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All sourcesNASA NTRSDOE OSTI
NASA NTRS2000

From Interstellar PAHs and Ices to the Origin of Life

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. Twenty years ago the composition of interstellar dust was largely guessed at, the concept of ices in dense molecular clouds ignored, and the notion of large, abundant, gas phase, carbon rich molecules widespread throughout the interstellar medium (ISM) considered impossible. Today the composition of dust in the diffuse 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. In dense molecular clouds, the birthplace of stars and planets, these cold dust particles are coated with mixed molecular ices whose composition is very well constrained. Lastly, the signature of carbon-rich polycyclic aromatic hydrocarbons (PAHs), shockingly large molecules by earlier interstellar chemistry standards, is widespread throughout the Universe. The first part of this lecture will describe how infrared studies of interstellar space, combined with laboratory simulations, have revealed the composition of interstellar ices (the building blocks of comets) and the high abundance and nature of interstellar PAHs. The laboratory database has now enabled us to gain insight into the identities, concentrations, and physical state of many interstellar materials. Within a dense molecular cloud, and especially in the solar nebula during the star and planet formation stage, the materials frozen into interstellar/precometary ices are photoprocessed by ultraviolet light, producing more complex molecules. The remainder of the presentation will focus on the photochemical evolution of these materials and the possible role of these compounds on the early Earth. As these materials are thought to be the building blocks of comets and related to the carbonaceous components of micrometeorites, they are likely to have been important sources of complex organic materials on the early Earth and their composition may be related to the origin of life.

Allamandola, Louis J.↗
NASA NTRS1994

Microphysical growth state of ice particles and large-scale electrical structure of clouds

Cloud temperature, liquid water content, and vertical air velocity are all considered in evaluating the microphysical growth state of ice phase precipitation particles in the atmosphere. The large-scale observations taken together with in situ measurements indicated that the most prevalent growth condition for large ice particles in active convection is sublimation during riming, whereas the most prevalent growth condition in stratiform precipitation is vapor deposition. The large-scale electrical observations lend further support to the idea that particles warmed by riming into sublimation charge negatively and particles in vapor deposition charge positively in collisions with small ice particles.

Williams, Earle↗
NASA NTRS2014

Cold Water Vapor in the Barnard 5 Molecular Cloud

After more than 30 yr of investigations, the nature of gas-grain interactions at low temperatures remains an unresolved issue in astrochemistry. Water ice is the dominant ice found in cold molecular clouds; however, there is only one region where cold ((is) approximately 10 K) water vapor has been detected-L1544. This study aims to shed light on ice desorption mechanisms under cold cloud conditions by expanding the sample. The clumpy distribution of methanol in dark clouds testifies to transient desorption processes at work-likely to also disrupt water ice mantles. Therefore, the Herschel HIFI instrument was used to search for cold water in a small sample of prominent methanol emission peaks. We report detections of the ground-state transition of o-H2O (J = 110-101) at 556.9360 GHz toward two positions in the cold molecular cloud, Barnard 5. The relative abundances of methanol and water gas support a desorption mechanism which disrupts the outer ice mantle layers, rather than causing complete mantle removal.

ISM: molecules↗
NASA NTRS2005

Impact of Cirrus Crystal Shape on Solar Spectral Irradiance: A Case Study for Subtropical Cirrus

Profiles of in situ measurements of ice crystal size distribution of subtropical cirrus were used to calculate solar spectral irradiances above and below the clouds. Spheres and nonspherical ice crystal habits (columns, hollows, plates, bullets, and aggregates) were assumed in the calculations. The simulation results were compared to irradiance measurements from the NASA Solar Spectral Flux Radiometer. The microphysical and radiation data were collected by three aircraft during CRYSTAL-FACE. Two cirrus cases (optical thickness of about 1 and 7) from two mission dates (26 and 23 July 2002) were investigated in detail. The measured downwelling and upwelling irradiance spectra above the cirrus could mostly be reproduced by the radiation model to within +/- 5-10% for most ice crystal habits. Below the cirrus the simulations disagreed with the measured irradiances due to surface albedo variability along the flight track, and nonoptimal colocation between the microphysical and irradiance measurements. The impact of shape characteristics of the crystals was important for the reflected irradiances above the optically thin cirrus, especially for small solar zenith angles, because in this case single-scattering dominated the solar radiation field. For the cirrus of moderate optical thickness the enhanced multiple scattering tended to diminish particular shape features caused by nonspherical single-scattering. Within the ice absorption bands the shape-related differences in the absorption characteristics of the individual nonspherical ice crystals were amplified if multiple scattering prevailed. Furthermore, it was found that below the cloud the shape sensitivity of the downwelling irradiance spectra is larger compared to the nonsphericity effects on reflected irradiances above the cirrus. Finally, it was shown that the calculated cirrus solar radiative forcing could vary by as much as 26% depending on the ice crystal habit.

