Using infrared and optical absorption spectroscopy ill combination wit
h photoconductivity measurements on uranium-doped calcium fluorite cry
stals, we clarify a controversy in the assignment of U2+ and U4+ ion v
alences in CaF2 crystals which exhibit different coloration. The energ
y thresholds of donor-like processes (photoionization) follow the sequ
ence of ionization potentials for uranium ions of different valences a
nd indicate the green and yellow colors to be due to U4+ Of different
charge compensation.