Energy levels of the4f2electronic configuration of Pr3+in SrAl12O19(SAM) have been determined from polarized absorption and fluorescence spectra using crystals, charge-compensated with Mg2+, at temperatures between about 20 and 300 K. Energy level assignments were made initially by comparing the crystal spectra with energy levels calculated by using crystal-field parameters,Bkm, compatible with those previously reported for Nd3+in SAM. TheBkmwere varied to obtain a best fit between experimental and theoretical energies, and the final values:B20=−94,B40=1047,B60=−1397, andB66=−1245cm−1give an rms fit of 14.5 cm−1. TheBkmfor Pr3+in SAM were also used along with a result relating theBkmto crystal-field components,Anm, derived in a lattice sum calculation to obtainBkmvalues for all the triply ionized rare-earth ions in SAM. Odd-foldAkmare also given that are required in the intensity and lifetime calculations and yield results in good agreement with the measurements. In addition, the results of our energy level fitting were useful in estimating absorption and emission cross sections, as well as lifetimes and branching ratios, for the variousJmultiplets. The evidence given here that the room temperature fluorescence quantum efficiency of3P0in lightly doped Pr in SAM is near unity strengthens the case that this is a potentially useful laser material. The theoretical model and method of analysis used is useful for the calculation of energy levels, wave functions, transition probabilities, etc., for any rare-earth RE3+ion in any host of known crystal structure. ©1997 American Institute of Physics.