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  Ligand Field Theory and Angular Overlap Model Based Analysis of the Electronic Structure of Homovalent Iron–Sulfur Dimers

Chilkuri, V. G., DeBeer, S., & Neese, F. (2020). Ligand Field Theory and Angular Overlap Model Based Analysis of the Electronic Structure of Homovalent Iron–Sulfur Dimers. Inorganic Chemistry, 59(2), 984-995. doi:10.1021/acs.inorgchem.9b00974.

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 Creators:
Chilkuri, Vijay Gopal1, Author           
DeBeer, Serena2, Author           
Neese, Frank1, Author           
Affiliations:
1Research Department Neese, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_2541710              
2Research Department DeBeer, Max Planck Institute for Chemical Energy Conversion, Max Planck Society, ou_3023871              

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 Abstract: The electronic structure of multinuclear transition metal complexes is a highly challenging problem for quantum chemical methods. The problems to be solved for a successful analysis include the following: (1) many unpaired electrons leading to “highly entangled” wave functions that cannot be calculated by standard electronic structure methods, (2) drastic differences between the one-particle and many-particle spectra and a high density of low-lying states, and (3) the interpretation of such highly complex wave functions in chemical terms. In this work, we continue our research on oligonuclear clusters by presenting an in-depth analysis of the electronic structure of a prototypical iron–sulfur (Fe2S2) dimer. Accurate wave functions are obtained from a variety of advanced wave function based methods. The wave function results are interpreted in terms of an effective Hamiltonian that in turn is parametrized in terms of the angular overlap model (AOM) that provides the chemical insights that we are striving for. A hierarchical analysis allows us to interpret the local electronic structure in terms of the thiolate, sulfide ligands, and metal–metal interaction strengths. The many-particle spectrum is analyzed in terms of configurations involving ligand and metal centers. Finally, we are able to derive simple yet effective interpretations of ligand interaction strengths, the metal–metal interaction strength, and the low-lying many-particle spectrum of the Fe2S2 dimer.

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Language(s): eng - English
 Dates: 2019-04-032019-06-202020-01-21
 Publication Status: Published in print
 Pages: 12
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/acs.inorgchem.9b00974
 Degree: -

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Title: Inorganic Chemistry
  Abbreviation : Inorg. Chem.
Source Genre: Journal
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Publ. Info: Washington, DC : American Chemical Society
Pages: - Volume / Issue: 59 (2) Sequence Number: - Start / End Page: 984 - 995 Identifier: ISSN: 0020-1669
CoNE: https://pure.mpg.de/cone/journals/resource/0020-1669