X‐ray Crystallographic Analysis of a Tailor‐Made Bis(phthalocyaninato)‐Tb III Single‐Molecule Magnet as a Fundamental Unit for Supramolecular Spintronic Devices

The single‐crystal X‐ray diffraction analysis of the title compound, the pyrene‐substituted unsymmetrical bis(phthalocyaninato)terbium(III) Single‐Molecule Magnet (SMM) [Pc–Tb–Pc*] 0 ( 1 ) (Pc = dianion of phthalocyanine, P* = dianion of phthalocyanine decorated with six flexible hexyl chains and one 4‐pyren‐1yl‐butoxy group), was carried out. Both phthalocyaninato ligands in 1 are distorted from planarity and, therefore, adopt a biconcave shape. Effective π–π interactions between the molecules lead to the formation of head‐to‐tail π dimers. These dimers are stacked in the crystal, forming adjacent, parallel columns, the axes of which are tilted by 30° with respect to the C 4 axes of the macrocycles. Herein, we also report the synthesis and characterization of the new isostructural Dy (compound 2 ) and Ho (compound 3 ) analogues of 1 .