Raman light scattering and c-axis resistivity evidence for a pressure-induced stage transformation in PdAl2Cl8 intercalated graphite

We have examined several samples of first- to third-stage PdAl2Cl8-intercalated graphite under hydrostatic pressures up to 1 GPa. In stage-1 highly oriented pyrolytic graphite-(HOPG) and single-crystal-graphite-based materials, the c-axis resistivity decreases sharply above a few kilobars; pressure release induces a reversible return to the initial value only in the case of the latter sample. Raman spectra taken in situ under pressure on a HOPG-based material show similarly irreversible effects. Analysis of the spectra taken on higher-stage samples leads to the conclusion that hydrostatic pressure beyond a few kilobars increases the density of the intercalate within the graphitic galleries, transforming the initial sample to a higher-stage material. Since there is no loss of intercalate, the overall intercalate-to-host charge transfer remains constant so that the Raman frequency is approximately the same for both first- and second-stage products. This is an unusual situation in which there is thus an apparent lack of Raman signature in spite of the stage change.