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Narrow linewidth tunable lasers augur a new kind of laser Doppler velocimetry employing resonant absorption and fluorescence from trace atomic species rather than scattering from particles. This technique may provide better turbulence and small volume information than present velocimetry.
The principles of spectral line formation and of techniques for retrieval of atmospheric temperature and constituent profiles are discussed. Applications to the atmospheres of Earth, Mars, Venus, and Jupiter are illustrated by results obtained with Fourier transform and infrared heterodyne spectrometers at resolving powers (lambda/delta hyperon lambda of approximately 10,000 and approximately 10 to the seventh power), respectively, showing the high complementarity of spectroscopy at these two widely different resolving powers. The principles of heterodyne spectroscopy are presented and its applications to atmospheric probing and to laboratory spectroscopy are discussed. Direct absorption spectroscopy with tuneable semiconductor lasers is discussed in terms of precision frequency-and line strength-measurements, showing substantial advances in laboratory infrared spectroscopy.
A technique is presented for visualizing and quantitatively measuring velocity, temperature, and pressure by shining a single frequency laser beam into a gaseous flow which is seeded with an atomic species. The laser is tuned through the absorption frequencies of the seeded species and the absorption profile is detected by observing fluorescence as the atoms relax back to the ground state. The flow velocity is determined by observing the Doppler shift in the absorption frequency. Spectroscopic absorption line broadening mechanisms furnish information regarding the static temperature and pressure of the moving gas. Results of experiments conducted in the free stream and in the bow shock of a conical model mounted in a hypersonic wind tunnel indicate that the experimental uncertainties in the measurement of average values for the velocity, temperature and pressure of the flow are 0.1, 5 and 10 percent respectively.
The vapor pressure of potassium has been measured in absorption using a CW tunable laser and calibrated against the accurate radiative lifetime of the 4s-4p doublet of potassium. An accurate value of 20,850 + or - 30 cal/mol for the heat of vaporization (from the liquid phase) at the melting point was determined.
Measurements were made of the elemental composition of particulate matter collected in flights in the Arctic in spring 1983 as part of the Arctic Gas and Aerosol Sampling Program (AGASP). Ten samples of size-selected particles were analyzed by four nondestructive techniques at Davis. Concentrations were determined for H, C, N, and O by Forward Alpha Scattering Techniques (FAST) and for elements heavier than fluorine by Particle Induced X-ray Emission (PIXE). Total mass was measured gravimetrically, and optical absorption was measured using the Laser Integrating Plate Method (LIPM). Results of the analyses show dramatic differences in concentrations and elemental ratios from the Alaskan Arctic to the Norwegian Arctic, with indications of wood smoke and sulfuric acid in the arctic atmosphere.
A high resolution spectrometer which incorporates a narrow line width tunable dye laser was used to make absorption profiles of 57 spectral lines in the Oxygen A-Band at pressures up to one atmosphere in pure O2. The observed line profiles are compared to the Voigt, and a collisionally narrowed, profile using a least squares fitting procedure. The collisionally narrowed profile compares more favorable to the observed profiles. Values of the line strengths and self broadening coeffiencients, determined from the least square fitting process, are presented in tabular form. It is found that the experssion by Watson are in closest agreement with the experimentally determined strengths. The self broadening coefficients are compared with the measurements of several other investigators.
The LaRC airborne lidar system was operated from the ARC DC-8 aircraft during the 1992 Airborne Arctic Stratospheric Expedition (ASEE-2) to investigate the distribution of stratospheric aerosols and O3 across the Arctic vortex from Jan. to Mar. 1992. Monthly flights were made across the Arctic vortex from Anchorage, Alaska, to Stavanger, Norway, and then back to Bangor, Maine, and additional round-trip flights north into the vortex were made each month from either Stavanger or Bangor depending on the location of the vortex that month. The airborne lidar system uses the differential absorption lidar (DIAL) technique at laser wavelengths of 301.5 and 310.8 nm to measure O3 profiles above the DC-8 over the 12-25 km altitude range. Lidar measurements of aerosol backscatter and depolarization profiles over the 12-30 km altitude range are made simultaneously with the O3 measurements using infrared (IR) and visible (VIS) laser wavelengths of 603 and 1064 nm, respectively. The measurements of Pinatubo aerosols, polar stratospheric clouds, and O3 made with the airborne DIAL system during the AASE-2 expedition and to chemical and dynamical process that contribute to O3 depletion in the wintertime Arctic stratosphere.
A tandem dual-beam spectrometer has been developed to determine ozone absorption cross sections for 13 selected wavelengths between 750 and 975 nm at room temperature. The increasingly pronounced structure in this region may interfere with atmospheric trace gas transitions that are useful for remote sensing and complicate the measurement of aerosols. Ozone concentrations were determined by absorption at the common HeNe laser transition near 632.8 nm using the absolute cross section reported previously. The overall accuracy of these room temperature measurements is generally better than 2 percent. A synoptic near-IR spectrum scaled to these measurements is employed for comparison with results of previous studies.
