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This report concerns one role of Raman spectroscopy for observing the behavior of solids under high pressures—that is, Raman spectroscopy is an experimental technique for characterizing in situ phases of solids that occur only at high pressures. This task has several aspects, three of which receive part cular attention in the work described here. These are: a. the detection of phase transformations in solids under pressure including determination of phase boundaries and other characteristics of the transition; b. assignment of the Raman spectrum in terms of plausible structures and other properties of the high-pressure phases; and c. interpretation of pressure dependences of vibrational spectra in terms of interatomic interaction; that may explain the occurrence of known transitions, with the goal of generalizing the analysis to describe properties of related materials under conditions that may not be accessible for experimentation.