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NASA NTRS1990

New findings and instrumentation from the NASA Lewis Microgravity Facility

The study of fundamental combustion and fluid physics phenomena in microgravity enables a new range of experiments to be performed since buoyancy-type flows are nearly eliminated, normally obscured forces and flows may be isolated, gravitational settling or sedimentation is nearly eliminated, and larger time or length scales in experiments become permissible. Some new phenomena found through ground-based microgravity research at NASA facilities is reviewed along with the instrumentation and drop tower facilities used in the research. Experiments are described in the areas of premixed gas combustion, droplet combustion, particle cloud combustion, liquid reorientation, and two-phase flow patterns. Future plans for instrumentation development are also outlined.

Ross, Howard D.↗

NASA NTRS1990

Diabatic forcing and initialization with assimilation of cloud and rain water in a forecast model: Methodology

The focus of this part of the investigation is to find one or more general modeling techniques that will help reduce the time taken by numerical forecast models to initiate or spin-up precipitation processes and enhance storm intensity. If the conventional data base could explain the atmospheric mesoscale flow in detail, then much of our problem would be eliminated. But the data base is primarily synoptic scale, requiring that a solution must be sought either in nonconventional data, in methods to initialize mesoscale circulations, or in ways of retaining between forecasts the model generated mesoscale dynamics and precipitation fields. All three methods are investigated. The initialization and assimilation of explicit cloud and rainwater quantities computed from conservation equations in a mesoscale regional model are examined. The physical processes include condensation, evaporation, autoconversion, accretion, and the removal of rainwater by fallout. The question of how to initialize the explicit liquid water calculations in numerical models and how to retain information about precipitation processes during the 4-D assimilation cycle are important issues that are addressed. The explicit cloud calculations were purposely kept simple so that different initialization techniques can be easily and economically tested. Precipitation spin-up processes associated with three different types of weather phenomena are examined. Our findings show that diabatic initialization, or diabatic initialization in combination with a new diabatic forcing procedure, work effectively to enhance the spin-up of precipitation in a mesoscale numerical weather prediction forecast. Also, the retention of cloud and rain water during the analysis phase of the 4-D data assimilation procedure is shown to be valuable. Without detailed observations, the vertical placement of the diabatic heating remains a critical problem.

Raymond, William H.↗

NASA NTRS1993

Michelson Interferometer (MINT)

MINT is a Michelson interferometer designed to measure the thermal emission from the earth at high spectral resolution (2/cm) over a broad spectral range (250-1700/cm, 6-40 mu m) with contiguous 3-pixel wide (12 mrad, 8 km field of view) along-track sampling. MINT is particularly well suited for monitoring cloud properties (cloud cover, effective temperature, optical thickness, ice/water phase, and effective particle size) both day and night, as well as tropospheric water vapor, ozone, and temperature. The key instrument characteristics that make MINT ideally suited for decadal monitoring purposes are: high wavelength to wavelength precision across the full IR spectrum with high spectral resolution; space-proven long-term durability and calibration stability; and small size, low cost, low risk instrument incorporating the latest detector and electronics technology. MINT also incorporates simplicity in design and operation by utilizing passively cooled DTGS detectors and nadir viewing geometry (with target motion compensation). MINT measurement objectives, instrument characteristics, and key advantages are summarized in this paper.

Lacis, Andrew↗

NASA NTRS1994

High altitude molecular clouds

A population of molecular clouds with a significantly greater scale height than that of giant molecular clouds (GMCs) has been identified by examining maps of the latitude distribution of the (12)CO(1 - 0) emission in the first quadrant of the Galaxy. These clouds are found by identifying emission more than 2.6 times the scale-height away from the Galactic midplane (centroid of CO emission) at the tangent points. Since the distance to the tangent points is known, we know the heights and the sizes of these clouds. They are smaller and fainter than the GMCs and do not seem to be gravitationally bound. These clouds have properties similar to the high-latitude clouds in the solar neighborhood. Although they lie outside the molecular cloud layer, the high-altitude clouds are well within the H I layer in the Galaxy and coincide with distinct peaks in the H I distribution. These clouds represent a Galaxy-wide population of small molecular clouds having a larger scale height. They may be clouds in transition between molecular and atomic phases.

