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Correlated wavefunction methods in bioinorganic chemistry

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Abstract

In this commentary the challenges faced in the application of wavefunction-based ab initio methods to (open-shell) transition metal complexes of (bio)inorganic interest are briefly touched on. Both single-reference and multireference methods are covered. It is stressed that the generation and nature of the reference wavefunction is a subject of major importance. How erroneous results can be easily obtained even with coupled-cluster theory is illustrated through the example of the septet–quintet separation in iron(IV)–oxo complexes. Second, the interplay between relativistic and correlation effects is important. This is demonstrated with coupled-cluster calculations on models for dinuclear copper active sites, where relativity has a major influence on the relative stabilities of the bis(μ-oxo) and side-on peroxo species.

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Acknowledgments

We gratefully acknowledge financial support of our work by the SFB 813 (“Chemistry at spin centers”), the SFB 624 (”Template effects in chemistry”), the Max Planck Society (via a Max Planck Society fellowship to F.N.), and the University of Bonn.

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Authors and Affiliations

  1. Institut für Physikalische und Theoretische Chemie, Universität Bonn, Wegelerstr 12, 53115, Bonn, Germany

    Frank Neese, Dimitrios G. Liakos & Shengfa Ye

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  1. Frank Neese
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  2. Dimitrios G. Liakos
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  3. Shengfa Ye
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Correspondence to Frank Neese.

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Neese, F., Liakos, D.G. & Ye, S. Correlated wavefunction methods in bioinorganic chemistry. J Biol Inorg Chem 16, 821–829 (2011). https://doi.org/10.1007/s00775-011-0787-6

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