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Characterization of Spectral Absorption Properties of Aerosols Using Satellite Observations

The wavelength-dependence of aerosol absorption optical depth (AAOD) is generally represented in terms of the Angstrom Absorption Exponent (AAE), a parameter that describes the dependence of AAOD with wavelength. The AAE parameter is closely related to aerosol composition. Black carbon (BC) containing aerosols yield AAE values near unity whereas Organic carbon (OC) aerosol particles are associated with values larger than 2. Even larger AAE values have been reported for desert dust aerosol particles. Knowledge of spectral AAOD is necessary for the calculation of direct radiative forcing effect of aerosols and for inferring aerosol composition. We have developed a satellitebased method of determining the spectral AAOD of absorbing aerosols. The technique uses high spectral resolution measurements of upwelling radiation from scenes where absorbing aerosols lie above clouds as indicated by the UV Aerosol Index. For those conditions, the satellite measured reflectance (rho lambda) is approximately given by Beer's law rho lambda = rho (sub 0 lambda) e (exp -mtau (sub abs lambda)) where rho(sub 0 lambda) is the cloud reflectance, m is the geometric slant path and tau (sub abs lambda) is the spectral AAOD. The rho (sub 0 lambda) term is determined by means of radiative transfer calculations using as input the cloud optical depth derived as described in Torres et al. [JAS, 2012] that accounts for the effects of aerosol absorption. In the second step, corrections for molecular and aerosol scattering effects are applied to the cloud reflectance term, and the spectral AAOD is then derived by inverting the equation above. The proposed technique will be discussed in detail and application results will be presented. The technique can be easily applied to hyper-spectral satellite measurements that include UV such as OMI, GOME and SCIAMACHY, or to multi-spectral visible measurements by other sensors provided that the aerosol-above-cloud events are easily identified.

Torres, O.

Absorption-line spectra of quasi-stellar objects - Physical properties of absorbing gas

The optical absorption lines of quasars are examined, and implications of the lines for the physical properties of the absorbing gas are discussed. Consideration is given to the characteristics of broad absorption lines observed in such quasars as PHL 5200 and Q 1246-057 and of the more prevalent extremely narrow lines, with discussion of the presumed physical conditions in the absorbing gas and the distribution of absorption-line redshifts with respect to emission-line redshifts. It is pointed out that absorption features become more prevalent in quasar spectra with emission redshifts greater than 2.3, and results of studies of column densities and abundances and of the presence of absorption in radio compact quasars are indicated. Research programs currently under way are then described, including a search for the distribution of absorption lines in a fixed wavelength range less than the Lyman alpha emission wavelength, study of low absorption-redshift systems, a study of individual objects such as the quasar pair 1548+114a and b, and various theoretical investigations.

Burbidge, E. M.

Nanodiamond in Colloidal Suspension: Electrophoresis; Other Observations

Selective laser extraction has demonstrated that meteoritic diamonds may consist of subpopulations with different optical absorption properties, but it is not clear what makes them optically different. More work is needed to understand the mechanism for selective laser extraction. Additional information is contained in the original extended abstract.

Meshik, A. P.

Coaxial carbon plasma gun deposition of amorphous carbon films

A unique plasma gun employing coaxial carbon electrodes was used in an attempt to deposit thin films of amorphous diamond-like carbon. A number of different structural, compositional, and electrical characterization techniques were used to characterize these films. These included scanning electron microscopy, scanning transmission electron microscopy, X ray diffraction and absorption, spectrographic analysis, energy dispersive spectroscopy, and selected area electron diffraction. Optical absorption and electrical resistivity measurements were also performed. The films were determined to be primarily amorphous, with poor adhesion to fused silica substrates. Many inclusions of particulates were found to be present as well. Analysis of these particulates revealed the presence of trace impurities, such as Fe and Cu, which were also found in the graphite electrode material. The electrodes were the source of these impurities. No evidence of diamond-like crystallite structure was found in any of the film samples. Details of the apparatus, experimental procedure, and film characteristics are presented.

Sater, D. M.

