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NASA NTRS2003

Composition Dependence of the Hydrostatic Pressure Coefficients of the Bandgap of ZnSe(1-x)Te(x) Alloys

Optical absorption experiments have been performed using diamond anvil cells to measure the hydrostatic pressure dependence of the fundamental bandgap of ZnSe(sub 1-xTe(sub x) alloys over the entire composition range. The first and second-order pressure coefficients are obtained as a function of composition. Starting from the ZnSe side, the magnitude of both coefficients increases slowly until x approx. 0.7, where the ambient-pressure bandgap reaches a minimum. For larger values of x the coefficients rapidly approach the values of ZnTe. The large deviations of the pressure coefficients from the linear interpolation between ZnSe and ZnTe are explained in terms of the band anticrossing model.

Wu, J.↗
NASA NTRS2003

[Activities of Texas University]

All the principal investigator's current projects investigate aspects of radio-loud, radio-quiet, BAL QSOs, and buried (IRAS-selected) QSOs and the relationships among these different classes, with the aim of probing the nature of accretion onto the massive central black hole - via relativistic jets, X-ray and optical absorption outflows, and the kinematics of the surrounding gas whose emission lines are excited by the accretion continuum.

Oliversen, R.↗
NASA NTRS2003

GOME Total Ozone and Calibration Error Derived Usign Version 8 TOMS Algorithm

The Global Ozone Monitoring Experiment (GOME) is a hyper-spectral satellite instrument measuring the ultraviolet backscatter at relatively high spectral resolution. GOME radiances have been slit averaged to emulate measurements of the Total Ozone Mapping Spectrometer (TOMS) made at discrete wavelengths and processed using the new TOMS Version 8 Ozone Algorithm. Compared to Differential Optical Absorption Spectroscopy (DOAS) techniques based on local structure in the Huggins Bands, the TOMS uses differential absorption between a pair of wavelengths including the local stiucture as well as the background continuum. This makes the TOMS Algorithm more sensitive to ozone, but it also makes the algorithm more sensitive to instrument calibration errors. While calibration adjustments are not needed for the fitting techniques like the DOAS employed in GOME algorithms, some adjustment is necessary when applying the TOMS Algorithm to GOME. Using spectral discrimination at near ultraviolet wavelength channels unabsorbed by ozone, the GOME wavelength dependent calibration drift is estimated and then checked using pair justification. In addition, the day one calibration offset is estimated based on the residuals of the Version 8 TOMS Algorithm. The estimated drift in the 2b detector of GOME is small through the first four years and then increases rapidly to +5% in normalized radiance at 331 nm relative to 385 nm by mid 2000. The lb detector appears to be quite well behaved throughout this time period.

Gleason, J.↗
NASA NTRS2003

Total Ozone from the Ozone Monitoring System (OMI) using TOMS and DOAS Methods

The Ozone Monitoring Instrument (OMI) is the Dutch-Finnish contribution to NASA's EOS-Aura satellite scheduled for launch in January 2004. OMI is an imaging spectrometer that will measure the back-scattered Solar radiance in the wavelength range of 270 to 500 nm. The instrument provides near global coverage in one day with a spatial resolution of 13x24 square kilometers. OMI is a new instrument, with a heritage from TOMS, SBW, GOME, GOMOS and SCIAMACHY. OMI'S unique capabilities for measuring important trace gases and aerosols with a small footprint and daily global coverage, in conjunction with the other Aura instruments, will make a major contribution to our understanding of stratospheric and tropospheric chemistry and climate change. OMI will provide data continuity with the 23-year ozone record of TOMS. There are three ozone products planned for OMI: total column ozone, ozone profile and tropospheric column ozone. We are developing two different algorithms for total column ozone: one similar to the algorithm currently being used to process the TOMS data, and the other an improved version of the differential optical absorption spectroscopy (DOAS) method, which has been applied to GOME and SCIAMACHY data. The main reasons for starting with two algorithms for total ozone have to do with heritage and past experience; our long-term goal is to combine the two to develop a more accurate and reliable total ozone product for OMI. We will compare the performance of these two algorithms by applying both of them to the GOME data. We will examine where and how the results differ, and use the extensive TOMS-Dobson comparison studies to assess the performance of the DOAS algorithm.

