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NASA NTRS2009

Studies of Minerals, Organic and Biogenic Materials through Time-Resolved Raman Spectroscopy

A compact remote Raman spectroscopy system was developed at NASA Langley Research center and was previously demonstrated for its ability to identify chemical composition of various rocks and minerals. In this study, the Raman sensor was utilized to perform time-resolved Raman studies of various samples such as minerals and rocks, Azalea leaves and a few fossil samples. The Raman sensor utilizes a pulsed 532 nm Nd:YAG laser as excitation source, a 4-inch telescope to collect the Raman-scattered signal from a sample several meters away, a spectrograph equipped with a holographic grating, and a gated intensified CCD (ICCD) camera system. Time resolved Raman measurements were carried out by varying the gate delay with fixed short gate width of the ICCD camera, allowing measurement of both Raman signals and fluorescence signals. Rocks and mineral samples were characterized including marble, which contain CaCO3. Analysis of the results reveals the short (approx.10-13 s) lifetime of the Raman process, and shows that Raman spectra of some mineral samples contain fluorescence emission due to organic impurities. Also analyzed were a green (pristine) and a yellow (decayed) sample of Gardenia leaves. It was observed that the fluorescence signals from the green and yellow leaf samples showed stronger signals compared to the Raman lines. Moreover, it was also observed that the fluorescence of the green leaf was more intense and had a shorter lifetime than that of the yellow leaf. For the fossil samples, Raman shifted lines could not be observed due the presence of very strong short-lived fluorescence.

Garcia, Christopher S.↗

NASA NTRS1994

Visible-infrared remote-sensing model and applications for ocean waters

Remote sensing has become important in the ocean sciences, especially for research involving large spatial scales. To estimate the in-water constituents through remote sensing, whether carried out by satellite or airplane, the signal emitted from beneath the sea surface, the so called water-leaving radiance (L(w)), is of prime importance. The magnitude of L(w) depends on two terms: one is the intensity of the solar input, and the other is the reflectance of the in-water constituents. The ratio of the water-leaving radiance to the downwelling irradiance (E(d)) above the sear surface (remote-sensing reflectance, R(sub rs)) is independent of the intensity of the irradiance input, and is largely a function of the optical properties of the in-water constituents. In this work, a model is developed to interpret r(sub rs) for ocean water in the visible-infrared range. In addition to terms for the radiance scattered from molecules and particles, the model includes terms that describe contributions from bottom reflectance, fluorescence of gelbstoff or colored dissolved organic matter (CDOM), and water Raman scattering. By using this model, the measured R(sub rs) of waters from the West Florida Shelf to the Mississippi River plume, which covered a (concentration of chlorophyll a) range of 0.07 - 50 mg/cu m, were well interpreted. The average percentage difference (a.p.d.) between the measured and modeled R(sub rs) is 3.4%, and, for the shallow waters, the model-required water depth is within 10% of the chart depth. Simple mathematical simulations for the phytoplankton pigment absorption coefficient (a(sub theta)) are suggested for using the R(sub rs) model. The inverse problem of R(sub rs), which is to analytically derive the in-water constituents from R(sub rs) data alone, can be solved using the a(sub theta) functions without prior knowledge of the in-water optical properties. More importantly, this method avoids problems associated with a need for knowledge of the shape and value of the chlorophyll-specific absorption coefficient. The simulation was tested for a wide range of water types, including waters from Monterey Bay, the West Florida Shelf, and the Mississippi River plume. Using the simulation, the R(sub rs)-derived in-water absorption coefficients were consistent with the values from in-water measurements (r(exp 2) greater than 0.94, slope approximately 1.0). In the remote-sensing applications, a new approach is suggested for the estimation of primary production based on remote sensing. Using this approach, the calculated primary production (PP) values based upon remotely sensed data were very close to the measured values for the euphotic zone (r(exp 2) = 0.95, slope 1.26, and 32% average difference), while traditional, pigment-based PP model provided values only one-third the size of the measured data. This indicates a potential to significantly improve the accuracy of the estimation of primary production based upon remote sensing.

Lee, Zhongping↗

NASA NTRS1981

The Sun among stars. IV - Albedos of Uranus and Neptune and the solar color

Geometric albedos in 48 adjacent 50 A bands from 3250 to 5600 A have been derived from observations of Uranus and Neptune. The solar analog found in earlier papers (Hardorp 1978, 1980) was chosen for these reductions, so these albedos are more reliable systematically than earlier ones and allow a choice among the scattering models of Savage et al. (1980). Green methane bands are stronger on Neptune. Strong solar absorption lines are found to be partially filled in by Raman-scattering. Neglect of this effect caused Croft et al. (1972) to find a solar color that is too blue. It probably also affected the classification of G-type stars in the Michigan Spectral Catalogue as well as Garrison's (1979) interpretation of IUE observations.

