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NASA NTRS2006

Evaluation of Daytime Measurements of Aerosols and Water Vapor made by an Operational Raman Lidar over the Southern Great Plains

Raman lidar water vapor and aerosol extinction profiles acquired during the daytime over the Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) site in northern Oklahoma (36.606 N, 97.50 W, 315 m) are evaluated using profiles measured by in situ and remote sensing instruments deployed during the May 2003 Aerosol Intensive Operations Period (IOP). The automated algorithms used to derive these profiles from the Raman lidar data were first modified to reduce the adverse effects associated with a general loss of sensitivity of the Raman lidar since early 2002. The Raman lidar water vapor measurements, which are calibrated to match precipitable water vapor (PWV) derived from coincident microwave radiometer (MWR) measurements were, on average, 5-10% (0.3-0.6 g/m(exp 3) higher than the other measurements. Some of this difference is due to out-of-date line parameters that were subsequently updated in the MWR PWV retrievals. The Raman lidar aerosol extinction measurements were, on average, about 0.03 km(exp -1) higher than aerosol measurements derived from airborne Sun photometer measurements of aerosol optical thickness and in situ measurements of aerosol scattering and absorption. This bias, which was about 50% of the mean aerosol extinction measured during this IOP, decreased to about 10% when aerosol extinction comparisons were restricted to aerosol extinction values larger than 0.15 km(exp -1). The lidar measurements of the aerosol extinction/backscatter ratio and airborne Sun photometer measurements of the aerosol optical thickness were used along with in situ measurements of the aerosol size distribution to retrieve estimates of the aerosol single scattering albedo (omega(sub o)) and the effective complex refractive index. Retrieved values of omega(sub o) ranged from (0.91-0.98) and were in generally good agreement with omega(sub o) derived from airborne in situ measurements of scattering and absorption. Elevated aerosol layers located between about 2.6 and 3.6 km were observed by the Raman lidar on May 25 and May 27. The airborne measurements and lidar retrievals indicated that these layers, which were likely smoke produced by Siberian forest fires, were primarily composed of relatively large particles (r(sub eff) approximately 0.23 micrometers), and that the layers were relatively nonabsorbing (omega(sub o) approximately 0.96-0.98). Preliminary results show that major modifications that were made to the Raman lidar system during 2004 have dramatically improved the sensitivity in the aerosol and water vapor channels and reduced random errors in the aerosol scattering ratio and water vapor retrievals by an order of magnitude.

Ferrare, Richard↗

NASA NTRS2010

Simultaneous Spectral Temporal Adaptive Raman Spectrometer - SSTARS

Raman spectroscopy is a prime candidate for the next generation of planetary instruments, as it addresses the primary goal of mineralogical analysis, which is structure and composition. However, large fluorescence return from many mineral samples under visible light excitation can render Raman spectra unattainable. Using the described approach, Raman and fluorescence, which occur on different time scales, can be simultaneously obtained from mineral samples using a compact instrument in a planetary environment. This new approach is taken based on the use of time-resolved spectroscopy for removing the fluorescence background from Raman spectra in the laboratory. In the SSTARS instrument, a visible excitation source (a green, pulsed laser) is used to generate Raman and fluorescence signals in a mineral sample. A spectral notch filter eliminates the directly reflected beam. A grating then disperses the signal spectrally, and a streak camera provides temporal resolution. The output of the streak camera is imaged on the CCD (charge-coupled device), and the data are read out electronically. By adjusting the sweep speed of the streak camera, anywhere from picoseconds to milliseconds, it is possible to resolve Raman spectra from numerous fluorescence spectra in the same sample. The key features of SSTARS include a compact streak tube capable of picosecond time resolution for collection of simultaneous spectral and temporal information, adaptive streak tube electronics that can rapidly change from one sweep rate to another over ranges of picoseconds to milliseconds, enabling collection of both Raman and fluorescence signatures versus time and wavelength, and Synchroscan integration that allows for a compact, low-power laser without compromising ultimate sensitivity.

