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NASA NTRS2012

Correction Technique for Raman Water Vapor Lidar Signal-Dependent Bias and Suitability for Water Wapor Trend Monitoring in the Upper Troposphere

The MOHAVE-2009 campaign brought together diverse instrumentation for measuring atmospheric water vapor. We report on the participation of the ALVICE (Atmospheric Laboratory for Validation, Interagency Collaboration and Education) mobile laboratory in the MOHAVE-2009 campaign. In appendices we also report on the performance of the corrected Vaisala RS92 radiosonde measurements during the campaign, on a new radiosonde based calibration algorithm that reduces the influence of atmospheric variability on the derived calibration constant, and on other results of the ALVICE deployment. The MOHAVE-2009 campaign permitted the Raman lidar systems participating to discover and address measurement biases in the upper troposphere and lower stratosphere. The ALVICE lidar system was found to possess a wet bias which was attributed to fluorescence of insect material that was deposited on the telescope early in the mission. Other sources of wet biases are discussed and data from other Raman lidar systems are investigated, revealing that wet biases in upper tropospheric (UT) and lower stratospheric (LS) water vapor measurements appear to be quite common in Raman lidar systems. Lower stratospheric climatology of water vapor is investigated both as a means to check for the existence of these wet biases in Raman lidar data and as a source of correction for the bias. A correction technique is derived and applied to the ALVICE lidar water vapor profiles. Good agreement is found between corrected ALVICE lidar measurments and those of RS92, frost point hygrometer and total column water. The correction is offered as a general method to both quality control Raman water vapor lidar data and to correct those data that have signal-dependent bias. The influence of the correction is shown to be small at regions in the upper troposphere where recent work indicates detection of trends in atmospheric water vapor may be most robust. The correction shown here holds promise for permitting useful upper tropospheric water vapor profiles to be consistently measured by Raman lidar within NDACC (Network for the Detection of Atmospheric Composition Change) and elsewhere, despite the prevalence of instrumental and atmospheric effects that can contaminate the very low signal to noise measurements in the UT.

MOHAVE-2009↗

NASA NTRS2013

Liquid Water Cloud Measurements Using the Raman Lidar Technique: Current Understanding and Future Research Needs

This paper describes recent work in the Raman lidar liquid water cloud measurement technique. The range-resolved spectral measurements at the National Aeronautics and Space Administration Goddard Space Flight Center indicate that the Raman backscattering spectra measured in and below low clouds agree well with theoretical spectra for vapor and liquid water. The calibration coefficients of the liquid water measurement for the Raman lidar at the Atmospheric Radiation Measurement Program Southern Great Plains site of the U.S. Department of Energy were determined by comparison with the liquid water path (LWP) obtained with Atmospheric Emitted Radiance Interferometer (AERI) and the liquid water content (LWC) obtained with the millimeter wavelength cloud radar and water vapor radiometer (MMCR-WVR) together. These comparisons were used to estimate the Raman liquid water cross-sectional value. The results indicate a bias consistent with an effective liquid water Raman cross-sectional value that is 28%-46% lower than published, which may be explained by the fact that the difference in the detectors' sensitivity has not been accounted for. The LWP of a thin altostratus cloud showed good qualitative agreement between lidar retrievals and AERI. However, the overall ensemble of comparisons of LWP showed considerable scatter, possibly because of the different fields of view of the instruments, the 350-m distance between the instruments, and the horizontal inhomogeneity of the clouds. The LWC profiles for a thick stratus cloud showed agreement between lidar retrievals andMMCR-WVR between the cloud base and 150m above that where the optical depth was less than 3. Areas requiring further research in this technique are discussed.

vapor and liquid water↗

NASA NTRS2022

Reduction of Raman Spectroscopy Data for H2-CO2-Air Tubular Flame Measurements

An approach of reducing spontaneous Raman spectroscopy data, based on the matrix inversion method which logically removes undesired sources of the Raman scattering signals including cross-talk due to the signals from other species, is discussed. The approach contains extensive calibration of temperature-dependent system response. The Raman spectra of several cold and hot calibration flames and their resulting calibration matrix are elaborated. The structure of H2-CO2-air tubular flames, in terms of major species (CO2, O2, N2, H2O, and H2) concentrations and temperature, was successfully measured with the optical technique. The Raman spectra data used in this study are taken from a uniquely designed experimental apparatus – a tubular burner and Raman spectroscopy system at Vanderbilt University. The characteristic uncertainties for chemical species are approximately ±2% by mole fraction for hot products and ±0.5% for room temperature reactants. The approach described here for hydrogen/air tubular flames may be adapted to hydrocarbon/air tubular flames when other necessary major species, for example, CH4 and CO for methane/air tubular flame, are considered in the whole process.