Malhotra, Sangeeta↗

NASA NTRS2003

Measurements of the Ice Water Content of Cirrus in the Tropics and Subtropics: Instrument Details and Validation - I

We describe an instrument mounted in a pallet on the NASA WB-57 aircraft that is designed to measure the sum of gas phase and solid phase water, or total water, in cirrus clouds. Using an isokinetic inlet, a 600-watt heater mounted directly in the flow, and Lyman-alpha photofragment fluorescence technique for detection, accurate measurements of total water have been made over almost three orders of magnitude. Isokinetic flow is achieved with an actively controlled roots pump by referencing aircraft pressure, temperature, and true air speed, together with instrument flow velocity, temperature, and pressure. During CRYSTAL FACE, the instrument operated at duct temperatures sufficiently warm to completely evaporate particles up to 150 microns diameter. In flight diagnostics, intercomparison with water measured by absorption in flight, as well as intercomparisons in clear air with water vapor measured by the Harvard water vapor instrument and the JPL infrared tunable diode laser hygrometer validate the detection sensitivity of the instrument and illustrate minimal hysteresis from instrument surfaces. The simultaneous measurement of total water and water vapor in cirrus clouds yields their ice water content.

Weinstock, E. M.↗

NASA NTRS1993

Laboratory Studies of Atmospheric Heterogeneous Chemistry

In the laboratory, ice films formed by freezing from the liquid or more frequently by deposition from the vapor phase have been used to simulate stratospheric cloud surfaces for measurements of reaction and uptake rates. To obtain intrinsic surface reaction probabilities that can be used in atmospheric models, the area of the film surface that actually takes part in the reaction must be known. It is important to know not only the total surface area but also the film morphology in order to determine where and how the surface is situated and, thus, what fraction of it is available for reaction. Information on the structure of these ice films has been obtained by using several experimental methods. In the sections that follow, these methods will be discussed, then the results will be used to construct a working model of the ice films, and finally the model will be applied to an experimental study of HC1 uptake by H_2O ice.

Keyser, L. F.↗

NASA NTRS2007

The Abundance and Distribution of Presolar Materials in Cluster IDPS

Presolar grains and remnants of interstellar organic compounds occur in a wide range of primitive solar system materials, including meteorites, interplanetary dust particles (IDPs), and comet Wild-2 samples. Among the most abundant presolar phases are silicate stardust grains and molecular cloud material. However, these materials have also been susceptible to destruction and alteration during parent body and nebular processing. In addition to their importance as direct samples of remote and ancient astrophysical environments, presolar materials thus provide a measure of how well different primitive bodies have preserved the original solar system starting materials. The matrix normalized abundances of presolar silicate grains in meteorites range from 20 ppm in Semarkona and Bishunpur to 170 ppm for Acfer 094. The lower abundances of presolar silicates in Bishunpur and Semarkona has been ascribed to the destruction of presolar silicates during aqueous processes. Presolar silicates appear to be significantly more abundant in anhydrous IDPs, possibly because these materials did not experience parent body hydrothermal alteration. Among IDPs the estimated abundances of presolar silicates vary by more than an order of magnitude, from 480 to 5500 ppm. The wide disparity in the abundances of presolar silicates of IDPs may be a consequence of the relatively small total area analyzed in those studies and the fine grain sizes of the IDPs. Alternatively, there may be a wide range in presolar silicate abundances between different IDPs. This view is supported by the observation that 15N-rich IDPs have higher presolar silicate abundances than those with isotopically normal N.

