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At least 1,585 records · Page 88

On the Correspondence Between Atmosphere-Only and Coupled Simulations for Radiative Feedbacks and Forcing From CO 2

Atmosphere-only experiments are widely used to investigate climate feedbacks simulated in more computationally expensive fully coupled global climate model simulations. We confirm that this remains a valid approach by comparing the radiative feedbacks and forcing between coupled and atmosphere-only simulations for the latest models taking part in the 6th phase of the Coupled Model Intercomparison Project (CMIP6). For global-mean cloud feedbacks, we find a better than previously known correspondence between these experiments, which applies even to the response of individual cloud properties (amount, altitude, and optical depth) and holds even when considering atmosphere-only simulations of only 1 yr duration. For regional cloud feedbacks, the correspondence between the two experiments is generally present at every geographic location except for the tropical Pacific but takes longer experiments to reveal. For the lapse rate and surface albedo feedbacks, the correspondence between the two experiments is weaker due to the non-uniform warming pattern and loss of sea ice in the coupled experiment. For the across-model relationship between 4xCO 2 effective radiative forcing and feedback, we find a different behavior across experiments in CMIP6 than in CMIP5, casting doubt on the physical significance of previous results that highlighted an anti-correlation between the two quantities. Overall, these results confirm the utility of atmosphere-only experiments particularly to study cloud feedbacks, which are the dominant source of inter-model spread in climate sensitivity.

58 GEOSCIENCES↗

Molecular Chemistry of Organic Aerosols Through the Application of High Resolution Mass Spectrometry

Understanding of molecular composition and fundamental chemical transformations of organic aerosols (OA) during their formation and aging is both a major challenge and the area of greatest uncertainty in atmospheric research. Particularly little is known about fundamental relationship between the chemical composition and physicochemical properties of OA, their atmospheric history, evolution, and impact on the environment. Ambient soft-ionization methods combined with high-resolution mass spectrometry (HR-MS) analysis provide detailed information on the molecular content of OA that is pivotal for improved understanding of their complex composition, multi-phase aging chemistry, direct (light absorption and scattering) and indirect (aerosol-cloud interactions) effects on atmospheric radiation and climate, and health effects. The HR-MS methods can detect thousands of individual OA constituents at once, provide their elemental formulae from accurate mass measurements, and provide structural information based on tandem mass spectrometry. Integration with additional analytical tools, such as chromatography and UV/Vis absorption spectroscopy, makes it possible to further separate OA compounds by their polarity and ability to absorb solar radiation. The goal of this perspective is to describe modern HR-MS methods, review recent applications to field and laboratory studies of OA, and explain how the information obtained from HR-MS methods can be translated into improved understanding of OA chemistry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Surfactants and cloud droplet activation: A systematic extension of Köhler theory based on analysis of droplet stability

The activation of aerosol particles to form cloud droplets, a necessary first step in cloud formation, controls much of the impact that aerosols have on clouds and climate. Recently, there has been a surge of interest in extending the Köhler theory of cloud droplet activation to include surface active (typically organic) as well as water-soluble (typically inorganic) aerosol components, but a systematic framework for doing this has yet to be developed. Here, we apply a droplet stability analysis to this end. Ideal and Szyszkowski–Langmuir surfactant models are analyzed to demonstrate the new approach, but the underlying theoretical framework is fundamental and model free. A key finding is that superficial densities at the cloud activation threshold (Köhler maximum) are significantly sub-monolayer, with fractional coverage ranging from 69% to 85% for the organic compounds and mixtures studied. The result, significant for model inventories of cloud condensation nuclei, is a weakening of the surfactant effect relative to expectations based on bulk sample measurements. Analytical results are obtained for the loci of Köhler maxima and applied to aerosol mixtures containing an arbitrary number of water-soluble and surfactant components.

