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Spin-inversion mechanisms in O-2 binding to a model heme complex revisited by density function theory calculations

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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 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 . 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)
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)

Submitter: 長谷川 淳也

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