Messenger, Scott↗

NASA NTRS2007

The Abundance and Distribution of Presolar Materials in Cluster IDPS

Messenger, Scott↗

NASA NTRS2002

The Exobiological Role of Interstellar Polycyclic Aromatic Hydrocarbons and Ices

Tremendous strides have been made in our understanding of interstellar material over the past twenty years thanks to significant, parallel developments in observational astronomy and laboratory astrophysics. Before this time, the composition of interstellar dust was largely guessed-at, the presence of ices in interstellar clouds ignored, and the notion that large, gas phase, carbon rich molecules might be abundant and widespread throughout the interstellar medium (ISM) considered impossible. Today, the composition of dust in the ISM is reasonably well constrained to micron-sized cold refractory materials comprised of amorphous and crystalline silicates mixed with an amorphous carbonaceous material containing aromatic structural units and short, branched aliphatic chains. Shrouded within the protective confines of cold, opaque molecular clouds--the birthplace of stars and planets--these cold dust particles secrete mantles of mixed molecular ices whose compositions are also well constrained. Finally, amidst the molecular inventory of these ice mantles are likely to be found polycyclic aromatic hydrocarbons (PAHs), shockingly large molecules by the standards of interstellar chemistry, the telltale infrared spectral signature of which is now recognized throughout the Universe. In the first part of this talk, we will review the spectroscopic evidence that forms the basis for the currently accepted abundance and ubiquity of PANs in the ISM. We will then look at a few specific examples which illustrate how experimental and theoretical data can be applied to interpret the interstellar spectra and track how the PAN population evolves as it passes from its formation site in the circumstellar outflows of dying stars, through the various phases of the ISM, and into forn~iing planetary systems. Nevertheless, despite the fact that PANs likely represent the single largest molecular reservoir of organic carbon in evolving planetary systems, they are not what would be considered "biogenic" molecules. Although interesting from a chemical and astrophysical standpoint, in the absence of a mechanism by which this population can be dislodged from the precipitous thermodynamic well afforded by their extensive aromatic networks, they are of little Astrobiological significance. Consequently, for the remainder of the talk, we will consider the photochemical evolution of PANS under conditions similar to those found in the ISM and in proto-planetary systems with an eye toward means by which this rich repository of pre-biotic organic "ore" might be converted into materials of greater importance to Astrobiology.

Hudgins, Douglas M.↗

DOE OSTI2025

Advancing Aerosol Chemical Characterization and Vertical Profiling over the Southern Great Plains Using Uncrewed Aerial Sampling and Offline Aerosol Mass Spectrometry

Recent advancements in uncrewed aerial systems (UASs) and particulate matter (PM) analytical techniques have provided opportunities for atmospheric research. In this study, we deployed the Department of Energy’s fixed-wing ArcticShark UAS to examine PM 2.5 composition at varying altitudes─within and above the planetary boundary layer (PBL)─over the Southern Great Plains atmospheric observatory (SGP). A total of 22 flights were conducted across March, June, and August 2023. Composite filter samples were collected during each flight and analyzed with offline aerosol mass spectrometry (AMS), complemented by on-board real-time sensors and ground-based instrumentation, to provide a comprehensive view of regional aerosol characteristics. Results show clear vertical and seasonal differences in the aerosol composition. Relative to ground-level measurements, aloft samples exhibited shifts in the distribution of organic and inorganic PM, with the organic composition varying distinctly across seasons. Particulate organic nitrogen (ON) was elevated, with bulk compositions similar in March and June but strongly altered in August, likely driven by biomass burning and enhanced photochemical activity. Combined AMS and chemical ionization mass spectrometry analyses detected amines, amides, and amino acids. PM above the planetary boundary layer was enriched in oxidized organic aerosols, while ground-level PM contained higher nitrate and sulfate. Seasonal differences in aqueous-phase processing were also observed, which were strongest in March during persistent cloud cover and weaker in the drier August period, suggesting a shift from aqueous- to gas-phase SOA formation. In conclusion, these findings highlight the value of UAS in advancing PM measurements and vertical profiling of aerosol composition.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1988

Observations of interstellar HOCO(+) - Abundance enhancements toward the Galactic center

The 4(04)-3(03) and 1(01)-0(00) transitions of HOCO(+) toward several molecular clouds have been monitored. Of the molecular clouds considered, the HOCO(+) molecule has been detected only in Sgr B2 and Sgr A. The results suggest that gas phase CO2 is not a major carbon reservoir in typical molecular clouds. For Sgr B2, the column density of HOCO(+) at the northern peak is found to be about 3 x 10 to the 14th/sq cm, and a fractional abundance relative to H2 is obtained which is about 2 orders of magnitude greater than recent theoretical predictions.

