Monitoring of All Hydrogen Isotopologues at Tritium Laboratory Karlsruhe Using Raman Spectroscopy

We have recorded Raman spectra for all hydrogen isotopologues, using a CW Nd:YVO4 laser (5 W output power at 532 nm) and a high-throughput (f/1.8) spectrograph coupled to a Peltier-cooled (200 K) CCD-array detector (512 x 2048 pixels). A (static) gas cell was used in all measurements. We investigated (i) pure fillings of the homonuclear isotopologues H-2, D-2, and T-2; (ii) equilibrated binary fillings of H-2 + D-2, H-2 + T-2, and D-2 + T-2, thus providing the heteronuclear isotopologues HD, HT, and DT in a controlled manner; and (iii) general mixtures containing all isotopologues at varying concentration levels. Cell fillings within the total pressure range 13-985 mbar were studied, in order to determine the dynamic range of the Raman system and the detection limits for all isotopologues. Spectra were recorded for an accumulation period of 1000 s. The preliminary data evaluation was based on simple peak-height analysis of the ro-vibrational Q(1)-branches, yielding 3 sigma measurement sensitivities of 5 x 10(-3), 7 x 10(-3), and 25 x 10(-3) mbar for the tritium-containing isotopologues T-2, DT, and HT, respectively. These three isotopologues are the relevant ones for the KATRIN experiment and in the ITER fusion fuel cycle. While the measurement reported here were carried out with static-gas fillings, the cells are also ready for use with flowing-gas samples.