This NASA-Ames University Consortium Project has focused on the design and demonstration of optical absorption sensors using tunable diode laser to target atomic copper impurities from electrode erosion in thc arc-heater metastable electronic excited states of molecular nitrogen, atomic argon, aid atomic oxygen in the arcjet plume. Accomplishments during this project include: 1. Design, construction, and assembly of optical access to the arc-heater gas flow. 2. Design of diode laser sensor for copper impurities in the arc-heater flow. 3 . Diode laser sensor design and test in laboratory plasmas for metastable Ar(3P), O(5S), N(4P), and N2(A). 4. Diode laser sensor demonstration measurements in the test cell to monitor species in the arc-jet plume.
Ground-based LIDAR observations can potentially provide continuous profiles of CO2 through the planetary boundary layer and into the free troposphere. We will present initial atmospheric measurements from a prototype system that is based on components developed by the telecommunications industry. Preliminary measurements and instrument performance calculations indicate that an optimized differential absorption LIDAR (DIAL) system will be capable of providing continuous hourly averaged profiles with 250m vertical resolution and better than 1 ppm precision at 1 km. Precision increases (decreases) at lower (higher) altitudes and is directly proportional to altitude resolution and acquisition time. Thus, precision can be improved if temporal or vertical resolution is sacrificed. Our approach measures absorption by CO2 of pulsed laser light at 1.6 microns backscattered from atmospheric aerosols. Aerosol concentrations in the planetary boundary layer are relatively high and are expected to provide adequate signal returns for the desired resolution. The long-term goal of the project is to develop a rugged, autonomous system using only commercially available components that can be replicated inexpensively for deployment in a monitoring network.
This study tests a novel methodology to add value to satellite data sets. This methodology, data fusion, is similar to data assimilation, except that the background modelbased field is replaced by a satellite data set, in this case AIRS (Atmospheric Infrared Sounder) carbon monoxide (CO) measurements. The observational information comes from CO measurements with lower spatial coverage than AIRS, namely, from TES (Tropospheric Emission Spectrometer) and MLS (Microwave Limb Sounder). We show that combining these data sets with data fusion uses the higher spectral resolution of TES to extend AIRS CO observational sensitivity to the lower troposphere, a region especially important for air quality studies. We also show that combined CO measurements from AIRS and MLS provide enhanced information in the UTLS (upper troposphere/lower stratosphere) region compared to each product individually. The combined AIRS-TES and AIRS-MLS CO products are validated against DACOM (differential absorption mid-IR diode laser spectrometer) in situ CO measurements from the INTEX-B (Intercontinental Chemical Transport Experiment: MILAGRO and Pacific phases) field campaign and in situ data from HIPPO (HIAPER Pole-to-Pole Observations) flights. The data fusion results show improved sensitivities in the lower and upper troposphere (20-30% and above 20%, respectively) as compared with AIRS-only version 5 CO retrievals, and improved daily coverage compared with TES and MLS CO data.
The dissociation of aligned, electronically excited H 2 (E,F 1 Σ g + ), followed by ionization of the produced H atom, is analyzed via the velocity mapped imaging technique. The dissociation and ionization processes are accomplished, respectively, by a two- and a onephoton absorption from a single 532-nm laser pulse, while the alignment is induced by a separate 1064-nm laser pulse. The velocity of the produced H + photofragments shows a weak perpendicular alignment at low alignment laser field values, evolving to strongly parallel for larger fields. We modeled this alignment behavior with a simple two-state model involving the Stark mixing of the initially-prepared J = 0 with the J = 2 rotational state. This model is able to reproduce all of the observed angular distribution, and permits us to extract from the fit the polarizability anisotropy of H 2 (E,F) electronic state. We determine this value to be (3.7 ± 1.2) x 10 3 a.u. As this value is extremely large in comparison to what one would expect from the pure H 2 (E,F) electronic state, we hypothesize that this value comes from the 1064-nm laser beam mixing nearby electronic states with the initially laser prepared (E,F) state generating a mixed state (EF**) with an extremely large polarizability anisotropy.
The results of field measurements of concentration of some gaseous components of the atmosphere along the paths, in Sofia, Bulgaria, using a gas analyzer based on the use of a CO2 laser radiation frequency-doubled with ZnGeP2 monocrystals are presented. The gas analyzer is a traditional long path absorption meter. Radiation from the tunable CO2 laser of low pressure and from an additional He-Ne laser is directed to a colliminating hundredfold Gregori telescope with a 300 mm diameter of the principal mirror. The dimensions of the mirrors of a retroreflector 500 x 500 mm and a receiving telescope allow one to totally intercept the beam passed through the atmospheric layer under study and back.
