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NASA NTRS1994

Measurements of thermal infrared spectral reflectance of frost, snow, and ice

Because much of Earth's surface is covered by frost, snow, and ice, the spectral emissivities of these materials are a significant input to radiation balance calculations in global atmospheric circulation and climate change models. Until now, however, spectral emissivities of frost and snow have been calculated from the optical constants of ice. We have measured directional hemispherical reflectance spectra of frost, snow, and ice from which emissivities can be predicted using Kirchhoff's law (e = 1-R). These measured spectra show that contrary to conclusions about the emissivity of snow drawn from previously calculated spectra, snow emissivity departs significantly from blackbody behavior in the 8-14 micrometer region of the spectrum; snow emissivity decreases with both increasing particle size and increasing density due to packing or grain welding; while snow emissivity increases due to the presence of meltwater.

Salisbury, John W.↗

NASA NTRS1995

Thermal emission from particulate surfaces: A comparison of scattering models with measured spectra

Emissivity spectra of particulate mineral samples are highly dependent on particle size when that size is comparable to the wavelength of light emitted (5-50 micrometers for the midinfrared). Proper geologic interpretation of data from planetary infrared spectrometers will require that these particle size effects be well understood. To address this issue, samples of quartz powders were produced with narrow, well-characterized particle size distributions. Mean particle diameters in these samples ranged from 15 to 227 micrometers. Emission spectra of these powders allow the first detailed comparison of the complex spectral variations with particle size observed in laboratory data with the predictions of radiative transfer models. Four such models are considered here. Hapke's relectance theory (converted to emissivity via Kirchoff's law) is the first model tested. Hapke's more recently published emission theory is also employed. The third model, the 'Mie/Conel' model, uses Mie single scattering with a two-stream approximation for multiple scattering. This model, like the first, is a converted reflec- tance model. Mie scattering assumes particles are both spherical and well separated, which is not true for the quartz powders, but includes diffraction effects. The fourth model uses the Mie solution for single scattering by spheres and inputs those results into the multiple scattering formalism of Hapke's emission theory. The results of the four models are considered in relation to the values of the optical constants n and k. We have grouped these as class 1 (k large), class 2 (k moderate, n is approximately 2), class 3 (k small, n is approximately 2), and class 4 (k small, n is approximately 1). In general, the Mie/Hapke hybrid model does best at predicting variations with grain size. In particular, it predicts changes of the correct pattern, although incorrect magnitude, for class 1 bands, where large increases in emissivity with decreasing grain size are observed. This model also does an excellent job on moderate (class 2) and very weak and intraband (class 3) regions, and correctly predicts the emission maximum and its invariance with grain size near the Christiansen frequency (class 4). The Mie/Hapke hybrid model also has the fewest free parameters of the four models examined, while maintaining the most physical treatment of the radiative transfer. The Mie/Conel model performs as well as the Mie/Hapke hybrid model in strong bands (class 1) but does not accurately model the behavior of moderate (class 2) and very weak (class 3) bands.

Moersch, J. E.↗

NASA NTRS1995

Spectrophotometry and organic matter on Iapetus. 1: Composition models

Iapetus shows a greater hemispheric albedo asymmetry than any other body in the solar system. Hapke scattering theory and optical constants measured in the laboratory are used to identify possible compositions for the dark material on the leading hemisphere of Iapetus. The materials considered are poly-HCN, kerogen, Murchison organic residue, Titan tholin, ice tholin, and water ice. Three-component mixtures of these materials are modeled in intraparticle mixture of 25% poly-HCN, 10% Murchison residue, and 65% water ice is found to best fit the spectrum, albedo, and phase behavior of the dark material. The Murchison residue and/or water ice can be replaced by kerogen and ice tholin, respectively, and still produce very good fits. Areal and particle mixtures of poly-HCN, Titan tholin, and either ice tholin or Murchison residue are also possible models. Poly-HCN is a necessary component in almost all good models. The presence of poly-HCN can be further tested by high-resolution observations near 4.5 micrometers.