Blacksberg, Jordana↗

NASA NTRS1973

Atmospheric Temperature from Raman Scattering

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.

Lapp, M.↗

NASA NTRS2005

Active Raman sounding of the earth's water vapor field

The typically weak cross-sections characteristic of Raman processes has historically limited their use in atmospheric remote sensing to nighttime application. However, with advances in instrumentation and techniques, it is now possible to apply Raman lidar to the monitoring of atmospheric water vapor, aerosols and clouds throughout the diurnal cycle. Upper tropospheric and lower stratospheric measurements of water vapor using Raman lidar are also possible but are limited to nighttime and require long integration times. However, boundary layer studies of water vapor variability can now be performed with high temporal and spatial resolution. This paper will review the current state-of-the-art of Raman lidar for high-resolution measurements of the atmospheric water vapor, aerosol and cloud fields. In particular, we describe the use of Raman lidar for mapping the vertical distribution and variability of atmospheric water vapor, aerosols and clouds throughout the evolution of dynamic meteorological events. The ability of Raman lidar to detect and characterize water in the region of the tropopause and the importance of high-altitude water vapor for climate-related studies and meteorological satellite performance are discussed.

Earth (Planet)↗

NASA NTRS2013

Assessing the Temperature Dependence of Narrow-Band Raman Water Vapor Lidar Measurements: A Practical Approach

Narrow-band detection of the Raman water vapor spectrum using the lidar technique introduces a concern over the temperature dependence of the Raman spectrum. Various groups have addressed this issue either by trying to minimize the temperature dependence to the point where it can be ignored or by correcting for whatever degree of temperature dependence exists. The traditional technique for performing either of these entails accurately measuring both the laser output wavelength and the water vapor spectral passband with combined uncertainty of approximately 0.01 nm. However, uncertainty in interference filter center wavelengths and laser output wavelengths can be this large or larger. These combined uncertainties translate into uncertainties in the magnitude of the temperature dependence of the Raman lidar water vapor measurement of 3% or more. We present here an alternate approach for accurately determining the temperature dependence of the Raman lidar water vapor measurement. This alternate approach entails acquiring sequential atmospheric profiles using the lidar while scanning the channel passband across portions of the Raman water vapor Q-branch. This scanning is accomplished either by tilt-tuning an interference filter or by scanning the output of a spectrometer. Through this process a peak in the transmitted intensity can be discerned in a manner that defines the spectral location of the channel passband with respect to the laser output wavelength to much higher accuracy than that achieved with standard laboratory techniques. Given the peak of the water vapor signal intensity curve, determined using the techniques described here, and an approximate knowledge of atmospheric temperature, the temperature dependence of a given Raman lidar profile can be determined with accuracy of 0.5% or better. A Mathematica notebook that demonstrates the calculations used here is available from the lead author.

Raman lidar↗

NASA NTRS1987

Raman spectra of adsorbed layers on space shuttle and AOTV thermal protection system surface

Surfaces of interest to space vehicle heat shield design were struck by a 2 W argon ion laser line while subjected to supersonic arc jet flow conditions. Emission spectra were taken at 90 deg to the angle of laser incidence on the test object. Results showed possible weak Raman shifts which could not be directly tied to any particular parameter such as surface temperature or gas composition. The investigation must be considered exploratory in terms of findings. Many undesirable effects were found and corrected as the project progressed. For instance, initial spectra settings led to ghosts which were eliminated by closing the intermediate of filter slit of the Spex from 8 to 3 mm. Further, under certain conditions, plasma lines from the laser were observed. Several materials were also investigated at room temperature for Raman shifts. Results showed Raman shifts for RCC and TEOS coated materials. The HRSI materials showed only weak Raman shifts, however, substantial efforts were made in studying these materials. Baseline materials showed the technique to be sound. The original goal was to find a Raman shift for the High-temperature Reusable Surface Insulation (HRSI) Reaction Cured borosilicate Glass (RCG) coated material and tie the amplitude of this peak to Arc jet conditions. Weak Raman shifts may be present, however, time limitations prevented confirmation.

