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Report describes state of art of tunable-diode-laser second-harmonic spectroscopy applied to measurements of concentrations of trace constituents of atmosphere. Combination of temperature, composition, and drive-current tuning, wavelengths of tunable diode lasers varied over infrared range of 3 to 30 micrometer, containing spectral lines of many molecules of interest in atmospheric research.
A high-sensitivity spectroscopic measurement of O2 using two-tone frequency modulation spectroscopy with a GaAlAs diode laser is presented. An oxygen sensor based on this technique would be non-intrusive, compact and possess high sensitivity and fast time response.
Blocked impurity band (BIB) detectors have allowed extension of highly sensitive tunable diode laser (TDL) spectroscopy to over 20 micron spectral region. BIB detectors present low noise equivalent power. Here the apparatus and its components are described and an example of molecular spectra is presented.
The nu 5 antisymmetric stretching vibration of 1 sigma+g C9 has been observed using direct infrared diode laser absorption spectroscopy of a pulsed supersonic cluster beam. Twenty-eight rovibrational transitions measured in the region of 2079-2081 cm-1 were assigned to this band. A combined least squares fit of these transitions with previously reported nu 6 transitions yielded the following molecular constants for the nu 5 band: nu 0 = 2 079.673 58(17) cm-1, B"= 0.014 321 4(10) cm-1, and B'=0.014 288 9(10) cm-1. The IR intensity of the nu 5 band relative to nu 6 was found to be 0.108 +/- 0.006. Theoretical predictions for the relative intensities vary widely depending upon the level of theory employed, and the experimental value reported here is in reasonable agreement only with the result obtained from the most sophisticated ab initio calculation considered (CCSD).
We report the first structural characterization of the triplet isomer of C6. Forty-one rovibrational/fine structure transitions in the nu 4(sigma u) antisymmetric stretch fundamental of the C6 cluster have been measured by diode laser absorption spectroscopy of a supersonic carbon cluster beam. The observed spectrum is characteristic of a centrosymmetric linear triplet state with cumulene-type bonding. The measured ground state rotational constant B0 = 0.048 479 (10)cm-1 and the effective bond length r(eff) = 1.2868 (1) angstroms are in good agreement with ab initio predictions for the linear triplet (3 sigma g-) state of C6.
The simultaneous measurement of temperature and density using laser-induced fluorescence of oxygen in combination with Q-branch Raman scattering of nitrogen and oxygen is demonstrated in a low-speed air flow. The lowest density and temperature measured in the experiment correspond to the freestream values at Mach 5 in the Ames 3.5-Foot Hypersonic Wind Tunnel for stagnation conditions of 100 atm and 1000 K. The experimental results demonstrate the viability of the optical technique for measurements that support the study of compressible turbulence and the validation of numerical codes in supersonic and hypersonic wind tunnel flows.
The paper examines the rapidly expanding use of lasers for spectroscopic studies of alkali metal vapors. Since the alkali metals (lithium, sodium, potassium, rubidium and cesium) are theoretically simple ('visible hydrogen'), readily ionized, and strongly interacting with laser light, they represent ideal systems for quantitative understanding of microscopic interconversion mechanisms between photon (e.g., solar or laser), chemical, electrical and thermal energy. The possible implications of such understanding for a wide variety of practical applications (sodium lamps, thermionic converters, magnetohydrodynamic devices, new lasers, 'lithium waterfall' inertial confinement fusion reactors, etc.) are also discussed.
A novel tunable diode laser spectrometer operating at 8-28 microns is described. A blocked impurity band Si:As chip is employed as detector. This device operates in this wavelength range with high detectivity and adequate frequency response for the high-sensitivity techniques used. A combination of sweep averaging and second-harmonic detection at 22 kHz yielded signal-to-noise ratios of 1200 at wavelengths above 20 microns. The sensitivity and spectral resolution achieved are an order of magnitude better than those of Fourier instruments in this range, with an improvement in instrument time response of about 3000. Several molecular bands of CO2 and N2O are observed for what is, to our knowledge, the first time with this instrument. Examples of spectral line measurements are presented.
A CdTe phase modulator and low power RF sources have been used with Pb-salt tunable diode lasers operating near 8 microns to generate optical sidebands for high sensitivity absorption spectroscopy. Sweep averaged, first-derivative sample spectra of CH4 were acquired by wideband phase sensitive detection of the electrooptically (EO) generated carrier-sideband beat signal. EO generated beat signals were also used to frequency lock the TDL to spectral lines. This eliminates low frequency diode jitter, and avoids the excess laser linewidth broadening that accompanies TDL current modulation frequency locking methods.
Ratios of C-12/C-13 in CO2 have been measured using a tunable diode laser (TDL) spectrometer to an accuracy of better than 0.4 percent. These results were made possible by the use of state-of-the-art high-temperature TDLs, an etalon and wavenumber calibration technique, high-speed assembly language controlled data acquisition, and the ratioing of absorbances from simultaneously acquired sample and reference data scans. The dual beam spectrometer that is employed uses the sweep integration technique in a spectral region where adjacent spectral lines are of approximately equal absorbance at the expected isotopic abundances.
