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Fragment-Based Excited-State Calculations Using the GW Approximation and the Bethe–Salpeter Equation
https://repo.qst.go.jp/records/84624
https://repo.qst.go.jp/records/8462467d87182-6ffb-4b1b-9f01-5dd0a8ae7c1c
| Item type | 学術雑誌論文 / Journal Article(1) | |||||
|---|---|---|---|---|---|---|
| 公開日 | 2021-12-27 | |||||
| タイトル | ||||||
| タイトル | Fragment-Based Excited-State Calculations Using the GW Approximation and the Bethe–Salpeter Equation | |||||
| 言語 | ||||||
| 言語 | eng | |||||
| 資源タイプ | ||||||
| 資源タイプ識別子 | http://purl.org/coar/resource_type/c_6501 | |||||
| 資源タイプ | journal article | |||||
| アクセス権 | ||||||
| アクセス権 | metadata only access | |||||
| アクセス権URI | http://purl.org/coar/access_right/c_14cb | |||||
| 著者 |
Fujita, Takatoshi
× Fujita, Takatoshi× Noguchi, Yoshifumi× Takatoshi, Fujita |
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| 抄録 | ||||||
| 内容記述タイプ | Abstract | |||||
| 内容記述 | Herein, we present a fragment-based approach for calculating the charged and neutral excited states in molecular systems, based on the many-body Green’s function method within the GW approximation and the Bethe–Salpeter equation (BSE). The implementation relies on the many-body expansion of the total irreducible polarizability on the basis of fragment molecular orbitals. The GW quasi-particle energies in complex molecular environments are obtained by the GW calculation for the target fragment plus induced polarization contributions of the surrounding fragments at the static Coulomb-hole plus screened exchange level. In addition, we develop a large-scale GW/BSE method for calculating the delocalized excited states of molecular aggregates, based on the fragment molecular orbital method and the exciton model. The accuracy of fragment-based GW and GW/BSE methods was evaluated on molecular clusters and molecular crystals. We found that the accuracy of the total irreducible polarizability can be improved systematically by including two-body correction terms, and the fragment-based calculations can reasonably reproduce the results of the corresponding unfragmented calculations with a relative error of less than 100 meV. The proposed approach enables efficient excited-state calculations for large molecular systems with reasonable accuracy. | |||||
| 書誌情報 |
The Journal of Physical Chemistry A 巻 125, p. 10580-10592, 発行日 2021-12 |
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| ISSN | ||||||
| 収録物識別子タイプ | ISSN | |||||
| 収録物識別子 | 1520-6106 | |||||
| DOI | ||||||
| 識別子タイプ | DOI | |||||
| 関連識別子 | 10.1021/acs.jpca.1c07337 | |||||
| 関連サイト | ||||||
| 識別子タイプ | URI | |||||
| 関連識別子 | https://pubs.acs.org/doi/full/10.1021/acs.jpca.1c07337 | |||||