Minh, Y. C.↗

NASA NTRS2000

GCSS Cirrus Parcel Model Comparison Project

The Cirrus Parcel Model Comparison Project, a project of GCSS Working Group on Cirrus Cloud Systems (WG2), involves the systematic comparison of current models of ice crystal nucleation and growth for specified, typical, cirrus cloud environments. The goal of this project is to document and understand the factors resulting in significant inter-model differences. The intent is to foment research leading to model improvement and validation. In Phase 1 of the project reported here, simulated cirrus cloud microphysical properties are compared for situations of "warm" (-40 C) and "cold" (-60 C) cirrus subject to updrafts of 4, 20 and 100 cm/s, respectively. Five models participated. These models employ explicit microphysical schemes wherein the size distribution of each class of particles (aerosols and ice crystals) is resolved into bins. Simulations are made including both homogeneous and heterogeneous ice nucleation mechanisms. A single initial aerosol population of sulfuric acid particles is prescribed for all simulations. To isolate the treatment of the homogeneous freezing (of haze drops) nucleation process, the heterogeneous nucleation mechanism is disabled for a second parallel set of simulations. Qualitative agreement is found for the homogeneous-nucleation-only simulations, e.g., the number density of nucleated ice crystals increases with the strength of the prescribed updraft. However, non-negligible quantitative differences are found. Detailed analysis reveals that the homogeneous nucleation formulation, aerosol size, ice crystal growth rate (particularly the deposition coefficient), and water vapor uptake rate are critical components that lead to differences in predicted microphysics. Systematic bias exists between results based on a modified classical theory approach and models using an effective freezing temperature approach to the treatment of nucleation. Each approach is constrained by critical freezing data from laboratory studies, but each includes assumptions that can only be justified by further laboratory data. Consequently, it is not yet clear if the two approaches can be made consistent. Large haze particles may deviate considerably from equilibrium size in moderate to strong updrafts (20-100 cm/s) at -60 C when the commonly invoked equilibrium assumption is lifted. The resulting difference in particle-size-dependent solution concentration of haze particles may significantly affect the ice nucleation rate during the initial nucleation interval. The uptake rate for water vapor excess by ice crystals is another key component regulating the total number of nucleated ice crystals. This rate, the product of ice number concentration and ice crystal diffusional growth rate, which is sensitive to the deposition coefficient when ice particles are small, partially controls the peak nucleation rate achieved in an air parcel and the duration of the active nucleation time period. The effects of heterogeneous nucleation are most pronounced in weak updraft situations. Vapor competition by the nucleated (heterogeneous) ice crystals limits the achieved ice supersaturation and thus suppresses the contribution of homogeneous nucleation. Correspondingly, ice crystal number density is markedly reduced. Definitive laboratory and atmospheric benchmark data are needed for the heterogeneous nucleation process. Inter-model differences are correspondingly greater than in the case of the homogeneous nucleation process acting alone.

Lin, Ruei-Fong↗

NASA NTRS2005

A New Unsteady Model for Dense Cloud Cavitation in Cryogenic Fluids

A new unsteady, cavitation model is presented wherein the phase change process (bubble growth/collapse) is coupled to the acoustic field in a cryogenic fluid. It predicts the number density and radius of bubbles in vapor clouds by tracking both the aggregate surface area and volume fraction of the cloud. Hence, formulations for the dynamics of individual bubbles (e.g. Rayleigh-Plesset equation) may be integrated within the macroscopic context of a dense vapor cloud i.e. a cloud that occupies a significant fraction of available volume and contains numerous bubbles. This formulation has been implemented within the CRUNCH CFD, which has a compressible real fluid formulation, a multi-element, unstructured grid framework, and has been validated extensively for liquid rocket turbopump inducers. Detailed unsteady simulations of a cavitating ogive in liquid nitrogen are presented where time-averaged mean cavity pressure and temperature depressions due to cavitation are compared with experimental data. The model also provides the spatial and temporal history of the bubble size distribution in the vapor clouds that are shed, an important physical parameter that is difficult to measure experimentally and is a significant advancement in the modeling of dense cloud cavitation.