Raman Spectroscopy↗

NASA NTRS1973

Laser radar studies: A study of the feasibility of remote measurement of atmospheric density and turbidity by means of rotational Raman scattering of laser light

A remote sensing technique is described which utilizes elastic scattering and rotational Raman scattering of laser light in the atmosphere to obtain soundings of turbidity, transmissivity and density. A scheme is devised whereby, through selective weighting of the rotational Raman lines, the effect of atmospheric temperature structure may be eliminated. The close spectral proximity of the elastic and Raman-scattered signals, combined with the fact that the Raman scattering is quite weak, produces special requirements for the spectroscopic and light-gathering components of a rotational Raman laser radar system. These requirements are investigated. A computation of typical signal-to-noise ratios is made. It is shown that daytime signal-to-noise ratios greater than 10 db are to be expected for observation heights of 5 km and below. For nighttime work, 10 db signal-to-noise ratios are achievable to altitudes as high as 15 km.

Reiss, N.↗

NASA NTRS1981

Raman scattering as a probe of planetary atmospheres

The observable effects of Raman scattering on the spectra of the giant planets may provide new information on the composition and structure of these atmospheres. Satellite observations have already shown the influence of Raman scattering on the UV continuum albedo. A cross correlation technique is presented for detecting rotational and vibrational transitions of the Raman active gases in the atmosphere. This technique has been applied to ground-based visible spectra of Venus, Jupiter, Saturn and Uranus. Extension of this method into the UV would improve the detectability of the Raman lines because the ratio of Raman to Rayleigh cross section increases with decreasing wavelength. The technology currently exists to efficiently obtain high-signal-to-noise ratio UV spectra through the use of silicon diode array detectors. Application of the cross-correlation technique to UV spectra obtained from space vehicles would give a new important probe of the structure and composition of planetary atmospheres by enabling the use of the UV spectra of a planet to observe what would normally be an infrared molecular transition.

Cochran, W. D.↗

NASA NTRS1988

Concentration, temperature, and density in a hydrogen-air flame by excimer-induced Raman scattering

Single-pulse, vibrational Raman scattering (VRS) is an attractive laser diagnostic for the study of supersonic hydrogen-air combustion. The VRS technique gives a complete thermodynamic description of the gas mixture at a point in the reacting flow. Single-pulse, vibrational Raman scattering can simultaneously provide independent measurements of density, temperature, and concentration of each major species (H2, H2O, O2 and N2) in a hydrogen/air turbulent combustor. Also the pressure can be calculated using the ideal gas law. However, single-pulse VRS systems in current use for measurement of turbulent combustion have a number of shortcomings when applied to supersonic flows: (1) slow repetition rate (1 to 5 Hz), (2) poor spatial resolution (0.5x0.3x0.3 cu mm), and (3) marginal time resolution. Most of these shortcomings are due to the use of visible wavelength flash-lamp pumped dye lasers. The advent of UV excimer laser allows the possibility of dramatic improvements in the single-pulse, vibrational Raman scattering. The excimer based VRS probe will greatly improve repetition rate (100 to 500 Hz), spatial resolution (0.1x0.1x0.1 cu mm) and time resolution (30ns). These improvements result from the lower divergence of the UV excimer, higher repetition rate, and the increased Raman cross-sections (15 to 20 times higher) at ultra-violet (UV) wavelengths. With this increased capability, single-pulse vibrational Raman scattering promises to be an ideal non-intrusive probe for the study of hypersonic propulsion flows.

Wehrmeyer, Joseph A.↗

NASA NTRS1989

Optical Stark effect in the four-wave mixing and stimulated Raman spectra of N2

The influence of the optical Stark effect on spectral line shapes in four-wave-mixing Raman spectroscopy (FWMRS) and stimulated Raman spectroscopy (SRS) is investigated experimentally and theoretically. Using an experimental setup capable of rapid alternation between the simultaneous measurement of coherent Stokes Raman spectroscopy and inverse Raman spectroscopy at low and high intensities, together with a sophisticated frequency reference scheme, it was possible to perform a rather direct comparison between Stark-broadened and non-Stark-broadened spectra of both classes of Raman spectroscopies. The results demonstrate that SRS spectra show more Stark shift and broadening than their FWMRS counterparts. A discrepancy with theoretical results is pointed out, and an attempt is made to explain it.