Wendisch, Manfred↗
NASA NTRS1983

Laboratory and field observations related to ice particle and aircraft charging in convective storms

Graupel particle charging in simulated cloud conditions which show the need for the presence of ice crystals and cloud water simultaneously except under conditions where secondary ice crystal production occurs when charging initially occurs in the absence of ice crystals was examined. The magnitude of the charging increases with size of ice crystals, and impact velocity; it is also sensitive to impurities. The magnitude of the charge is also sensitive to temperature and the sign changes between -10 and -20 C, depending on cloud liquid water content. Aircraft studies were carried out in Montana convective clouds to test the validity of the extrapolation of the laboratory data to the atmosphere from the viewpoint of generation of charge, electric field, and aircraft charging during cloud penetration.

Christian, H.↗
NASA NTRS2005

Influence of Nucleation Mechanisms on the Radiative Properties of Deep Convective Clouds and Subvisible Cirrus in CRYSTAL/FACE

During the past few years we have conducted work on several different topics, as reflected by our publications. As one of the Co-Project scientists for The Cirrus Regional Study of Tropical Anvils and Cirrus Layers - Florida Area Cirrus Experiment (CRYSTAL FACE) we worked to help design the mission and then conduct it in the field. Another major activity during the past two years has been to pull together various groups to formulate plans for follow on missions to CRYSTAL FACE. We organized a workshop at the University of Colorado during the summer of 2003 to assess the best locations for future missions. Working with a group of about 10 scientists from around the country we prepared a science-planning document (Tropical Composition, Cloud and Climate Coupling Experiment (TC(sup 4)) that outlined the rationale, locations, strategy to accomplish the goals, and possible payloads for a set of three tropical missions. We also prepared background materials for various NRAs being prepared at NASA Headquarters for missions in Costa Rica, Darwin and Guam. In conjunction with the group at NASA Ames we have helped build a new numerical model for deep convection and have applied that model to simulate the CRYSTAL data. Our goal in particular has been to better understand how convection distributes water vapor isotopes. CRYSTAL observations of water isotopes are very different from those suggested by previous workers who assumed the isotopes would obey Rayleigh fractionation. The water isotope study has several implications. First it is a check on the realism of the deep convection model. Second, the isotopes are a measure of the precipitation removal in the atmosphere. Hence they provide a constraint on a parameter that is difficult to otherwise measure. Finally it has been suggested that isotopes may be the key to unraveling the water transport into the stratosphere and upper troposphere. Such transport is critical both for the radiation balance and for stratospheric chemistry. Ours is the first model that is able to treat this transport. Our initial results have just been submitted to Geophys. Res. Lett (Smith et al., 2005). Essentially we are able to explain the vertical profiles of isotopes in the tropical tropopause transition layer. We are also able to account for stratospheric humidity and isotope abundances with this model. We have also been heavily involved in trying to improve our understanding of nitric acid condensation on ice. Gao et al (2004) have shown that water supersaturations above ice occur when the atmosphere is supersaturated with respect to nitric acid trihydrate. As one of the co-authors of that work, we suggested the mechanism that may explain why this is occurring. Essentially, ice does not like to grow near unit supersaturation, but does so because the water molecules can find sites on the ice surface to attach themselves to before they fly off the ice surface. This phenomena was well known in the 1960s when it was a source of debate about whether condensation and evaporation coefficients for ice would be the same. Evaporation does not require any molecular orientation, while condensation does, so it was possible that the coefficients would differ. They don't differ because the water molecules rapidly move across the surface and find places to attach. Nitric acid may be occupying these preferred sites and therefore the water molecules can't find a desirable place to attach. We anticipate that this research will be the subject of laboratory work during the coming few years. Another possibility that has been suggested is that cubic ice is forming in clouds. We have measured the vapor pressure of cubic ice, and plan to publish that result in the next few months. We have also been working on additional aspects of the condensation of nitric acid on ice. With Y. Kondo we studied the condensation of NOy on ice using the SOLVE data. Gamblin et al. have continued this work. The CRYSTAL NOy and HNO, groups have shown th their data can be fit using standard Langmuir isotherms as suggested in some, but not all, laboratory studies. We have found in the SOLVE data set that this is not the case. Moreover some laboratory studies show there are important kinetic effects that may be occurring in the atmosphere limiting the transfer of nitric acid to the ice. The SOLVE data seem consistent with these studies. We are currently re-analyzing the CRYSTAL data to look for these kinetic effects. There are a number of implications of these studies. One of the more interesting is that the nitric acid coating on ice can be used as a cloud clock to determine how long the cloud parcel has been in existence. We have also been involved with several laboratory studies. We have worked to improve the database on ice optical constants, which are critical for remote sensing. We have also studied the ways in which ice nucleates on clays. We suspect now that the standard theories used for depositional ice nucleation are completely incorrect. Further work will be needed to develop a new theory.