Remote sensing of atmospheric chemistry; Proceedings of the Meeting, Orlando, FL, Apr. 1-3, 1991

The present volume on remote sensing of atmospheric chemistry discusses special remote sensing space observations and field experiments to study chemical change in the atmosphere, network monitoring for detection of stratospheric chemical change, stratospheric chemistry studies, and the combining of model, in situ, and remote sensing in atmospheric chemistry. Attention is given to the measurement of tropospheric carbon monoxide using gas filter radiometers, long-path differential absorption measurements of tropospheric molecules, air quality monitoring with the differential optical absorption spectrometer, and a characterization of tropospheric methane through space-based remote sensing. Topics addressed include microwave limb sounder experiments for UARS and EOS, an overview of the spectroscopy of the atmosphere using an FIR emission experiment, the detection of stratospheric ozone trends by ground-based microwave observations, and a FIR Fabry-Perot spectrometer for OH measurements.

Mcelroy, James L.

Growth of new materials for solid state laser applications. The growth of ZnGeP2 by the vertical Bridgman method

This is the final technical report on the cooperative NASA program 'Growth of New Materials for Solid State Laser Applications,' covering the period from 9-1-86 through 3-31-91. The first two and one half years of the program, from 9-1-86 through 3-31-89, was devoted to the development of new eye-safe laser sources. Single crystal fibers of rare earth doped and co-doped YAG were grown by the laser-heated pedestal growth method, characterized for their structural properties and supplied to NASA/Langley for spectroscopic evaluation. From 4-1-89 though 3-31-91, research focused on the growth of zinc germanium phosphide for nonlinear optical applications in the IR. The vertical Bridgman growth process was evaluated as a means to achieve better control over the short wavelength optical absorption in this material that adversely affects 2 micron-pumped optical parametric oscillators.

Feigelson, R. S.

Reduced chromium in olivine grains from lunar basalt 15555 - X-ray Absorption Near Edge Structure (XANES)

The oxidation state of Cr in 200-micron regions within individual lunar olivine and pyroxene grains from lunar basalt 15555 was inferred using X-ray Absorption Near Edge Structure (XANES). Reference materials had previously been studied by optical absorption spectroscopy and included Cr-bearing borosilicate glasses synthesized under controlled oxygen fugacity and Cr-doped olivines. The energy dependence of XANES spectral features defined by these reference materials indicated that Cr is predominantly divalent in the lunar olivine and trivalent in the pyroxene. These results, coupled with the apparent f(02)-independence of partitioning coefficients for Cr into olivine, imply that the source magma was dominated by divalent Cr at the time of olivine crystallization.

Sutton, S. R.

Continuum laser absorption spectroscopy of C 2 (a 3 Π u ) in a sublimating cloud of carbon black

A direct optical absorption diagnostic has been developed for rotationally resolved measurements of diatomic carbon (a 3 Π u →d 3 Π g (0,0) and (1,1)) at a repetition rate of 525 kHz and resolution of 7.3 pm over the range of 511.1–514.1 nm. The diagnostic utilizes a high-power pulsed continuum laser light source dispersed in a spectrograph and imaged by a high-speed camera. Measurements have been performed that capture the temporal evolution of C 2 number density and temperature of a cloud of carbon black sublimating in shock heated gas at high temperature and pressure (T = 5500 K, P = 3.7 atm). A simultaneous light absorption measurement of the condensed phase enables comparisons of the gaseous C 2 number density to the condensed phase mass. The continuum laser absorption diagnostic is applied to C 2 in this work but shows promise in being a simple “drop-in” system for absorption spectroscopy in the visible range at rapid repetition rates and high dispersion, filling an important gap for laser diagnostic systems.

Willhardt, Colton Dean [Univ. of Illinois at Urban

Rise kinetics of light-induced modulation of absorption for a CdS crystal

An experimental study has been made of the rise kinetics for changes in optical absorption in a single crystal of CdS which was bulk excited by pulsed laser light. The experimental data were compared to calculations from a simple model involving a bimolecular process. Experimental and calculated values agreed to within the experimental error and confirmed that light-induced modulation of absorption is a bimolecular process.

Long, E. R., Jr.

