[en] Raman light scattering, infrared reflection, and infrared absorption spectra are reported for the mineral pollucite and other cesium aluminosilicate formulations of interest to the beneficial use program of Sandia Laboratories. In addition, Raman spectra of crystals of a pure-phase pollucite are presented. Assignment of the active normal modes is made; a resonance at 200 cm^-1 is tentatively assigned to a Cs cage mode; the remaining resonances are assigned to oxygen stretching vibrations of the Al-0 and Si-0 bonds, external vibrations of the aluminosilicate framework, and to more complex vibrations involving all of the atoms of the crystal. It is shown that by using a reference crystalline spectrum, oher cesium aluminosilicate structures can be identified as polycrystalline in nature with a makeup similar to pollucite. Structural alterations (broken bonds) as well as state changes (crystalline to amorphous) can also be ascertained by Raman spectroscopy. Water is found only in mineral pollucite, where it exists as a monomer, hydrogen-bonded to oxygen atoms that form its cage. Satisfactory results were obtained from a range of materials; black to milky to clear in appearance