In conclusion, we have carried out the first RT-TDDFT study of excited-state dynamics in PFAS pollutants to understand their photo-induced degradation mechanisms. By explicitly accounting for non-adiabatic excited-state interactions in solvated PFOA/PFOS, we show that these photo-induced excitations enable a charge-transfer process that polarizes the C-F bond, resulting in a dynamic dissociation on a femtosecond time scale. Moreover, we show that this photo-induced process is highly selective and only affects the PFOA/PFOS molecules while keeping the surrounding water molecules intact. The parameters used in these calculations are commensurate with commercially available monochromatic light/laser sources and shed crucial mechanistic insight into their excited-state degradation dynamics.