54 ENVIRONMENTAL SCIENCES↗

Merged-beams reaction studies of O + H{sub 3}{sup +}

We have measured the reaction of O+H{sub 3}{sup +} forming OH{sup +} and H{sub 2}O{sup +}. This is believed to be one of the key gas-phase astrochemical processes initiating the formation of water molecules in dense molecular clouds. For this work, we have used a novel merged fast-beams apparatus that overlaps a beam of H{sub 3}{sup +} onto a beam of ground-term neutral O. Here, we present cross-section data for forming OH{sup +} and H{sub 2}O{sup +} at relative energies from ≈3.5 meV to ≈15.5 and 0.13 eV, respectively. Measurements were performed for statistically populated O({sup 3}P{sub J}) in the ground term reacting with hot H{sub 3}{sup +} (with an internal temperature of ∼2500–3000 K). From these data, we have derived rate coefficients for translational temperatures from ≈27 K to ∼10{sup 5} K for the formation of OH{sup +} and ∼10{sup 3} K for the formation of H{sub 2}O{sup +}. In order to convert these results to a thermal rate coefficient suitable for astrochemistry, we have added the results together for both exit channels and scaled the summed data on statistically populated oxygen to thermally populated oxygen. For this we have used theory as a guide, thereby accounting for the temperature dependence of the O fine-structure levels. Our results are in good agreement with two independent flowing afterglow measurements at a temperature of ≈300 K, and with a corresponding level of H{sub 3}{sup +} internal excitation. This good agreement suggests that the internal excitation of the H{sub 3}{sup +} does not play a significant role in this reaction. The Langevin rate coefficient is in reasonable agreement with the experimental results at 10 K but a factor of ∼2 larger at 300 K. The two published classical trajectory studies using quantum-mechanical potential energy surfaces lie a factor of ∼1.5 above our experimental results over this 10–300 K range.

74 ATOMIC AND MOLECULAR PHYSICS↗

Unexpectedly acidic nanoparticles formed in dimethylamine-ammonia-sulfuric-acid nucleation experiments at CLOUD

New particle formation driven by acid–base chemistry was initiated in the CLOUD chamber at CERN by introducing atmospherically relevant levels of gas-phase sulfuric acid and dimethylamine (DMA). Ammonia was also present in the chamber as a gas-phase contaminant from earlier experiments. The composition of particles with volume median diameters (VMDs) as small as 10 nm was measured by the Thermal Desorption Chemical Ionization Mass Spectrometer (TDCIMS). Particulate ammonium-to-dimethylaminium ratios were higher than the gas-phase ammonia-to-DMA ratios, suggesting preferential uptake of ammonia over DMA for the collected 10–30 nm VMD particles. This behavior is not consistent with present nanoparticle physicochemical models, which predict a higher dimethylaminium fraction when NH 3 and DMA are present at similar gas-phase concentrations. Despite the presence in the gas phase of at least 100 times higher base concentrations than sulfuric acid, the recently formed particles always had measured base : acid ratios lower than 1 : 1. The lowest base fractions were found in particles below 15 nm VMD, with a strong size-dependent composition gradient. The reasons for the very acidic composition remain uncertain, but a plausible explanation is that the particles did not reach thermodynamic equilibrium with respect to the bases due to rapid heterogeneous conversion of SO 2 to sulfate. Furthermore, these results indicate that sulfuric acid does not require stabilization by ammonium or dimethylaminium as acid–base pairs in particles as small as 10 nm.

54 ENVIRONMENTAL SCIENCES↗

Night-time observations of snow using visible imagery

Consideration is given to the possibility of increasing the frequency of satellite snow cover observations in the visible range by using the light reflected off the moon as an illumination source for nighttime observations. Images obtained at night by DMSP satellites orbiting in the noon-midnight plane are presented which were obtained at various phases of the moon. It is concluded that DMSP visible imagery can be used to detect snow cover during those periods when the moon is over the local horizon and is between the first quarter phase and the last quarter phase, which amounts to around five additional days a month allowing for cloud cover. The high frequency of observation of a given area provided by a light-sensitivity imager would be an important feature of a dedicated water-resources satellite.

Foster, J. L.↗

Remote sensing of cloud radiation and microphysical parameters

Multispectral cloud radiometer (MCR) data, retrieved from a radiometer installed in a nadir viewing position on a high-altitude aircraft flying at 200 m/s and at an altitude of 60,000 ft above the mean sea level, are analyzed. The data discussed were obtained in the 0.754, 0.7609, 0.7634, 1.626, 2.125, and 11.38-micron channels, and are compared to lidar-derived profiles. Among the cloud parameters under consideration are the cloud scaled optical thickness, cloudtop altitude, scaled volume scattering coefficient, particle thermodynamic phase, mean particle size, and cloudtop temperature.

Wu, M.-L. C.↗

Tropical synoptic composites in VAS, OLR and TOVS radiance data

The horizontal structure of specific tropical synoptic features are compared with the features of a zonal mean ITCZ using four different forms of satellite radiance data: daily gridded OLR data, GOES VAS water vapor imagery, brightness temperatures from TOVS water vapor channels (6.7 and 7.3 microns), and brightness temperature vectors for a complete set of TOVS channels. All of the data are composited over many events to minimize the effects of missing data, sampling errors, and system variability. The major differences between the observing systems are examined, focusing on resolution and clouds. It is found that the ITCZ exhibits a zonally symmetric convective phase and an enhanced regional convective phase (plumes), both of which can be differentiated from climatological mean behavior.