Filtered Rayleigh scattering (FRS) is a laser diagnostic where the intensity of elastically scattered light is measured after it passes through a molecular absorption filter. The filter removes background interference that overwhelms the relatively weak scattering from the gas molecules. However, with a filter, the measured light intensity depends on many of the scattering gas properties, including pressure, density, temperature, and velocity. In this work, CFD simulations of an isolator shock train flow field are input into a physics-based model to predict the values of FRS intensity measurements in a proposed experiment. The goal is to evaluate if a simplistic FRS setup (that utilizes one camera, laser, and absorption filter) can be used to accurately quantify number density despite the fact that the scattered light intensity also depends on other gas properties. It is found that the experimental setup can be optimized such that a linear relationship describes the number density with an average prediction error of 2%. The vast majority of the flow exhibits prediction errors of less than 3%, but small regions of the flow reach up to 11% error. A sensitivity analysis shows that the prediction error increases with the central wavelength of the incident laser light and decreases with the angle between the camera and laser propagation directions. The optimal experimental parameters are chosen based on a compromise between the prediction error, spatial resolution, and the amount of unfiltered light. In the future, the proposed FRS setup will be implemented to acquire new and valuable information on an isolator shock train, a flow field that has been traditionally studied using wall static pressure measurements and path-integrated visualization techniques, such as schlieren and shadowgraphy.
Platinum(II) mono- and di-benzoporphyrins carrying either ester or imide peripheral groups have been successfully synthesized. These benzoporphyrins possessing C 2v and D 2h symmetry were investigated using a range of techniques including UV-Vis and phosphorescence spectroscopy, differential pulse voltammetry, and transient absorption spectroscopy covering wide spatial and temporal ranges. Up to three oxidation and three reductions within the accessible potential window of dichlorobenzene were observed. Facile reductions for both mono- and dibenzoporphyrin derivatives, more so with imide peripheral substituents were witnessed. Computational studies were supportive of push-pull type interactions within these molecular systems. Here, the formation of triplet excited states within 5 ps after laser excitation was confirmed by femtosecond transient absorption studies. Nanosecond transient absorption studies coupled with phosphorescence lifetime studies revealed relatively rapid relaxation of the triplet excited states as compared to a controlled platinum porphyrin suggesting push-pull type interactions on a slower time scale.
A research program on remote optical measurements of humidity and temperature is summarized, and new results are given of such measurements as well as new data on the near IR absorption spectrum of H2O. The basic atmospheric technique is differential absorption lidar (DIAL) using narrow band, tunable dye lasers. Approximate wavelengths are 720, 820, 940 nm (H2O) and 690, 760 nm (O2; temperature). The requisite absorption line strengths and widths are measured in a controlled environment by means of grating spectroscopy and tunable lasers. Prospects for routine lidar meteorology, even from airplane and satellite platforms, appear excellent in several important applications; the conditions and the optical properties of the atmosphere can be obtained remotely by these means.
Langley Research Center has developed a novel external path sensor which monitors water vapor along an optical path between an airplane window and reflective material on the plane's engine. An infrared tunable diode laser is wavelength modulated across a water vapor absorption line at a frequency f. The 2f and DC signals are measured by a detector mounted adjacent to the laser. The 2f/DC ratio depends on the amount of wavelength modulation, the water vapor absorption line being observed, and the temperature, pressure, and water vapor content of the atmosphere. The present work concerns efforts to quantify the contributions of these factors and to derive a method for extracting the water vapor mixing ratio from the measurements. A 3 m cell was fabricated in order to perform laboratory tests of the sensor. Measurements of 2f/DC were made for a series of pressures and modulation amplitudes. During my 1994 faculty fellowship, a computer program was created which allowed 2f/DC to be calculated for any combination of the variables which effect it. This code was used to generate 2f/DC values for the conditions measured in the laboratory. The experimental and theoretical values agreed to within a few percent. As a result, the laser modulation amplitude can now be set in the field by comparing the response of the instrument to the calculated response as a function of modulation amplitude. Once the validity of the computer code was established, it was used to investigate possible candidate absorption lines. 2f/DC values were calculated for pressures, temperatures, and water vapor mixing ratios expected to be encountered in future missions. The results have been incorporated into a database which will be used to select the best line for a particular mission. The database will also be used to select a retrieval technique. For examples under some circumstances there is little temperature dependence in 2f/DC so temperature can be neglected. In other cases, there is a dependence with temperature for a particular pressure, requiring a more complicated retrieval algorithm. Future experimental work is necessary to test agreement with the theoretical values over a range of temperatures and mixing ratios. Additionally, retrieval algorithms for forthcoming missions must be incorporated into the software package which controls the instrument.
The rudiments of a rocket thruster, which receives its enthalpy from an energy source which is remotely beamed from a laser, is described. An experimental study, now partially complete, is discussed which will eventually provide a detailed understanding of the physics for assessing the feasibility of using hydrogen plasmas for accepting and converting this energy to enthalpy. A plasma ignition scheme which uses a pulsed CO2 laser was develped and the properites of the ignition spark documented, including breakdown intensities in hydrogen. A complete diagnostic system capable of determining plasma temperature and the plasma absorptivitiy for subsequent steady-state absorption of a high power CO2 laser beam are developed and demonstrative use is discussed for the preliminary case study, a two atmosphere laser supported argon plasma.