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Title: The melting point of lithium: an orbital-free first-principles molecular dynamics study

Abstract

The melting point of liquid lithium near zero pressure is studied with large-scale orbital-free first-principles molecular dynamics (OF-FPMD) in the isobaric-isothermal ensemble. Here, we adopt the Wang-Govind-Carter (WGC) functional as our kinetic energy density functional (KEDF) and construct a bulk-derived local pseudopotential (BLPS) for Li. Our simulations employ both the ‘heat-until-melts’ method and the coexistence method. We predict 465 K as an upper bound of the melting point of Li from the ‘heat-until-melts’ method, while we predict 434 K as the melting point of Li from the coexistence method. These values compare well with an experimental melting point of 453 K at zero pressure. Furthermore, we calculate a few important properties of liquid Li including the diffusion coefficients, pair distribution functions, static structure factors, and compressibilities of Li at 470 K and 725 K in the canonical ensemble. This theoretically-obtained results show good agreement with known experimental results, suggesting that OF-FPMD using a non-local KEDF and a BLPS is capable of accurately describing liquid metals.

Authors:
 [1];  [2];  [3];  [1];  [4]
  1. Princeton Univ., NJ (United States). Dept. of Mechanical and Aerospace Engineering
  2. Ecole Polytechnique Federale Lausanne, Palaiseau (France). Lab. of Irradiated Solids
  3. Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Theoretical Division
  4. Princeton Univ., NJ (United States). Dept. of Mechanical and Aerospace Engineering, Andlinger Center for Energy and the Environment, Program in Applied and Computational Mathematics
Publication Date:
Research Org.:
Princeton Univ., NJ (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Fusion Energy Sciences (FES)
OSTI Identifier:
1390521
Grant/Contract Number:  
SC0008598
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Molecular Physics
Additional Journal Information:
Journal Volume: 111; Journal Issue: 22-23; Journal ID: ISSN 0026-8976
Publisher:
Taylor & Francis
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; orbital-free density functional theory; molecular dynamics; melting temperature; liquid lithium; superheating effect

Citation Formats

Chen, Mohan, Hung, Linda, Huang, Chen, Xia, Junchao, and Carter, Emily A. The melting point of lithium: an orbital-free first-principles molecular dynamics study. United States: N. p., 2013. Web. doi:10.1080/00268976.2013.828379.
Chen, Mohan, Hung, Linda, Huang, Chen, Xia, Junchao, & Carter, Emily A. The melting point of lithium: an orbital-free first-principles molecular dynamics study. United States. https://doi.org/10.1080/00268976.2013.828379
Chen, Mohan, Hung, Linda, Huang, Chen, Xia, Junchao, and Carter, Emily A. Sun . "The melting point of lithium: an orbital-free first-principles molecular dynamics study". United States. https://doi.org/10.1080/00268976.2013.828379. https://www.osti.gov/servlets/purl/1390521.
@article{osti_1390521,
title = {The melting point of lithium: an orbital-free first-principles molecular dynamics study},
author = {Chen, Mohan and Hung, Linda and Huang, Chen and Xia, Junchao and Carter, Emily A.},
abstractNote = {The melting point of liquid lithium near zero pressure is studied with large-scale orbital-free first-principles molecular dynamics (OF-FPMD) in the isobaric-isothermal ensemble. Here, we adopt the Wang-Govind-Carter (WGC) functional as our kinetic energy density functional (KEDF) and construct a bulk-derived local pseudopotential (BLPS) for Li. Our simulations employ both the ‘heat-until-melts’ method and the coexistence method. We predict 465 K as an upper bound of the melting point of Li from the ‘heat-until-melts’ method, while we predict 434 K as the melting point of Li from the coexistence method. These values compare well with an experimental melting point of 453 K at zero pressure. Furthermore, we calculate a few important properties of liquid Li including the diffusion coefficients, pair distribution functions, static structure factors, and compressibilities of Li at 470 K and 725 K in the canonical ensemble. This theoretically-obtained results show good agreement with known experimental results, suggesting that OF-FPMD using a non-local KEDF and a BLPS is capable of accurately describing liquid metals.},
doi = {10.1080/00268976.2013.828379},
url = {https://www.osti.gov/biblio/1390521}, journal = {Molecular Physics},
issn = {0026-8976},
number = 22-23,
volume = 111,
place = {United States},
year = {2013},
month = {8}
}

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Cited by: 23 works
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    Challenges in large scale quantum mechanical calculations: Challenges in large scale quantum mechanical calculations
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