Automatic Locking of Laser Frequency to an Absorption Peak

An electronic system adjusts the frequency of a tunable laser, eventually locking the frequency to a peak in the optical absorption spectrum of a gas (or of a Fabry-Perot cavity that has an absorption peak like that of a gas). This system was developed to enable precise locking of the frequency of a laser used in differential absorption LIDAR measurements of trace atmospheric gases. This system also has great commercial potential as a prototype of means for precise control of frequencies of lasers in future dense wavelength-division-multiplexing optical communications systems. The operation of this system is completely automatic: Unlike in the operation of some prior laser-frequency-locking systems, there is ordinarily no need for a human operator to adjust the frequency manually to an initial value close enough to the peak to enable automatic locking to take over. Instead, this system also automatically performs the initial adjustment. The system (see Figure 1) is based on a concept of (1) initially modulating the laser frequency to sweep it through a spectral range that includes the desired absorption peak, (2) determining the derivative of the absorption peak with respect to the laser frequency for use as an error signal, (3) identifying the desired frequency [at the very top (which is also the middle) of the peak] as the frequency where the derivative goes to zero, and (4) thereafter keeping the frequency within a locking range and adjusting the frequency as needed to keep the derivative (the error signal) as close as possible to zero. More specifically, the system utilizes the fact that in addition to a zero crossing at the top of the absorption peak, the error signal also closely approximates a straight line in the vicinity of the zero crossing (see Figure 2). This vicinity is the locking range because the linearity of the error signal in this range makes it useful as a source of feedback for a proportional + integral + derivative control scheme that constantly adjusts the frequency in an effort to drive the error to zero. When the laser frequency deviates from the midpeak value but remains within the locking range, the magnitude and sign of the error signal indicate the amount of detuning and the control circuitry adjusts the frequency by what it estimates to be the negative of this amount in an effort to bring the error to zero.

Koch, Grady J.

High-Power Single-Mode 2.65-micron InGaAsSb/AlInGaAsSb Diode Lasers

Central to the advancement of both satellite and in-situ science are improvements in continuous-wave and pulsed infrared laser systems coupled with integrated miniaturized optics and electronics, allowing for the use of powerful, single-mode light sources aboard both satellite and unmanned aerial vehicle platforms. There is a technological gap in supplying adequate laser sources to address the mid-infrared spectral window for spectroscopic characterization of important atmospheric gases. For high-power applications between 2 to 3 micron, commercial laser technologies are unsuitable because of limitations in output power. For instance, existing InP-based laser systems developed for fiber-based telecommunications cannot be extended to wavelengths longer than 2 micron. For emission wavelengths shorter than 3 micron, intersubband devices, such as infrared quantum cascade lasers, become inefficient due to band-offset limitations. To date, successfully demonstrated singlemode GaSb-based laser diodes emitting between 2 and 3 micron have employed lossy metal Bragg gratings for distributed- feedback coupling, which limits output power due to optical absorption. By optimizing both the quantum well design and the grating fabrication process, index-coupled distributed-feedback 2.65-micron lasers capable of emitting in excess of 25 mW at room temperature have been demonstrated. Specifically, lasers at 3,777/cm (2.65 micron) have been realized to interact with strong absorption lines of HDO and other isotopologues of H2O. With minor modifications of the optical cavity and quantum well designs, lasers can be fabricated at any wavelength within the 2-to-3-micron spectral window with similar performance. At the time of this reporting, lasers with this output power and wavelength accuracy are not commercially available. Monolithic ridge-waveguide GaSb lasers were fabricated that utilize secondorder lateral Bragg gratings to generate single-mode emission from InGaAsSb/ AlInGaAsSb multi-quantum well structures. The device fabrication utilizes etched index-coupled gratings in the top AlGaAsSb cladding of the laser chip along the ridge waveguide, whereas commercial lasers that emit close to this wavelength include loss-coupled metal gratings that limit the output power of the laser. Semiconductor-laser-based spectrometers can be used to replace gas sensors currently used in industry and government. With the availability of high-power laser sources at mid-infrared wavelengths, sensors can target strong fundamental gas absorption lines to maximize instrument sensitivity.

Frez, Clifford F.

