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Water vapor is one of the most important constituents of the earth's atmosphere. It has a major impact on both atmospheric dynamics and radiative transfer. From a dynamic standpoint, the distribution of water vapor with height determines convective stability which is the major indicator of destructive storm development. Also, water vapor stored in the planetary boundary layer acts as the fuel to intensify severe weather. In regards to radiative transfer, water vapor is the most active IR molecule in the atmosphere. It is more effective in absorbing and emitting IR radiation than either carbon dioxide or methane, and thus plays an important role in global change. The main objective of FIRE (First ISSCCP (International Satellite Cloud Climatology Project) Regional Experiment) was to study the development and radiative characteristics of cirrus clouds. The SPECTRE (Spectral Radiation Experiment) project was designed to acquire the necessary atmospheric observations to compare radiative measurements with radiative transfer theory, with special emphasis on understanding the water vapor spectral continuum. The FIRE/SPECTRE field campaign was conducted during Nov. - Dec. 1991 in Coffeyville, Kansas. A complete understanding of water vapor, its distribution with height, and its temporal variation was important for both experiments.

The Atmospheric Radiation Measurement (ARM) Program was initiated by the Department of Energy's Atmospheric and Climate Research Division (DOE/ACRD) to improve parameterizations of cloud radiative effects in general circulation models of the Earth's climate. The Instrument Development Program (IDP), a major component of ARM, is directed toward the improvement of radiometric and remote sensing instrumentation pertinent to near real-time characterizations of atmospheric parameters. The ultimate goal of this program is to provide state-of-the-art instruments suitable for installation and extended use in ARM's field measurement component, the Cloud and Radiation Testbed (CART).

We describe preliminary results from a comprehensive computer model developed to guide optimization of a Raman lidar system for measuring daytime profiles of atmospheric water vapor, emphasizing an ultraviolet, solar-blind approach.

The first quantitative, time- and space-resolved measurements have been obtained for probability density functions of OH concentration in nonpremixed flames. Measurements using single-pulse, laser-saturated fluorescence in laminar, transitional, and turbulent nonpremixed H2-air flames provide unambiguous evidence for substantial OH superequilibrium concentrations, in qualitative agreement with predictions of laminar and turbulent combustion models. The average degree of superequilibrium, OH/OH(AE), is typically 4-5 near the jet exit and approaches unity far downstream. The maximum instantaneous OH concentration measured in transitional and turbulent H2-air flames is about 6 x 10 to the 16th molecules/cc, in accord with the maximum determined by partial equilibrium thermodynamic calculations and with the maximum OH concentrations measured in premixed H2-air flames.

A new optical technique has been developed for ultra-sensitive attenuation measurements in gaseous media and, in particular, for determination of low levels of smoke emitted from jet engines. It is a variation on direct light transmission where the sample gas density in a cell is modulated acoustically by a speaker. The amplitude variation of the light transmission is proportional to the gas density and is insensitive to window contamination and detector instabilities. Preliminary analysis and experiments indicate that the instrument promises to measure light absorption to less than 1 percent per meter and allow measurment of smoke emissions from 1 to 100 mg/cu m. The technique has been demonstrated through the use of an absorbing gas, viz., 200 ppm of NO2 in N2 which produces 25 percent per meter absorption.

A single-pulse, laser-saturated fluorescence technique has been developed for absolute OH concentration measurements with a temporal resolution of 2 nsec, a spatial resolution of less than 0.1 cu mm, and an estimated accuracy of + or - 30 percent. It has been applied in laminar, transitional, and turbulent hydrogen-air diffusion flames, providing the first reported quantitative measurements of average values, rms fluctuations, and probability-density functions of OH-radical concentration in nonpremixed flames.