Wilson, Peter D.↗

NASA NTRS1995

Characterization and Application of a Grazing Angle Objective for Quantitative Infrared Reflection Microspectroscopy

A grazing angle objective on an infrared microspectrometer is studied for quantitative spectroscopy by considering the angular dependence of the incident intensity within the objective's angular aperture. The assumption that there is no angular dependence is tested by comparing the experimental reflectance of Si and KBr surfaces with the reflectance calculated by integrating the Fresnel reflection coefficient over the angular aperture under this assumption. Good agreement was found, indicating that the specular reflectance of surfaces can straight-forwardly be quantitatively integrated over the angular aperture without considering non-uniform incident intensity. This quantitative approach is applied to the thickness determination of dipcoated Krytox on gold. The infrared optical constants of both materials are known, allowing the integration to be carried out. The thickness obtained is in fair agreement with the value determined by ellipsometry in the visible. Therefore, this paper illustrates a method for more quantitative use of a grazing angle objective for infrared reflectance microspectroscopy.

Pepper, Stephen V.↗

NASA NTRS1995

Spectroscopic Evidence Against Nitric Acid Trihydrate in Polar Stratospheric Clouds

Heterogeneous reactions on polar stratospheric clouds (PSC's) play a key role in the photochemical mechanism thought to be responsible for ozone depletion in the Antarctic and Arctic. Reactions of PSC particles activate chlorine to forms that are capable of photochemical ozone destruction, and sequester nitrogen oxides (NOx) that would otherwise deactivate the chlorine. Although the heterogeneous chemistry is now well established, the composition of the clouds themselves is uncertain. It is commonly thought that they are composed of nitric acid trihydrate, although observations have left this question unresolved. Here we reanalyse infrared spectra of type 1 PSCs obtained in Antarctica in September 1987, using recently measured optical constants of the various compounds that might be present in PSCs. We find these PSCs were not composed of nitric acid trihydrate but instead had a more complex compositon, perhaps that of a ternary solution. Because cloud formation is sensitive to their composition, this finding will alter our understanding of the locations and conditions in which PSCs form. In addition, the extent of ozone loss depends on the ability of the PSCs to remove NOx permanently through sedimentation, The sedimentation rates depend on PSC particle size which in turn is controlled by the composition and formation mechanism.

Toon, Owen B.↗

NASA NTRS1996

The 11 micron Silicon Carbide Feature in Carbon Star Shells

Silicon carbide (SiC) is known to form in circumstellar shells around carbon stars. SiC can come in two basic types - hexagonal alpha-SiC or cubic beta-SiC. Laboratory studies have shown that both types of SiC exhibit an emission feature in the 11-11.5 micron region, the size and shape of the feature varying with type, size and shape of the SiC grains. Such a feature can be seen in the spectra of carbon stars. Silicon carbide grains have also been found in meteorites. The aim of the current work is to identity the type(s) of SiC found in circumstellar shells and how they might relate to meteoritic SiC samples. We have used the CGS3 spectrometer at the 3.8 m UKIRT to obtain 7.5-13.5 micron spectra of 31 definite or proposed carbon stars. After flux-calibration, each spectrum was fitted using a chi(exp 2)-minimisation routine equipped with the published laboratory optical constants of six different samples of small SiC particles, together with the ability to fit the underlying continuum using a range of grain emissivity laws. It was found that the majority of observed SiC emission features could only be fitted by alpha-SiC grains. The lack of beta-SiC is surprising, as this is the form most commonly found in meteorites. Included in the sample were four sources, all of which have been proposed to be carbon stars, that appear to show the SiC feature in absorption.

