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A smoothly tunable, narrow-linewidth, cw, 32-mW, 2.066-mum Ho:YLF laser was constructed and used for the first time in preliminary spectroscopic measurements of atmospheric CO(2) and H(2)O. The laser was constructed with a 4.5-mm-long, TE-cooled, codoped 5% Tm and 0.5% Ho yttrium lithium fluoride crystal (cut at Brewster's angle) pumped by an Ar(+)-pumped 500-mW Ti:sapphire laser operating at 792 nm. Intracavity etalons were used to reduce the laser linewidth to approximately 0.025 cm(-1) (0.75 GHz), and the laser wavelength was continuously and smoothly tunable over approximately 6 cm(-1) (180 GHz). The Ho:YLF laser was used to perform spectroscopic measurements on molecular CO(2) in a laboratory absorption cell and to measure the concentration of CO(2) and water vapor in the atmosphere with an initial accuracy of approximately 5-10%. The measurement uncertainty was found to be due to several noise sources, including the effect of asymmetric intensity of the laser modes within the laser linewidth, fluctuations caused by atmospheric turbulence and laser beam/target movement, and background spectral shifts.

Laser beams can be used as long-range spectroscopic probes of the chemical composition and physical state of the atmosphere. The spectroscopic, optical, and laser requirements for atmospheric laser remote sensing are reviewed, and the sensitivity and limitations of the technique are described. A sampling of recent measurements includes the detection of urban air pollution and toxic chemicals in the atmosphere, the measurement of global circulation of volcanic ash in the upper atmosphere, and the observation of wind shear near airports.

For the first time to the best of our knowledge, a simultaneous 10.6 mum CO(2) laser pulse has been used to enhance the Laser Induced Breakdown Spectroscopy (LIBS) emission from a 1.064 mum Nd:YAG laser induced plasma on a hard target. The enhancement factor was on the order of 25 to 300 times, depending upon the emission lines observed. For an alumina ceramic substrate the Al emission lines at 308 nm and Fe impurity line at 278 nm showed an increase of 60x and 119x, respectively. The output energy of the Nd:YAG laser was 50 mJ/pulse focused to a 1 mm diameter spot to produce breakdown. The CO(2) laser pulse had a similar energy density of 40 mJ/mm(2). Timing overlap of the two laser pulses within 1 microsecond was important for enhancement to be observed. An observed feature was the differential enhancement between different elemental species and also between different ionization states, which may be helpful in the application of LIBS for multi-element analysis.