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The  35 Cl NQR spin-lattice relaxation mechanism in isomorphous Ni(H 2 O) 6 SnCl 6  and Mg(H 2 O) 6 SnCl 6  crystals is reported. The spin-lattice relaxation time T 1Q  in the Ni compound is determined mainly by a paramagnetic relaxation. However, above ca. 400 K T 1Q  decreased rapidly and a log vs. T 1  curve was almost linear. This steep decrease of T 1Q  was explained by reorientational motions of the anions with an activation energy of 73 kJ mol -1 . In addition, a double minimum in T 1Q , which can be interpreted as arising from the fluctuation o f the electric field gradient (EFG) at the chlorine site caused by cationic thermal motions, was observed around room temper ature. The temperature dependence of the  35 Cl NQR T 1Q  in the Mg salt is re-analysed in the light of the EFG -modulation effect caused by a 180° flip motion of the H 2 O molecules and an overall reorientational motion of the [Mg(H 2 O) 6 ] 2+  octahedral cations as a whole.

35 Cl NQR Spin-Lattice Relaxation Mechanism in Ni(H 2 O) 6 SnCl 6 and Mg(H 2 O) 6 SnCl 6 Crystals