Hardorp, J.↗

NASA NTRS1986

Linewidth characteristics of Raman-shifted dye laser output at 720 and 940 nm

Existing DIAL systems for water vapor measurements in the troposphere operate at wavelengths near 720 nm. The use of stronger water vapor absorption lines in the range 930 to 960 nm will significantly improve DIAL measurements in the upper troposphere and lower stratosphere where water vapor concentrations are low. The generation of light at 940 nm using a frequency doubled Nd:YAG pumped dye laser is inefficient due to the small absorption if infrared dyes at the pump wavelength. However, 940 nm generation utilizing stimulated Raman scattering of dye lasers is attractive because of a potentially high conversion efficiency plus the possibility of retaining the narrow linewidth available from some dye lasers. The Raman conversion efficiency and line broadening are presented for first Stokes operation at 720 and 940 nm using hydrogen and deuterium as the Raman media.

Grossmann, B. E.↗

NASA NTRS1999

Coherent Pump-Probe Interactions and Terahertz Intersubband Gain in Semiconductor Quantum Wells

In recent years there has been considerable interest in intersubband-transition-based infrared semiconductor quantum well (QW) lasers because of their potential applications. In the mid-infrared range, both electrically-injected quantum cascade lasers [1] and optically-pumped multiple QW lasers [2] have been experimentally realized. In these studies, optical gain is due to population inversion between the lasing subbands. It was also proposed that stimulated Raman scattering in QW systems can produce net infrared optical gain [3j. In such a nonlinear optical scheme, the appearance of optical gain that may lead to intersubband Raman lasers does not rely on the population inversion. Since, in tile resonant Raman process (Raman gain is the largest in this case), the pump field induces population redistribution among subbands in the QW s ystem, it seems that a realistic estimate of the optical gain has to include this effect. Perturbative calculations used in the previous work [3] may overestimate the Raman gain. In this paper we present a nonperturbative calculation of terahertz gain of optically-pumped semiconductor step quantum wells. Limiting optical transitions within the conduction band of QW, we solve the pump-field-induced nonequilibrium distribution function for each subband of the QW system from a set of coupled rate equations. Both intrasubband and intersubband relaxation processes in the quantum well system are included. Taking into account the coherent interactions between pump and THz (signal) waves, we we derive the susceptibility of the QW system for the THz field. For a GaAs/AlGaAs step QW, we calculate the Thz gain spectrum for different pump frequencies and intensities. Under moderately strong pumping (approximately 0.3 MW/sq cm), a significant THz gain (approximately 300/m) is predicted. It is also shown that the coherent wave interactions (resonant stimulated Raman processes) contribute significantly to the THz gain.

Liu, Ansheng↗

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 NTRS1989

Progress of research on water vapor lidar

Research is summarized on applications of stimulated Raman scattering (SRS) of laser light into near infrared wavelengths suitable for atmospheric monitoring. Issues addressed are conversion efficiency, spectral purity, optimization of operating conditions, and amplification techniques. A Raman cell was developed and built for the laboratory program, and is now available to NASA-Langley, either as a design or as a completed cell for laboratory or flight applications. The Raman cell has been approved for flight in NASA's DC-8 aircraft. The self-seeding SRS technique developed here is suggested as an essential improvement for tunable near-IR DIAL applications at wavelengths of order 1 micrometer or greater.

Wilkerson, Thomas D.↗

NASA NTRS2021

Perseverance’s Scanning Habitable Environments with Raman and Luminescence for Organics and Chemicals (SHERLOC) Investigation

The Scanning Habitable Environments with Raman and Luminescence for Organics and Chemicals (SHERLOC) is a robotic arm-mounted instrument on NASA’s Perseverance rover. SHERLOC has two primary boresights. The Spectroscopy boresight generates spatially resolved chemical maps using fluorescence and Raman spectroscopy coupled to microscopic images (10.1 μm/pixel). The second boresight is a Wide Angle Topographic Sensor for Operations and eNgineering (WATSON); a copy of the Mars Science Laboratory (MSL) Mars Hand Lens Imager (MAHLI) that obtains color images from microscopic scales (∼13 μm/pixel) to infinity. SHERLOC Spectroscopy focuses a 40 μs pulsed deep UV neon-copper laser (248.6 nm), to a ∼100 μm spot on a target at a working distance of ∼48 mm. Fluorescence emissions from organics, and Raman scattered photons from organics and minerals, are spectrally resolved with a single diffractive grating spectrograph with a spectral range of 250 to ∼370 nm. Because the fluorescence and Raman regions are naturally separated with deep UV excitation (<250 nm), the Raman region ∼ 800 – 4000 cm−1 (250 to 273 nm) and the fluorescence region (274 to ∼370 nm) are acquired simultaneously without time gating or additional mechanisms. SHERLOC science begins by using an Autofocus Context Imager (ACI) to obtain target focus and acquire 10.1 μm/pixel greyscale images. Chemical maps of organic and mineral signatures are acquired by the orchestration of an internal scanning mirror that moves the focused laser spot across discrete points on the target surface where spectra are captured on the spectrometer detector. ACI images and chemical maps (< 100 μm/mapping pixel) will enable the first Mars in situ view of the spatial distribution and interaction between organics, minerals, and chemicals important to the assessment of potential biogenicity (containing CHNOPS). Single robotic arm placement chemical maps can cover areas up to 7x7 mm in area and, with the < 10 min acquisition time per map, larger mosaics are possible with arm movements. This microscopic view of the organic geochemistry of a target at the Perseverance field site, when combined with the other instruments, such as Mastcam-Z, PIXL, and SuperCam, will enable unprecedented analysis of geological materials for both scientific research and determination of which samples to collect and cache for Mars sample return.

