Assessing the accuracy of compound formation energies with quantum Monte Carlo
| العنوان: | Assessing the accuracy of compound formation energies with quantum Monte Carlo |
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| المؤلفون: | Eric B. Isaacs, Hyeondeok Shin, Abdulgani Annaberdiyev, Chris Wolverton, Lubos Mitas, Anouar Benali, Olle Heinonen |
| المصدر: | Physical Review B. 105 |
| بيانات النشر: | American Physical Society (APS), 2022. |
| سنة النشر: | 2022 |
| مصطلحات موضوعية: | Condensed Matter - Materials Science, Materials Science (cond-mat.mtrl-sci), FOS: Physical sciences, Computational Physics (physics.comp-ph), Physics - Computational Physics |
| الوصف: | Accurately predicting the formation energy of a compound, which describes its thermodynamic stability, is a key challenge in materials physics. Here, we employ many-body quantum Monte Carlo (QMC) with single-reference trial functions to compute the formation energy of two electronically disparate compounds, the intermetallic VPt$_2$ and the semiconductor CuI, for which standard density functional theory (DFT) predictions using both the Perdew-Burke Ernzerhof (PBE) and the strongly constrained and appropriately normed (SCAN) density functional approximations deviate markedly from available experimental values. For VPt$_2$, we find an agreement between QMC, SCAN, and PBE0 estimates, which therefore remain in disagreement with the much less exothermic experimental value. For CuI, the QMC result agrees with neither SCAN nor PBE pointing towards DFT exchange-correlation biases, likely related to the localized Cu $3d$ electrons. Compared to the behavior of some density functional approximations within DFT, spin-averaged QMC exhibits a smaller but still appreciable deviation when compared to experiment. The QMC result is slightly improved by incorporating spin-orbit corrections for CuI and solid I$_2$, so that experiment and theory are brought into imperfect but reasonable agreement within about 120~meV/atom. |
| تدمد: | 2469-9969 2469-9950 |
| URL الوصول: | https://explore.openaire.eu/search/publication?articleId=doi_dedup___::eb198b1dd71eee3ecefcdfb94d33f11b https://doi.org/10.1103/physrevb.105.224110 |
| حقوق: | OPEN |
| رقم الأكسشن: | edsair.doi.dedup.....eb198b1dd71eee3ecefcdfb94d33f11b |
| قاعدة البيانات: | OpenAIRE |
| تدمد: | 24699969 24699950 |
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