A lidar instrument based on pulsed frequency-doubled carbon-dioxide lasers has been used at 4.88 microns for remote sensing of atmospheric carbon dioxide. A tunable-diode laser spectrometer provided the high-resolution spectroscopic data on carbon-dioxide line strength and line broadening needed for an accurate differential absorption measurement. Initial field measurements are presented, and instrument improvements necessary for accurate carbon dioxide measurement are discussed.
The formation of CN radicals by flash photolysis of a number of parent molecules was monitored by laser induced fluorescence in the B2Sigma(plus)-X2Sigma(plus) transition of CN. The rotational and vibrational energy of the newly formed radicals in the X state was measured directly. Formation of CN(A2Pi) in the lower vibrational levels was determined by an indirect method based on resonant energy transfer to higher vibrational levels of the ground state. These laboratory studies have shown that high initial internal excitation of CN with rotational levels of maximum N equals 50-70 is the rule. In general, the formation of simple molecules in excited states is commonly the case. There appear to be astrophysical systems where radiation from these excited levels may be detectable. Such observations would serve as a probe of molecular formation.
The nu 3(sigma u) fundamental vibration of 1 sigma g+ Si2C3 has been observed using a laser vaporization-supersonic cluster beam-diode laser spectrometer. Forty rovibrational transitions were measured in the range of 1965.8 to 1970.9 cm-1 with a rotational temperature of 10-15 K. A least-squares fit of these transitions yielded the following molecular constants: nu 3(sigma u)=1968.188 31(18) cm-1, B"=0.031 575 1(60) cm-1, and B'=0.031 437 4(57) cm-1. These results are in excellent agreement with recent Fourier transform infrared (FTIR) measurements of Si2C3 trapped in a solid Ar matrix [J. Chem. Phys. 100, 181(1994)] and with ab initio calculations [J. Chem. Phys. 100, 175 (1994)] which suggest cumulenic-like bonding for Si2C3, analogous to the isovalent C5 carbon cluster.
The infrared absorption spectrum of a linear, 13-atom carbon cluster (C13) has been observed by using a supersonic cluster beam-diode laser spectrometer. Seventy-six rovibrational transitions were measured near 1809 wave numbers and assigned to an antisymmetric stretching fundamental in the 1 sigma g+ ground state of C13. This definitive structural characterization of a carbon cluster in the intermediate size range between C10 and C20 is in apparent conflict with theoretical calculations, which predict that clusters of this size should exist as planar monocyclic rings.
Seven rovibrational transitions of the (01/1/0)-(00/0/0) fundamental bending band of C3 have been measured with high precision with the use of a tunable far-infrared laser spectrometer. The C3 molecules were produced by laser vaporization of a graphite rod and cooled in a supersonic expansion. The astrophysically important nu-2 fundamental frequency is determined to be 63.416529(40)/cm. These measurements provide the basis for studies of C3 in the interstellar medium with far-infrared astronomy.
Nonintrusive measurements of density, temperature, and their turbulent fluctuation levels were obtained in the boundary layer of an unseeded, Mach 2 wind tunnel flow. The spectroscopic technique that was used to make the measurements is based on the combination of laser-induced oxygen fluorescence and Raman scattering by oxygen and nitrogen from the same laser pulse. Results from this demonstration experiment are compared with previous measurements obtained in the same facility using conventional probes and an earlier spectroscopic technique. Densities and temperatures measured with the current technique agree with the previous surveys to within 3 percent and 2 percent, respectively. The fluctuation amplitudes for both variables agree with the measurements obtained using the earlier spectroscopic technique and show evidence of an unsteady, weak shock wave that perturbs the boundary layer.
Nonintrusive measurements of density and temperature and their turbulent fluctuation levels have been obtained in the boundary layer of an unseeded, Mach 2 wind tunnel flow. The spectroscopic technique that was used to make the measurements is based on the combination of laser-induced oxygen fluorescence and Raman scattering by oxygen and nitrogen from the same laser pulse. Results from this demonstration experiment compare favorably with previous measurements obtained in the same facility from conventional probes and an earlier spectroscopic technique.
Measurement of Total Organic Carbon (TOC) is an important tool on manned spaceflight missions for determining water quality. TOC quantification can be accomplished by oxidizing dissolved organic carbon to carbon dioxide (CO2) and analyzing the CO2 after volatilization. For human spaceflight applications, size, weight, and power need to be minimized while maintaining high sensitivity and accuracy. To this end, a tunable laser spectrometer tuned to measure CO2 was coupled to a miniature combustion reactor and the performance of the system for measuring the TOC was assessed. This combined system can be potentially reduced to around 1000 cm3 while offering the benefit afforded by combustion of converting all organics to CO2.