Density-functional theory of spin polarization and spin coupling in iron—sulfur clusters

Louis Noodleman, David A. Case

Research output: Contribution to journalArticle

572 Scopus citations


This chapter discusses recent progress toward the development of a unified picture of the electronic structures and spin interactions of iron–sulfur and related systems; these concepts provide a close connection between a spin Hamiltonian description and a more detailed orbital picture of the electron distribution. The iron–sulfur proteins and synthetic analogs are challenging systems for quantum mechanical methods because they contain a large number of electrons and because spin polarization and spin coupling are essential features of the complexes. Standard approaches of ab initio quantum chemistry start from a spin-restricted picture, which is poorly adapted to problems involving high-spin transition metal centers. For this reason, a combination has been developed of broken symmetry and spin-unrestricted methods that is particularly well adapted to study spin-polarized and spin-coupled systems. These ideas are well adapted for use with density-functional methods. In the chapter, the basic ideas are developed of this approach, using a perturbation theory formalism to rationalize the spin Hamiltonian and energy-splitting formulas that should be appropriate for spin-coupled transition metal clusters.

Original languageEnglish (US)
Pages (from-to)423-458
Number of pages36
JournalAdvances in Inorganic Chemistry
Issue numberC
StatePublished - Jan 1 1992
Externally publishedYes

All Science Journal Classification (ASJC) codes

  • Inorganic Chemistry

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