Raman-shifting ArF excimer laser radiation for vacuum-ultraviolet multiphoton spectroscopy

We present the results of Raman shifting the radiation from an ArF laser in HD and D2 to produce tunable high-power vacuum-ultraviolet radiation. Calculations of the Raman gain for H2, D2 and HD at 193 nm are presented Modifications made to the ArF laser to improve beam quality are described. Wavelengths as short as 132 nm are achieved by Raman shifting in D2. The gas must be cooled below room temperature for efficient Raman shifting in HD. We obtain energies as high as 1 mJ at 170 nm by Raman shifting in HD at liquid-nitrogen temperature. The Raman-shifted radiation is used to perform two-photon spectroscopy in atomic and molecular fluorine and molecular hydrogen.