Accelerating equilibration in first-principles molecular dynamics with orbital-free density functional theory
We introduce a practical hybrid approach that combines orbital-free density functional theory (DFT) with Kohn-Sham DFT for speeding up first-principles molecular dynamics simulations. Equilibrated ionic configurations are generated using orbital-free DFT for subsequent Kohn-Sham DFT molecular dynami...
| Main Authors: | , , , , , , |
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| Format: | Article |
| Language: | English |
| Published: |
American Physical Society
2022-10-01
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| Series: | Physical Review Research |
| Online Access: | http://doi.org/10.1103/PhysRevResearch.4.043033 |
| _version_ | 1797210642790219776 |
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| author | Lenz Fiedler Zhandos A. Moldabekov Xuecheng Shao Kaili Jiang Tobias Dornheim Michele Pavanello Attila Cangi |
| author_facet | Lenz Fiedler Zhandos A. Moldabekov Xuecheng Shao Kaili Jiang Tobias Dornheim Michele Pavanello Attila Cangi |
| author_sort | Lenz Fiedler |
| collection | DOAJ |
| description | We introduce a practical hybrid approach that combines orbital-free density functional theory (DFT) with Kohn-Sham DFT for speeding up first-principles molecular dynamics simulations. Equilibrated ionic configurations are generated using orbital-free DFT for subsequent Kohn-Sham DFT molecular dynamics. This leads to a massive reduction of the simulation time without any sacrifice in accuracy. We assess this finding across systems of different sizes and temperature, up to the warm dense matter regime. To that end, we use the cosine distance between the time series of radial distribution functions representing the ionic configurations. Likewise, we show that the equilibrated ionic configurations from this hybrid approach significantly enhance the accuracy of machine-learning models that replace Kohn-Sham DFT. Our hybrid scheme enables systematic first-principles simulations of warm dense matter that are otherwise hampered by the large numbers of atoms and the prevalent high temperatures. Moreover, our finding provides an additional motivation for developing kinetic and noninteracting free-energy functionals for orbital-free DFT. |
| first_indexed | 2024-04-24T10:13:51Z |
| format | Article |
| id | doaj.art-578854d94ebe4d69889413261dddd397 |
| institution | Directory Open Access Journal |
| issn | 2643-1564 |
| language | English |
| last_indexed | 2024-04-24T10:13:51Z |
| publishDate | 2022-10-01 |
| publisher | American Physical Society |
| record_format | Article |
| series | Physical Review Research |
| spelling | doaj.art-578854d94ebe4d69889413261dddd3972024-04-12T17:25:18ZengAmerican Physical SocietyPhysical Review Research2643-15642022-10-014404303310.1103/PhysRevResearch.4.043033Accelerating equilibration in first-principles molecular dynamics with orbital-free density functional theoryLenz FiedlerZhandos A. MoldabekovXuecheng ShaoKaili JiangTobias DornheimMichele PavanelloAttila CangiWe introduce a practical hybrid approach that combines orbital-free density functional theory (DFT) with Kohn-Sham DFT for speeding up first-principles molecular dynamics simulations. Equilibrated ionic configurations are generated using orbital-free DFT for subsequent Kohn-Sham DFT molecular dynamics. This leads to a massive reduction of the simulation time without any sacrifice in accuracy. We assess this finding across systems of different sizes and temperature, up to the warm dense matter regime. To that end, we use the cosine distance between the time series of radial distribution functions representing the ionic configurations. Likewise, we show that the equilibrated ionic configurations from this hybrid approach significantly enhance the accuracy of machine-learning models that replace Kohn-Sham DFT. Our hybrid scheme enables systematic first-principles simulations of warm dense matter that are otherwise hampered by the large numbers of atoms and the prevalent high temperatures. Moreover, our finding provides an additional motivation for developing kinetic and noninteracting free-energy functionals for orbital-free DFT.http://doi.org/10.1103/PhysRevResearch.4.043033 |
| spellingShingle | Lenz Fiedler Zhandos A. Moldabekov Xuecheng Shao Kaili Jiang Tobias Dornheim Michele Pavanello Attila Cangi Accelerating equilibration in first-principles molecular dynamics with orbital-free density functional theory Physical Review Research |
| title | Accelerating equilibration in first-principles molecular dynamics with orbital-free density functional theory |
| title_full | Accelerating equilibration in first-principles molecular dynamics with orbital-free density functional theory |
| title_fullStr | Accelerating equilibration in first-principles molecular dynamics with orbital-free density functional theory |
| title_full_unstemmed | Accelerating equilibration in first-principles molecular dynamics with orbital-free density functional theory |
| title_short | Accelerating equilibration in first-principles molecular dynamics with orbital-free density functional theory |
| title_sort | accelerating equilibration in first principles molecular dynamics with orbital free density functional theory |
| url | http://doi.org/10.1103/PhysRevResearch.4.043033 |
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