The energy levels of
Gd3+ in the
6P,
6I, and
6D 4
f7 configuration in cubic, tetragonal, and cluster sites in
CaF2 have been excited by two-photon absorption. The relative two-photon intensities and polarization dependence show behavior which is similar to that previously observed for
Gd3+:
LaF3 and
Eu2+:
CaF2 and which requires higher-order perturbation theory in the virtual intermediate 4${f}^{6}$5d configuration.