Toon, Owen B.↗
NASA NTRS1995

Cloud Masking and Surface Temperature Distribution in the Polar Regions Using AVHRR and other Satellite Data

Surface temperature is one of the key variables associated with weather and climate. Accurate measurements of surface air temperatures are routinely made in meteorological stations around the world. Also, satellite data have been used to produce synoptic global temperature distributions. However, not much attention has been paid on temperature distributions in the polar regions. In the polar regions, the number of stations is very sparse. Because of adverse weather conditions and general inaccessibility, surface field measurements are also limited. Furthermore, accurate retrievals from satellite data in the region have been difficult to make because of persistent cloudiness and ambiguities in the discrimination of clouds from snow or ice. Surface temperature observations are required in the polar regions for air-sea-ice interaction studies, especially in the calculation of heat, salinity, and humidity fluxes. They are also useful in identifying areas of melt or meltponding within the sea ice pack and the ice sheets and in the calculation of emissivities of these surfaces. Moreover, the polar regions are unique in that they are the sites of temperature extremes, the location of which is difficult to identify without a global monitoring system. Furthermore, the regions may provide an early signal to a potential climate change because such signal is expected to be amplified in the region due to feedback effects. In cloud free areas, the thermal channels from infrared systems provide surface temperatures at relatively good accuracies. Previous capabilities include the use of the Temperature Humidity Infrared Radiometer (THIR) onboard the Nimbus-7 satellite which was launched in 1978. Current capabilities include the use of the Advance Very High Resolution Radiometer (AVHRR) aboard NOAA satellites. Together, these two systems cover a span of 16 years of thermal infrared data. Techniques for retrieving surface temperatures with these sensors in the polar regions have been developed. Errors have been estimated to range from 1K to 5K mainly due to cloud masking problems. With many additional channels available, it is expected that the EOS-Moderate Resolution Imaging Spectroradiometer (MODIS) will provide an improved characterization of clouds and a good discrimination of clouds from snow or ice surfaces.

Comiso, Joey C.↗
NASA NTRS1980

Infrared radiative properties of tropical cirrus clouds inferred with aircraft measurements

Longwave emissivities and the vertical profile of cooling rates of tropical cirrus clouds are determined using broadband hemispheric irradiance data. Additionally, a broadband mass absorption coefficient is defined and used to relate emissivity to water content. The data used were collected by the National Center for Atmospheric Research (NCAR) Sabreliner during the GARP Atlantic Tropical Experiment (GATE) in the summer of 1974. Three case studies are analyzed showing that these tropical cirrus clouds approached an emissivity of 1.0 within a vertical distance of 1.0 km. Broadband mass absorption coefficients ranging from 0.076 to 0.096 sq m per g are derived. A comparison of these results with other work suggests that tropical cirrus cloud emissivities may be significantly larger than heretofore believed. Ice water content of the clouds were deduced from data collected by a one-dimensional particle spectrometer. Analyses of the ice water content and the observed particle size distributions are presented.

