Isoreticular Modulation of Electrical Conduction and Magnetic Properties in Semiconducting Lanthanide‐based Metal−Organic Frameworks

ABSTRACT The integration of tunable magnetic properties and electrical conductivity within a single material presents significant opportunities for spintronic applications and quantum information processing. This paper describes the first systematic investigation of electrical conduction and magnetism in four novel isostructural electrically conductive metal−organic frameworks (cMOFs), Ln‐HHTP (Ln = Sm, Eu, Gd, Tb), constructed using lanthanide ions and hexahydroxytriphenylene (HHTP) ligands. These materials show tunable semiconducting properties arising from efficient interlayer charge transport, which can be modulated by the density of states of the metal centers. Ln‐HHTP cMOFs exhibit different magnetic properties, with magnetic interactions varying from antiferromagnetism in Tb‐HHTP to ferromagnetism in Gd‐HHTP and Sm‐HHTP. The magnetic properties in Ln‐HHTP are modulated by single‐ion anisotropies of Ln 3+ spins and inherent geometric frustration within the kagome lattice. Moreover, Gd‐HHTP and Tb‐HHTP demonstrate robust quantum tunneling of magnetization. This work advances the understanding of cMOF magnets and underscores their potential as tunable platforms for next‐generation spintronic and quantum technologies.