Spectroscopic, laser, and χ(3) nonlinear optical properties of tetragonal PbWO4, NaY(WO4)2, CaWO4, and monoclinic CdWO4 and ZnWO4 were investigated. Particular attention was paid to Nd3+-doped and undoped PbWO4 and NaY(WO4)2 crystals. Their absorption and luminescence intensity characteristics, including the peak cross sections of induced transitions, were determined. Pulsed and continuous-wave lasing in the two 4 F 3/2→ 4 I 11/2 and 4 F 3/2 →4 I 13/2 channels was excited. For these five tungstates, highly efficient (greater than 50%) multiple Stokes generation and anti-Stokes picosecond generation were achieved. All the observed scattered laser components were identified. These results were analyzed and compared with spectroscopic data from spontaneous Raman scattering. A new crystalline Raman laser based on PbWO4 was developed for the χ(3) conversion frequency of 1-µm pump radiation to the first Stokes emission with efficiency up to 40%. We classify all the tungstates as promising media for lasers and neodymium-doped crystals for self-stimulated Raman scattering lasers.
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