Griffith, K. T.↗
NASA NTRS2009

Diagnosing the Ice Crystal Enhancement Factor in the Tropics

Recent modeling studies have revealed that ice crystal number concentration is one of the dominant factors in the effect of clouds on radiation. Since the ice crystal enhancement factor and ice nuclei concentration determine the concentration, they are both important in quantifying the contribution of increased ice nuclei to global warming. In this study, long-term cloud-resolving model (CRM) simulations are compared with field observations to estimate the ice crystal enhancement factor in tropical and midlatitudinal clouds, respectively. It is found that the factor in tropical clouds is ~10 3-104 times larger than that of mid-latitudinal ones, which makes physical sense because entrainment and detrainment in the Tropics are much stronger than in middle latitudes. The effect of entrainment/detrainment on the enhancement factor, especially in tropical clouds, suggests that cloud microphysical parameterizations should be coupled with subgrid turbulence parameterizations within CRMs to obtain a more accurate depiction of cloud-radiative forcing.

Zeng, Xiping↗
DOE OSTI2020

Characterizing the Small-Scale Dynamical, Ice Microphysical, and Residual Aerosol Properties of Mid-Latitude Cold Clouds: A Pilot Study (Final Report)

Our understanding of cirrus clouds has been advancing rapidly due to improvements in measurements made inside clouds, computer cloud models, and laboratory experimentation. This advancement in knowledge has made it clear that cirrus are complicated systems where the intricate interactions among dynamic air motions, solar and terrestrial radiation, ice crystal growth, and water and air chemistry can substantially influence cirrus structure and evolution. Measurements made inside clouds have shown that cirrus crystals are often complex with shapes that are often unclassifiable, especially at small sizes. Laboratory measurements have revealed that the ice crystal surface is complex, even at small sizes. Recent laboratory and satellite studies show that this surface complexity modifies the radiative properties of cirrus clouds in important ways. Moreover, observations and computer cloud modeling work show that the larger and smaller scale properties of cirrus are sensitive to the interplay between small-scale air motions and the aerosol articles upon which cirrus ice crystals form. Taken together, these studies indicate that accurately accounting for the radiative properties of cirrus clouds requires knowing the air motions and aerosol properties that influence the number concentration and crystal size, along with an understanding of the surface properties of vapor grown ice. Although this prior work has been illuminating, there have been few studies that provide detailed shape and surface complexity measurements for the small ice crystals that often compose cirrus clouds.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1998

Tropical Oceanic Precipitation Processes over Warm Pool: 2D and 3D Cloud Resolving Model Simulations

Rainfall is a key link in the hydrologic cycle as well as the primary heat source for the atmosphere, The vertical distribution of convective latent-heat release modulates the large-scale circulations of the tropics, Furthermore, changes in the moisture distribution at middle and upper levels of the troposphere can affect cloud distributions and cloud liquid water and ice contents. How the incoming solar and outgoing longwave radiation respond to these changes in clouds is a major factor in assessing climate change. Present large-scale weather and climate models simulate cloud processes only crudely, reducing confidence in their predictions on both global and regional scales. One of the most promising methods to test physical parameterizations used in General Circulation Models (GCMS) and climate models is to use field observations together with Cloud Resolving Models (CRMs). The CRMs use more sophisticated and physically realistic parameterizations of cloud microphysical processes, and allow for their complex interactions with solar and infrared radiative transfer processes. The CRMs can reasonably well resolve the evolution, structure, and life cycles of individual clouds and cloud systems, The major objective of this paper is to investigate the latent heating, moisture and momenti,im budgets associated with several convective systems developed during the TOGA COARE IFA - westerly wind burst event (late December, 1992). The tool for this study is the Goddard Cumulus Ensemble (CCE) model which includes a 3-class ice-phase microphysical scheme, The model domain contains 256 x 256 grid points (using 2 km resolution) in the horizontal and 38 grid points (to a depth of 22 km depth) in the vertical, The 2D domain has 1024 grid points. The simulations are performed over a 7 day time period. We will examine (1) the precipitation processes (i.e., condensation/evaporation) and their interaction with warm pool; (2) the heating and moisture budgets in the convective and stratiform regions; (3) the cloud (upward-downward) mass fluxes in convective and stratiform regions; (4) characteristics of clouds (such as cloud size, updraft intensity and cloud lifetime) and the comparison of clouds with Radar observations. Differences and similarities in organization of convection between simulated 2D and 3D cloud systems. Preliminary results indicated that there is major differences between 2D and 3D simulated stratiform rainfall amount and convective updraft and downdraft mass fluxes.

