Stimulated Raman shifting of the Nd:YAG fourth harmonic (266 nm) in H2, HD, and D2

The dependence of the first Stokes stimulated Raman conversion efficiency of fourth-harmonic radiation from a Nd:YAG laser at 266 nm has been studied for the isotopic species H2, HD, and D2 as a function of gas pressure and laser energy using a low numerical aperture (about 0.0045) pumping geometry. While the laser energy threshold for first Stokes conversion varies significantly among the species, photon conversion efficiencies of at least 50 percent can be achieved for all of them for laser pump energies at 266 nm of 50 mJ/pulse or less. This study provides a new measurement of the differential cross section for stimulated Raman scattering in HD of 8.1 + or - 2.4 x 10 to the -29th sq cm/sr at 266 nm and at high pressures, and agreement is found with previous measurements of the cross sections for H2 and D2. The results have been used to optimize the laser transmitter system for a differential-absorption lidar to measure tropospheric ozone concentration profiles.