A method using the
2H-NMR spectra was shown to be useful to study the solid state physics in diamagnetic and paramagnetic compounds and in crystals having a modulated structure. The spectra and
T1 of NMR in solids were measured for [
M(H
2O)
6][
AB6] crystals to investigate the static and dynamic structure of H
2O and [
M(H
2O)
6]
2+ as well as the dynamics of the electron spin in the paramagnetic
M2+ ion. The physical properties of [
M(H
2O)
6][
AB6] were found to be as follows: (1) The spin-lattice relaxations of the electron spin of
M2+ in [
M(H
2O)
6][SiF
6] (
M2+=Fe
2+, Co
2+, Ni
2+) are dominated by the Orbach process, the Orbach process, and the Raman process, respectively. The spin-lattice relaxation of the electron spin of Cu
2+ in [Cu(H
2O)
6][PtCl
6] is caused by jumping between the Jahn-Teller configurations. (2) In [Cu(H
2O)
6][PtCl
6], H
2O and [Cu(H
2O)
6]
2+ undergo 180° flips and jumping between the different Jahn-Teller configurations, respectively. A weakening of the hydrogen bond O-H…Cl upon deuteration results in a lowering of the transition temperature. (3) In [
M(H
2O)
6][SiF
6], H
2O and [
M(H
2O)
6]
2+ undergo 180° flips and reorientation about the
C3 axis, respectively. The order-disorder transition is closely related to a freezing of this reorientation. (4) By elongation of [
M(H
2O)
6]
2+ along the
C3 axis, the mobility becomes higher. (5) The disorder of [Fe(H
2O)
6]
2+ in the high-temperature phase of [Fe(H
2O)
6][SiF
6] is dynamic. Rotational modulation of [Mg(H
2O)
6]
2+ along the
C3 axis exists in the incommensurate phase of [Mg(H
2O)
6][SiF
6].
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