Pasquier, Remi and Graml, Maximilian and Wilhelm, Jan (2026) Gaussian Basis Sets for All-Electron Excited-State Calculations of Large Molecules. JOURNAL OF CHEMICAL THEORY AND COMPUTATION, 22 (1). pp. 540-557. ISSN 1549-9618, 1549-9626
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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.
| Item Type: | Article |
|---|---|
| Uncontrolled Keywords: | AUXILIARY BASIS-SETS; GREENS-FUNCTION; ORBITAL METHODS; GW; EXPANSIONS; RESOLUTION; CHEMISTRY; APPROXIMATIONS; ENERGIES; VALENCE; |
| Subjects: | 500 Science > 530 Physics 500 Science > 540 Chemistry & allied sciences |
| Divisions: | Physics > Institute of Theroretical Physics Regensburg Center for UltrafastNanoscopy (RUN) |
| Depositing User: | Dr. Gernot Deinzer |
| Date Deposited: | 07 May 2026 07:55 |
| Last Modified: | 07 May 2026 07:55 |
| URI: | https://pred.uni-regensburg.de/id/eprint/65787 |
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