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| Main Authors: | , , , |
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| Format: | Preprint |
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2025
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| Online Access: | https://arxiv.org/abs/2509.00953 |
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| _version_ | 1866914323725549568 |
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| author | Francisco, H. Thapa, B. Trickey, S. B. Cancio, A. C. |
| author_facet | Francisco, H. Thapa, B. Trickey, S. B. Cancio, A. C. |
| contents | Deorbitalization of a conventional meta-generalized-gradient exchange-correlation approximation replaces its dependence upon the Kohn-Sham kinetic energy density with a dependence on the density gradient and Laplacian. In principle, that simplification should provide improved computational performance relative to the original meta-GGA form because of the shift from an orbital-dependent generalized Kohn-Sham potential to a true KS local potential. Often that prospective gain is lost because of problematic roughness in the density caused by the density Laplacian and consequent roughness in the exchange-correlation potential from the resulting higher-order spatial derivatives of the density in it. We address the problem by constructing a deorbitalizer based on the RPP deorbitalizer [Phys. Rev. Mater. 6, 083803 (2022)] with comparative smoothness of the potential along with retention of constraint satisfaction as design goals. Applied to the r^2SCAN exchange-correlation functional [J. Phys. Chem. Lett. 11, 8208 (2020)], we find substantial timing improvements for solid-state calculations over both r^2SCAN and its earlier deorbitalization for high precision calculations of structural properties, while improving upon the accuracy of RPP deorbitalization for both solids and molecules. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2509_00953 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Performance Improvement of Deorbitalized Exchange-Correlation Functionals Francisco, H. Thapa, B. Trickey, S. B. Cancio, A. C. Materials Science Deorbitalization of a conventional meta-generalized-gradient exchange-correlation approximation replaces its dependence upon the Kohn-Sham kinetic energy density with a dependence on the density gradient and Laplacian. In principle, that simplification should provide improved computational performance relative to the original meta-GGA form because of the shift from an orbital-dependent generalized Kohn-Sham potential to a true KS local potential. Often that prospective gain is lost because of problematic roughness in the density caused by the density Laplacian and consequent roughness in the exchange-correlation potential from the resulting higher-order spatial derivatives of the density in it. We address the problem by constructing a deorbitalizer based on the RPP deorbitalizer [Phys. Rev. Mater. 6, 083803 (2022)] with comparative smoothness of the potential along with retention of constraint satisfaction as design goals. Applied to the r^2SCAN exchange-correlation functional [J. Phys. Chem. Lett. 11, 8208 (2020)], we find substantial timing improvements for solid-state calculations over both r^2SCAN and its earlier deorbitalization for high precision calculations of structural properties, while improving upon the accuracy of RPP deorbitalization for both solids and molecules. |
| title | Performance Improvement of Deorbitalized Exchange-Correlation Functionals |
| topic | Materials Science |
| url | https://arxiv.org/abs/2509.00953 |