Lidar Measurements of Methane and Applications for Aircraft and Spacecraft

Atmospheric methane levels have remained relatively constant over the last decade around 1.78 parts per million (ppm) but observations since 2007 show that levels may be increasing. This trend may be caused by increased fossil fuel production, rice farming, livestock and landfills, but the underlying causes are quite uncertain. One hypothesis is that reservoirs of carbon trapped in the permafrost regions of northern Canada, Europe, and Siberia thaw as global temperatures rise and are releasing increasing amounts of methane. Another hypothesis points to increased production of methane by microbes as the permafrost warms. Currently most observations of greenhouse gases are limited to in-situ (surface and tower sites) and limited airborne in-situ measurements. Space column density measurements are starting to become available from the GOSAT mission. Although methane survives for a shorter time in the atmosphere than CO2, its impact on climate change per molecule is about 23 times than that of CO2. Accurate global observations of several greenhouse gases, including methane, are urgently needed in order to better understand climate change processes and to reduce the uncertainty in the carbon budget. Differential absorption lidar is a well-established technique to measure atmospheric gases, and methane has optical absorption bands near 1.65,2.2,3.4 and 7.8 micron. The near infrared overtones lines of CH4 near 1650 nm are relatively free of interference from other species. There are absorption lines near 1651 nm which are both temperature insensitive and have line strengths well suited for lidar measurements. We have developed a laser and demonstrated lidar measurements of CH4 using lines in this band. Our laser uses a narrow linewidth 1064 nm laser pulse passing through a nonlinear crystal. We generate the tunable laser signals near 1651 nm by using the optical parametric amplification (OPA) process. Inside the crystal the 1064 nm beam overlaps with an injection seed laser near 1651 nm from a wavelength tunable diode laser. Incident photons from the pump laser pulse are converted into two photons, with one at the wavelength of the injection seeder. The wavelength of the OPA output is tuned via the wavelength of diode laser. Our laser is tunable, operates near 1651 nm and generates approximately 4 uJ/pulse at 6 KHz. We vary the emission wavelengths within this band by tuning the diode laser's wavelength. We have used this OPA transmitter to make measurements of CH4 at various pressures in a gas cell and over open outdoor horizontal paths. We have measured the lineshape of methane in a 6 cm long cell at various energy levels with this transmitter, with excellent agreement with the lineshape calculated by HITRAN. We have also measured the absorption lineshape of atmospheric methane in an open 3 km outdoor path. The agreement between the measurements and HITRAN, for 1746 ppb and 760 Torr was quite good. We have also made pulsed two wavelength lidar measurements of methane line absorption in the column to a tower at 1.5 km range. These used on- and off-line wavelengths of 1650.957 nm, and 1651.072 nm, and a 20 cm diameter receiver telescope with an infrared PMT detector. The absorption of the on-line photons was 30%. The methane column absorption was estimated via HITRAN, and was in good agreement with the expected methane absorption for a concentration of 1750 ppm. Finally we have calculated the measurement performance of an airborne methane lidar using this transmitter, as well as the energy and telescope scaling needed for a lidar for space. These results, and more details of our experiments will be described in the presentation.

Riris, Haris

Spontaneous Formation of Single-Crystalline Spherulites in a Chiral 2D Hybrid Perovskite

In two-dimensional (2D) chiral metal-halide perovskites (MHPs), chiral organic spacers induce structural chirality and chiroptical properties in the metal-halide sublattice. This structural chirality enables reversible crystalline-glass phase transitions in (S-NEA) 2 PbBr 4 , a prototypical chiral 2D MHP where NEA + represents 1-(1-naphthyl)ethylammonium. Here, in this study, we investigate two distinct spherulite states of (S-NEA) 2 PbBr 4 , exhibiting either radial-like or stripe-like banded patterns depending on the annealing conditions of the amorphous film. Despite similarities in optical absorption and photoluminescence, the stripe-like, banded spherulite exhibits higher crystallinity and improved optical transparency compared to those of radial-like spherulite. X-ray nanoprobe measurements reveal tilting-angle modulations in the octahedral plane of stripe-like spherulites, correlating with the film’s surface geometry. Transfer matrix calculations indicate that the optical contrast in stripe-like patterns, seen in bright-field optical microscopy, arises from optical interference effects, differing from the contrast mechanism observed in polymer spherulites. Ultrafast carrier dynamics experiments suggest that the stripe-like spherulites resemble single crystals more closely than radial-like spherulites, while electrical conductivity measurements show enhanced charge carrier transport in stripe-like spherulites. These findings offer insights into MHP spherulite states with a single composition but different morphologies, previously observed only in polymers, highlighting their potential for optoelectronic applications.

36 MATERIALS SCIENCE

Origin of the Bandgap Bowing in ZNSe(1-x)Te(x) Alloys

Photomodulated reflection and optical absorption spectroscopies were used to measure the composition and hydrostatic pressure dependencies of interband optical transitions in ZnSe(1-x)Te(x) alloys. On the Te-rich side, the bandgap reduction and the reduction in the pressure dependence of the bandgap are well explained by the band anticrossing interaction between the ZnTe conduction band states and the Se localized state located at 2.85 eV above the valence band top of ZnTe. On the Se-rich side, an interaction between the degenerate Gamma valence bands of ZnSe and the localized Te state located at 0.1 eV above the valence band top of ZnSe is proposed to generate the bandgap reduction and the rapid increase of the spin-orbit splitting with increasing Te concentration. A linear interpolation between these two models accounts for the composition and pressure dependencies of the bandgap in the entire composition range.

