Enhancing Intramolecular Ferromagnetic Coupling in Tetrathiafulvalene-Nitronyl Nitroxide-Based Compounds through Spin Polarization Mechanism

distort the BTBN radical arrangement within the molecular crystal as little as possible, in the event the material can be synthesized. NICSiso(1) and Wiberg’s Bond Order are analyzed to further assist in identifying promising potential candidates, since the decrease in aromaticity is expected to enhance the diradical character and give rise to a larger magnetic coupling value. The most favorable diradical building block to replace the BTBN moiety results from using a hydroxyl-ethylene ( (H)C=C(OH) ) as a coupler preserving BTBN original radicals, namely, NN and TTF + * units. This study aims at illustrating the feasibility of improving the intramolecular FM interaction between radical moieties, which is fully realized, as a first step towards the synthesis of new materials with (possibly) enhanced magnetoresistance properties.