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Published December 9, 2011 | public
Journal Article

A Theoretical Study of the 3d-M(smif)_2 Complexes: Structure, Magnetism, and Oxidation States

Abstract

We carry out a theoretical investigation of the recently reported M(smif)_2 series1, 2 and find a number of interesting phenomena. These include complex potential energy surfaces with near-degenerate stationary points, low-lying states, non-trivial electron configurations, as well as non-innocent ligand behavior. The M(smif)_2 exhibit a delicate balance between geometry and electronic structure, which has implications not only for their reactivity but also for controlling their properties through ligand design. We address methodological issues and show how conceptual quantities such as oxidation states and electronic configurations can be extracted through a simple analysis of the electron and spin densities—without a complicated examination of the underlying orbitals.

Additional Information

© 2011 Wiley-VCH Verlag GmbH& Co. KGaA, Weinheim. Received: April 14, 2011. Published online on September 27, 2011. We thank Prof. Thomas R. Cundari for providing his preliminary B3LYP results on some of the studied complexes, Profs. Troy Van Voorhis, Roald Hoffmann, and Emily A. Carter for helpful discussions on oxidation states, as well as Profs. Christopher J. Cramer and Frank Neese for discussions on the application of DFT and CASSCF in transition metal chemistry. G.K.C. acknowledges support from the National Science Foundation NSF CAREER award.

Additional details

Created:
August 22, 2023
Modified:
October 24, 2023