Graduation Year

2008

Document Type

Dissertation

Degree

Ph.D.

Degree Granting Department

Physics

Major Professor

Dennis Killinger, Ph.D.

Keywords

Laser breakdown spectroscopy, DIAL, Lidar, Raman spectroscopy, Boltzmann temperature measurements

Abstract

Several different laser remote sensing techniques related to the detection of trace chemical species were studied. In particular, a Differential-Absorption lidar (DIAL), a Laser-Induced-Breakdown Spectroscopy (LIBS) lidar, and a Raman lidar were studied. Several of the laser spectroscopic techniques that were used were common throughout these different studies. More precisely, 10.6 µm CO2 laser related spectroscopy was common for the DIAL and LIBS studies, and 266 nm Nd:YAG laser related spectroscopy was used for the LIBS and Raman studies. In the first system studied a tunable CO2 DIAL system was developed for the first time to our knowledge for the potential detection of the explosive Triacetone Triperoxide (TATP) gas clouds. The system has been used to measure gas samples of SF6, and has shown initial absorption measurements of samples of TATP contained within an enclosed optical absorption cell.

The LIBS plasma emission covering the range of 240 - 800 nm was enhanced by use of a nearly simultaneous 10.6 µm CO2 laser that increased the LIBS plasma emission by several orders of magnitude. The emission spectrum was used to detect and identify the species of interest. Plasma temperatures on various solid substrates were measured. An increase in the plasma temperature of about 5000 K was measured and analyzed, for the first to our knowledge, due to the addition of the CO2 laser pulse to the LIBS plasma generated by the Nd:YAG laser. An optimum temporal overlap of the two laser pulses was found to be important for the enhancement. Finally, in a third related lidar system, initial 266 nm Raman lidar studies were conducted at detection ranges of 15 m. However, significant spectroscopic background interferences were observed at these wavelengths and additional optical filtering is required.

DIAL/Lidar returns from a remote retro-reflector target array were used for the DIAL measurements after passage through a laboratory cell containing the TATP gas. DIAL measured concentrations agreed well with those obtained using a calibrated Ion Mobility Spectrometer. DIAL detection sensitivity of the TATP gas concentration in the cell was about 0.5 ng/µl for a 0.3 m path-length. However, the concentration of TATP was found to be unstable over long periods of time possibly due to re-absorption and crystallization of the TATP vapors on the absorption cell windows. A heated cell partially mitigated these effects. In the second set of studies, a Deep UV LIBS system was developed and studied for the remote detection of solid targets, and potentially chemical, biological, and explosive substances. A 4th harmonic Q-Switched Nd:YAG laser operating at 266 nm was used for excitation of the LIBS plasma at standoff ranges up to 50 m .

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