Magnet Design by Integration of Layer and Chain Magnetic Systems in a π‐Stacked Pillared Layer Framework

The control of inter-lattice magnetic interactions is a crucial issue when long-range ordered magnets that are based on low-dimensional magnetic frameworks are designed. A "pillared layer framework (PLF)" model could be an efficient system for this purpose. In this report, A magnet based on a π-stacked PLF with a phase transition temperature of 82 K, which can be increased to 107 K by applying a pressure of 12.5 kbar, is rationally constructed. Two types of low-dimensional magnetic framework systems, an electron donor/acceptor magnetic layer and a charge transfer [FeCp*2](+)TCNQ(.-) columnar magnet ([FeCp*2](+) = decamethylferrocenium; TCNQ = 7,7,8,8-tetracyano-p-quinodimethane), are integrated to fabricate the magnet. This synthetic strategy employing a combination of layers and chains is widely useful not only for magnet design, but also for the creation of multifunctional materials with pores and anisotropic frameworks.