Veefkind, J. P.↗
NASA NTRS2003

Retrieval and Analysis of Stratospheric NO2 from GOME

In this paper we describe the retrieval of stratospheric NO2 from the GOME (Global Ozone Monitoring Experiment) spectrometer. For this retrieval the Differential Optical Absorption Spectroscopy (DOAS) is used and we describe the influence of the instrument s characteristics on this measurement technique. This analysis led to an improved version of the DOAS algorithm resulting in results with lower systematic errors. Subsequently these results were used to separate the tropospheric and stratospheric fraction of the measured NO;! in the atmosphere. This paper is focusing on the annual variations of the stratospheric distribution of nitrogen oxides. For this examination the satellite data from beginning of 1996 to the end of 2001 was used and has been visualized in a plot zonal means versus time of the year, a visualization which proved to be very useful for Ozone. Additionally the so called "Noxon Cliff", a drop of NO2 column densities Noxon measured in 1975-77 while traveling northwards towards the pole in Canada, is shown. Also its southern equivalent could be discovered in the GOME data.

Wenig, M.↗
NASA NTRS2003

Quantitative Species Measurements In Microgravity Combustion Flames

The capability of models and theories to accurately predict and describe the behavior of low gravity flames can only be verified by quantitative measurements. Although video imaging, simple temperature measurements, and velocimetry methods have provided useful information in many cases, there is still a need for quantitative species measurements. Over the past decade, we have been developing high sensitivity optical absorption techniques to permit in situ, non-intrusive, absolute concentration measurements for both major and minor flames species using diode lasers. This work has helped to establish wavelength modulation spectroscopy (WMS) as an important method for species detection within the restrictions of microgravity-based measurements. More recently, in collaboration with Prof. Dahm at the University of Michigan, a new methodology combining computed flame libraries with a single experimental measurement has allowed us to determine the concentration profiles for all species in a flame. This method, termed ITAC (Iterative Temperature with Assumed Chemistry) was demonstrated for a simple laminar nonpremixed methane-air flame at both 1-g and at 0-g in a vortex ring flame. In this paper, we report additional normal and microgravity experiments which further confirm the usefulness of this approach. We also present the development of a new type of laser. This is an external cavity diode laser (ECDL) which has the unique capability of high frequency modulation as well as a very wide tuning range. This will permit the detection of multiple species with one laser while using WMS detection.

Chen, Shin-Juh↗
NASA NTRS2004

Aerosol Absorption Effects in the TOMS UV Algorithm

The availability of global long-term estimates of surface UV radiation is very important, not only for preventive medicine considerations, but also as an important tool to monitor the effects of the stratospheric ozone recovery expected to occur in the next few decades as a result of the decline of the stratospheric chlorine levels. In addition to the modulating effects of ozone and clouds, aerosols also affect the levels of UV-A and W-B radiation reaching the surface. Oscillations in surface W associated with the effects of aerosol absorption may be comparable in magnitude to variations associated with the stratospheric ozone recovery. Thus, the accurate calculation of surface W radiation requires that both the scattering and absorption effects of tropospheric aerosols be taken into account. Although absorption effects of dust and elevated carbonaceous aerosols are already accounted for using Aerosol Index technique, this approach does not work for urban/industrial aerosols in the planetary boundary layer. The use of the new TOMS long-term global data record on UV aerosol absorption optical depth, can improve the accuracy of TOMS spectral UV products, by properly including the spectral attenuation effects of carbonaceous, urban/industrial and mineral aerosols. The TOMS data set on aerosol properties will be discussed, and results of its use in the TOMS surface W algorithm will be presented.

Torres, O.↗
NASA NTRS2003

Deposition of Nanostructured Thin Film from Size-Classified Nanoparticles

Materials comprising nanometer-sized grains (approximately 1_50 nm) exhibit properties dramatically different from those of their homogeneous and uniform counterparts. These properties vary with size, shape, and composition of nanoscale grains. Thus, nanoparticles may be used as building blocks to engineer tailor-made artificial materials with desired properties, such as non-linear optical absorption, tunable light emission, charge-storage behavior, selective catalytic activity, and countless other characteristics. This bottom-up engineering approach requires exquisite control over nanoparticle size, shape, and composition. We describe the design and characterization of an aerosol system conceived for the deposition of size classified nanoparticles whose performance is consistent with these strict demands. A nanoparticle aerosol is generated by laser ablation and sorted according to size using a differential mobility analyzer. Nanoparticles within a chosen window of sizes (e.g., (8.0 plus or minus 0.6) nm) are deposited electrostatically on a surface forming a film of the desired material. The system allows the assembly and engineering of thin films using size-classified nanoparticles as building blocks.

