Site-selective laser spectroscopy of Pr3+C4v symmetry centers in hydrogenated CaF2:Pr3+ and SrF2:Pr3+ crystals

Abstract
Laser-selective excitation and optical-absorption techniques have been used to establish comprehensive sets of energy levels for both the F and hydrogenic varieties of the tetragonal symmetry (C4v) centers in SrF2 and CaF2. Polarization of the various spectral lines was used to determine the symmetry labels of many of the energy levels. Reversals of the ordering of some levels between SrF2 and CaF2 are found and, in particular, the two lowest levels (D1 and D2) of the 1 D2 multiplet, which are the originating levels for many of the observed emission transitions, have reversed-symmetry label assignments in SrF2 and CaF2. Differences were found between the ground-state Zeeman splittings for the C4v F and D centers for both SrF2 and CaF2. Fluorescence lifetimes of the C4v hydrogenic centers show a strong dependence on the particular charge-compensating ion present through nonradiative decay processes involving the respective local mode phonons. The upconversion spectra observed for F, T, and D varieties of the C4v centers in SrF2 and for the C4v F center in CaF2 are all consistent with excitation of specific subsets of nearby C4v centers.