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At least 469 records · Page 26

In-SITU Raman Spectroscopy of Single Microparticle Li-Intercalation Electrodes

Modifications in the vibrational properties of a single microparticle of LiMn2O4 induced by extraction and subsequent injection of Li(+) into the lattice have been monitored in situ via simultaneous acquisition of Raman scattering spectra and cyclic voltammetry data in 1M LiC1O4 solutions in ethylene carbonate (EC):diethyl carbonate (DEC) mixtures (1:1 by volume). Statistical analyses of the spectra in the range 15 < SOD < 45%, where SOD represents the state of discharge (in percent) of the nominally fully charged material, i.e. lambda-MnO2, were found to be consistent with the coexistence of two distinct phases of lithiated metal oxide in agreement with information derived from in situ X-ray diffraction (XRD) measurements involving more conventional battery-type electrodes.

Dokko, Kaoru↗

Retrieval Studies with LIDORT

This short program of LIDORT-based research in atmospheric trace gas retrieval was conducted over the 1 year period 01 July 2002 to 30 June 2003. After consultation with the NASA reporting officer, the first of the two original proposal activities (development of a direct-fitting total O3 column retrieval algorithm with operational capability for GOME data) was replaced by other tasks. The three activities addressed were: (1) Sensitivity studies for column and profile retrieval of NO2 distributions from a new generation of multi-axis ground-based spectrometers; (2) use of the LIDORT-RRS model to determine the effect of inelastic rotational Raman scattering at SBUV wavelengths; (3) an examination of ozone profile weighting functions in the presence of optically thick tropospheric clouds.

Bhartia, P. K.↗

Spectroscopy-Based Characterization of Single Wall Carbon Nanotubes

We present the initial results of our combined investigation of Raman scattering and optical absorption spectroscopy in a batch of single wall carbon nanotubes (SWNTs). The SWNT diameters are first estimated from the four radial breathing mode (RBM) peaks using a simple relation of omega(sub RBM) = 248/cm nm/d(sub t)(nm). The calculated diameter values are related to the optical absorption peaks through the expressions of first interband transition energies, i.e., E(sup S)(sub 11) = 2a gamma/d(sub t) for semiconducting and E(sup S)(sub 11) = 6a gamma/d(sub t) for metallic SWNTs, respectively, where a is the carbon-carbon bond length (0.144 nm) and gamma is the energy of overlapping electrons from nearest neighbor atoms, which is 2.9 eV for a SWNT. This analysis indicates that three RBM peaks are from semiconducting tubes, and the remaining one is from metallic tubes. The detailed analysis in the present study is focused on these three peaks of the first absorption band by determining the values of the representative (n,m) pairs. The first step of analysis is to construct a list of possible (n,m) pairs from the diameters calculated from the positions of the RBM peaks. The second step is to compute the first interband transition energy, E(sub 11), by substituting the constructed list of (n,m) into the expression of Reich and Thomsen, and Saito et al. Finally, the pairs with the energies closest to the experimental values are selected.

Namkung, Min↗

Development of a High-Pressure Gaseous Burner for Calibrating Optical Diagnostic Techniques

In this work-in-progress report, we show the development of a unique high-pressure burner facility (up to 60 atm) that provides steady, reproducible premixed flames with high precision, while having the capability to use multiple fuel/oxidizer combinations. The highpressure facility has four optical access ports for applying different laser diagnostic techniques and will provide a standard reference flame for the development of a spectroscopic database in high-pressure/temperature conditions. Spontaneous Raman scattering (SRS) was the first diagnostic applied, and was used to successfully probe premixed hydrogen-air flames generated in the facility using a novel multi-jet micro-premixed array burner element. The SRS spectral data include contributions from H2, N2, O2, and H2O and were collected over a wide range of equivalence ratios ranging from 0.16 to 4.9 at an initial pressure of 10-atm via a spatially resolved point SRS measurement with a high-performance optical system. Temperatures in fuel-lean to stoichiometric conditions were determined from the ratio of the Stokes to anti-Stokes scattering of the Q-branch of N2, and those in fuel-rich conditions via the rotational temperature of H2. The SRS derived temperatures using both techniques were consistent and indicated that the flame temperature was approximately 500 K below that predicted by adiabatic equilibrium, indicating a large amount of heat-loss at the measurement zone. The integrated vibrational SRS signals show that SRS provides quantitative number density data in high-pressure H2-air flames.