Rohit Bhartia↗

NASA NTRS1990

Progress of research on water vapor lidar

Research is described on several aspects of stimulated Raman scattering (SRS) of 532 nm laser light in H2, D2, and CH4. The goals of this work are to develop a more thorough understanding of nonlinear processes involving the Raman effect and four-wave mixing, and to find the best way to generate radiation at several wavelengths simultaneously, for lidar applications. Issues addressed are conversion efficiency, optimization of operating conditions (gas pressure, confocal parameter, etc.) and the distribution of output pulse energy over three Stokes components, the first anti-Stokes component, and the zeroth order (pump) wavelength. The described research and results constitute another step in the development of SRS applications for NASA's atmospheric lidar program.

Wilkerson, T. D.↗

NASA NTRS1980

Remote sensing of subsurface water temperature by laser Raman spectroscopy

This paper describes experimental remote sensing of subsurface water temperature using the Raman spectroscopic technique. By the use of a pulsed laser and range gating detection techniques, Raman scattering is analyzed as a function of depth in a radar-like echo mode, and thus subsurface profiles of temperature and transmission are obtained. Experiments are described in which Raman data using polarization spectroscopy has been obtained from a ship as a function of depth in ocean water near Grand Bahama Island. A spectral temperature accuracy of + or - 1 C has been obtained from this data in the first two optical attenuation lengths. Raman data obtained from ocean water using the NASA airborne oceanographic lidar is also presented.

Leonard, D. A.↗

NASA NTRS1981

Remote Raman measurement techniques

The use of laser Raman measurement techniques in remote sensing applications is surveyed. A feasibility index is defined as a means to characterize the practicality of a given remote Raman measurement application. Specific applications of Raman scattering to the measurement of atmospheric water vapor profiles, methane plumes from liquid natural gas spills, and subsurface ocean temperature profiles are described. This paper will survey the use of laser Raman measurement techniques in remote sensing applications using as examples specific systems that the Computer Genetics Corporation (CGC) group has developed and engineered.

Leonard, D. A.↗

NASA NTRS1986

Observation of atmospheric ozone by dial with Raman lasers pumped by a KrF laser

Since the XeCl excimer laser (308 nm) was first used in Differential Absorption Lidar (DIAL) for stratospheric ozone detection, the XeCl ozone lidar became a useful tool for the monitoring of the stratospheric ozone concentration. Shorter wavelength lasers are needed for the observation of ozone in the troposphere where the ozone concentration is about one order of magnitude smaller than in the stratosphere. In 1983, tropospheric ozone was observed with the combination of the second Stokes line (290.4 nm) of stimulated Raman scattering from methane pumped by a KrF laser and the XeCl laser line. The measurement of the ozone distribution from ground to 30 km was reported, using three Stokes lines of Raman lasers pumped by a KrF laser. At wavelengths shorter than 295 nm, the background solar radiation is effectively suppressed by atmospheric ozone. Such a solar-blind effect can be expected when two wavelengths 277 and 290.4 nm are used for DIAL ozone detection. A preliminary measurement of the day time ozone distribution in the troposphere is presented using these wavelengths generated by a KrF laser with a Raman shifter. Analysis using the lidar equation predicts the maximum detectable range is 7 km.

