Structural and electronic tuning of hybrid metal thiocyanate <i>N</i>-oxides

Hybrid metal thiocyanates are highly tailorable materials isolable under mild synthetic conditions. By varying pyridine-<i>N</i>-oxide derivatives within manganese, cobalt, and nickel congeners, we show fine-tuning of structural and electronic features depending on molecular substituent and metal selection, providing a roadmap for application-specific customization and potential property-tuning.