open access

https://hdl.handle.net/2115/83178

Spin‐inversion mechanisms in O2 binding to a model heme compound : A perspective from nonadiabatic wave packet calculations

英語

2020-11

John Wiley & Sons

Journal of Computational Chemistry

41(29)

2527-2537

Spin-inversion dynamics in O(2)binding to a model heme complex, which consisted of Fe(II)-porphyrin and imidazole, were studied using nonadiabatic wave packet dynamics calculations. We considered three active nuclear degrees of freedom in the dynamics, including the motions along the Fe-O distance, Fe-O-O angle, and Fe out-of-plane distance. Spin-free potential energy surfaces for the singlet, triplet, quintet, and septet states were developed using density functional theory calculations, and spin-orbit coupling elements were obtained from CASSCF-level electronic structure calculations. The spin-inversion mainly occurred between the singlet state and one of the triplet states due to large spin-orbit couplings and the contributions of other states were extremely small. The present quantum dynamics calculations suggested that the narrow crossing region model plays a dominant role in the O(2)binding dynamics. In addition, the one-dimensional Landau-Zener model underestimated the nonadiabatic transition probability.

学術雑誌論文

Accepted Manuscript

This is the peer reviewed version of the following article: Saito, K, Watabe, Y, Miyazaki, T, Takayanagi, T, Hasegawa, J. Spin‐inversion mechanisms in O2 binding to a model heme compound: A perspective from nonadiabatic wave packet calculations. J Comput Chem. 2020; 41: 2527– 2537, which has been published in final form at https://doi.org/10.1002/jcc.26409 . This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions.

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