atomic liquids
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2020 ◽  
Author(s):  
Jan-Michael Mewes ◽  
Odile Smits

<div>The normal boiling point (NBP) is a fundamental property of liquids and marks the intersection of the Gibbs energies of the liquid and the gas phase at ambient pressure.</div><div>This work provides the first comprehensive demonstration of the calculation of boiling points of atomic liquids through first-principles molecular-dynamics simulations.</div><div>To this end, thermodynamic integration (TDI) and perturbation theory (TPT) are combined with a density-functional theory (DFT) Hamiltonian, which provides absolute Gibbs energies, internal energies, and entropies of atomic liquids with an accuracy of a few meV/atom. </div><div>Linear extrapolation to the intersection with the Gibbs energy of a non-interacting gas phase eventually pins-down the NBPs. While these direct results can already be quite accurate, they are susceptible to a systematic over- or underbinding of the employed density functional. We show how the resulting errors can be strongly reduced by increasing the robustness of the method through a simple linear correction based on a high-level theoretical or experimental cohesive energy termed $\lambda$-scaling.</div><div>By carefully tuning the technical parameters, the walltime per element could be reduced from weeks to about a day (10-20k core-hours), which enabled extensive testing for B, Al, Na, K, Ca, Sr, Ba, Mn, Cu, Xe and Hg. </div><div>This comprehensive benchmark demonstrates the excellent performance and robustness of the approach with a mean absolute deviation (MAD) of less than 2% from experimental NBPs and very similar accuracy for liquid entropies (MAD 2.3 J/(mol*K), 2% relative). In some cases, the uncertainty in the predictions are several times smaller than the variation between literature values, allowing us to clear out ambiguities in the NBPs of B and Ba.</div>


2020 ◽  
Author(s):  
Jan-Michael Mewes ◽  
Odile Smits

<div>The normal boiling point (NBP) is a fundamental property of liquids and marks the intersection of the Gibbs energies of the liquid and the gas phase at ambient pressure.</div><div>This work provides the first comprehensive demonstration of the calculation of boiling points of atomic liquids through first-principles molecular-dynamics simulations.</div><div>To this end, thermodynamic integration (TDI) and perturbation theory (TPT) are combined with a density-functional theory (DFT) Hamiltonian, which provides absolute Gibbs energies, internal energies, and entropies of atomic liquids with an accuracy of a few meV/atom. </div><div>Linear extrapolation to the intersection with the Gibbs energy of a non-interacting gas phase eventually pins-down the NBPs. While these direct results can already be quite accurate, they are susceptible to a systematic over- or underbinding of the employed density functional. We show how the resulting errors can be strongly reduced by increasing the robustness of the method through a simple linear correction based on a high-level theoretical or experimental cohesive energy termed $\lambda$-scaling.</div><div>By carefully tuning the technical parameters, the walltime per element could be reduced from weeks to about a day (10-20k core-hours), which enabled extensive testing for B, Al, Na, K, Ca, Sr, Ba, Mn, Cu, Xe and Hg. </div><div>This comprehensive benchmark demonstrates the excellent performance and robustness of the approach with a mean absolute deviation (MAD) of less than 2% from experimental NBPs and very similar accuracy for liquid entropies (MAD 2.3 J/(mol*K), 2% relative). In some cases, the uncertainty in the predictions are several times smaller than the variation between literature values, allowing us to clear out ambiguities in the NBPs of B and Ba.</div>


2020 ◽  
Vol 22 (41) ◽  
pp. 24041-24050
Author(s):  
Jan-Michael Mewes ◽  
Odile R. Smits

Thermodynamic integration with a DFT Hamiltonian has been used to obtain accurate absolute Gibbs energies of atomic liquids and normal boiling points in excellent agreement with experimental references (MAD < 2%).


2017 ◽  
Vol 146 (18) ◽  
pp. 184506 ◽  
Author(s):  
Edilio Lázaro-Lázaro ◽  
Patricia Mendoza-Méndez ◽  
Luis Fernando Elizondo-Aguilera ◽  
Jorge Adrián Perera-Burgos ◽  
Pedro Ezequiel Ramírez-González ◽  
...  

2015 ◽  
Vol 142 (12) ◽  
pp. 124504 ◽  
Author(s):  
S. Bernini ◽  
F. Puosi ◽  
D. Leporini

2014 ◽  
Vol 394 ◽  
pp. 1-16 ◽  
Author(s):  
Patricia Mendoza-Méndez ◽  
Leticia López-Flores ◽  
Alejandro Vizcarra-Rendón ◽  
Luis E. Sánchez-Díaz ◽  
Magdaleno Medina-Noyola

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