Tao, W.- K.↗
NASA NTRSDate not supplied

Clouds in the Arctic Climate System: A Force for Change?

Clouds play a central role in the global climate system through the modulation of Earth’s energy flows and as a mediator of precipitation. In the Arctic, clouds are also a major player; however, the processes that govern cloud evolution in the Arctic differ from most of the other regions of the globe. Thus, clouds are a key “wildcard” within the Arctic climate system that could have a substantial influence on the Arctic climate system response to anthropogenic forcing. What is the role of clouds within the phenomenon known as Arctic Amplification? This is question does not have a clear answer. Clouds seem to be a center to the important processes driving Arctic Amplification (e.g., the atmospheric response to sea ice loss and airmass transformation), however feedback analysis studies indicate that net cloud feedback in the Arctic is small. This seminar discusses the role of clouds within the Arctic Amplification processes reviewing aspects of what we know about Arctic clouds and the uncertainties that limit our ability to model them. Results from recently published and ongoing work are presented that provide an observationally-based estimate of the cloud-sea ice feedback and evaluate cloud properties within models. The goal of this presentation is to ignite a discussion and new collaborations around the best approaches to resolving uncertainties related to the role of clouds with the Arctic system and how to better represent Arctic clouds in models.

Patrick C Taylor↗
NASA NTRS1989

Diffusion and infrared properties of molecules in ice mantles

Within dense molecular clouds the formation of frozen icy mantles on interstellar dust grains is thought to be the result of various growth conditions. The molecules, which make up the ice mantles are probably completely mixed. To study the physical properties of such ice mixtures the experiments were performed on the evaporation processes and on the spectroscopic properties of CO, CO2, and CH4 in water rich ices. The decrease in concentration of volatile molecules in ice samples deposited at 10 K and subsequently heated is found to occur essentially in two steps. The first one, corresponding to an evaporation of part of the volatile molecules, starts at about 25 K for CO, 32 K for CH4, and 70 K for CO2. During the crystallization of H2O ice at temperatures greater than 120 K a second evaporation occurs leading to the complete disappearance of the volatile molecules in the solid phase. The main astrophysical implications of the diffusion and spectroscopic behaviors are presented. The possible effects of a heating source on the fraction of volatile molecules, such as CO trapped in grain mantles, are discussed.