Kojima, Jun↗

A Hardened CARS System Utilized for Temperature Measurements in a Supersonic Combustor

A coherent anti-Stokes Raman scattering (CARS) system has been hardened for use in a NASA Langley supersonic combustion test cell. The system can obtain temperature cross sections of the flow at three locations. The system is environmentally protected and remotely operated. Measurements were made in a scram-jet combustor model consisting of a rear- ward-facing step, followed by an expansion duct. The duct is nominally 4 feet in length. The free stream conditions were Mach 2, with static pressure which ranged from 0.8 to 1.9 atm, and a static temperature of approximately 800K. Three vertical slots were machined into each side of the duct to allow optical access. The CARS system utilized a planar BOXCARS beam arrangement. This arrangement allowed the laser beams to pass through the vertical slots in the tunnel. Translation stages were utilized to move the focussing volume within the tunnel. These stages allowed complete cross sections to be obtained at each slot location. A fiber optic carried the signal to a remotely located monochrometer and reticon detector.Data for two different flow conditions were taken at each of the three slot locations. These two conditions provided a comparison between reacting and non-reacting mixing of injected hydrogen fuel with the combustion heated supersonic stream.

Antcliff, Richard R.↗

Computational and Experimental Study of Energetic Materials in a Counterflow Microgravity Environment

Counterflow diffusion flames are studied for various fuels flowing against decomposition products from solid ammonium perchlorate (AP) pellets in order to obtain fundamental understanding of composite propellant flame structure and chemistry. We illustrate this approach through a combined experimental and numerical study of a fuel mixture consisting of C2H4 CO + H2, and C2H2 + C2H4 flowing against solid AP. For these particular AP-fuel systems, the resulting flame zone simulates the various flame structures that are ex+ to exist between reaction products from Ap crystals and a hydrocarbon binder. As in all our experimental studies, quantitative species and temperature profiles have been measured between the fuel exit and AP surface. Species measured included CN, NH, NO, OH, N2, CO2, CO, H2, CO, HCl, and H2O. Temperature was measured using a thermocouple at the exit, spontaneous Raman scattering measurements throughout the flame, OH rotational population distributions, and NO vibrational population distributions. The burning rate of AP was also measured as a function of strain rate, given by the separation distance between the AP surface and the gaseous hydrocarbon fuel tube exit plane. This distance was nominally set at 5 mm, although studies have been performed for variations in separation distance. The measured 12 scalars are compared with predictions from a detailed gas-phase kinetics model consisting of 86 species and 531 reactions. Model predictions are found to be in good agreement with experiment and illustrate the type of kinetic features that may be expected to occur in propellants when AP particle size distributions are varied. Furthermore, the results constitute the continued development of a necessary database and validation of a comprehensive model for studying more complex AP-solid fuel systems in microgravity. Exploratory studies have also been performed with liquid and solid fuels at normal gravity. Because of melting (and hence dripping) and deep thermal wave penetration into the liquid, these experiments were found feasible, but not used for obtaining quantitative data. Microgravity experiments are needed to eliminate the dripping and boiling phenomena of these systems at normal gravity. Microgravity tests in the NASA Glenn 2.2 second drop tower were performed (1) to demonstrate the feasibility of performing propellant experiments using the NASA Glenn microgravity facilities, (2) to develop the operational procedures for safe handing of the energetic materials and disposal of their toxic combustion by-products and (3) to obtain initial measurements of the AP burning rate and flame structure under microgravity conditions. Experiments were conducted on the CH4/AP system previously studied at normal gravity using a modified design of the counterflow burner and a NASA Glenn Pig Rig, i.e., one of the existing drop rigs for general-purpose usage. In these experiments, the AP burning rate was measured directly with a linear variable differential transducer (LVDT) and video imaging of the flame structure was recorded ignition was achieved by hot wires stretched across the AP surfaces. Initial drop tower combustion data show that with the same burner separation distance and flow conditions of the normal gravity experiments, the AP burning rate is approximately a factor of two lower. This difference is likely a result of radiation effects, but further tests with longer test times need to be conducted to verify that steady state conditions were achieved under microgravity conditions.

