Thermodynamic Properties, Structural Characteristics, and Cation Dynamics of Perovskite-Type Layer Crystal [NH(3)(CH(2))(2)NH(3)]ZnCl(4)

[Image: see text] In this study, we investigated the structural dynamic features of the [NH(3)(CH(2))(2)NH(3)]ZnCl(4) crystal as a function of temperature through magic angle spinning (MAS) (1)H nuclear magnetic resonance (NMR), MAS (13)C NMR, and static (14)N NMR. From the chemical shifts, changes in the structural environments of (13)C and (14)N were evident. The (1)H spin–lattice relaxation time (T(1ρ)) values at high temperatures undergo molecular motion according to the Bloembergen–Purcell–Pound theory, and the (13)C T(1ρ) value also varied abruptly with increasing temperature. Although the phase-transition temperature was not detected from the differential scanning calorimetry result, the chemical shifts and T(1ρ) results showed discontinuities around 300 K. Herein, the activation energies of molecular motion for (1)H and (13)C obtained from T(1ρ) are discussed. In addition, we compare the structural dynamics of diammonium-type [NH(3)(CH(2))(2)NH(3)]ZnCl(4) obtained in this study and monoammonium-type [CH(3)NH(3)](2)ZnCl(4) previously reported. The findings reported herein can provide important insights for potential applications of [NH(3)(CH(2))(2)NH(3)]ZnCl(4) crystals.