Speck, A. K.↗

NASA NTRS1996

The Surfaces of Pluto and Charon

Much of the surface of Pluto consists of high-albedo regions covered to an unknown depth by Beta-N2, contaminated with CH4, CO, and other molecules. A portion of the exposed surface appears to consist of solid H2O. The remainder is covered by lower albedo material of unknown composition. The N2 ice may occur as polar caps of large extent, leaving ices and other solids of lower volatility in the equatorial regions. The low-albedo material found primarily in the equatorial regions may consist in part of solid hydrocarbons and nitriles produced from N2 and CH4 in the atmosphere or in the surface ices. Alternatively, it may arise from deposition from impacting bodies and/or the chemistry of the impact process itself. Charon's surface is probably more compositionally uniform than that of Pluto, and is covered by H2O ice with possible contaminants or exposures of other materials that are as yet unidentified. The molecular ices discovered on Pluto and Charon have been identified from near-infrared spectra obtained with Earth-based telescopes. The quantitative interpretation of those data has been achieved through the computation of synthetic spectra using the Hapke scattering theory and the optical constants of various ices observed in the laboratory. Despite limitations imposed by the availability of laboratory data on ices in various mixtures, certain specific results have been obtained. It appears that CH4 and CO are trace constituents, and that some fraction of the CH4 (and probably the CO) on Pluto is dissolved in the matrix of solid N2. Pure CH4 probably also occurs on Pluto's surface, allowing direct access to the atmosphere. Study of the nitrogen absorption band at 2.148 micrometers shows that the temperature of the N2 in the present epoch is 40 +/-2 K. The global temperature regime of Pluto can be modeled from observations of the thermal flux at far-infrared and millimeter wavelengths. The low-albedo equatorial regions must be significantly warmer than the polar regions covered by N2 (at T = 40 K) to account for the total thermal flux measured. At the present season, the diurnal skin depth of the insolation-driven thermal wave is small, and the observed mm-wave fluxes may arise from a greater depth. Alternatively, the mm-wave flux may arise from the cool, sublimation source region. The surface microstructure in the regions covered by N2 ice is likely governed by the sintering properties of this highly volatile material. The observed nitrogen infrared band strength requires that expanses of the surface be covered with cm-sized crystals of N2. Grains of H2O ice on Charon, in contrast, are probably of order 50 micrometers in size, and do not metamorphose into larger grains at a significant rate. Because of the similarities in size, density, atmosphere and surface composition between Pluto and Neptune's satellite Triton, the surface structures observed by Voyager on Triton serve as a plausible paradigm for what might be expected on Pluto. Such crater forms, tectonic structures, aeolian features, cryovolcanic structures, and sublimation-degraded topography as are eventually observed on Pluto and Charon by spacecraft will give information on their interior compositions and structures, as well as on the temperature and wind regimes over the planet's extreme seasonal cycle.

Cruikshank, Dale P.↗

NASA NTRS1997

Use of Variable Angle Spectroscopic Ellipsometry in Order to Determine Contaminant Optical Properties

In order to measure contaminant levels found in the manufacture of the Redesigned Solid Rocket Motor (RSRM), optical properties of the contaminants are needed to develop standards for calibration purposes. Specific to our efforts is the determination of the complex index of refraction for a hydrocarbon mixture and a commercial methyl siloxane. Using ellipsometric measurements with multiple angles of incident and a range of wavelengths in the near infrared a determination of the index of refraction and the extinction coefficient were made for the contaminants. This paper will present the optical techniques and modeling approach used to determine these optical constants of the hydrocarbon mixture and the methyl siloxane studied.

Hughes, C.↗

NASA NTRS1994

Multilayer Thin Film Polarizer Design for Far Ultraviolet using Induced Transmission and Absorption Technique

Good theoretical designs of far ultraviolet polarizers have been reported using a MgF2/Al/MgF2 three layer structure on a thick Al layer as a substrate. The thicknesses were determined to induce transmission and absorption of p-polarized light. In these designs Al optical constants were used from films produced in ultrahigh vacuum (UHV: 10(exp -10) torr). Reflectance values for polarizers fabricated in a conventional high vacuum (p approx. 10(exp -6 torr)) using the UHV design parameters differed dramatically from the design predictions. Al is a highly reactive material and is oxidized even in a high vacuum chamber. In order to solve the problem other metals have been studied. It is found that a larger reflectance difference is closely related to higher amplitude and larger phase difference of Fresnel reflection coefficients between two polarizations at the boundary of MgF2/metal. It is also found that for one material a larger angle of incidence from the surface normal brings larger amplitude and phase difference. Be and Mo are found good materials to replace Al. Polarizers designed for 121.6 nm with Be at 60 deg and with Mo at 70 deg are shown as examples.