Takahashi, Fumiaki↗

Observations over Hurricanes from the Ozone Monitoring Instrument

There is an apparent inconsistency between the total column ozone derived from the total ozone mapping spectrometer (TOMS) and aircraft observations within the eye region of tropical cyclones. The higher spectral resolution, coverage, and sampling of the ozone monitoring instrument (OMI) on NASA s Aura satellite as compared with TOMS allows for improved ozone retrievals by including estimates of cloud pressure derived simultaneously using the effects of rotational Raman scattering. The retrieved cloud pressures from OM1 are more appropriate than the climatological cloud-top pressures based on infrared measurements used in the TOMS and initial OM1 algorithms. We find that total ozone within the eye of hurricane Katrina is significantly overestimated when we use climatological cloud pressures. Using OMI-retrieved cloud pressures, total ozone in the eye is similar to that in the surrounding area. The corrected total ozone is in better agreement with aircraft measurements that imply relatively small or negligible amounts of stratospheric intrusion into the eye region of tropical cyclones.

Joiner, J.↗

Cascaded Photoenhancement: Implications for Photonic Chemical and Biological Sensors

Our analysis shows that coupling of gold nanoparticles to microspheres will evoke a cascading effect from the respective photoenhancement mechanisms. We refer to this amplification process as cascaded photoenhancement, and the resulting cavity amplification of surface-enhanced Raman scattering (SERS) and fluorescence as CASERS and CAF, respectively. Calculations, based on modal analysis of scattering and absorption by compound spheres, presented herein indicate that the absorption cross sections of metal nanoparticles immobilized onto dielectric microspheres can be greatly enhanced by cavity resonances in the microspheres without significant degradation of the resonators. Gain factors associated with CSP of 10(exp 3) - 10(exp 4) are predicted for realistic experimental conditions using homogenous microspheres. Cascaded surface photoenhancement thus has the potential of dramatically increasing the sensitivities of fluorescence and vibrational spectroscopies.

Fuller, Kirk A.↗

Fiber Optic Raman Sensor to Monitor Concentration Ratio of Nitrogen and Oxygen in a Cryogenic Mixture

A spontaneous Raman scattering optical fiber sensor is developed for a specific need of NASA/SSC for long-term detection and monitoring of the quality of liquid oxygen (LOX) in the delivery line during ground testing of rocket engines. The sensor performance was tested in the laboratory and with different excitation light sources. To evaluate the sensor performance with different excitation light sources for the LOX quality application, we have used the various mixtures of liquid oxygen and liquid nitrogen as samples. The study of the sensor performance shows that this sensor offers a great deal of flexibility and provides a cost effective solution for the application. However, an improved system response time is needed for the real-time, quantitative monitoring of the quality of cryogenic fluids in harsh environment.

Tiwari, Vidhu S.↗

Three Way Comparison between Two OMI/Aura and One POLDER/PARASOL Cloud Pressure Products

The cloud pressures determined by three different algorithms, operating on reflectances measured by two space-borne instruments in the "A" train, are compared with each other. The retrieval algorithms are based on absorption in the oxygen A-band near 760 nm, absorption by a collision induced absorption in oxygen near 477nm, and the filling in of Fraunhofer lines by rotational Raman scattering. The first algorithm operates on data collected by the POLDER instrument on board PARASOL, while the latter two operate on data from the OMI instrument on board Aura. The satellites sample the same air mass within about 15 minutes. Using one month of data, the cloud pressures from the three algorithms are found to show a similar behavior, with correlation coefficients larger than 0.85 between the data sets for thick clouds. The average differences in the cloud pressure are also small, between 2 and 45 hPa, for the whole data set. For optically thin to medium thick clouds, the cloud pressure the distribution found by POLDER is very similar to that found by OMI using the O2 - O2 absorption. Somewhat larger differences are found for very thick clouds, and we hypothesise that the strong absorption in the oxygen A-band causes the POLDER instrument to retrieve lower pressures for those scenes.

