Gaussian basis sets for all-electron excited-state calculations of large molecules
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| Format: | Preprint |
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2025
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| _version_ | 1866908706756624384 |
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| author | Pasquier, Rémi Graml, Maximilian Wilhelm, Jan |
| author_facet | Pasquier, Rémi Graml, Maximilian Wilhelm, Jan |
| contents | We introduce a family of all-electron Gaussian basis sets, augmented MOLOPT, optimized for excited-state calculations on large molecules. We generate these basis sets by augmenting existing STO-3G, STO-6G, and MOLOPT basis sets optimized for ground state energy calculations. The augmented MOLOPT basis sets achieve fast convergence of $GW$ gaps and Bethe-Salpeter excitation energies, while maintaining low condition numbers of the overlap matrix to ensure numerical stability. For $GW$ HOMO-LUMO gaps, the double-zeta augmented MOLOPT basis yields a mean absolute deviation of 60 meV to the complete basis set limit. The basis set convergence for excitation energies from time-dependent density functional theory and the Bethe-Salpeter equation is similar. We use our smallest generated augmented MOLOPT basis (aug-SZV-MOLOPT-ae-mini) to demonstrate $GW$ calculations on nanographenes with 9224 atoms requiring only 34300 core hours of computational resources. |
| format | Preprint |
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arxiv_https___arxiv_org_abs_2508_12884 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Gaussian basis sets for all-electron excited-state calculations of large molecules Pasquier, Rémi Graml, Maximilian Wilhelm, Jan Chemical Physics Materials Science We introduce a family of all-electron Gaussian basis sets, augmented MOLOPT, optimized for excited-state calculations on large molecules. We generate these basis sets by augmenting existing STO-3G, STO-6G, and MOLOPT basis sets optimized for ground state energy calculations. The augmented MOLOPT basis sets achieve fast convergence of $GW$ gaps and Bethe-Salpeter excitation energies, while maintaining low condition numbers of the overlap matrix to ensure numerical stability. For $GW$ HOMO-LUMO gaps, the double-zeta augmented MOLOPT basis yields a mean absolute deviation of 60 meV to the complete basis set limit. The basis set convergence for excitation energies from time-dependent density functional theory and the Bethe-Salpeter equation is similar. We use our smallest generated augmented MOLOPT basis (aug-SZV-MOLOPT-ae-mini) to demonstrate $GW$ calculations on nanographenes with 9224 atoms requiring only 34300 core hours of computational resources. |
| title | Gaussian basis sets for all-electron excited-state calculations of large molecules |
| topic | Chemical Physics Materials Science |
| url | https://arxiv.org/abs/2508.12884 |