Hosangadi, A.↗

NASA NTRS2008

Near-Real Time Cloud Retrievals from Operational and Research Meteorological Satellites

A set of cloud retrieval algorithms developed for CERES and applied to MODIS data have been adapted to analyze other satellite imager data in near-real time. The cloud products, including single-layer cloud amount, top and base height, optical depth, phase, effective particle size, and liquid and ice water paths, are being retrieved from GOES- 10/11/12, MTSAT-1R, FY-2C, and Meteosat imager data as well as from MODIS. A comprehensive system to normalize the calibrations to MODIS has been implemented to maximize consistency in the products across platforms. Estimates of surface and top-of-atmosphere broadband radiative fluxes are also provided. Multilayered cloud properties are retrieved from GOES-12, Meteosat, and MODIS data. Native pixel resolution analyses are performed over selected domains, while reduced sampling is used for full-disk retrievals. Tools have been developed for matching the pixel-level results with instrumented surface sites and active sensor satellites. The calibrations, methods, examples of the products, and comparisons with the ICESat GLAS lidar are discussed. These products are currently being used for aircraft icing diagnoses, numerical weather modeling assimilation, and atmospheric radiation research and have potential for use in many other applications.

Minnis, Patrick↗

NASA NTRS2000

The Abundances of Solid N2 and Gaseous CO2 in Interstellar Dense Molecular Clouds

We present 2338-2322 per centimeter (4.277-4.307 micrometer) infrared spectra of a number of N2-containing mixed molecular ices and demonstrate that the strength of the infrared "forbidden" band due to the N=N stretch near 2328 per centimeter (4.295 micrometer) is extremely sensitive to the composition of the ice. The strength of the 2328 per centimeter N2 fundamental is significantly enhanced relative to that of pure N2 ice when NH3, H2O, or CO2 are present, but is largely unaffected by the presence of CO, CH4 or O2. We use the laboratory data in coil junction with ISO data that probes several lines-of-sight through dense molecular clouds to place limits on the abundance of interstellar solid phase N2 and the composition of the ices. Deriving upper limits is complicated by the presence of overlapping absorptions due to CO2 gas in the clouds and, in some cases, to photospheric CO in the background star. These upper limits are just beginning to be low enough to constrain interstellar grain models and the composition of possible N2-bearing interstellar ices. We outline the search criteria that will need to be met if solid interstellar N2 is to be detected in the future. We also discuss some of the implications of the presence of warm CO2 gas along the lines-of-sight to embedded protostars and demonstrate that its presence may help resolve certain puzzles associated with the previously derived gas/solid CO2 ratios and the relative abundances of polar and nonpolar ices towards these objects. Finally, we briefly comment on the possible implications of these results for the interpretation of N2 detections on outer solar system bodies.

Sandford, Scott A.↗

NASA NTRS2006

From Astrochemistry to Astrobiology ...... and Back Again

Tremendous strides have been made in our understanding of interstellar material over the past twenty five years thanks to significant developments in observational infrared astronomy and laboratory astrophysics. Twenty five years ago the composition of interstellar dust was largely guessed at, the concept of ices in dense molecular clouds generally ignored, and the notion of large, abundant, gas phase, carbon-rich molecules widespread throughout the interstellar medium (ISM) considered impossible. Today the composition of interstellar dust is reasonably well understood. In molecular clouds, the birthplace of stars and planets, these cold dust particles are coated with mixed molecular ices whose composition is reasonably well constrained. Lastly, the signature of carbon-rich polycyclic aromatic hydrocarbons (PAHs), shockingly large molecules by early interstellar chemistry standards, is widespread throughout the Universe. The first part of this talk will describe how infrared spectroscopic studies of interstellar space, combined with laboratory simulations and theoretical studies of PAHs and interstellar ices, have revealed the widespread presence of interstellar PAHs and the composition of interstellar precometary ices. The remainder of the presentation will focus on the photochemical evolution of these icy materials. Within a molecular cloud, and especially the presolar nebula, materials frozen into the ices are photoprocessed by ultraviolet light and more complex molecules are produced. As these materials are the building blocks of comets and related to carbonaceous micrometeorites, they are likely to be important sources of complex materials delivered to habitable planets and their composition may be related to the origin of life.