Sneep, M.↗

Single-Shot Scalar-Triplet Measurements in High-Pressure Swirl-Stabilized Flames for Combustion Code Validation

In support of NASA ARMD's code validation project, we have made significant progress by providing the first quantitative single-shot multi-scalar data from a turbulent elevated-pressure (5 atm), swirl-stabilized, lean direct injection (LDI) type research burner operating on CH4-air using a spatially-resolved pulsed-laser spontaneous Raman diagnostic technique. The Raman diagnostics apparatus and data analysis that we present here were developed over the past 6 years at Glenn Research Center. From the Raman scattering data, we produce spatially-mapped probability density functions (PDFs) of the instantaneous temperature, determined using a newly developed low-resolution effective rotational bandwidth (ERB) technique. The measured 3-scalar (triplet) correlations, between temperature, CH4, and O2 concentrations, as well as their PDF s, also provide a high-level of detail into the nature and extent of the turbulent mixing process and its impact on chemical reactions in a realistic gas turbine injector flame at elevated pressures. The multi-scalar triplet data set presented here provides a good validation case for CFD combustion codes to simulate by providing both average and statistical values for the 3 measured scalars.

Kojima, Jun↗

Dual-Pump CARS Temperature and Species Concentration Measurements in a Supersonic Combustor

The dual-pump coherent anti-Stokes Raman scattering (CARS) method was used to measure temperature and the mole fractions of N2 and O2 in a supersonic combustor. Experiments were conducted in NASA Langley Research Center s Direct Connect Supersonic Combustion Test Facility. In this facility, H2 and oxygen-enriched air burn to increase the enthalpy of the simulated air test gas. This gas is expanded through a Mach 2 nozzle and into a combustor model consisting of a short constant-area section followed by a small rearward-facing step and another constant-area section. At the end of this straight section, H2 fuel is injected at Mach 2 and at a 30 angle with respect to the freestream. One wall of the duct then expands at a 3 angle for over 1 meter. The ensuing combustion is probed optically through ports in the side of the combustor. Dual-pump CARS measurements were performed at the facility nozzle exit and at four planes downstream of fuel injection. Maps are presented of the mean temperature, as well as N2 and O2 mean mole fraction fields. Correlations between fluctuations of the different measured parameters are also presented.

O'Byrne, S.↗

Focal-Plane Imaging of Crossed Beams in Nonlinear Optics Experiments

An application of focal-plane imaging that can be used as a real time diagnostic of beam crossing in various optical techniques is reported. We discuss two specific versions and demonstrate the capability of maximizing system performance with an example in a combined dual-pump coherent anti-Stokes Raman scattering interferometric Rayleigh scattering experiment (CARS-IRS). We find that this imaging diagnostic significantly reduces beam alignment time and loss of CARS-IRS signals due to inadvertent misalignments.

Bivolaru, Daniel↗

Absorption in Extended Inhomogeneous Clouds

The launch of several different sensors, including CloudSat, into the A-train constellation of satellites allows us for the first time to compute absorption that can occur in realistic vertically inhomogeneous clouds including multiple cloud decks. CloudSat data show that these situations are common. Therefore, understanding vertically inhomogeneous clouds is important from both climate and satellite atmospheric composition remote sensing perspectives. Satellite passive sensors that operate from the near IR to the UV often rely on radiative cloud pressures derived from absorption in oxygen bands (A, B, gamma, or O2-O2 bands) or from rotational-Raman scattering in order to retrieve information about atmospheric trace gases. The radiative cloud pressure is distinct from the physical cloud top derived from thermal infrared measurements. Therefore, the combination of information from different passive sensors yields some information about the cloud vertical profile. When either or both the clouds or atmospheric absorbers (trace gases and aerosols) are vertically inhomogeneous, the use of an effective cloud pressure derived from these approaches may lead to errors. Here, we focus on several scenarios (deep convective clouds and distinct two layer clouds) based on realistic cloud optical depth vertical profiles derived from the CloudSatfMODIS combination. We focus on implications for trace-gas column amount retrievals (specifically ozone and NO2) and derived surface UV irradiance from the Ozone Monitoring Instrument (OMI) on the Atrain Aura platform.