Kim, Jongmin↗

NASA NTRS1998

Magnesium-Aluminum-Zirconium Oxide Amorphous Ternary Composite: A Dense and Stable Optical Coating

In the present work, the process parameter dependent optical and structural properties of MgO-Al(2)O(3)-ZrO(2) ternary mixed-composite material have been investigated. Optical properties were derived from spectrophotometric measurements. The surface morphology, grain size distributions, crystallographic phases and process dependent material composition of films have been investigated through the use of Atomic Force Microscopy (AFM), X-ray diffraction analysis and Energy Dispersive X- ray (EDX) analysis. EDX analysis made evident the correlation between the optical constants and the process dependent compositions in the films. It is possible to achieve environmentally stable amorphous films with high packing density under certain optimized process conditions.

Sahoo, N. K.↗

NASA NTRS1998

MgO-Al2O3-ZrO2 Amorphous Ternary Composite: A Dense and Stable Optical Coating

The process-parameter-dependent optical and structural properties of MgO-Al2O3-ZrO2 ternary mixed-composite material were investigated. Optical properties were derived from spectrophotometric measurements. The surface morphology, grain size distributions, crystallographic phases, and process- dependent material composition of films were investigated through the use of atomic force microscopy, x-ray diffraction analysis, and energy-dispersive x-ray analysis. Energy-dispersive x-ray analysis made evident the correlation between the optical constants and the process-dependent compositions in the films. It is possible to achieve environmentally stable amorphous films with high packing density under certain optimized process conditions.

Shaoo, Naba K.↗

NASA NTRS1999

Contamination Effects on EUV Optics

During ground-based assembly and upon exposure to the space environment, optical surfaces accumulate both particles and molecular condensibles, inevitably resulting in degradation of optical instrument performance. Currently, this performance degradation (and the resulting end-of-life instrument performance) cannot be predicted with sufficient accuracy using existing software tools. Optical design codes exist to calculate instrument performance, but these codes generally assume uncontaminated optical surfaces. Contamination models exist which predict approximate end-of-life contamination levels, but the optical effects of these contamination levels can not be quantified without detailed information about the optical constants and scattering properties of the contaminant. The problem is particularly pronounced in the extreme ultraviolet (EUV, 300-1,200 A) and far (FUV, 1,200-2,000 A) regimes due to a lack of data and a lack of knowledge of the detailed physical and chemical processes involved. Yet it is in precisely these wavelength regimes that accurate predictions are most important, because EUV/FUV instruments are extremely sensitive to contamination.

Tveekrem, J.↗

NASA NTRS1984

The Specular Reflectance of IR-Opaque Coatings

A reflecting-layer model of the specular reflectance of a rough, thick, absorbing, dielectric film has been developed and fitted to the spectra of seven optical-black coatings between 12 and 300 micrometers. The coatings were quite different. At 100 micrometers their reflectance varied by a factor of nearly 10(exp 3). The model determines optical constants and surface parameters, and indicates which parameters control reflectance in the far IR.

Smith, Sheldon M.↗

NASA NTRS1998

Calculation of the Bulk Electromagnetic Properties of Thunderclouds Using a Two-Space Scattering Formalism

A two-space scatterer formalism and equivalent medium approach of Twersky are used to obtain formulae for the bulk electromagnetic parameters of a thundercloud medium that is illuminated by lightning optical emissions. A modified WKB approximation is applied to derive the two-space scattering amplitude. Optical constants of dry air, moist atmosphere, and water,.are inserted into the formulae to generate numerical values via iteration. The two-space scatterer formalism results are close to those obtained from free- or sin-le-space formalisms for the dilute case. The numerical values of the bulk parameters are required to successfully transform the scattering problem to that of an equivalent obstacle excited by an incident wave traveling in K - space but radiating in k(sub 1) -space.

