NMR-spectroscopic studies on solutions as well as X-ray structural inv
estigations of the solids reveal that both Me2Si[N(Li)SiMe3]2 (1) and
(Me3Si)2N-SiH[Me3SiN(Li)]2 (2) are dimeric molecular compounds in both
phases. Moreover, in spite of their different reactivity and constitu
tion, the Li, N, and Si atoms of both dimers from similar ''basketshap
ed'' molecular cages in the solid state. H-1-, Li-6/7-, and C-13-NMR s
pectra in toluene show temperature dependence which is ascribed to int
ramolecular bond fluctuations within the molecular cages causing an eq
uilibration of the two enantiomers of both compounds which cocrystalli
ze in the solid state. The different activation energies for the motio
ns of 1 and 2, which are deduced by inspection of the spectra, can be
explained by participation of the hydride hydrogen in the intramolecul
ar process in 2.