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Proposed spectral imaging system used to detect leaking hydrogen from distance of 100 ft or more. Video cameras form images of leaking hydrogen by use of Raman scattering of laser beam from hydrogen. By indicating potentially explosive concentrations of hydrogen in air, system contributes to safety at facilities producing and handling hydrogen, such as fueling stations for hydrogen-burning automobiles of near future.
The motivation of this work was to have robust spectroscopic sensors for sensitive detection and chemical analysis of organic and molecular compounds. The solution is to use silica sphere optical resonators to provide surface-enhanced spectroscopic signal. Whispering-gallery mode (WGM) resonators made from silica microspheres were used for surface-enhanced Raman scattering (SERS) without coupling to a plasmonic mechanism. Large Raman signal enhancement is observed by exclusively using 5.08-micron silica spheres with 785-nm laser excitation. The advantage of this non-plasmonic approach is that the active substrate is chemically inert silica, thermally stable, and relatively simple to fabricate. The Raman signal enhancement is broadly applicable to a wide range of molecular functional groups including aliphatic hydrocarbons, siloxanes, and esters. Applications include trace organic analysis, particularly for in situ planetary instruments that require robust sensors with consistent response.
We report the first observations, to our knowledge, of nonlinear optical effects in large (millimeter-sized) droplets. Stimulated Raman scattering (SRS) and laser-induced breakdown (LIB) are simultaneously observed in acoustically levitated millimeter-sized glycerol droplets irradiated by either a frequency-doubled (532-nm) or a frequency-tripled (355-nm) Nd:YAG laser. The two processes, which occur above a nearby coincident irradiation threshold, are conjectured to arise from a common initiation mechanism: self-focusing. LIB generates vapor bubbles within the droplet, resulting in the quenching of SRS emission.
Vibrational and rotational population distributions in expanding nitrogen in the supersonic nozzle of a reflected shock tunnel were investigated using spontaneous Raman scattering spectroscopy. The experimental data are compared with two multitemperature nonequilibrium calculations, one based on the Landau-Teller model for vibrational relaxation, the other on the solution of the vibrational master equations. Good agreement was found between both the Landau-Teller and the master equation solutions for the vibrational energy mode, but the experimentally inferred rotational temperatures were found to be systematically low, due to collisional narrowing. The dramatic increase in vibrational relaxation rates for a cooling flowfield reported in most previous studies was not reproduced by the present experiments.
In this paper we examine differences between cloud pressures retrieved from the Ozone Monitoring Instrument (OMI) using the ultraviolet rotational Raman scattering (RRS) algorithm and those from the thermal infrared (IR) Aqua/MODIS. Several cloud data sets are currently being used in OMI trace gas retrieval algorithms including climatologies based on IR measurements and simultaneous cloud parameters derived from OMI. From a validation perspective, it is important to understand the OMI retrieved cloud parameters and how they differ with those derived from the IR. To this end, we perform radiative transfer calculations to simulate the effects of different geophysical conditions on the OMI RRS cloud pressure retrievals. We also quantify errors related to the use of the Mixed Lambert-Equivalent Reflectivity (MLER) concept as currently implemented of the OMI algorithms. Using properties from the Cloudsat radar and MODIS, we show that radiative transfer calculations support the following: (1) The MLER model is adequate for single-layer optically thick, geometrically thin clouds, but can produce significant errors in estimated cloud pressure for optically thin clouds. (2) In a two-layer cloud, the RRS algorithm may retrieve a cloud pressure that is either between the two cloud decks or even beneath the top of the lower cloud deck because of scattering between the cloud layers; the retrieved pressure depends upon the viewing geometry and the optical depth of the upper cloud deck. (3) Absorbing aerosol in and above a cloud can produce significant errors in the retrieved cloud pressure. (4) The retrieved RRS effective pressure for a deep convective cloud will be significantly higher than the physical cloud top pressure derived with thermal IR.
