric D. Journal of Physics: Condensed Matter, Vol. 28, Issue 18 https://doi.org/10.1088/0953-8984/28/18/185101	journal	April 2016
V-T theory for the self-intermediate scattering function in a monatomic liquid Wallace, Duane C.; Chisolm, Eric D.; De Lorenzi-Venneri, Giulia Journal of Physics: Condensed Matter, Vol. 29, Issue 5 https://doi.org/10.1088/1361-648X/29/5/055101	journal	December 2016
Dynamics, thermodynamics and structure of liquids and supercritical fluids: crossover at the Frenkel line Fomin, Yu D.; Ryzhov, V. N.; Tsiok, E. N. Journal of Physics: Condensed Matter, Vol. 30, Issue 13 https://doi.org/10.1088/1361-648X/aaaf39	journal	March 2018
Entropy of Liquid Metals Wallace, D. C. Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 433, Issue 1889 https://doi.org/10.1098/rspa.1991.0067	journal	June 1991
Compressibility and Binding Energy of the Simple Metals Ashcroft, N. W.; Langreth, David C. Physical Review, Vol. 155, Issue 3 https://doi.org/10.1103/PhysRev.155.682	journal	March 1967
Pseudopotential Calculation of the Thermal Expansion Coefficient of Sodium and Potassium Wallace, Duane C. Physical Review, Vol. 176, Issue 3 https://doi.org/10.1103/PhysRev.176.832	journal	December 1968
Test of a theoretical equation of state for elemental solids and liquids Chisolm, Eric D.; Crockett, Scott D.; Wallace, Duane C. Physical Review B, Vol. 68, Issue 10 https://doi.org/10.1103/PhysRevB.68.104103	journal	September 2003
Heat capacity of liquids: An approach from the solid phase Trachenko, Kostya Physical Review B, Vol. 78, Issue 10 https://doi.org/10.1103/PhysRevB.78.104201	journal	September 2008
Structure discovery for metallic glasses using stochastic quenching Holmström, E.; Bock, N.; Peery, T. Physical Review B, Vol. 82, Issue 2 https://doi.org/10.1103/PhysRevB.82.024203	journal	July 2010
Liquid-state properties from first-principles density functional theory calculations: Static properties Bock, Nicolas; Holmström, Erik; Peery, Travis B. Physical Review B, Vol. 82, Issue 14 https://doi.org/10.1103/PhysRevB.82.144101	journal	October 2010
Application of density functional theory calculations to the statistical mechanics of normal and anomalous melting Rudin, Sven P.; Bock, Nicolas; Wallace, Duane C. Physical Review B, Vol. 90, Issue 17 https://doi.org/10.1103/PhysRevB.90.174109	journal	November 2014
Multiphase aluminum equations of state via density functional theory Sjostrom, Travis; Crockett, Scott; Rudin, Sven Physical Review B, Vol. 94, Issue 14 https://doi.org/10.1103/PhysRevB.94.144101	journal	October 2016
Statistical mechanics of monatomic liquids Wallace, Duane C. Physical Review E, Vol. 56, Issue 4 https://doi.org/10.1103/PhysRevE.56.4179	journal	October 1997
Nature of the many-particle potential in the monatomic liquid state: Energetics, kinetics, and stability Wallace, D. C.; Clements, B. E. Physical Review E, Vol. 59, Issue 3 https://doi.org/10.1103/PhysRevE.59.2942	journal	March 1999
Improved model for the transit entropy of monatomic liquids Wallace, Duane C.; Chisolm, Eric D.; Bock, Nicolas Physical Review E, Vol. 79, Issue 5 https://doi.org/10.1103/PhysRevE.79.051201	journal	May 2009
Ab initio method for locating characteristic potential-energy minima of liquids Holmström, E.; Bock, N.; Peery, Travis B. Physical Review E, Vol. 80, Issue 5 https://doi.org/10.1103/PhysRevE.80.051111	journal	November 2009
Statistical mechanics model for the transit free energy of monatomic liquids Wallace, Duane C.; Chisolm, Eric D.; Bock, N. Physical Review E, Vol. 81, Issue 4 https://doi.org/10.1103/PhysRevE.81.041201	journal	April 2010
Emergence and Evolution of the k Gap in Spectra of Liquid and Supercritical States Yang, C.; Dove, M. T.; Brazhkin, V. V. Physical Review Letters, Vol. 118, Issue 21 https://doi.org/10.1103/PhysRevLett.118.215502	journal	May 2017
Wide-range multiphase equation of state for iron Medvedev, A. B. Combustion, Explosion, and Shock Waves, Vol. 50, Issue 5 https://doi.org/10.1134/S0010508214050141	journal	September 2014

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