Direct first-principles chemical potential calculations of liquids
Abstract
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.
Document Details
- Document Type
- Pub Defense Publication
- Publication Date
- Sep 07, 2012
- Source ID
- 10.1063/1.4749287
Entities
People
- Axel van de Walle
- Qi-Jun Hong
Organizations
- Brown University
- California Institute of Technology
- Office of Naval Research