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The temperature dependence of the spin-lattice relaxation time (T 1H ) of  1 H NMR measured in tetramethylammonium hexachloroplumbate(IV), (Me 4 N) 2 [PbCl 6 ], showed a deep and a shallow minimum near 190 and 115 K, respectively. Since the presence of two kinds of crystallographically nonequivalent cations in the room-temperature Fd 3c unit cell has been reported, the deep T 1H  minimum was assigned to the overall reorientation of three quarters of the Me 4 N +  ions and the shallow minimum to that of the remaining cations. Two different temperature dependences of the chlorine NQR spin-lattice relaxation time (T 1Q ), attributable to a modulated electric-field-gradient by the protonic motion, were observed in (Me 4 N) 2 [MCl 6 ] (M = Pb, Sn, Te). One is found in the Pb complex whose T 1Q  stems from the cationic motion responsible for the deep T 1H  minimum, and the other one is determined by the cationic motion giving the shallow T 1H  minimum. Although all room-temperature phases of these complexes are well described by the Fd 3c unit cell, the presence of different temperature dependences of T 1Q  suggests that the CH 3  groups in the respective complexes take different orientations in the crystals

Unusual Temperature Dependence of 35 Cl NQR Spin-Lattice Relaxation Time in [(CH 3 ) 4 N] 2 [MCl 6 ] (M = Pb, Sn, Te)