Extension of the Einstein molecule method for solid free energy calculation to nonperiodic and semiperiodic systems
Abstract
Free energy calculations on solid phases are important for understanding the phase behavior of various systems. For periodic crystalline solids, the Einstein molecule approach can be used to determine the free energy difference between the solid of interest and an ideal crystal for which the free energy can be found analytically. In this work, we show how this method is extensible to systems which are nonperiodic or periodic in some dimensions but not in others. This allows for the calculation of exact absolute free energies of finitesized crystals having specific shapes and surface geometries. We illustrate this using the fcc LennardJones solid and also illustrate how surface contributions to free energies can easily be extracted from simulations of this solid in semiinfinite slab geometries. We have created a software package which interfaces with the LAMMPS molecular dynamics code to perform these calculations.
 Authors:

 Lehigh Univ., Bethlehem, PA (United States)
 Publication Date:
 Research Org.:
 Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of California, Oakland, CA (United States); Lehigh Univ., Bethlehem, PA (United States)
 Sponsoring Org.:
 USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC22). Materials Sciences & Engineering Division; USDOE
 OSTI Identifier:
 1577597
 Alternate Identifier(s):
 OSTI ID: 1546111
 Grant/Contract Number:
 AC0205CH11231; SC0013979
 Resource Type:
 Accepted Manuscript
 Journal Name:
 Journal of Chemical Physics
 Additional Journal Information:
 Journal Volume: 151; Journal Issue: 5; Journal ID: ISSN 00219606
 Publisher:
 American Institute of Physics (AIP)
 Country of Publication:
 United States
 Language:
 English
 Subject:
 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Pretti, Evan, and Mittal, Jeetain. Extension of the Einstein molecule method for solid free energy calculation to nonperiodic and semiperiodic systems. United States: N. p., 2019.
Web. doi:10.1063/1.5100960.
Pretti, Evan, & Mittal, Jeetain. Extension of the Einstein molecule method for solid free energy calculation to nonperiodic and semiperiodic systems. United States. doi:https://doi.org/10.1063/1.5100960
Pretti, Evan, and Mittal, Jeetain. Fri .
"Extension of the Einstein molecule method for solid free energy calculation to nonperiodic and semiperiodic systems". United States. doi:https://doi.org/10.1063/1.5100960. https://www.osti.gov/servlets/purl/1577597.
@article{osti_1577597,
title = {Extension of the Einstein molecule method for solid free energy calculation to nonperiodic and semiperiodic systems},
author = {Pretti, Evan and Mittal, Jeetain},
abstractNote = {Free energy calculations on solid phases are important for understanding the phase behavior of various systems. For periodic crystalline solids, the Einstein molecule approach can be used to determine the free energy difference between the solid of interest and an ideal crystal for which the free energy can be found analytically. In this work, we show how this method is extensible to systems which are nonperiodic or periodic in some dimensions but not in others. This allows for the calculation of exact absolute free energies of finitesized crystals having specific shapes and surface geometries. We illustrate this using the fcc LennardJones solid and also illustrate how surface contributions to free energies can easily be extracted from simulations of this solid in semiinfinite slab geometries. We have created a software package which interfaces with the LAMMPS molecular dynamics code to perform these calculations.},
doi = {10.1063/1.5100960},
journal = {Journal of Chemical Physics},
number = 5,
volume = 151,
place = {United States},
year = {2019},
month = {8}
}
Web of Science
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