Moosmuller, H.↗

NASA NTRS1999

Fine Structure of the Low-Frequency Raman Phonon Bands of Single-Wall Carbon Nanotubes

The Raman spectra of singled-wall carbon nanotubes (SWNT) produced by laser and are process were studied between 5 and 500 kappa. The line width vs. temperature dependence of the low-frequency Raman bands between 150 and 200/ cm deviates from that expected for phonon decay through phonon-phonon scattering mechanism. The experimental results and their analysis provided convincing evidence that each of the low-frequency Raman lines is a superposition of several narrower Raman lines corresponding to tubes of nearly the same diameter. The application of Raman spectroscopy to probe the distribution of SWNT by both diameter and chirality is discussed.

Iliev, M. N.↗

NASA NTRS2000

Raman Gas Species Measurements in Hydrocarbon-Fueled Rocket Engine Injector Flows

Rocket engine propellent injector development at NASA-Marshall includes experimental analysis using optical techniques, such as Raman, fluorescence, or Mie scattering. For the application of spontaneous Raman scattering to hydrocarbon-fueled flows a technique needs to be developed to remove the interfering polycyclic aromatic hydrocarbon fluorescence from the relatively weak Raman signals. A current application of such a technique is to the analysis of the mixing and combustion performance of multijet, impinging-jet candidate fuel injectors for the baseline Mars ascent engine, which will burn methane and liquid oxygen produced in-situ on Mars to reduce the propellent mass transported to Mars for future manned Mars missions. The Raman technique takes advantage of the strongly polarized nature of Raman scattering. It is shown to be discernable from unpolarized fluorescence interference by subtracting one polarized image from another. Both of these polarized images are obtained from a single laser pulse by using a polarization-separating calcite rhomb mounted in the imaging spectrograph. A demonstration in a propane-air flame is presented, as well as a high pressure demonstration in the NASA-Marshall Modular Combustion Test Artice, using the liquid methane-liquid oxygen propellant system

Wehrmeyer, Joseph↗

NASA NTRS2000

AROTEL Temperature Retrievals Within PSC's Using Raman Scattering

NASA Goddard Space Flight Center's Airborne Raman Ozone Temperature Lidar (AROTEL) made temperature retrievals within Polar Stratospheric Clouds (PSCs) on several flights during the SAGE III Ozone Loss and Validation Experiment (SOLVE) campaign. The location of the PSCs was confirmed using simultaneously acquired data from the NASA Langley Aerosol lidar. Retrievals were made on flight dates 991207, 991210 and 000127 from just above the aircraft to 25 kilometers geometric altitude. Raman temperature retrievals are, to first order, insensitive to Mie interference because the Raman signals are red shifted by 2331 cm(exp -1) from the initial laser wavelength. Backscattering from clouds and aerosols is consequently not observed by the detector; however, extinction does impact the measurement and limits retrievals to optically thin clouds. Comparisons between retrievals employing Rayleigh and Raman scattering show the Raman temperatures to be significantly warmer than those employing Rayleigh scattering. Uncertainties are a function of altitude: at 25 km they were approximately 3 K. Temperature profiles could not be retrieved for optically thick clouds.

Burris, John↗

NASA NTRS2003

New Examination of the Raman Lidar Technique for Water Vapor and Aerosols: Evaluating the Temperature Dependent Lidar Equations - Paper 1

The intent of this paper and its companion is to compile together the essential information required for the analysis of Raman lidar water vapor and aerosol data acquired using a single laser wavelength. In this first paper several details concerning the evaluation of the lidar equation when measuring Raman scattering are considered. These details include the influence of the temperature dependence of both pure rotational and vibrational-rotational Raman scattering on the lidar profile. These are evaluated for the first time using a new form of the lidar equation. The results indicate that, for the range of temperatures encountered in the troposphere, the magnitude of the temperature dependent effect can reach 10% or more for narrowband Raman water vapor measurements. Also the calculation of atmospheric transmission is examined carefully including the effects of depolarization. Different formulations of Rayleigh cross section determination commonly used in the lidar field are compared revealing differences up to 5% among the formulations. The influence of multiple scattering on the measurement of aerosol extinction using the Raman lidar technique is considered as are several photon pulse-pileup correction techniques.

