Globally-Optimized Local Pseudopotentials for (Orbital-Free) Density Functional Theory Simulations of Liquids and Solids

Beatriz G. Del Rio, Johannes M. Dieterich, Emily A. Carter

Research output: Contribution to journalArticle

5 Scopus citations

Abstract

The accuracy of local pseudopotentials (LPSs) is one of two major determinants of the fidelity of orbital-free density functional theory (OFDFT) simulations. We present a global optimization strategy for LPSs that enables OFDFT to reproduce solid and liquid properties obtained from Kohn-Sham DFT. Our optimization strategy can fit arbitrary properties from both solid and liquid phases, so the resulting globally optimized local pseudopotentials (goLPSs) can be used in solid and/or liquid-phase simulations depending on the fitting process. We show three test cases proving that we can (1) improve solid properties compared to our previous bulk-derived local pseudopotential generation scheme; (2) refine predicted liquid and solid properties by adding force matching data; and (3) generate a from-scratch, accurate goLPS from the local channel of a non-local pseudopotential. The proposed scheme therefore serves as a full and improved LPS construction protocol.

Original languageEnglish (US)
Pages (from-to)3684-3695
Number of pages12
JournalJournal of Chemical Theory and Computation
Volume13
Issue number8
DOIs
StatePublished - Aug 8 2017

All Science Journal Classification (ASJC) codes

  • Computer Science Applications
  • Physical and Theoretical Chemistry

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