Phanord, Dieudonne D.↗

NASA NTRS1999

Interacting Surfaces and Atmospheres in the Outer Solar System

The work reported here is an extension of ongoing efforts in data reduction and modeling of the spectral reflectances of several objects in the outer Solar System. In general terms, this requires an evaluation of the data obtained at the telescope, conversion of those data into geometric albedo units, and the combination of individual spectrum segments into a complete spectrum over the wavelength interval of interest. The modeling effort to produce a synthetic spectrum of a given Solar System object requires the complex refractive indices (the optical constants) of candidate surface materials, including ices, minerals, and organic solids. Those indices are primarily available only through contacts with other researchers, including colleagues at NASA Ames and at other institutions. Once obtained, the indices must be convolved with the telescopic data and then used in a computational model to produce the required synthetic spectrum for comparison with the data obtained at the telescope. In this way, we reach a convergence on the chemical composition and microstructural properties of the surfaces of objects in the outer Solar System.

DalleOre, Cristina↗

NASA NTRS1995

Composition of Polar Stratospheric Clouds from Infrared Spectroscopy

Heterogeneous reactions on polar stratospheric clouds (PSCs) have recently been implicated in Arctic and Antarctic ozone destruction. Although the chemistry is well documented, the composition of the clouds remains uncertain. The most common PSCs (type I) are thought to be composed of HNO3/H2O mixtures. Although the exact process is not clear, type I PSCs are believed to nucleate on preexisting stratospheric sulfate aerosols (SSAs) composed of sulfuric acid and water. We are using infrared spectroscopy to study the composition and formation mechanism of type I PSCs. In the laboratory, we have used FTIR spectroscopy to probe the composition and phase of H2SO4/HNO3/H2O aerosols under winter polar stratospheric conditions. We have also used recently measured infrared optical constants for HNO3/H2O mixtures to analyze solar infrared extinction measurements of type I PSCs obtained in September 1987 over Antarctica. The results of these studies will be discussed in the context of current theories for polar stratospheric clouds formation.

Tolbert, M. A.↗

NASA NTRS1996

The 2140 cm(exp -1) (4.673 Microns) Solid CO Band: The Case for Interstellar O2 and N2 and the Photochemistry of Non-Polar Interstellar Ice Analogs

The infrared spectra of CO frozen in non-polar ices containing N2, CO2, O2, and H2O, and the ultraviolet photochemistry of these interstellar/precometary ice analogs are reported. The spectra are used to test the hypothesis that the narrow 2140/cm (4.673 micrometer) interstellar absorption feature attributed to solid CO might be produced by CO frozen in ices containing non-polar species such as N2 and O2. It is shown that mixed molecular ices containing CO, N2, O2, and CO2 provide a very good match to the interstellar band at all temperatures between 12 and 30 K both before and after photolysis. The optical constants (real and imaginary parts of the index of refraction) in the region of the solid CO feature are reported for several of these ices.

Elsila, Jamie↗

NASA NTRS2003

Spectral Characteristic of Tholin Produced from Possible Early Earth Atmospheres and its Role in Antigreenhouse Effect on Early Earth

We have produced organic material simulating a methane photochemical haze in a CO2- rich atmosphere of the early Earth by irradiating gas mixtures in an inductively coupled cold plasma chamber with pressure approx. 0.25 mbar at 100 W total power. The flow rate was 24 cm3 min. We added progressively higher levels of CH, by combining gas mixtures of N2/CH4 (9/1) and N2/CO2 (9/1) to change the ratio of CH4/CO2. Tholin was accumulated for 5 hours in each experiment; the onset of tholin formation is in the range CH4/CO2 = 0.5 to 1. As the mixing ratio of CH, is increased, the production rate of the brownish tholin film increases. IR spectra showed the C-H and N-H bands similar to that of Titan tholin and closely resemble Titan tholin made at 0.13 mbar pressure. A decrease in the CH bonds on decreasing CH4/CO2 is noted. Ether bands (-(2-O-C) were tentatively detected, but no detectable carbonyl (C=O) band was found. The absorption in the UV region for the early Earth tholin is found to be substantially greater than the Titan tholin. Quantitative values of the optical constants of early Earth tholin are currently being measured.

Khare, B. N.↗