Willey, Ronald J.↗

NASA NTRS1990

Raman spectroscopic studies of carbon in extra-terrestrial materials

The measurements obtained here indicate ways in which micro-Raman spectroscopy can be used to elucidate structural characteristics and distribution of carbon in meteorites and interplanetary dust particles (IDPs). Existing information about structurally significant aspects of Raman measurements of graphite is combined with structurally relevant findings from the present micro-Raman studies of carbons prepared by carbonization of polyvinylidine chloride (PVDC) at various temperatures and natural material, as well as several acid residues from the Allende and Murchison meteorites in order to establish new spectra-structure relationships. Structural features of many of the materials in this study have been measured by x ray analysis and electron microscopy: thus, their structural differences can be directly correlated with differences in the Raman spectra. The spectral parameters consequently affirmed as indicators of structure are used as a measure of structure in materials that have unknown carbon structure, especially IDPs. The unique applicability of micro-Raman spectroscopy is realized not only in the ability to conveniently measure spectra of micron-size IDPs, but also micro-sized parts of an inhomogeneous material. Microcrystalline graphite is known to give Raman spectra that differ dependent on crystallite size (see e.g., Lespade, et. al., 1984, or Nemanich and Solin, 1979). The spectral changes that accompany decreasing particle size include increase in the ratio (R) of the intensity of the band near 1350 cm(-1) (D band) to that of the band near 1600 cm(-1) (G band) increase in the half width of the D band (wD) increase in the frequency maximum of the G band and increase in the half-width (wG) of the 2nd order band near 2700 cm(-1) (G) band.

Macklin, John↗

NASA NTRS1992

Raman Lidar Measurements of Pinatubo Aerosols over Southeastern Kansas During November-december 1991

The eruptions of the Philippine volcano Pinatubo during June 1991 produced large amounts of stratospheric aerosols that could significantly affect earth's climate as well as trigger stratospheric ozone depletion through heterogeneous chemical reactions. Information regarding the physical and optical properties of these aerosols is required to quantify those effects. By measuring both the elastically backscattered signal and the inelastic signal produced by Raman scattering from nitrogen molecules, Raman lidar can provide some of this information. In this presentation we discuss Raman lidar measurements of the scattering ratio, backscattering, extinction, extinction/backscattering ratio, and optical thickness of the Pinatubo aerosols over southeastern Kansas made on 10 nights during November and December, 1991. The Raman lidar developed at GSFC is a trailer-based system which uses an XeF excimer laser to transmit light at 351 nm. The light backscattered by molecules and aerosols at this wavelength is detected as well as Raman scattered light from water vapor, nitrogen, and oxygen molecules. Since background skylights interfere with the detection of the Raman signals the data discussed in this paper were acquired only at night.

Ferrare, R. A.↗

NASA NTRS1997

Modulated FT- Raman Fiber-Optic Spectroscopy: A technique for Remotely Monitoring High-Temperature Reactions in Real-Time

A modification to a commercial FT-Raman spectrometer is presented for the elimination of thermal backgrounds in FT-Raman spectra. The modification involves the use of a mechanical chopper to modulate the CW laser, remote collection of the signal via fiber optics, and connection of a dual-phase digital signal processor lock-in amplifier between the detector and the spectrometer's collection electronics to demodulate and filter the optical signals. The resulting modulated FT-Raman fiber-optic spectrometer is capable of completely eliminating thermal backgrounds at temperatures exceeding 370 C. In addition, the signal/noise of generated Raman spectra is greater than for spectra collected with the conventional FT-Raman under identical conditions and incident laser power. This is true for both room-temperature and hot samples. The method allows collection of data using preexisting spectrometer software. The total cost of the modification (excluding fiber optics) is approximately $3000 and requires less than 2 h to implement. This is the first report of Fr-Raman spectra collected at temperatures in excess of 300 C in the absence of thermal backgrounds.