Camata, Renato P.↗
NASA NTRS1999

Water transport by the bacterial channel alpha-hemolysin

This study is an investigation of the ability of the bacterial channel alpha-hemolysin to facilitate water permeation across biological membranes. alpha-Hemolysin channels were incorporated into rabbit erythrocyte ghosts at varying concentrations, and water permeation was induced by mixing the ghosts with hypertonic sucrose solutions. The resulting volume decrease of the ghosts was followed by time-resolved optical absorption at pH 5, 6, and 7. The average single-channel permeability coefficient of alpha-hemolysin for water ranged between 1.3x10-12 cm/s and 1.5x10-12 cm/s, depending on pH. The slightly increased single-channel permeability coefficient at lower pH-values was attributed to an increase in the effective pore size. The activation energy of water transport through the channel was low (Ea=5.4 kcal/mol), suggesting that the properties of water inside the alpha-hemolysin channel resemble those of bulk water. This conclusion was supported by calculations based on macroscopic hydrodynamic laws of laminar water flow. Using the known three-dimensional structure of the channel, the calculations accurately predicted the rate of water flow through the channel. The latter finding also indicated that water permeation data can provide a good estimate of the pore size for large channels.

Non-NASA Center↗
NASA NTRS2006

Volume Ice Radiolysis in the Outer Solar System

The primary energy flux of charged particle components of the heliospheric and magnetospheric environments of the solar system is primarily carried by highly penetrating energetic particles. Although laboratory experiments on production of organics and oxidants typically only address effects on very thin surface layers, energy deposition occurs on surfaces of icy bodies of the outer solar system to meters in depth. Time scales for significant radiolytic deposition vary from thousands of years at millimeter depths on Europa to billions of years in the meters-deep regolith of Kuiper Belt Objects. Radioisotope decay (e.g., K-40) also contributes to volume radiolysis as the only energy source at much greater depths. Radiolytic oxygen is a potential resource for life within Europa and a partial source of oxygen for Saturn's magnetosphere and Titan's upper atmosphere. Interactions of very high energy cosmic rays with ices at Titan's surface may provide one of the few sources of oxidants in that highly reducing environment. The red colors of low-inclination classical Kuiper Belt Objects at 40-50 AU, and Centaur objects originating from this same population, may arise from volume radiolysis of deep ice layers below more refractory radiation crusts eroded away by surface sputtering and micrometeoroid impacts. A variety of techniques are potentially available to measure volume radiolysis products and have been proposed for study as part of the new Space Physics of Life initiative at NASA Goddard Space Flight Center. The technique of Electron Paramagnetic Resonance (EPR) has been used in medical studies to measure oxidant production in irradiated human tissue for cancer treatment. Other potential techniques include optical absorption spectroscopy and standard wet chemical analysis. These and other potential techniques are briefly reviewed for applicability to problems in solar system ice radiolysis and astrobiology.

