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Boosting Vis/NIR Charge-Transfer Absorptions of Iron(II) Complexes by N-Alkylation and N-Deprotonation in the Ligand Backbone.
Chemistry : a European Journal 2017 June 13
Reversing the metal-to-ligand charge transfer (3 MLCT)/metal-centered (3 MC) excited state order in iron(II) complexes is a challenging objective, yet would finally result in long-sought luminescent transition-metal complexes with an earth-abundant central ion. One approach to achieve this goal is based on low-energy charge-transfer absorptions in combination with a strong ligand field. Coordinating electron-rich and electron-poor tridentate oligopyridine ligands with large bite angles at iron(II) enables both low-energy MLCT absorption bands around 590 nm and a strong ligand field. Variations of the electron-rich ligand by introducing longer alkyl substituents destabilizes the iron(II) complex towards ligand substitution reactions while hardly affecting the optical properties. On the other hand, N-deprotonation of the ligand backbone is feasible and reversible, yielding deep-green complexes with charge-transfer bands extending into the near-IR region. Time-dependent density functional theory calculations assign these absorption bands to transitions with dipole-allowed ligand-to-ligand charge transfer character. This unique geometric and electronic situation establishes a further regulating screw to increase the energy gap between potentially emitting charge-transfer states and the non-radiative ligand field states of iron(II) dyes.
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