Cooper, John B.↗

NASA NTRS2002

Spontaneous Raman Scattering Diagnostics for High-pressure Gaseous Flames

A high-pressure (up to 60 atm) gaseous burner facility with optical access that provides steady, reproducible flames with high precision, and the ability to use multiple fuel/oxidizer combinations has been developed. In addition, a high-performance spontaneous Raman scattering system for use in the above facility has also been developed. Together, the two systems will be used to acquire and establish a comprehensive Raman scattering spectral database for use as a quantitative high-pressure calibration of single-shot Raman scattering measurements in high-pressure combustion systems. Using these facilities, the Raman spectra of H2-Air flames were successfully measured at pressures up to 20 atm. The spectra demonstrated clear rotational and ro-vibrational Raman features of H2, N2, and H2O. theoretical Raman spectra of pure rotational H2, vibrational H2, and vibrational N2 were calculated using a classical harmonic-oscillator model with pressure broadening effects and fitted to the data. At a gas temperature of 1889 K for a phi = 1.34 H2-Air flame, the model and the data showed good agreement, confirming a ro-vibrational equilibrium temperature.

Kojima, Jun↗

NASA NTRS2003

Raman Spectroscopic Characterization of the Feldspars: Implications for Surface Mineral Characterization in Planetary Exploration

The availability in the last decade of improved Raman instrumentation using small, stable, intense lasers, sensitive CCD array detectors, and advanced fast grating systems enabled us to develop the Mars Microbeam Raman Spectrometer (MMRS), a field-portable Raman spectrometer with precision and accuracy capable of identifying minerals and their different compositions. For example, we can determine Mg cation ratios in pyroxenes and olivines to +/-0.1 on the basis of Raman peak positions. Feldspar is another major mineral formed in igneous systems whose characterization is important for determining rock petrogenesis and alteration. From their Raman spectral pattern, feldspars can be readily distinguished from ortho- and chain-silicates and from other tecto-silicates such as quartz and zeolites. We show here how well Raman spectral analysis can distinguish among members within the feldspar group.

Freeman, J. J.↗

NASA NTRS2002

Water Measurements using a Raman Lidar

The research record for the usefulness of Raman Lidar in addressing a broad range of important atmospheric research topics is well established. Raman lidar technology has been used to measure tropospheric aerosols, stratospheric aerosols and cirrus clouds. Arguably the most important measurements offered by Raman lidar for both dynamic and radiative studies, however, is that of water vapor. We will describe large improvements in Raman lidar measurements of water vapor made possible through recent technology upgrades. Furthermore, we will present the use of Raman lidar to study liquid water in the atmosphere and describe current research into the use of Raman lidar measurements to estimate ice water content of cirrus clouds.

Whiteman, D. N.↗

NASA NTRS2005

Raman Lidar Measurements during the International HZO Project: Instrumentation and Analysis Techniques, Popular Summary - 1

The amount of water vapor in the atmosphere helps to determine the likelihood that severe storms may develop. The concentration of water vapor, though, is highly variable in space and time. And yet small changes in water vapor concentration over a short period of time or over a short spatial distance can determine whether a storm may or may not develop. Therefore, in order to improve the ability to forecast severe weather such as thunderstorms it is important to measure water vapor in the atmosphere with high spatial and temporal resolution. One of the most attractive research tools for measuring water vapor in the atmosphere with high spatial and temporal resolution is a Raman lidar. A Raman lidar consists of a laser transmitter, a telescope receiver and optics and electronics for processing opticand electronic signals. A laser pulse is emitted into the atmosphere and it interacts with molecules in the atmosphere causing them to become excited and to emit, through the Raman process, photons of different wavelength than emitted by the laser. The molecule that emitted these emitted. This is the way that a Raman lidar identifies water vapor molecules in the atmosphere. can be identified based on the wavelength of the photons One of the great challenges in Raman lidar measurements has been to make useful daytime measurements of the water vapor profile under bright daytime conditions. In this first of two papers, we describe the instrumentation and analysis of the first documented Raman lidar that is able to measure water vapor in the daytime with sufficient quality to permit the study of developing storm systems.

