Investigation of a Quantum Monte Carlo Protocol To Achieve High Accuracy and High-Throughput Materials Formation Energies
High-throughput calculations based on density functional theory (DFT) methods have been widely implemented in the scientific community. However, depending on both the properties of interest as well as particular chemical/structural phase space, accuracy even for correct trends remains a key challeng...
| Main Authors: | , , , |
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| Format: | Article |
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American Chemical Society (ACS)
2018
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| Online Access: | http://hdl.handle.net/1721.1/114820 https://orcid.org/0000-0002-2240-8520 https://orcid.org/0000-0003-1281-2359 |
| _version_ | 1826198979863379968 |
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| author | Saritas, Kayahan Mueller, Tim Wagner, Lucas Grossman, Jeffrey C. |
| author2 | Massachusetts Institute of Technology. Department of Materials Science and Engineering |
| author_facet | Massachusetts Institute of Technology. Department of Materials Science and Engineering Saritas, Kayahan Mueller, Tim Wagner, Lucas Grossman, Jeffrey C. |
| author_sort | Saritas, Kayahan |
| collection | MIT |
| description | High-throughput calculations based on density functional theory (DFT) methods have been widely implemented in the scientific community. However, depending on both the properties of interest as well as particular chemical/structural phase space, accuracy even for correct trends remains a key challenge for DFT. In this work, we evaluate the use of quantum Monte Carlo (QMC) to calculate material formation energies in a high-throughput environment. We test the performance of automated QMC calculations on 21 compounds with high quality reference data from the Committee on Data for Science and Technology (CODATA) thermodynamic database. We compare our approach to different DFT methods as well as different pseudopotentials, showing that errors in QMC calculations can be progressively improved especially when correct pseudopotentials are used. We determine a set of accurate pseudopotentials in QMC via a systematic investigation of multiple available pseudopotential libraries. We show that using this simple automated recipe, QMC calculations can outperform DFT calculations over a wide set of materials. Out of 21 compounds tested, chemical accuracy has been obtained in formation energies of 11 structures using our QMC recipe, compared to none using DFT calculations. |
| first_indexed | 2024-09-23T11:12:51Z |
| format | Article |
| id | mit-1721.1/114820 |
| institution | Massachusetts Institute of Technology |
| last_indexed | 2024-09-23T11:12:51Z |
| publishDate | 2018 |
| publisher | American Chemical Society (ACS) |
| record_format | dspace |
| spelling | mit-1721.1/1148202022-10-01T02:07:02Z Investigation of a Quantum Monte Carlo Protocol To Achieve High Accuracy and High-Throughput Materials Formation Energies Saritas, Kayahan Mueller, Tim Wagner, Lucas Grossman, Jeffrey C. Massachusetts Institute of Technology. Department of Materials Science and Engineering Saritas, Kayahan Grossman, Jeffrey C. High-throughput calculations based on density functional theory (DFT) methods have been widely implemented in the scientific community. However, depending on both the properties of interest as well as particular chemical/structural phase space, accuracy even for correct trends remains a key challenge for DFT. In this work, we evaluate the use of quantum Monte Carlo (QMC) to calculate material formation energies in a high-throughput environment. We test the performance of automated QMC calculations on 21 compounds with high quality reference data from the Committee on Data for Science and Technology (CODATA) thermodynamic database. We compare our approach to different DFT methods as well as different pseudopotentials, showing that errors in QMC calculations can be progressively improved especially when correct pseudopotentials are used. We determine a set of accurate pseudopotentials in QMC via a systematic investigation of multiple available pseudopotential libraries. We show that using this simple automated recipe, QMC calculations can outperform DFT calculations over a wide set of materials. Out of 21 compounds tested, chemical accuracy has been obtained in formation energies of 11 structures using our QMC recipe, compared to none using DFT calculations. National Science Foundation (U.S.) (Grant DMR 1206242) National Science Foundation (U.S.) (Grant DMR 1352373) United States. Department of Energy (Award INCITE MAT307) United States. Department of Energy (Award INCITE MAT141) National Science Foundation (U.S.) (Grant XSEDE TG-DMR090027) 2018-04-20T18:32:34Z 2018-04-20T18:32:34Z 2017-05 2016-12 2018-04-19T14:18:22Z Article http://purl.org/eprint/type/JournalArticle 1549-9618 1549-9626 http://hdl.handle.net/1721.1/114820 Saritas, Kayahan et al. “Investigation of a Quantum Monte Carlo Protocol To Achieve High Accuracy and High-Throughput Materials Formation Energies.” Journal of Chemical Theory and Computation 13, 5 (April 2017): 1943–1951 © 2017 American Chemical Society https://orcid.org/0000-0002-2240-8520 https://orcid.org/0000-0003-1281-2359 http://dx.doi.org/10.1021/ACS.JCTC.6B01179 Journal of Chemical Theory and Computation Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use. application/pdf American Chemical Society (ACS) MIT Web Domain |
| spellingShingle | Saritas, Kayahan Mueller, Tim Wagner, Lucas Grossman, Jeffrey C. Investigation of a Quantum Monte Carlo Protocol To Achieve High Accuracy and High-Throughput Materials Formation Energies |
| title | Investigation of a Quantum Monte Carlo Protocol To Achieve High Accuracy and High-Throughput Materials Formation Energies |
| title_full | Investigation of a Quantum Monte Carlo Protocol To Achieve High Accuracy and High-Throughput Materials Formation Energies |
| title_fullStr | Investigation of a Quantum Monte Carlo Protocol To Achieve High Accuracy and High-Throughput Materials Formation Energies |
| title_full_unstemmed | Investigation of a Quantum Monte Carlo Protocol To Achieve High Accuracy and High-Throughput Materials Formation Energies |
| title_short | Investigation of a Quantum Monte Carlo Protocol To Achieve High Accuracy and High-Throughput Materials Formation Energies |
| title_sort | investigation of a quantum monte carlo protocol to achieve high accuracy and high throughput materials formation energies |
| url | http://hdl.handle.net/1721.1/114820 https://orcid.org/0000-0002-2240-8520 https://orcid.org/0000-0003-1281-2359 |
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