[N(CH3)3H]2ZnCl4 has been studied by X-ray powder diffraction patterns, differential scanning calorimetry (DSC), and impedance spectroscopy. The [N(CH3)3H]2ZnCl4 hybrid compound is crystallized at room temperature (T ≈ 300 K) in the orthorhombic system with Pnma space group. Five phase transitions (T1 = 255 K, T2 = 282 K, T3 = 302 K, T4 = 320 K, and T5 = 346 K) have been proved by DSC measurements. The electrical technique was measured in the 10−1-107 Hz frequency range and 233–363 K temperature interval. The frequency dependence of alternative current (AC) conductivity is interpreted in terms of Jonscher's law. The AC electrical conduction in [N(CH3)3H]2ZnCl4 is analyzed by different processes, which can be attributed to several models: the correlated barrier hopping model in phase I, the overlapping large polaron tunneling model in phase II, the quantum mechanical tunneling model in phase IV, and the non-overlapping small polaron tunneling model in phases III, V, and VI. The conduction mechanism is studied with the help of Elliot's theory, and the Elliot's parameters are determined.
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