Whiteman, D. N.↗

NASA NTRS2005

Single Pulse Remote Raman Detection of Minerals and Organics Under Illuminated Condition from 10 Meters Distance

A directly coupled portable remote Raman instrument developed by the University of Hawaii has been shown here to identify several minerals, chemicals and organics from a distance of 10 m using a single laser pulse in a well illuminated background. Raman spectra, obtained during a very short period of time, of common minerals e.g., dolomite, calcite, marble, barite, gypsum, quarts, rutile, fluorapatite etc. clearly show Raman features which could be used as fingerprints for mineral identification. Raman features of organics such as benzene, cyclohexane, 2-propanol, naphthalene, etc. and other chemicals containing various functional groups like oxides, silicates, sulphates, nitrates, phosphates and carbonates were also easily detected. Ability to measure Raman spectra with a single laser pulse would be promising for future space missions where power consumption is critical and a rapid survey of the minerals with moderate to high Raman cross section might be desirable for selecting rocks that would provide high scientific return or for acquiring rocks for sample return to the Earth.

Misra, A. K.↗

NASA NTRS2005

Improvement of Raman lidar algorithm for quantifying aerosol extinction

Aerosols are particles of different composition and origin and influence the formation of clouds which are important in atmospheric radiative balance. At the present there is high uncertainty on the effect of aerosols on climate and this is mainly due to the fact that aerosol presence in the atmosphere can be highly variable in space and time. Monitoring of the aerosols in the atmosphere is necessary to better understanding many of these uncertainties. A lidar (an instrument that uses light to detect the extent of atmospheric aerosol loading) can be particularly useful to monitor aerosols in the atmosphere since it is capable to record the scattered intensity as a function of altitude from molecules and aerosols. One lidar method (the Raman lidar) makes use of the different wavelength changes that occur when light interacts with the varying chemistry and structure of atmospheric aerosols. One quantity that is indicative of aerosol presence is the aerosol extinction which quantifies the amount of attenuation (removal of photons), due to scattering, that light undergoes when propagating in the atmosphere. It can be directly measured with a Raman lidar using the wavelength dependence of the received signal. In order to calculate aerosol extinction from Raman scattering data it is necessary to evaluate the rate of change (derivative) of a Raman signal with respect to altitude. Since derivatives are defined for continuous functions, they cannot be performed directly on the experimental data which are not continuous. The most popular technique to find the functional behavior of experimental data is the least-square fit. This procedure allows finding a polynomial function which better approximate the experimental data. The typical approach in the lidar community is to make an a priori assumption about the functional behavior of the data in order to calculate the derivative. It has been shown in previous work that the use of the chi-square technique to determine the most likely functional behavior of the data prior to actually calculating the derivative eliminates the need for making a priori assumptions. We note that the a priori choice of a model itself can lead to larger uncertainties as compared to the method that is validated here. In this manuscript, the chi-square technique that determines the most likely functional behavior is validated through numerical simulation and by application to a large body of Raman lidar measurements. In general, we show that the chi-square approach to evaluate aerosol extinction yields lower extinction uncertainty than the traditional technique. We also use the technique to study the feasibility of developing a general characterization of the extinction uncertainty that could permit the uncertainty in Raman lidar aerosol extinction measurements to be estimated accurately without the use of the chi-square technique.