Enhanced scattering and fluorescence processes in the visible and UV were investigated which will enable improved remote measurements of gas properties. The theoretical relationship between scattering and fluorescence from an isolated molecule in the approach to resonance is examined through analysis of the time dependence of re-emitted light following excitation of pulsed incident light. Quantitative estimates are developed for the relative and absolute intensities of fluorescence and resonance scattering. New results are obtained for depolarization of scattering excited by light at wavelengths within a dissociative continuum. The experimental work was performed in two separate facilities. One of these utilizes argon and krypton lasers, single moded by a tilted etalon, and a 3/4 meter double monochromator. This facility was used to determine properties of the re-emission from NO2, I2 and O3 excited by visible light. The second facility involves a narrow-line dye laser, and a 3/4 meter single monochromator. The dye laser produces pulsed light with 5 nsec pulse duration and 0.005 nm spectral width.

Raman scattering signatures are functions of the scattering-gas temperature, and are therefore of potential use for practical atmospheric temperature probes. The method described uses either ratios of pure rotational Raman scattering intensities for air utilizing various spectral bandpasses, or, alternatively, ratios of air-rotational to nitrogen-vibrational scattering intensities. Three aspects of work relating to the development of such probes are discussed in this presentation: (1) fundamental absolute Raman data, (2) construction of air spectra from these data, and (3) temperature-sensitivity of the signature. The fundamental data described are the absolute rotational and vibrational scattering cross sections. Recent measurements in this laboratory of rotational cross sections for N2, O2, and CO2 are emphasized, as are their use in predicting absolute magnitudes of Raman scattering signals. Next is described the computation of air rotational Raman spectra as a function of temperature calculated through use of the experimentally-measured cross sections. The spectra are based additively upon nitrogen and oxygen contributions, since pure rotational Raman scattering from water vapor is very weak. Finally, the sensitivity of the scattering intensity ratios to temperature is explored as a function of choice of spectral bandpass for the monitored rotational Raman scattering. Various compromises will be discussed which must be made in choosing bandpasses appropriate for specific purposes and experimental conditions.

A portion of the fluorescence spectrum of SO2 has been studied using a narrow wavelength doubled dye laser as the exciting source. One purpose of this study is to evaluate the use of SO2 resonance re-emission as a probe of SO2 in the atmosphere. When the SO2 is excited by light at 300.2 nm, for example, a strong reemission peak is observed which is Stokes-shifted from the incident light wavelength by the usual Raman shift (the VI symmetric vibration frequency 1150.5/cm ). The intensity of this peak is sensitive to small changes (.01 nm) in the incident wavelength. Measurements of the N2 quenching and self quenching of this re-emission have been obtained. Preliminary analysis of this data indicates that the quenching is weak but not negligible. The dye laser in our system is pumped by a pulsed N2 laser. Tuning 'and spectral narrowing are accomplished using a telescope-echelle grating combination. In a high power configuration the resulting pulses have a spectral width of about 5 x 10(exp -3) nm and a time duration of about 6 nsec. The echelle grating is rotated by a digital stepping motor, such that each step shifts the wavelength by 6 x 10(exp -4) nm. In addition to the tunable, narrow wavelength uv source and spectral analysis of the consequent re-emission, the system also provides time resolution of the re-emitted light to 6 nsec resolution. This capability is being used to study the lifetime of low pressure S02 fluorescence at different wavelengths and pressures.

An experimental examination of the absolute intensity, polarization, and relative line intensities of rotational Raman scattering (RRS) from N2, O2, and CO2 is reported. The absolute scattering intensity for N2 is characterized by its differential cross section for backscattering of incident light at 647.1 nm, which is calculated from basic measured values. The ratio of the corresponding cross section for O2 to that for N2 is 2.50 plus or minus 5 percent. The intensity recent for N2, O2, and CO2 are shown to compare favorably to values calculated from recent measurements of the depolarization of Rayleigh scattering plus RRS. Measured depolarizations of various RRS lines agree to within a few percent with the theoretical value of 3/4. Detailed error analyses are presented for intensity and depolarization measurements. Finally, extensive RRS spectra at nominal gas temperatures of 23 C, 75 C, and 125 C are presented and shown to compare favorably to theoretical predictions.