Effects of quantum mechanical interferences on third-order susceptibilities in molecules are studied. First principle calculations for molecular hydrogen are presented and shown to agree with results derived from experimental stimulated Raman gain and spontaneous Raman cross-section data. 10 percent third-harmonic conversion efficiency in H2 at 1 atm without phase matching should require a 150 MW per sq cm at 4.81 microns. As little as 5.9-MW power is sufficient when the beam is properly focused. Resonance Raman scattering (RRS) is proposed for experimentally investigating the interference effects, which tend to reduce the strength of third-order nonlinear susceptibilities.
Researchers from NASA Glenn Research Center s Combustion Branch and the Ohio Aerospace Institute (OAI) have developed a transferable calibration standard for an optical technique called spontaneous Raman scattering (SRS) in high-pressure flames. SRS is perhaps the only technique that provides spatially and temporally resolved, simultaneous multiscalar measurements in turbulent flames. Such measurements are critical for the validation of numerical models of combustion. This study has been a combined experimental and theoretical effort to develop a spectral calibration database for multiscalar diagnostics using SRS in high-pressure flames. However, in the past such measurements have used a one-of-a-kind experimental setup and a setup-dependent calibration procedure to empirically account for spectral interferences, or crosstalk, among the major species of interest. Such calibration procedures, being non-transferable, are prohibitively expensive to duplicate. A goal of this effort is to provide an SRS calibration database using transferable standards that can be implemented widely by other researchers for both atmospheric-pressure and high-pressure (less than 30 atm) SRS studies. A secondary goal of this effort is to provide quantitative multiscalar diagnostics in high pressure environments to validate computational combustion codes.
Goal of sensor-development program to measure concentrations as low as few parts per billion in continuous monitoring as well as peak concentrations up to hundreds of parts per million, such as encountered near leaks. Sensors based on Raman scattering from hydrazine or monomethyl hydrazine adsorbed on roughened metal or metal oxide substrates. Similar systems developed to detect nitrogen oxides and other gases.
Reliable cloud pressure estimates are needed for accurate retrieval of ozone and other trace gases using satellite-borne backscatter ultraviolet (buv) instruments such as the global ozone monitoring experiment (GOME). Cloud pressure can be derived from buv instruments by utilizing the properties of rotational-Raman scattering (RRS) and absorption by O2-O2. In this paper we estimate cloud pressure from GOME observations in the 355-400 nm spectral range using the concept of a Lambertian-equivalent reflectivity (LER) surface. GOME has full spectral coverage in this range at relatively high spectral resolution with a very high signal-to-noise ratio. This allows for much more accurate estimates of cloud pressure than were possible with its predecessors SBUV and TOMS. We also demonstrate the potential capability to retrieve chlorophyll content with full-spectral buv instruments. We compare our retrieved LER cloud pressure with cloud top pressures derived from the infrared ATSR instrument on the same satellite. The findings confirm results from previous studies that showed retrieved LER cloud pressures from buv observations are systematically higher than IR-derived cloud-top pressure. Simulations using Mie-scattering radiative transfer algorithms that include O2-O2 absorption and RRS show that these differences can be explained by increased photon path length within and below cloud.
The OMI cloud pressure product is necessary for accounting for cloud effects on the mission- critical total ozone product. One of the OM1 cloud pressure algorithms uses UV measurements to derive cloud pressures from the high frequency structure of top- of-atmosphere reflectance caused by rotational Raman scattering (RRS) in the atmosphere. RRS results in filling-in of Fraunhofer lines in the backscatter UV spectra (also known as the Ring effect). The magnitude of filling-in of the Fraunhofer lines is roughly proportional to the average number of solar photon scatterings in the atmosphere above the clouds. This property of RRS is used to deduce an effective cloud pressure. The cloud pressure algorithm retrieves the cloud pressure and cloud fraction using a concept of the Mixed Lambert Equivalent Reflectivity (MLER) also used for the TOMS-V8 OM1 total column ozone algorithm. Currently, this OMI total column ozone algorithm utilizes information about cloud top pressures from a climatology based on IR measurements. The IR-derived cloud top pressure is known to be lower than UV-derived cloud top pressure because UV radiation penetrates clouds deeper than IR radiation. That is why the UV-derived cloud pressure may be more consistent withthe total ozone algorithm. We estimate total column ozone differences caused by replacing the cloud pressure climatology with cloud pressures retrieved from GOME data same as used for retrieval of ozone.
