We have examined the utility of a gas-filled, Nd:YAG-laser-pumped Rama
n shifter as a possible broad-spectrum light source. Six to nine new o
utput frequencies with pulse energies above 1 muJ are produced when a
pure-hydrogen or pure-methane Raman shifter is pumped with 40 mJ of se
cond-harmonic, 20 mJ of third-harmonic, or 11 mJ of fourth-harmonic pu
mp pulse energy. Optimum output occurs at pressures of approximately 1
0 atm for the pure-gas experiments. We also report the output frequenc
ies and pulse energies of a mixed hydrogen-methane Raman shifter pumpe
d by 20 mJ of the third harmonic of the laser for various proportions
of the two gases at pressures up to nearly 20 atm. Depending on compos
ition and pressure, over a dozen new output lines with pulse energies
over 1 muJ can be produced. We discuss the nonlinear processes involve
d, the optimum operating conditions, and the suitability of the source
for our application of groundwater monitoring.