Maeda, M.↗

NASA NTRS2017

Rotational Raman-Based Temperature Measurements in a High-Velocity Turbulent Jet

Spontaneous rotational Raman scattering spectroscopy is used to acquire the first ever high quality, spatially-resolved measurements of the mean and root mean square (rms) temperature fluctuations in turbulent, high-velocity heated jets. Raman spectra in air were obtained across a matrix of radial and axial locations downstream from a 50 mm diameter nozzle operating from subsonic to supersonic conditions over a wide range of temperatures and Mach numbers, in accordance with the Tanna matrix frequently used in jet noise studies. These data were acquired in the hostile, high noise (115 dB) environment of a large scale open air test facility at NASA Glenn Research Center (GRC). Temperature estimates were determined by performing nonlinear least squares fitting of the single shot spectra to the theoretical rotational Stokes spectra of N2 and O2, using a custom in-house code developed specifically for this investigation. The laser employed in this study was a high energy, long-pulsed, frequency doubled Nd:YAG laser. One thousand single-shot spectra were acquired at each spatial coordinate. Mean temperature and rms temperature variations were calculated at each measurement location. Excellent agreement between the averaged and single-shot temperatures was observed with an accuracy better than 2.5 percent for temperature, and rms variations in temperature between +/-2.2 percent at 296 K and +/-4.5 percent at 850 K. The results of this and planned follow-on studies will support NASA GRC's development of physics-based jet noise prediction, turbulence modeling and aeroacoustic source modeling codes.

Randy J Locke↗

NASA NTRS2017

Rotational Raman-Based Temperature Measurements in a High-Velocity Turbulent Jet

Randy J Locke↗

NASA NTRS1981

Absolute tracer dye concentration using airborne laser-induced water Raman backscatter

The use of simultaneous airborne-laser-induced dye fluorescence and water Raman backscatter to measure the absolute concentration of an ocean-dispersed tracer dye is discussed. Theoretical considerations of the calculation of dye concentration by the numerical comparison of airborne laser-induced fluorescence spectra with laboratory spectra for known dye concentrations using the 3400/cm OH-stretch water Raman scatter as a calibration signal are presented which show that minimum errors are obtained and no data concerning water mass transmission properties are required when the laser wavelength is chosen to yield a Raman signal near the dye emission band. Results of field experiments conducted with an airborne conical scan lidar over a site in New York Bight into which rhodamine dye had been injected in a study of oil spill dispersion are then indicated which resulted in a contour map of dye concentrations, with a minimum detectable dye concentration of approximately 2 ppb by weight.

Hoge, F. E.↗

NASA NTRS2009

Enhancing SERS by Means of Supramolecular Charge Transfer

In a proposed method of sensing small quantities of molecules of interest, surface enhanced Raman scattering (SERS) spectroscopy would be further enhanced by means of intermolecular or supramolecular charge transfer. There is a very large potential market for sensors based on this method for rapid detection of chemical and biological hazards. In SERS, the Raman signals (vibrational spectra) of target molecules become enhanced by factors of the order of 108 when those molecules are in the vicinities of nanostructured substrate surfaces that have been engineered to have plasmon resonances that enhance local electric fields. SERS, as reported in several prior NASA Tech Briefs articles and elsewhere, has remained a research tool and has not yet been developed into a practical technique for sensing of target molecules: this is because the short range (5 to 20 nm) of the field enhancement necessitates engineering of receptor molecules to attract target molecules to the nanostructured substrate surfaces and to enable reliable identification of the target molecules in the presence of interferants. Intermolecular charge-transfer complexes have been used in fluorescence-, photoluminescence-, and electrochemistry-based techniques for sensing target molecules, but, until now, have not been considered for use in SERS-based sensing. The basic idea of the proposed method is to engineer receptor molecules that would be attached to nanostructured SERS substrates and that would interact with the target molecules to form receptor-target supramolecular charge-transfer complexes wherein the charge transfer could be photoexcited.

Wong, Eric↗

NASA NTRS1990

Flow diagnostics in unseeded air

Several approaches are presented for the quantitative measurement of flowfield parameters in high-speed flows. The techniques are developed for the study of air flows in the Mach 2 to Mach 3 regime and can be extended to the hypersonic and subsonic regimes in a straightforward manner. Instantaneous two-dimensional cross-sectional images of the density using UV Rayleigh scattering and the measurement of velocity profiles using the RELIEF technique are shown. The RELIEF technique employs two high-powered lasers separated in frequency by the vibrational frequency of oxygen molecules to write lines across the flowfield by stimulated Raman scattering. The preliminary results indicate that the UV Rayleigh scattering may also be extended to the measurement of velocity and temperature fields by using an atomic or molecular absorption filter window, and that the RELIEF technique can be extended to marking shaped volumetric points or arrays of points in the flowfield for velocity and vorticity measurements.

Miles, R.↗

NASA NTRS1993

Intense backward Raman lasers in CH4 and H2

The conversion efficiency of the first Stokes radiation generated by backward stimulated Raman scattering is measured in CH4 and H2 that are pumped by a third harmonic of a Nd:YAG laser in the 12-55-mJ energy range and in the 0.86-6.00-MPa pressure range. Our experimental results show that CH4 is a better Raman medium than H2 at moderate pressures (a few megapascals) to efficiently generate backward Raman lines.

Sentrayan, Karuppasamy↗