Orbital energy mismatch engenders high-spin ground states in heterobimetallic complexes.
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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.
Coste, S. C., Pearson, T. J., Altman, A. B., Klein, R. A., Finney, B. A., Hu, M. Y., ... Freedman, D. E.
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Coste, Scott C||Pearson, Tyler J||Altman, Alison B||Klein, Ryan A||Finney, Brian A||Hu, Michael Y||Alp, E Ercan||Vlaisavljevich, Bess||Freedman, Danna E