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The temperature dependence of the chlorine NQR spin-lattice relaxation time T 1Q  was observed for trimethylsulfonium hexachlorometallates(IV), [(CH 3 ) 3 S] 2 MCl 6  (M = Pt, Sn), trimethylammonium hexachlorostannate(IV), [(CH 3 ) 3 NH] 2 SnCl 6 , and tetramethylphosphonium hexachlorostannate(IV), [(CH 3 ) 4 P] 2 SnCl 6 . The quadrupolar relaxation in [(CH 3 ) 3 NH] 2 SnCl 6  and [(CH 3 ) 4 P] 2 SnCl 6  can be described by the usual librational and reorientational motion of the complex anion at lower and higher temperatures, respectively. Besides T 1Q  due to these two mechanisms, T 1Q  minimum was observed at ca. 90 and 120 K for [(CH 3 ) 3 S] 2 PtCl 6  and [(CH 3 ) 3 S] 2 SnCl 6 , respectively, which is attributable to the electric field gradient modulation by the motion of the [(CH 3 ) 3 S] +  cation having lone-pair electrons. The activation energies for the isotropic reorientation of the complex anion were determined as 46, 65, 59, and 60 kJ mol  -1  for [(CH 3 ) 4 P] 2 SnCl 6 , [(CH 3 ) 2 NH] 2 SnCl 6 , [(CH 3 ) 3 S] 2 PtCl 6 , and [(CH 3 ) 3 S] 2 SnCl 6 , respectively

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Electric field Gradient Modulation by Motion of Lone-Pair Electrons in [(CH 3 ) 3 S] 2 MCl 6  (M = Pt, Sn) as a Possible Relaxation Mechanism of Chlorine Nuclear Quadrupole Resonance