New thiocyanato and azido adducts of the redox-active Fe(η5-C5Me5)(η2-dppe) center: Synthesis and study of the Fe(II) and Fe(III) complexes

► The thiocyanato- (5/5+) and azido- (6/6+) Fe(II)/Fe(III) complexes were synthesized. ► These new compounds were extensively characterized and modelled by DFT. ► The g-tensor anisotropy was determined for 5[PF6] by single-crystal ESR measurements. ► An accurate picture of their electronic structures is provided.