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Spin-inversion mechanisms in O-2 binding to a model heme complex revisited by density function theory calculations
| Title: | Spin-inversion mechanisms in O-2 binding to a model heme complex revisited by density function theory calculations |
| Authors: | Saito, Kohei Browse this author | | Watabe, Yuya Browse this author | | Fujihara, Takashi Browse this author | | Takayanagi, Toshiyuki Browse this author →KAKEN DB | | Hasegawa, Jun-ya Browse this author →KAKEN DB |
| Keywords: | spin crossover | | spin-forbidden | | spin inversion |
| Issue Date: | 30-Apr-2020 |
| Publisher: | John Wiley & Sons |
| Journal Title: | Journal of Computational Chemistry |
| Volume: | 41 |
| Issue: | 11 |
| Start Page: | 1130 |
| End Page: | 1138 |
| Publisher DOI: | 10.1002/jcc.26159 |
| Abstract: | Spin-inversion mechanisms in O-2 binding to a model heme complex, consisting of Fe(II)-porphyrin and imidazole, were investigated using density-functional theory calculations. First, we applied the recently proposed mixed-spin Hamiltonian method to locate spin-inversion structures between different total spin multiplicities. Nine spin-inversion structures were successfully optimized for the singlet-triplet, singlet-quintet, triplet-quintet, and quintet-septet spin-inversion processes. We found that the singlet-triplet spin-inversion points are located around the potential energy surface region at short Fe-O distances, whereas the singlet-quintet and quintet-septet spin-inversion points are located at longer Fe-O distances. This suggests that both narrow and broad crossing models play roles in O-2 binding to the Fe-porphyrin complex. To further understand spin-inversion mechanisms, we performed on-the-fly Born-Oppenheimer molecular dynamics calculations. The reaction coordinates, which are correlated to the spin-inversion dynamics between different spin multiplicities, are also discussed. |
| Rights: | This is the peer reviewed version of the following article: Saito, K, Watabe, Y, Fujihara, T, Takayanagi, T, Hasegawa, J‐y. Spin‐inversion mechanisms in O2 binding to a model heme complex revisited by density function theory calculations. J Comput Chem. 2020; 41: 1130– 1138, which has been published in final form at https://doi.org/10.1002/jcc.26159 . This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions." |
| Type: | article (author version) |
| URI: | http://hdl.handle.net/2115/81206 |
| Appears in Collections: | 触媒科学研究所 (Institute for Catalysis) > 雑誌発表論文等 (Peer-reviewed Journal Articles, etc)
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Submitter: 長谷川 淳也
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