Russo, Felicita↗

NASA NTRS2007

Remote Raman Sensor System for Testing of Rocks and Minerals

Recent and future explorations of Mars and lunar surfaces through rovers and landers have spawned great interest in developing an instrument that can perform in-situ analysis of minerals on planetary surfaces. Several research groups have anticipated that for such analysis, Raman spectroscopy is the best suited technique because it can unambiguously provide the composition and structure of a material. A remote pulsed Raman spectroscopy system for analyzing minerals was demonstrated at NASA Langley Research Center in collaboration with the University of Hawaii. This system utilizes a 532 nm pulsed laser as an excitation wavelength, and a telescope with a 4-inch aperture for collecting backscattered radiation. A spectrograph equipped with a super notch filter for attenuating Rayleigh scattering is used to analyze the scattered signal. To form the Raman spectrum, the spectrograph utilizes a holographic transmission grating that simultaneously disperses two spectral tracks on the detector for increased spectral range. The spectrum is recorded on an intensified charge-coupled device (ICCD) camera system, which provides high gain to allow detection of inherently weak Stokes lines. To evaluate the performance of the system, Raman standards such as calcite and naphthalene are analyzed. Several sets of rock and gemstone samples obtained from Ward s Natural Science are tested using the Raman spectroscopy system. In addition, Raman spectra of combustible substances such acetone and isopropanol are also obtained. Results obtained from those samples and combustible substances are presented.

Garcia, Christopher S.↗

NASA NTRS2004

Coronagraphic Notch Filter for Raman Spectroscopy

A modified coronagraph has been proposed as a prototype of improved notch filters in Raman spectrometers. Coronagraphic notch filters could offer alternatives to both (1) the large and expensive double or triple monochromators in older Raman spectrometers and (2) holographic notch filters, which are less expensive but are subject to environmental degradation as well as to limitations of geometry and spectral range. Measurement of a Raman spectrum is an exercise in measuring and resolving faint spectral lines close to a bright peak: In Raman spectroscopy, a monochromatic beam of light (the pump beam) excites a sample of material that one seeks to analyze. The pump beam generates a small flux of scattered light at wavelengths slightly greater than that of the pump beam. The shift in wavelength of the scattered light from the pump wavelength is known in the art as the Stokes shift. Typically, the flux of scattered light is of the order of 10 7 that of the pump beam and the Stokes shift lies in the wave-number range of 100 to 3,000 cm 1. A notch filter can be used to suppress the pump-beam spectral peak while passing the nearby faint Raman spectral lines. The basic principles of design and operation of a coronagraph offer an opportunity for engineering the spectral transmittance of the optics in a Raman spectrometer. A classical coronagraph may be understood as two imaging systems placed end to end, such that the first system forms an intermediate real image of a nominally infinitely distant object and the second system forms a final real image of the intermediate real image. If the light incident on the first telescope is collimated, then the intermediate image is a point-spread function (PSF). If an appropriately tailored occulting spot (e.g., a Gaussian-apodized spot with maximum absorption on axis) is placed on the intermediate image plane, then the instrument inhibits transmission of light from an on-axis source. However, the PSFs of off-axis light sources are formed off axis - that is, away from the occulting spot - so that they become refocused onto the final image plane.

Cohen, David↗

NASA NTRS2013

UV Resonant Raman Spectrometer with Multi-Line Laser Excitation

A Raman spectrometer employs two or more UV (ultraviolet) laser wavel engths to generate UV resonant Raman (UVRR) spectra in organic sampl es. Resonant Raman scattering results when the laser excitation is n ear an electronic transition of a molecule, and the enhancement of R aman signals can be several orders of magnitude. In addition, the Ra man cross-section is inversely proportional to the fourth power of t he wavelength, so the UV Raman emission is increased by another fact or of 16, or greater, over visible Raman emissions. The Raman-scatter ed light is collected using a high-resolution broadband spectrograph . Further suppression of the Rayleigh-scattered laser light is provi ded by custom UV notch filters.

Lambert, James L.↗