Whiteman, David N.↗

NASA NTRS2005

Extracting Olivine (Fo-Fa) Compositions from Raman Spectral Peak Positions

Olivine and pyroxene are two major basaltic minerals that have been identified at Gusev Crater and Meridiani Planum by the Mars Exploration Rovers. Full petrologic characterization of a sample (rock or soil), however, requires determining the range of mineral compositions, extent of zoning, range of grain sizes, mineral associations, presence of xenocrysts, etc. Information of this sort will aid the interpretation of sample crystallization and differentiation histories and help discriminate between lithologies. In Raman spectroscopic experiments, minerals are identified by their spectral patterns and mineral compositions can be inferred from the peak positions. Instruments currently in use or slated for impending surface exploration missions provide only average elemental compositions for relatively large rock or soil targets or bulk mineral analysis. No techniques currently in use or scheduled for flight can characterize both structure and composition of individual mineral grains, in-situ, like the Mars Microbeam Raman Spectrometer (MMRS). The MMRS is designed to take 100 spectra along a 1 cm linear traverse on the surface of a sample, with contributions from one or a few mineral phases per spectrum. We presented a method to extract structural and compositional information from the Raman spectra of quadrilateral pyroxenes. The pyroxene calibration was applied to a Raman spectroscopic study of Martian meteorite EETA79001 along with a preliminary olivine calibration, where we demonstrated the capability to discriminate related lithologies using Raman point counts. This paper presents an improved olivine calibration that will further aid sample characterization and the study of alteration processes.

Kuebler, K.↗

NASA NTRS2001

One-Dimensional Spontaneous Raman Measurements Made in a Gas Turbine Combustor

The NASA Glenn Research Center and the aerospace industry are designing and testing low-emission combustor concepts to build the next generation of cleaner, more fuel efficient aircraft powerplants. These combustors will operate at much higher inlet temperatures and at pressures that are up to 3 to 5 times greater than combustors in the current fleet. From a test and analysis viewpoint, there is an increasing need for measurements from these combustors that are nonintrusive, simultaneous, multipoint, and more quantitative. Glenn researchers have developed several unique test facilities (refs. 1 and 2) that allow, for the first time, optical interrogation of combustor flow fields, including subcomponent performance, at pressures ranging from 1 to 60 bar (1 to 60 atm). Experiments conducted at Glenn are the first application of a visible laser-pumped, one-dimensional, spontaneous Raman-scattering technique to analyze the flow in a high-pressure, advanced-concept fuel injector at pressures thus far reaching 12 bar (12 atm). This technique offers a complementary method to the existing two- and three-dimensional imaging methods used, such as planar laser-induced fluorescence. Raman measurements benefit from the fact that the signal from each species is a linear function of its density, and the relative densities of all major species can be acquired simultaneously with good precision. The Raman method has the added potential to calibrate multidimensional measurements by providing an independent measurement of species number-densities at known points within the planar laser-induced fluorescence images. The visible Raman method is similar to an ultraviolet-Raman technique first tried in the same test facility (ref. 3). However, the visible method did not suffer from the ultraviolet technique's fuel-born polycyclic aromatic hydrocarbon fluorescence interferences.

DeGroot, Wilhelmus A.↗

NASA NTRS2006

Remote Pulsed Laser Raman Spectroscopy System for Detecting Qater, Ice, and Hydrous Minerals

For exploration of planetary surfaces, detection of water and ice is of great interest in supporting existence of life on other planets. Therefore, a remote Raman spectroscopy system was demonstrated at NASA Langley Research Center in collaboration with University of Hawaii for detecting ice-water and hydrous minerals on planetary surfaces. In this study, a 532 nm pulsed laser is utilized as an excitation source to allow detection in high background radiation conditions. The Raman scattered signal is collected by a 4-inch telescope positioned in front of a spectrograph. The Raman spectrum is analyzed using a spectrograph equipped with a holographic super notch filter to eliminate Rayleigh scattering, and a holographic transmission grating that simultaneously disperses two spectral tracks onto the detector for higher spectral range. To view the spectrum, the spectrograph is coupled to an intensified charge-coupled device (ICCD), which allows detection of very weak Stokes line. The ICCD is operated in gated mode to further suppress effects from background radiation and long-lived fluorescence. The sample is placed at 5.6 m from the telescope, and the laser is mounted on the telescope in a coaxial geometry to achieve maximum performance. The system was calibrated using the spectral lines of a Neon lamp source. To evaluate the system, Raman standard samples such as calcite, naphthalene, acetone, and isopropyl alcohol were analyzed. The Raman evaluation technique was used to analyze water, ice and other hydrous minerals and results from these species are presented.

