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Spin Crossover Dynamics Studies of Thermal Activated Molecular Oxygen Binding Mechanism on a Model Copper Complex

Abstract

The theoretical description of the primary dioxygen (O2) binding and activation step in many copper or iron enzymes, suffers from instrinsically electronic non-adiabaticity of the spin flip events of the triplet dioxygen molecule (3O2), mediated by spin-orbit couplings. In this work, we presented the early-stage ultrafast spin flip dynamics of O2 binding for a simplified monocopper complex, involving the coupled singlet and triplet electronic states. The on-the-fly trajectory surface hopping (TSH) simulations have identified the dynamical effects that may influence the mode of O2 coordination (end-on vs side-on), and the electronic structures can be viewed as complexes of molecular O2 with Cu(I) or as Cu(II)-superoxide compounds. In addition, the significant spin flip events are obversed within the sub-picosecond regime. We hope this work may provide complimentary insights on the traditional interpreting of O2 binding on copper complexes and subsequent catalytic reaction mechanisms.

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Publication details

The article was accepted on 08 May 2018 and first published on 09 May 2018


Article type: Paper
DOI: 10.1039/C8CP02482K
Citation: Phys. Chem. Chem. Phys., 2018, Accepted Manuscript
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    Spin Crossover Dynamics Studies of Thermal Activated Molecular Oxygen Binding Mechanism on a Model Copper Complex

    L. Bie, F. Liu, Y. Li, T. Dong, J. Gao, L. Du and Q. Yuan, Phys. Chem. Chem. Phys., 2018, Accepted Manuscript , DOI: 10.1039/C8CP02482K

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