The temperature‐dependent structure of crystalline methylammoniumtrihalogenoplumbates (II)—CH3NH+3PbX3 (X=Cl, Br, I)—as determined by x‐ray diffraction, is compared with measurements of the temperature‐dependent complex permittivity at frequencies of 50–150 GHz. The dielectric measurements reveal a picosecond relaxation process which corresponds to a dynamic disorder of the methylammonium group in the high‐temperature phases of the trihalogenoplumbates.

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