Garcia, Christopher S.↗

NASA NTRS2007

Application of Raman Spectroscopy for Nondestructive Evaluation of Composite Materials

This paper will present an overview of efforts to investigate the application of Raman spectroscopy for the characterization of Kevlar materials. Raman spectroscopy is a laser technique that is sensitive to molecular interactions in materials such as Kevlar, graphite and carbon used in composite materials. The overall goal of this research reported here is to evaluate Raman spectroscopy as a potential nondestructive evaluation (NDE) tool for the detection of stress rupture in Kevlar composite over-wrapped pressure vessels (COPVs). Characterization of the Raman spectra of Kevlar yarn and strands will be presented and compared with analytical models provided in the literature. Results of testing to investigate the effects of creep and high-temperature aging on the Raman spectra will be presented.

Washer, Glenn A.↗

NASA NTRS2004

Multiplex coherent raman spectroscopy detector and method

A multiplex coherent Raman spectrometer (10) and spectroscopy method rapidly detects and identifies individual components of a chemical mixture separated by a separation technique, such as gas chromatography. The spectrometer (10) and method accurately identify a variety of compounds because they produce the entire gas phase vibrational Raman spectrum of the unknown gas. This is accomplished by tilting a Raman cell (20) to produce a high-intensity, backward-stimulated, coherent Raman beam of 683 nm, which drives a degenerate optical parametric oscillator (28) to produce a broadband beam of 1100-1700 nm covering a range of more than 3000 wavenumber. This broadband beam is combined with a narrowband beam of 532 nm having a bandwidth of 0.003 wavenumbers and focused into a heated windowless cell (38) that receives gases separated by a gas chromatograph (40). The Raman radiation scattered from these gases is filtered and sent to a monochromator (50) with multichannel detection.

Chen, Peter↗

NASA NTRS2003

Assessing blood brain barrier dynamics or identifying or measuring selected substances or toxins in a subject by analyzing Raman spectrum signals of selected regions in the eye

A non-invasive method for analyzing the blood-brain barrier includes obtaining a Raman spectrum of a selected portion of the eye and monitoring the Raman spectrum to ascertain a change to the dynamics of the blood brain barrier. Also, non-invasive methods for determining the brain or blood level of an analyte of interest, such as glucose, drugs, alcohol, poisons, and the like, comprises: generating an excitation laser beam (e.g., at a wavelength of 600 to 900 nanometers); focusing the excitation laser beam into the anterior chamber of an eye of the subject so that aqueous humor, vitreous humor, or one or more conjunctiva vessels in the eye is illuminated; detecting (preferably confocally detecting) a Raman spectrum from the illuminated portion of the eye; and then determining the blood level or brain level (intracranial or cerebral spinal fluid level) of an analyte of interest for the subject from the Raman spectrum. In certain embodiments, the detecting step may be followed by the step of subtracting a confounding fluorescence spectrum from the Raman spectrum to produce a difference spectrum; and determining the blood level and/or brain level of the analyte of interest for the subject from that difference spectrum, preferably using linear or nonlinear multivariate analysis such as partial least squares analysis. Apparatus for carrying out the foregoing methods are also disclosed.

Lambert, James L.↗

NASA NTRS2008

Assessing blood brain barrier dynamics or identifying or measuring selected substances, including ethanol or toxins, in a subject by analyzing Raman spectrum signals

A non-invasive method for analyzing the blood-brain barrier includes obtaining a Raman spectrum of a selected portion of the eye and monitoring the Raman spectrum to ascertain a change to the dynamics of the blood brain barrier.Also, non-invasive methods for determining the brain or blood level of an analyte of interest, such as glucose, drugs, alcohol, poisons, and the like, comprises: generating an excitation laser beam at a selected wavelength (e.g., at a wavelength of about 400 to 900 nanometers); focusing the excitation laser beam into the anterior chamber of an eye of the subject so that aqueous humor, vitreous humor, or one or more conjunctiva vessels in the eye is illuminated; detecting (preferably confocally detecting) a Raman spectrum from the illuminated portion of the eye; and then determining the blood level or brain level (intracranial or cerebral spinal fluid level) of an analyte of interest for the subject from the Raman spectrum. In certain embodiments, the detecting step may be followed by the step of subtracting a confounding fluorescence spectrum from the Raman spectrum to produce a difference spectrum; and determining the blood level and/or brain level of the analyte of interest for the subject from that difference spectrum, preferably using linear or nonlinear multivariate analysis such as partial least squares analysis. Apparatus for carrying out the foregoing methods are also disclosed.

Lambert, James L.↗