Multi-Stokes ultrashort pulse shapes and their relative positions of synchronously pumped stimulated Raman scattering (SRS) on combined primary and secondary vibrational modes in a BaWO4 crystal are investigated. An original method of its simultaneous measurement with the help of a streak camera has been developed. The structure of SRS pulses at the pulse shortening effect down to the pulse duration, close to the dephasing time of the secondary Raman mode of the BaWO4 crystal, is registered and analyzed for the detuning of the Raman laser cavity length.

The extracavity parametric Raman CaCO anti-Stokes laser at 954 nm excited by two orthogonally polarized (pump and probe) equal frequency laser beams was proposed and investigated. Tangential phase matching conditions for the orthogonally polarized Raman components four-wave mixing in the CaCO crystal at stimulated Raman scattering (SRS) under 1064-nm excitation were theoretically studied and applied for a novel nanosecond parametric Raman laser allowing to increase the 954-nm anti-Stokes generation efficiency. In agreement with the theoretical modeling, using the high-Q external cavity scheme we have experimentally achieved the highest optical-to-optical (1064 nm to 954 nm) efficiency of 4% in comparison with the known crystalline parametric Raman anti-Stokes lasers. The ~3 ns anti-Stokes output pulse energy was 0.3 mJ with high beam quality factor M = 1.1 × 1.2.

For the first time to our knowledge, a single-phase solid solution Sr(MoO_4)0.8(WO_4)0.2 was used as an active medium of a Raman laser. Using the high-intensity synchronous picosecond pumping satisfying the condition of phase capture of the parametric Raman interaction on the second vibrational mode made it possible to oscillate six components of Raman radiation with a combined frequency shift on the first (888 cm-1) and second (327 cm-1) vibrational modes in the wavelength range of 1194-1396 nm. Oscillation efficiency of the multiwavelength Raman laser radiation was as high as 10%. By detuning the Raman laser cavity length, the pulse shortening down to 6 ps for the Raman laser radiation components with the combined frequency shift was obtained, which is an order of magnitude shorter than the pumping pulse duration (64 ps). Keywords: stimulated Raman scattering, single-phase solid solution, vibrational mode, synchronous pumping.

Comparative investigation of stimulated Raman scattering (SRS) characteristics in the YVO4, GdVO4, and Ca3(VO4)2 orthovanadate crystals at both low and high frequency anionic group vibrations is presented. It was found that GdVO4 is the most perspective for SRS generation on both the ν1 stretching and ν2 bending modes of internal anionic group vibrations with the strongest SRS pulse shortening under synchronous picosecond pumping. It is as a result of GdVO4‘s widest linewidth (17cm−1) of the homogeneously broadened scheelite-type component of the bending ν2 Raman line that led to the strongest SRS pulse shortening down to the dephasing time of the widest (scheelite-type) Raman mode at the secondary intracavity short-shifted SRS conversion. It allowed us to achieve SRS pulses with sub-picosecond duration under tens-of-picoseconds pumping due to the strongest 42-fold pulse shortening. Using the Ca3(VO4)2 crystal with essentially wider Raman lines (~50cm−1) did not allow us to generate SRS pulses shorter than 1 ps. It can be explained by inhomogeneous broadening of the Raman lines in Ca3(VO4)2 because of its structural disordering. Using the measured SRS pulse duration, the homogeneous broadening of the inhomogeneously broadened bending Raman line of Ca3(VO4)2 was estimated to be ~9cm−1. Among the orthovanadate crystals, the YVO4 crystal with the highest Raman gain and with homogeneously broadened Raman lines allowed us to realize the most efficient SRS lasing and SRS pulse shortening truly down to inverse half-width of the bending Raman line.

Collinear phase matching of the Stokes ↔ anti-Stokes interaction for Raman-active crystals with different birefringence was studied theoretically as well as experimentally. It was shown that collinear phase matching of the Stokes ↔ anti-Stokes interaction in low-birefringent crystals can be insensitive to angular mismatch if a phase matching angle is higher than 60°. We have developed and experimentally realized an extracavity parametric Raman anti-Stokes laser based on a low-birefringent SrWO4. Cyan 507-nm anti-Stokes conversion from green (532 nm) pump radiation of a 5-ns, 1-mJ second harmonic Nd:YAG laser has been obtained. Laser setup with a single beam excitation made it possible to use an output face of the SrWO4 crystal as an output coupler because of wide (6°) angular tolerance of collinear phase matching that resulted in an increase of slope efficiency of anti-Stokes generation higher than 3% at the anti-Stokes energy output of a 10-µJ level.