Joiner, Joanna↗

Phase Matching of Diverse Modes in a WGM Resonator

Phase matching of diverse electromagnetic modes (specifically, coexisting optical and microwave modes) in a whispering-gallery-mode (WGM) resonator has been predicted theoretically and verified experimentally. Such phase matching is necessary for storage of microwave/terahertz and optical electromagnetic energy in the same resonator, as needed for exploitation of nonlinear optical phenomena. WGM resonators are used in research on nonlinear optical phenomena at low optical intensities and as a basis for design and fabrication of novel optical devices. Examples of nonlinear optical phenomena recently demonstrated in WGM resonators include low-threshold Raman lasing, optomechanical oscillations, frequency doubling, and hyperparametric oscillations. The present findings regarding phase matching were made in research on low-threshold, strongly nondegenerate parametric oscillations in lithium niobate WGM resonators. The principle of operation of such an oscillator is rooted in two previously observed phenomena: (1) stimulated Raman scattering by polaritons in lithium niobate and (2) phase matching of nonlinear optical processes via geometrical confinement of light. The oscillator is partly similar to terahertz oscillators based on lithium niobate crystals, the key difference being that a novel geometrical configuration of this oscillator supports oscillation in the regime. The high resonance quality factors (Q values) typical of WGM resonators make it possible to achieve oscillation at a threshold signal level much lower than that in a non-WGM-resonator lithium niobate crystal.

Savchenkov, Anatoliy↗

Determination of Probe Volume Dimensions in Coherent Measurement Techniques

When investigating combustion phenomena with pump-probe techniques, the spatial resolution is given by the overlapping region of the laser beams and thus defines the probe volume size. The size of this probe volume becomes important when the length scales of interest are on the same order or smaller. In this work, we present a new approach to measure the probe volume in three dimensions (3-D), which can be used to determine the probe volume length, diameter, and shape. The optical arrangement and data evaluation are demonstrated for a dual-pump dual-broadband coherent anti-Stokes Raman scattering (CARS) setup which is used for combustion diagnostics. This new approach offers a simple, quick alternative with more capabilities than formerly used probe volume measurement methods.

Tedder, Sarah A.↗

Advanced Laser Based Measurements in Porous Media Combustion

We present measurements using dual-pump dual-broadband coherent anti-Stokes Raman scattering spectroscopy (DP-DBB-CARS) inside a porous media burner. This work continues our previous measurements in such combustion systems. The existing setup was significantly modified with the aim of providing improved data quality and data rate, reduction of interferences and additional species information. These changes are presented and discussed in detail. The CARS technique was expanded to a dual-pump dual-broadband CARS system which in principle enables acquisition of temperatures together with relative H2/N2- and O2/N2- species concentrations. Experimental complexity was reduced by the use of a modified spectrometer enabling the detection of both signals, vibrational and rotational CARS, with only one detection system.

Tedder, Sarah A.↗

Nanostructures Exploit Hybrid-Polariton Resonances

Nanostructured devices that exploit the hybrid-polariton resonances arising from coupling among photons, phonons, and plasmons are subjects of research directed toward the development of infrared-spectroscopic sensors for measuring extremely small quantities of molecules of interest. The spectroscopic techniques in question are surface enhanced Raman scattering (SERS) and surface enhanced infrared absorption (SEIRA). An important intermediate goal of this research is to increase the sensitivity achievable by these techniques. The basic idea of the approach being followed in this research is to engineer nanostructured devices and thereby engineer their hybrid-polariton resonances to concentrate infrared radiation incident upon their surfaces in such a manner as to increase the absorption of the radiation for SEIRA and measure the frequency shifts of surface vibrational modes. The underlying hybrid-polariton-resonance concept is best described by reference to experimental devices that have been built and tested to demonstrate the concept. The nanostructure of each such device includes a matrix of silicon carbide particles of approximately 1 micron in diameter that are supported on a potassium bromide (KBr) or poly(tetrafluoroethylene) [PTFE] window. These grains are sputter-coated with gold grains of 40-nm size (see figure). From the perspective of classical electrodynamics, in this nanostructure, that includes a particulate or otherwise rough surface, the electric-field portion of an incident electromagnetic field becomes concentrated on the particles when optical resonance conditions are met. Going beyond the perspective of classical electrodynamics, it can be seen that when the resonance frequencies of surface phonons and surface plasmons overlap, the coupling of the resonances gives rise to an enhanced radiation-absorption or -scattering mechanism. The sizes, shapes, and aggregation of the particles determine the frequencies of the resonances. Hence, the task of designing a nanostructure to exhibit the desired radiation-absorption properties translates, in large part, to selecting particle sizes and shapes to obtain the desired enhanced coupling of energy from photons to plasmons and phonons. To broaden the spectral region(s) of enhanced absorption, one would select a distribution of particle sizes and shapes.

Anderson, Mark↗