The reorientational spectra in the mid-and far infrared of OH Ϫ , OD Ϫ , SH Ϫ , SD Ϫ , SeH Ϫ , and TeH Ϫ in a variety of different alkali halides are studied. All of these systems have ϳ300 cm Ϫ1 modes due to librations of the diatomics about their centers of mass. A surprising change in the dynamics of these librational modes with increasing temperature is discovered: their absorption strengths are observed to disappear by ϳ150 K in the sodium-chloride-structure hosts and reappear in the millimeter-wave region in the forms of generalized-Debye spectra. This is in striking contrast to what is expected on the basis of the estimated orientational barrier heights using the known librational frequencies. It also contrasts with the cesium-chloride-structure salts, where the librational strengths of the molecules are conserved up to RT. The temperature-dependent variations of the fcc systems can be explained using a thermally activated jump-rotational-diffusion model wherein each defect hops with temperature-dependent dwell times between two distinct elastic configurations of the lattice-defect system: one involving librational and the second supporting diffusive rotational states.