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 language | English (US) |
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Pages (from-to) | 3684-3695 |
Number of pages | 12 |
Journal | Journal of Chemical Theory and Computation |
Volume | 13 |
Issue number | 8 |
DOIs | |
State | Published - Aug 8 2017 |
All Science Journal Classification (ASJC) codes
- Computer Science Applications
- Physical and Theoretical Chemistry