Excited State Properties from the Bethe--Salpeter Equation: State-to-State Transitions and Spin-Orbit Coupling
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arXiv
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| Hauptverfasser: | , |
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| Format: | Preprint |
| Veröffentlicht: |
2024
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| _version_ | 1866916541070573568 |
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| author | Himmelsbach, Paula Holzer, Christof |
| author_facet | Himmelsbach, Paula Holzer, Christof |
| contents | The formalism to calculate excited state properties from the $GW$-Bethe-Salpeter equation (BSE) method is introduced, providing convenient access to excited state absorption, excited state circular dichroism, and excited state optical rotation in the framework of the $GW$-BSE method. This is achieved using the second-order transition density, which can be obtained by solving a set of auxiliary equations similar to time-dependent density functional theory (TD-DFT). The proposed formulation therefore leads to no increase in the formal computational complexity when compared to the corresponding ground state properties. We further outline the calculation of fully relaxed spin-orbit coupling matrix elements within the $GW$-BSE method, allowing us to include perturbative corrections for spin-orbit coupling in aforementioned properties. These corrections are also extended to TD-DFT. Excited state absorption and perturbative spin-orbit coupling corrections within $GW$-BSE are evaluated for a selected set of molecular systems, yielding promising results. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2410_11406 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Excited State Properties from the Bethe--Salpeter Equation: State-to-State Transitions and Spin-Orbit Coupling Himmelsbach, Paula Holzer, Christof Chemical Physics The formalism to calculate excited state properties from the $GW$-Bethe-Salpeter equation (BSE) method is introduced, providing convenient access to excited state absorption, excited state circular dichroism, and excited state optical rotation in the framework of the $GW$-BSE method. This is achieved using the second-order transition density, which can be obtained by solving a set of auxiliary equations similar to time-dependent density functional theory (TD-DFT). The proposed formulation therefore leads to no increase in the formal computational complexity when compared to the corresponding ground state properties. We further outline the calculation of fully relaxed spin-orbit coupling matrix elements within the $GW$-BSE method, allowing us to include perturbative corrections for spin-orbit coupling in aforementioned properties. These corrections are also extended to TD-DFT. Excited state absorption and perturbative spin-orbit coupling corrections within $GW$-BSE are evaluated for a selected set of molecular systems, yielding promising results. |
| title | Excited State Properties from the Bethe--Salpeter Equation: State-to-State Transitions and Spin-Orbit Coupling |
| topic | Chemical Physics |
| url | https://arxiv.org/abs/2410.11406 |