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Topotactic low-temperature reactions such as intercalation, deintercalation and ionexchange reactions provide a rational design of new structures of non-molecular extended solids which are otherwise not accessible by conventional high-temperature solid-state reactions [1-4]. Among candidate oxide materials used as a precursor of such reactions, the most intensively studied system is the Dion-Jacobson (DJ) type layered perovskite (Figure 1). The chemical formula of the DJ phase is expressed as A [An–1BnO3n+1], where A is an alkali metal (Na, Rb, ...), A is an alkaline earth or rare earth metal (Ca, Sr, La, ...), B is a d0 transition metal (Ti, Nb, Ta, ...), and n is the number of perovskite layers (2, 3, 4, ...) [5, 6]. Here, alkali metal ions at the A site are highly reactive because of ionic (i.e., weak) A -O bonding, while the perovskite unit [An–1BnO3n+1] is strongly bonded and is chemically inert. By exploiting ion-exchange reactions with various reagents, a wide variety of new or improved chemical and physical functionalities including (photo)catalysis [7, 8], ionic conductivity [9] and superconductivity [10] have been developed. However, ion-exchange reactions are rarely employed for the purpose of materials design toward low-dimensional magnetism, because those who work in this filed (mostly physicists) are not familiar with such chemical processing. In addition, compounds obtained by soft-chemical approaches involve negative effects on the crystal structure, for example, poor crystallinity, nonstoichiometry and defects. In particular, it is known that a tiny defect can easily destroy or mask intrinsic magnetic properties of low-dimensional quantum systems.

Ion-Exchange Reactions for Two-Dimensional Quantum Antiferromagnetism