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Direct first-principles chemical potential calculations of liquids

Hong, Qi-Jun and van de Walle, Axel (2012) Direct first-principles chemical potential calculations of liquids. Journal of Chemical Physics, 137 (9). Art. No. 094114. ISSN 0021-9606. doi:10.1063/1.4749287.

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We propose a scheme that drastically improves the efficiency of Widom's particle insertion method by efficiently sampling cavities while calculating the integrals providing the chemical potentials of a physical system. This idea enables us to calculate chemical potentials of liquids directly from first-principles without the help of any reference system, which is necessary in the commonly used thermodynamic integration method. As an example, we apply our scheme, combined with the density functional formalism, to the calculation of the chemical potential of liquid copper. The calculated chemical potential is further used to locate the melting temperature. The calculated results closely agree with experiments.

Item Type:Article
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URLURL TypeDescription
van de Walle, Axel0000-0002-3415-1494
Additional Information:© 2012 American Institute of Physics. Received 23 May 2012; accepted 17 August 2012; published online 7 September 2012. Discussions with Ligen Wang and Ljubomir Miljacic are gratefully acknowledged. This research was supported by the ONR (Grant Nos. N00014-12-1-0196 and N00014-10- 1-0660) and by the NSF through TeraGrid and XSEDE resources provided by the NCSA, SDSC, and TACC.
Funding AgencyGrant Number
Office of Naval Research (ONR)N00014-12-1-0196
Office of Naval Research (ONR)N00014-10-1-0660
Subject Keywords:ab initio calculations, Brillouin zones, chemical potential, copper, density functional theory, integration, liquid metals, melting, voids (solid)
Issue or Number:9
Classification Code:PACS: 61.25.Mv; 82.60.-s; 71.15.Mb; 71.22.+i
Record Number:CaltechAUTHORS:20121101-082641274
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Official Citation:Direct first-principles chemical potential calculations of liquids Qi-Jun Hong and Axel van de Walle, J. Chem. Phys. 137, 094114 (2012), DOI:10.1063/1.4749287
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:35223
Deposited By: Tony Diaz
Deposited On:01 Nov 2012 22:16
Last Modified:09 Nov 2021 23:13

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