The higher spectral resolution, coverage, and sampling of the Aura satellite ozone monitoring instrument (OMI), as compared with the total ozone mapping spectrometer (TOMS) should allow for improved ozone retrievals, including estimates of tropospheric ozone. By default, the TOMS-like OMI total column ozone algorithm uses climatological cloud-top pressures based on infrared (IR) measurements to estimate the column ozone below the clouds. Alternatively, cloud pressure can be retrieved using atmospheric rotational Raman scattering with OMI. The retrieved cloud pressures should be more consistent with assumptions made in the total ozone algorithm. Here, we use data from the global ozone monitoring experiment (GOME) to estimate total ozone using both the IR-climatological and retrieved cloud pressures. The exceed approximately 15 DU. Use of the UV cloud pressure retrievals leads to a smoother distribution of ozone along a satellite track by reducing small spatial irregularities presumably caused by errors in the climatological cloud pressures.
This paper uses Mie theory to treat electromagnetic scattering and to evaluate field enhancement in the forward direction of a small droplet irradiated by a high-energy beam and compares the results of calculations with the field-enhancement evaluation obtained via geometrical optics treatment. Results of this comparison suggest that the field enhancement located at the critical ring region encircling the axis in the forward direction of the droplet can support laser-induced Raman scattering. The results are supported by experimental observations of the interaction of a 120-micron-diam water droplet with a high-energy Nd:YAG laser beam.
Light scattering measurements of the Raman active modes of vibration in the range from 10 to 4000 per cm are reported for the paraelectric phase of NH4H2AsO4 in the temperature range from 220 to 295 K. Through examination of these spectra the protonic, transverse optic, internal, and O-H-O valence vibrations are identified, their symmetries are determined.
A theoretical model for the Raman rotational spectrum of air was formulated, yielding the spectral temperature dependence; and an error analysis of temperature measurement accuracies was performed. The theoretical spectra and the predicted temperature measurement error of + or - 20 K (7 percent) compared well with experimental data. These experimental data consisted of Raman spectra of air obtained for temperatures ranging from 243 to 313 K at a pressure of 1 atmosphere. The use of selected lines resulted in an experimental accuracy of + or - 13 K (-5 percent).
Raman backscatter of frequency doubled ruby laser beam by water vapor in atmosphere observed by optical radar, calculating water vapor mixing ratio profile
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Raman spectra of ZnO and Co substituted Zn1-xCoxO (ZCO) were carried out using the Raman microprobe system with an p.,+ ion laser source of 514.5 nm wavelength. The shift towards the lower frequency side of the nonpolar E210w mode and the broadening due to Co substitution in ZnO were analyzed using the phonon confinement model. The magnetic measurements showed ferromagnetic behavior with the maximum saturation magnetization (1.2micron Beta/ErCo) for 10% Co substitution, which decreased wi th at further increase in Co concentrations. The intensities of E1(LO) at 584 cm-1 and multiphonon modes at 540 cm-1 were increased with an increase in Co substitution. The additional Raman modes in ceramic targets of ZCO spectra for higher concentration of Co substitution (x=15%-20%) were identified to be due to the spinel ZnCo2O4 secondary phase.
The solutions for the imaginary susceptibility of the Raman field transition with arbitrary relaxation rates and field strengths are examined for differing sets of relaxation rates with emphasis on alkali metal vapors which have spontaneous emission dominated relaxation. The model is further expanded to include Doppler broadening and used to predict the peak gain as a function of detuning for a frequency doubled alexandrite laser-pumped cesium vapor gain cell.