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Issue 36, 2020

Orbital energy mismatch engenders high-spin ground states in heterobimetallic complexes

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Abstract

The spin state in heterobimetallic complexes heavily influences both reactivity and magnetism. Exerting control over spin states in main group-based heterobimetallics requires a different approach as the orbital interactions can differ substantially from that of classic coordination complexes. By deliberately engendering an energetic mismatch within the two metals in a bimetallic complex we can mimic the electronic structure of lanthanides. Towards this end, we report a new family of complexes, [Ph,MeTpMSnPh3] where M = Mn (3), Fe (4), Co (5), Ni (6), Zn (7), featuring unsupported bonding between a transition metal and Sn which represent an unusual high spin electronic structure. Analysis of the frontier orbitals reveal the desired orbital mismatch with Sn 5s/5p primarily interacting with 4s/4p M orbitals yielding localized, non-bonding d orbitals. This approach offers a mechanism to design and control spin states in bimetallic complexes.

Graphical abstract: Orbital energy mismatch engenders high-spin ground states in heterobimetallic complexes

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Article information


Submitted
09 Jul 2020
Accepted
31 Aug 2020
First published
01 Sep 2020

This article is Open Access
All publication charges for this article have been paid for by the Royal Society of Chemistry

Chem. Sci., 2020,11, 9971-9977
Article type
Edge Article

Orbital energy mismatch engenders high-spin ground states in heterobimetallic complexes

S. C. Coste, T. J. Pearson, A. B. Altman, R. A. Klein, B. A. Finney, M. Y. Hu, E. E. Alp, B. Vlaisavljevich and D. E. Freedman, Chem. Sci., 2020, 11, 9971 DOI: 10.1039/D0SC03777J

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