Optimization of rare-earth-doped fluorides for infrared lasers

The rare-earth-doped fluoride crystals Tm,Dy:BaY₂F₈ (Tm,Dy:BYF), Yb,Pr:NaYF₄ (Yb,Pr:NYF), and Nd:NYF show considerable promise as infrared laser materials, operating at 3 μm, 1.3 μm, and 1.06 μm respectively. Lasing has been reported previously on all three ionic transitions, but not in these crystals. Optimization of these materials for laser applications requires a more complete spectroscopic characterization than is currently available, particularly with regard to the key parameters of fluorescence lifetime and stimulated emission cross section.; To further the optimization process, polarized absorption and emission have been measured for Tm,Dy:BYF, Yb,Pr:NYF, and Nd:NYF, and relevant fluorescence lifetimes have been measured or estimated. For Tm,Dy:BYF and Yb,Pr:NYF which rely upon sensitization, energy transfer parameters were calculated. Results were used in a mathematical model to determine the conditions in which lasing may be obtained. The long upper laser level lifetime in Tm,Dy:BYF translates into low threshold pump intensity, but the ability to reach threshold depends strongly on active ion concentration. The short lifetime in Yb,Pr:NYF leads to much higher threshold pump intensities, but lasing is still attainable if resonator loss is minimized. In Nd:NYF lasing was demonstrated, with a maximum of 60 mW output from an absorbed pump power of 345 mW, and a slope efficiency of 21%. Thresholds were high owing to resonator losses near 9%.; Two chief issues involving the optimization of these laser materials were identified and explored. First, identification of the orientation for which emission cross section is highest is complicated in Tm,Dy:BYF by the presence of strong magnetic dipole radiation on the 3 μm transition. This effect makes it necessary to account for the polarization of both the electric and magnetic fields of the emitted radiation when determining an optimal crystal orientation, an accounting further complicated by the low symmetry of the monoclinic BYF host crystal.; Second, the effect of host crystal on fluorescence lifetime was considered by comparing lifetime values for the same ionic manifolds in BYF, NYF, and other host crystals. NYF has especially low phonon energies, which leads to longer lifetimes on the longer wavelength transitions which are susceptible to multiphonon relaxation. This advantage is especially needed for lasing at 1.3 μm in Pr where the upper level lifetime is very short. On the shorter wavelength transitions in Tm and Nd, however, the role of phonons is negligible and lifetimes are somewhat shorter than in other fluoride hosts.