Allamandola, L. J.↗

DOE OSTI2019

Physical and Thermodynamic Properties of Secondary Organic Materials for Modeling (Final Technical Report)

Secondary organic material constitutes more than 50% of the submicron component of atmospheric aerosol particles. This organic material is produced by oxidation of biogenic and anthropogenic volatile organic compounds. The physicochemical properties of these aerosol particles and their variability with atmospheric conditions influence many climate-relevant endpoints, such as rates of chemical reactions, production of secondary organic material, number-diameter distributions, direct radiative forcing, and cloud condensation nuclei. The results of the project research highlight a nonlabile-to-labile transition for material representative of anthropogenic secondary organic particulate matter at a threshold humidity range. This behavior differs markedly from materials representing biogenic aerosol sources, which lack such a transition. More specifically, the mass lability of atmospheric organic particulate matter, meaning its tendency to evaporate, is an important property in the mechanisms governing the climate effects. This property is affected by both the volatility and the molecular diffusivity of the constituent organic species. Via a series of laboratory experiments, the project directly determined the mass labilities of films of secondary organic material representative of anthropogenic and biogenic organic particulate matter (PM). The evaporation rates for anthropogenic organic PM increased above a threshold relative humidity (RH) between 20% and 30%, indicating rapid partitioning above a transition RH. Below the threshold, the characteristic time for equilibration was estimated at up to 1 week for a typically sized particle. In contrast, for films representing biogenic PM, no RH threshold was observed, suggesting equilibrium partitioning is rapidly obtained for all RHs. The effective molecular diffusivity for the biogenic case was at least 1000 times greater than that of the anthropogenic case. The results allow for an improved representation of anthropogenic and biogenic secondary organic aerosol formation in climate models. The results of the project also provide new measurements on how organic aerosol particles take up water and serve as cloud condensation nuclei, thus explaining the observed complex thermodynamic behaviors using a simple thermodynamic model. The project results reconciled the discrepancy between sub-saturation hygroscopicity and super-saturation cloud condensation nuclei activity for organic aerosol particles. The key to the explanation is the phase separation between hydrophobic and hydrophilic organics and the induced surface tension lowering. The results are essential for the assessment of the aerosol indirect effect on climate. In more detail, hygroscopic growth and cloud condensation nuclei activation are key processes for accurately modeling the climate impacts of organic particulate matter. Nevertheless, the microphysical mechanisms of these processes remain unresolved. The project results focus on complex thermodynamic behaviors, including humidity-dependent hygroscopicity, diameter-dependent cloud condensation nuclei activity, and liquid-liquid phase separation in the laboratory for biogenically derived secondary organic material representative of similar atmospheric organic particulate matter. These behaviors can be explained by the non-ideal mixing of water with hydrophobic and hydrophilic organic components. The non-ideality-driven liquid-liquid phase separation further enhances water uptake and induces lowered surface tension at high relative humidity, which results in a lower barrier to cloud condensation nuclei activation. By comparison, secondary organic material representing anthropogenic sources does not exhibit complex thermodynamic behavior. The combined results highlight the importance of detailed thermodynamic representations of the hygroscopicity and cloud condensation nuclei activity in models of the Earth’s climate system.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1987

The effects of stimulated star formation on the evolution of the galaxy. III - The chemical evolution of nonlinear systems

The evolution of models for star formation in galaxies with disk and halo components is discussed. Two phases for the halo (gas and stars) and three for the disk (including clouds) are used in these calculations. The star-formation history is followed using nonlinear phase-coupling models which completely determine the populations of the phases as a function of time. It is shown that for a wide range of parameters, including the effects of both spontaneous and stimulated star formation and mass exchange between the spatial components of the system, the observed chemical history of the galaxy can easily be obtained. The most sensitive parameter in the detailed metallicity and star-formation history for the system is the rate of return of gas to the diffuse phase upon stellar death.

Shore, Steven N.↗