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Two  35 Cl NQR frequencies, V a = 9.148 and V b = 28.286 MHz, were observed at 77.3 K in NH 4 ICl 2 . V a  and V b  showed a strong temperature dependence with positive and negative temperature coefficient, respectively. This anomalous temperature dependence is explained by a temperature dependence of the mole fraction of the hydrogen-bonded ICl -  2  ion. The energy difference, ΔE anion , of the anion between the hydrogen-bonded and the non-bonded states was derived as ΔE anion  ≈ 700 K (5.8 kJ mol -1 ) and as ΔE anion  ≈ 640 K (5.3 kJ mol -1 ) for NH 4 ICl 2  and ND 4 ICl 2 , respectively. The temperature dependence of the spin-lattice relaxation time 1 showed a clear minimum in the ln 1 vs. 103K plots, which can be interpreted as due to EFG modulation by the reorientational motion of the ammonium ion. The reorientation of the ammonium ion among stable and meta-stable orientations is expected to be responsible to the temperature variation of electronic structure of the ICl -  2  anion.

Change in Electronic Structure of the ICl – 2 Anion in NH 4 ICl 2 Crystals due to an Excitation of Reorientational Motion of the Ammonium Ion