Walukiewicz, W.

Proton-induced coloring of multicomponent glasses

The paper describes the coloring induced by 85-MeV protons in three Schott glasses representative of glass types used as focusing elements in the International Ultraviolet Explorer Fine Error Sensor. It is shown that the absorption (i.e., coloring) induced in each glass by the radiation can be resolved into three optical absorption bands in the near UV-visible range. It is also discussed how that absorption grows with increasing dosages of protons, thus providing the means to predict degradation in any of the three glasses for a particular fluence of proton radiation.

Bartusiak, M. F.

Utilization of O4 Slant Column Density to Derive Aerosol Layer Height from a Space-Borne UV-Visible Hyperspectral Sensor: Sensitivity and Case Study

The sensitivities of oxygen-dimer (O4) slant column densities (SCDs) to changes in aerosol layer height are investigated using the simulated radiances by a radiative transfer model, the linearized pseudo-spherical vector discrete ordinate radiative transfer (VLIDORT), and the differential optical absorption spectroscopy (DOAS) technique. The sensitivities of the O4 index (O4I), which is defined as dividing O4 SCD by 10(sup 40) molecules (sup 2) per centimeters(sup -5), to aerosol types and optical properties are also evaluated and compared. Among the O4 absorption bands at 340, 360, 380, and 477 nanometers, the O4 absorption band at 477 nanometers is found to be the most suitable to retrieve the aerosol effective height. However, the O4I at 477 nanometers is significantly influenced not only by the aerosol layer effective height but also by aerosol vertical profiles, optical properties including single scattering albedo (SSA), aerosol optical depth (AOD), particle size, and surface albedo. Overall, the error of the retrieved aerosol effective height is estimated to be 1276, 846, and 739 meters for dust, non-absorbing, and absorbing aerosol, respectively, assuming knowledge on the aerosol vertical distribution shape. Using radiance data from the Ozone Monitoring Instrument (OMI), a new algorithm is developed to derive the aerosol effective height over East Asia after the determination of the aerosol type and AOD from the MODerate resolution Imaging Spectroradiometer (MODIS). About 80 percent of retrieved aerosol effective heights are within the error range of 1 kilometer compared to those obtained from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) measurements on thick aerosol layer cases.

Air Pollution

A 21 Centimeter Absorber Identified with a Spiral Galaxy: Hubble Space Telescope Faint Object Spectrograph and Wide-Field Camera Observations of 3CR 196

We present imaging and spectroscopy of the quasar 3CR 196 (z(sub e) = 0.871), which has 21 cm and optical absorption at z(sub a) = 0.437. We observed the region of Ly alpha absorption in 3CR 196 at z(sub a) = 0.437 with the Faint Object Spectrograph on the Hubble Space Telescope. This region of the spectrum is complicated because of the presence of a Lyman limit and strong lines from a z(sub a) approx. z(sub e) system. We conclude that there is Ly alpha absorption with an H I column density greater than 2.7 x 10(exp 19) cm(exp -2) and most probably 1.5 x 10(exp 20) cm(exp -2). Based on the existence of the high H I column density along both the optical and radio lines of sight, separated by more than 15 kpc, we conclude that the Ly alpha absorption must arise in a system comparable in size to the gaseous disks of spiral galaxies. A barred spiral galaxy, previously reported as a diffuse object in the recent work of Boisse and Boulade, can be seen near the quasar in an image taken at 0.1 resolution with the Wide Field Planetary Camera 2 on the HST. If this galaxy is at the absorption redshift, the luminosity is approximately L(sub *) and any H I disk should extend in front of the optical quasar and radio lobes of 3CR 196, giving rise to both the Ly alpha and 21 cm absorption. In the z(sub a) approx. z(sub e) system we detect Lyman lines and the Lyman limit, as well as high ion absorption lines of C III, N V, S VI, and O VI. This absorption probably only partially covers the emission-line region. The ionization parameter is approximately 0.1. Conditions in this region may be similar to those in broad absorption line QSOs.

Cohen, Ross D.