Cooper, John F.↗
NASA NTRS2007

Nanorod-Based Fast-Response Pressure-Sensitive Paints

A proposed program of research and development would be devoted to exploitation of nanomaterials in pressuresensitive paints (PSPs), which are used on wind-tunnel models for mapping surface pressures associated with flow fields. Heretofore, some success has been achieved in measuring steady-state pressures by use of PSPs, but success in measuring temporally varying pressures has been elusive because of the inherent slowness of the optical responses of these materials. A PSP contains a dye that luminesces in a suitable wavelength range in response to photoexcitation in a shorter wavelength range. The luminescence is quenched by oxygen at a rate proportional to the partial pressure of oxygen and thus proportional to the pressure of air. As a result, the intensity of luminescence varies inversely with the pressure of air. The major problem in developing a PSP that could be easily applied to a wind-tunnel model and could be useful for measuring rapidly varying pressure is to provide very high gas diffusivity for rapid, easy transport of oxygen to and from active dye molecules. Most PSPs include polymer-base binders, which limit the penetration of oxygen to dye molecules, thereby reducing responses to pressure fluctuations. The proposed incorporation of nanomaterials (somewhat more specifically, nanorods) would result in paints having nanostructured surfaces that, relative to conventional PSP surfaces, would afford easier and more nearly complete access of oxygen molecules to dye molecules. One measure of greater access is effective surface area: For a typical PSP as proposed applied to a given solid surface, the nanometer-scale structural features would result in an exposed surface area more than 100 times that of a conventional PSP, and the mass of proposed PSP needed to cover the surface would be less than tenth of the mass of the conventional PSP. One aspect of the proposed development would be to synthesize nanorods of Si/SiO2, in both tangle-mat and regular- array forms, by use of chemical vapor deposition (CVD) and wet chemical processes, respectively. The rods would be coated with a PSP dye, and the resulting PSP signals would be compared with those obtained from PSP dye coats on conventional support materials. Another aspect of the proposed development would be to seek to exploit the quantum properties of nanorods of a suitable semiconductor (possibly GaN), which would be synthesized by CVD. These quantum properties of semiconductor nanorods include narrow-wavelength-band optical absorption and emission characteristics that vary with temperature. The temperature sensitivity might enable simultaneous measurement of fluctuating temperature and pressure and to provide a temperature correction for the PSP response.

Bencic, Timothy↗
NASA NTRS2006

Pattern-Recognition Algorithm for Locking Laser Frequency

A computer program serves as part of a feedback control system that locks the frequency of a laser to one of the spectral peaks of cesium atoms in an optical absorption cell. The system analyzes a saturation absorption spectrum to find a target peak and commands a laser-frequency-control circuit to minimize an error signal representing the difference between the laser frequency and the target peak. The program implements an algorithm consisting of the following steps: Acquire a saturation absorption signal while scanning the laser through the frequency range of interest. Condition the signal by use of convolution filtering. Detect peaks. Match the peaks in the signal to a pattern of known spectral peaks by use of a pattern-recognition algorithm. Add missing peaks. Tune the laser to the desired peak and thereafter lock onto this peak. Finding and locking onto the desired peak is a challenging problem, given that the saturation absorption signal includes noise and other spurious signal components; the problem is further complicated by nonlinearity and shifting of the voltage-to-frequency correspondence. The pattern-recognition algorithm, which is based on Hausdorff distance, is what enables the program to meet these challenges.

Karayan, Vahag↗
NASA NTRS2011

Using OMI Observations to Measure Aerosol Absorption of Biomass Burning Aerosols Above Clouds

The presence of absorbing aerosol layers above clouds is unambiguously detected by the TOMS/OMI UV Aerosol Index (AI) that uses satellite observations at two near-UV channels. A sensitivity study using radiative transfer calculations shows that the AI signal of resulting from the presence of aerosols above clouds is mainly driven by the aerosol absorption optical depth and the optical depth of the underlying cloud. Based on these results, an inversion algorithm has been developed to retrieve the aerosol optical depth (AOD) of aerosol layers above clouds. In this presentation we will discuss the sensitivity analysis, describe the retrieval approach, and present results of applications of the retrieval method to OMI observations over the South Atlantic Ocean. Preliminary error analyses, to be discussed, indicate that the AOD can be underestimated (up to -30%) or overestimated (up to 60%) depending on algorithmic assumptions.

Torres, Omar↗
NASA NTRS2013

Airborne MAX-DOAS Measurements Over California: Testing the NASA OMI Tropospheric NO2 Product

