Interplay between Electronic, Magnetic, and Transport Properties in Metal Organic–Radical Frameworks

Development of modern electronic and spintronic technologies depends in large part on the ability to design materials exhibiting switchable magnetic electrical properties. Here, motivated by successful demonstration reversible redox switching order conductivity 2dimensional metal-organic frameworks (MOFs) based benzoquinoid linkers, we perform hybrid density functional theory calculations investigate this phenomenon at atomistic level. Electronic, charge transport properties have been systematically investigated for oxidized reduced forms Mn Fe (i.e., (Me 4 N) 2 [Mn L 3 ], [Fe ] Na Na(Me respectively with deprotonated chloranilic acid as L). We demonstrate that experimentally observed increase upon ligand-centered reduction MOF (10 9 S•cm ?1), is due cooperative effects arising from band gap presence electrons lower effective mass. Superior (by least orders magnitude) pair framework compared analog stems similar factors and, notably, a electron delocalization compound.