Schmitt, Bernard↗
NASA NTRS2018

Design and Development of a Laboratory-Scale Ice Adhesion Testing Device

When an aircraft traverses through clouds containing supercooled water droplets, in-flight icing can occur that negatively affects vehicle performance by increasing weight and drag leading to loss of lift. Super-cooled water droplets present in clouds that impact vehicle surfaces can lead to inflight icing any time during the year.1 Most events occur at temperatures ranging from 0 to -20degC. Ice generated on the aircraft can vary between clear/glaze, rime, and mixed (Fig. 1) depending on air temperature (-5 to -20degC), liquid water content (0.3-0.6 g/m3), and droplet size (median volumetric diameter of 15-40 μm). Current strategies to remove ice are based on active technologies such as pneumatic boots, heated surfaces, and deicing agents (i.e., ethylene- and propylene-based glycols). The latter have potential environmental concerns. A passive approach to mitigate accreting ice that is actively being investigated are protective coatings. An ice mitigating coating could potentially be used as a stand-alone material, but more likely in combination with an active approach. In the latter scenario, potential reduction in power consumption by the active approach may be realized. To determine the ice adhesion strength of impact ice that is representative of the aircraft environment is not a trivial matter. Test methods utilizing slowly formed ice (i.e., freezer ice) do not accurately simulate this environment. Likewise, some testing methodologies involve sample relocation from the icing environment to the test chamber that can result in thermal shock to the sample, thus affecting the results. The Adverse Environment Rotor Test Stand (AERTS) located at Pennsylvania State University (PSU) has been demonstrated to simulate impact icing conditions within the icing envelope for the determination of ice adhesion shear strength (IASS) without removal/relocation of the sample.2 Due to the confidence in results obtained from AERTS, this instrument is in high demand and requires a significant amount of lead time and capital investment to obtain IASS results. As a solution for quickly and economically screening coatings in a controlled manner under impact icing conditions, a laboratory-scale ice adhesion test and dead blades were then removed from the rotor/blade assembly to obtain the final mass. The IASS of the live blade was determined from the difference in mass (before and after testing) of the live and dead blades, the ice shed area, and the rpm of the shed event. The same live blade sample was tested in triplicate at all three test temperatures. Surface roughness was determined using a Bruker Dektak XT Stylus Profilometer. Measurements were conducted using a 12.5 μm tip at a vertical range of 65.5 μm with an applied force of 3 mg. Data were collected over a 1.0 mm length at a resolution of 0.056 μm/point. Five single line scans at different locations were collected and processed using a two-point leveling subtraction. The resultant Ra (arithmetic roughness) and Rq (root mean square roughness) average values were calculated.

Smith, Joseph G., Jr.↗
DOE OSTI2022

thermocldphase

ARM VAP deriving the thermodynamic phase of water in clouds.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2004

Dynamical Modeling of Mars' Paleoclimate

This report summarizes work undertaken under a one-year grant from the NASA Mars Fundamental Research Program. The goal of the project was to initiate studies of the response of the Martian climate to changes in planetary obliquity and orbital elements. This work was undertaken with a three-dimensional numerical climate model based on the Geophysical Fluid Dynamics Laboratory (GFDL) Skyhi General Circulation Model (GCM). The Mars GCM code was adapted to simulate various obliquity and orbital parameter states. Using a version of the model with a basic water cycle (ice caps, vapor, and clouds), we examined changes in atmospheric water abundances and in the distribution of water ice sheets on the surface. This work resulted in a paper published in the Journal of Geophysical Research - Planets. In addition, the project saw the initial incorporation of a regolith water transport and storage scheme into the model. This scheme allows for interaction between water in the pores of the near subsurface (<3m) and the atmosphere. This work was not complete by the end of the one-year grant, but is now continuing within the auspices of a three-year grant of the same title awarded by the Mars Fundamental Research Program in late 2003.

Richardson, Mark I.↗
NASA NTRS2001

Tropical Oceanic Precipitation Processes Over Warm Pool: 2D and 3D Cloud Resolving Model Simulations

Rainfall is a key link in the hydrologic cycle as well as the primary heat source for the atmosphere. The vertical distribution of convective latent-heat release modulates the large-scale circulations of the topics. Furthermore, changes in the moisture distribution at middle and upper levels of the troposphere can affect cloud distributions and cloud liquid water and ice contents. How the incoming solar and outgoing longwave radiation respond to these changes in clouds is a major factor in assessing climate change. Present large-scale weather and climate model simulate processes only crudely, reducing confidence in their predictions on both global and regional scales. One of the most promising methods to test physical parameterizations used in General Circulation Models (GCMs) and climate models is to use field observations together with Cloud Resolving Models (CRMs). The CRMs use more sophisticated and physically realistic parameterizations of cloud microphysical processes, and allow for their complex interactions with solar and infrared radiative transfer processes. The CRMs can reasonably well resolve the evolution, structure, and life cycles of individual clouds and clouds systems. The major objective of this paper is to investigate the latent heating, moisture and momentum budgets associated with several convective systems developed during the TOGA COARE IFA - westerly wind burst event (late December, 1992). The tool for this study is the Goddard Cumulus Ensemble (GCE) model which includes a 3-class ice-phase microphysics scheme.

Tao, W.-K.↗