Airborne Multi-AXis Differential Optical Absorption Spectroscopy (AMAX-DOAS) measurements of NO2 tropospheric vertical columns were performed over California for two months in summer 2010. The observations are compared to the NASA Ozone Monitoring Instrument (OMI) tropospheric vertical columns (data product v2.1) in two ways: (1) Median data were compared for the whole time period for selected boxes, and the agreement was found to be fair (R = 0.97, slope = 1.4 +/- 0.1, N= 10). (2) A comparison was performed on the mean of coincident AMAX-DOAS measurements within the area of the corresponding OMI pixels with the tropospheric NASA OMI NO2 assigned to that pixel. The effects of different data filters were assessed. Excellent agreement and a strong correlation (R = 0.85, slope = 1.05 +/- 0.09, N= 56) was found for (2) when the data were filtered to eliminate large pixels near the edge of the OMI orbit, the cloud radiance fraction was<50%, the OMI overpass occurred within 2 h of the AMAX-DOAS measurements, the flight altitude was>2 km, and a representative sample of the footprint was taken by the AMAX-DOAS instrument. The AMAX-DOAS and OMI data sets both show a reduction of NO2 tropospheric columns on weekends by 38 +/- 24% and 33 +/- 11%, respectively. The assumptions in the tropospheric satellite air mass factor simulations were tested using independent measurements of surface albedo, aerosol extinction, and NO2 profiles for Los Angeles for July 2010 indicating an uncertainty of 12%.

remote sensing↗
NASA NTRS2015

Aircraft Measurements of BrO, IO, Glyoxal, NO2, H2O, O2-O2 and Aerosol Extinction Profiles in the Tropics: Comparison with Aircraft-/Ship-Based in Situ and Lidar Measurements

Tropospheric chemistry of halogens and organic carbon over tropical oceans modifies ozone and atmospheric aerosols, yet atmospheric models remain largely untested for lack of vertically resolved measurements of bromine monoxide (BrO), iodine monoxide (IO) and small oxygenated hydrocarbons like glyoxal (CHOCHO) in the tropical troposphere. BrO, IO, glyoxal, nitrogen dioxide (NO2), water vapor (H2O) and O2-O2 collision complexes (O4/ were measured by the University of Colorado Airborne Multi-AXis Differential Optical Absorption Spectroscopy (CU AMAXDOAS) instrument, aerosol extinction by high spectral resolution lidar (HSRL), in situ aerosol size distributions by an ultra high sensitivity aerosol spectrometer (UHSAS) and in situ H2O by vertical-cavity surface-emitting laser (VCSEL) hygrometer. Data are presented from two research flights (RF12, RF17) aboard the National Science Foundation/ National Center for Atmospheric Research Gulfstream V aircraft over the tropical Eastern Pacific Ocean (tEPO) as part of the "Tropical Ocean tRoposphere Exchange of Reactive halogens and Oxygenated hydrocarbons" (TORERO) project (January/February 2012). We assess the accuracy of O4 slant column density (SCD) measurements in the presence and absence of aerosols. Our O4-inferred aerosol extinction profiles at 477 nm agree within 6% with HSRL in the boundary layer and closely resemble the renormalized profile shape of Mie calculations constrained by UHSAS at low (sub-Rayleigh) aerosol extinction in the free troposphere. CU AMAX-DOAS provides a flexible choice of geometry, which we exploit to minimize the SCD in the reference spectrum (SCDREF, maximize signal-to-noise ratio) and to test the robustness of BrO, IO and glyoxal differential SCDs. The RF12 case study was conducted in pristine marine and free tropospheric air. The RF17 case study was conducted above the NOAA RV Ka'imimoana (TORERO cruise, KA-12-01) and provides independent validation data from ship-based in situ cavity-enhanced DOAS and MAX-DOAS. Inside the marine boundary layer (MBL) no BrO was detected (smaller than 0.5 pptv), and 0.2-0.55 pptv IO and 32-36 pptv glyoxal were observed. The near-surface concentrations agree within 30% (IO) and 10% (glyoxal) between ship and air-craft. The BrO concentration strongly increased with altitude to 3.0 pptv at 14.5 km (RF12, 9.1 to 8.6 deg N; 101.2 to 97.4 deg W). At 14.5 km, 5-10 pptv NO2 agree with model predictions and demonstrate good control over separating tropospheric from stratospheric absorbers (NO2 and BrO). Our profile retrievals have 12-20 degrees of freedom (DoF) and up to 500m vertical resolution. The tropospheric BrO vertical column density (VCD) was 1.5 x 10(exp 13) molec cm(exp -2) (RF12) and at least 0.5 x 10(exp 13) molec cm(exp -2) (RF17, 0- 10 km, lower limit). Tropospheric IO VCDs correspond to 2.1 x 10(exp 12) molec cm(exp -2) (RF12) and 2.5 x 10(exp 12) molec cm(exp -2) (RF17) and glyoxal VCDs of 2.6 x 10(exp 14) molec cm(exp -2) (RF12) and 2.7 x 10(exp 14) molec cm(exp -2) (RF17). Surprisingly, essentially all BrO as well as the dominant IO and glyoxal VCD fraction was located above 2 km (IO: 58 plus or minus 5 %, 0.1-0.2 pptv; glyoxal: 52 plus or minus 5 %, 3-20 pptv). To our knowledge there are no previous vertically resolved measurements of BrO and glyoxal from aircraft in the tropical free troposphere. The atmospheric implications are briefly discussed. Future studies are necessary to better understand the sources and impacts of free tropospheric halogens and oxygenated hydrocarbons on tropospheric ozone, aerosols, mercury oxidation and the oxidation capacity of the atmosphere.

