The experimental data are provided in subfolders by species, which contain each three files: (i) the normalized intensities (Eq. 1 in the article) for the mass peaks corresponding to the parent cation and its fragments as a function of the VUV irradiation time, (ii) the experimental error bars associated with these intensities, (iii) the curves corresponding to the fitting functions that were derived with the procedure described in Sect. 2.4. Each folder is named by the parents species: Pyr+ for pyrene (C16H10+), H6-Pyr+ for 1,2,3,6,7,8-hexahydro-pyrene (C16H16+), MePyr+ for 1-methylpyrene (C17H12+), EtPyr+ for 4-ethyl-pyrene (C18H14+), Cor+ for coronene (C24H12+), MeCor+ for methyl-coronene (C25H14+), EtCor+ for ethyl-coronene (C26H16+). In addition, the VUV_source folder contains the measurements corresponding to the VUV source calibration (see Fig. A.1 in the article appendix). The folder for TD-DFT calculations gathers the calculated photoabsorption cross-sections for all species of interest (see Fig. D.1 in the article appendix).