Relationship between the Coordination Geometry and Spin Dynamics of Dysprosium(III) Heteroleptic Triple-Decker Complexes

When using single molecule magnets (SMMs) in spintronics devices, controlling the quantum tunneling of the magnetization (QTM) and spin-lattice interactions is important. To improve the functionality of SMMs, researchers have explored the effects of changing the coordination geometry of SMMs and the magnetic interactions between them. Here, we report on the effects of the octa-coordination geometry on the magnetic relaxation processes of dinuclear dysprosium(III) complexes in the low-temperature region. Mixed ligand dinuclear Dy3+ triple-decker complexes [(TPP)Dy(Pc)Dy(TPP)] (1), which have crystallographically equivalent Dy3+ ions, and [(Pc)Dy(Pc)Dy(TPP)] (2), which have non-equivalent Dy3+ ions, (Pc2- = phthalocyaninato; TPP2- = tetraphenylporphyrinato), undergo dual magnetic relaxation processes. This is due to the differences in the ground states due to the twist angle (phi) between the ligands. The relationship between the off-diagonal terms and the dual magnetic relaxation processes that appears due to a deviation from D-4h symmetry is discussed.