Volkamer, R.↗
NASA NTRS2015

Using Single-Scattering Albedo Spectral Curvature to Characterize East Asian Aerosol Mixtures

Spectral dependence of aerosol single-scattering albedo (SSA) has been used to infer aerosol composition. In particular, aerosol mixtures dominated by dust absorption will have monotonically increasing SSA with wavelength while that dominated by black carbon absorption has monotonically decreasing SSA spectra. However, by analyzing SSA measured at four wavelengths, 440, 675, 870, and 1020 nm from the Aerosol Robotic Network data set, we find that the SSA spectra over East Asia are frequently peaked at 675 nm. In these cases, we suggest that SSA spectral curvature, defined as the negative of the second derivative of SSA as a function of wavelength, can provide additional information on the composition of these aerosol mixtures. Aerosol SSA spectral curvatures for East Asia during fall and winter are considerably larger than those found in places primarily dominated by biomass burning or dust aerosols. SSA curvature is found to increase as the SSA magnitude decreases. The curvature increases with coarse mode fraction (CMF) to a CMF value of about 0.4, then slightly decreases or remains constant at larger CMF. Mie calculations further verify that the strongest SSA curvature occurs at approx. 40% dust fraction, with 10% scattering aerosol fraction. The nonmonotonic SSA spectral dependence is likely associated with enhanced absorption in the shortwave by dust, absorption by black carbon at longer wavelengths, and also the flattened absorption optical depth spectral dependence due to the increased particle size.

curvature↗
NASA NTRS2015

Evaluating a New Homogeneous Total Ozone Climate Data Record from GOME/ERS-2, SCIAMACHY/Envisat, and GOME-2/MetOp-A

The European Space Agency's Ozone Climate Change Initiative (O3-CCI) project aims at producing and validating a number of high-quality ozone data products generated from different satellite sensors. For total ozone, the O3-CCI approach consists of minimizing sources of bias and systematic uncertainties by applying a common retrieval algorithm to all level 1 data sets, in order to enhance the consistency between the level 2 data sets from individual sensors. Here we present the evaluation of the total ozone products from the European sensors Global Ozone Monitoring Experiment (GOME)/ERS-2, SCIAMACHY/Envisat, and GOME-2/MetOp-A produced with the GOME-type Direct FITting (GODFIT) algorithm v3. Measurements from the three sensors span more than 16 years, from 1996 to 2012. In this work, we present the latest O3-CCI total ozone validation results using as reference ground-based measurements from Brewer and Dobson spectrophotometers archived at the World Ozone and UV Data Centre of the World Meteorological Organization as well as from UV-visible differential optical absorption spectroscopy (DOAS)/Système D′Analyse par Observations Zénithales (SAOZ) instruments from the Network for the Detection of Atmospheric Composition Change. In particular, we investigate possible dependencies in these new GODFIT v3 total ozone data sets with respect to latitude, season, solar zenith angle, and different cloud parameters, using the most adequate type of ground-based instrument. We show that these three O3-CCI total ozone data products behave very similarly and are less sensitive to instrumental degradation, mainly as a result of the new reflectance soft-calibration scheme. The mean bias to the ground-based observations is found to be within the 1 plus or minus 1 percent level for all three sensors while the near-zero decadal stability of the total ozone columns (TOCs) provided by the three European instruments falls well within the 1-3 percent requirement of the European Space Agency's Ozone Climate Change Initiative project.

Satellite sensors↗