The current proposal is devoted to synthesis and characterization of multifunctional molecular materials by designing heterotrinuclear cationic complexes containing three different metal ions (3d-4f-3d’), which can be used as building blocks in the construction of magnetic systems containing four different spin carriers. The modular design of these systems is intended to control the dimensionality of the molecular architectures (by the proper use of the anionic metallocomplexes which can act as bridge, terminal ligands or non-coordinating counter-ions), and to modulate the chemical and physical properties by the appropriate selection of the metal ions used for the formation of the cationic trinuclear bricks and anionic metalloligands (e.g. a high value of the spin ground state, caused by a ferromagnetic coupling between the metal ions within the trinuclear unit, associated with large magnetic anisotropy originating from the 4f and/or 3d metal ions can generate a single molecule magnet behaviour). A topical trend in the field of molecular materials is to combine within the same material at least two different physical properties, such as magnetism and conductivity, which can coexist or interplay. In this direction, the co-crystallization of heterotrinuclear cationic complexes (3d-4f-3d’) with anionic species presenting multi-stability in different oxidation states and high tendency to self-organize in columns in solid state (TCNQ, bis-dithiolene complexes) can be envisaged as a rational method to obtain multifunctional materials (magnetic conductors).
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