Mcguirk, James P.↗

Empirical relationships between gas abundances and UV selective extinction

Several studies of gas-phase abundances in lines of sight through the outer edges of dense clouds are summarized. These lines of sight have 0.4 less than E(B-V) less than 1.1 and have inferred spatial densities of a few hundred cm(-3). The primary thrust of these studies has been to compare gaseous abundances in interstellar clouds that have various types of peculiar selective extinction. To date, the most notable result has been an empirical relationship between the CN/Fe I abundance ratio and the depth of the 2200 A extinction bump. It is not clear at the present time, however, whether these two parameters are linearly correlated or the data are organized into two discrete ensembles. Based on 19 samples and assuming the clouds form discrete ensembles, lines of sight that have a CN/Fe I abundance ratio greater than 0.3 (dex) appear to have a shallow 2.57 plus or minus 0.55 bump compared to 3.60 plus or minus 0.36 for other dense clouds and compared to the 3.6 Seaton (1979) average. The difference in the strength of the extinction bump between these two ensembles is 1.03 plus or minus 0.23. Although a high-resolution IUE survey of dense clouds is far from complete, the few lines of sight with shallow extinction bumps all show preferential depletion of certain elements, while those lines of sight with normal 2200 A bumps do not. Ca II, Cr II, and Mn II appear to exhibit the strongest preferential depletion compared to S II, P II, and Mg II. Fe II and Si II depletions also appear to be enhanced somewhat in the shallow-bump lines of sight. It should be noted that Copernicus data suggest all elements, including the so-called nondepletors, deplete in diffuse clouds (Snow and Jenkins 1980, Joseph 1988). Those lines of sight through dense clouds that have normal 2200 A extinction bumps appear to be extensions of the depletions found in the diffuse interstellar medium. That is, the overall level of depletion is enhanced, but the element-to-element abundances are similar to those in diffuse clouds. In a separate study, the abundances of neutral atoms were studied in a dense cloud having a shallow 2200 A bump and in one with a normal strength bump.

Joseph, Charles L.↗

Stratospheric Heterogeneous Chemistry and Microphysics: Model Development, Validation and Applications

The objectives of this project are to: define the chemical and physical processes leading to stratospheric ozone change that involve polar stratospheric clouds (PSCS) and the reactions occurring on the surfaces of PSC particles; study the formation processes, and the physical and chemical properties of PSCS, that are relevant to atmospheric chemistry and to the interpretation of field measurements taken during polar stratosphere missions; develop quantitative models describing PSC microphysics and heterogeneous chemical processes; assimilate laboratory and field data into these models; and calculate the extent of chemical processing on PSCs and the impact of specific microphysical processes on polar composition and ozone depletion. During the course of the project, a new coupled microphysics/physical-chemistry/ photochemistry model for stratospheric sulfate aerosols and nitric acid and ice PSCs was developed and applied to analyze data collected during NASA's Arctic Airborne Stratospheric Expedition-II (AASE-II) and other missions. In this model, detailed treatments of multicomponent sulfate aerosol physical chemistry, sulfate aerosol microphysics, polar stratospheric cloud microphysics, PSC ice surface chemistry, as well as homogeneous gas-phase chemistry were included for the first time. In recent studies focusing on AASE measurements, the PSC model was used to analyze specific measurements from an aircraft deployment of an aerosol impactor, FSSP, and NO(y) detector. The calculated results are in excellent agreement with observations for particle volumes as well as NO(y) concentrations, thus confirming the importance of supercooled sulfate/nitrate droplets in PSC formation. The same model has been applied to perform a statistical study of PSC properties in the Northern Hemisphere using several hundred high-latitude air parcel trajectories obtained from Goddard. The rates of ozone depletion along trajectories with different meteorological histories are presently being systematically evaluated to identify the principal relationships between ozone loss and aerosol state. Under this project, we formulated a detailed quantitative model that predicts the multicomponent composition of sulfate aerosols under stratospheric conditions, including sulfuric, nitric, hydrochloric, hydrofluoric and hydrobromic acids. This work defined for the first time the behavior of liquid ternary-system type-1b PSCS. The model also allows the compositions and reactivities of sulfate aerosols to be calculated over the entire range of environmental conditions encountered in the stratosphere (and has been incorporated into a trajectory/microphysics model-see above). Important conclusions that derived from this work over the last few years include the following: the HNO3 content of liquid-state aerosols dominate PSCs below about 195 K; the freezing of nitric acid ice from sulfate aerosol solutions is likely to occur within a few degrees K of the water vapor frost point; the uptake and reactions of HCl in liquid aerosols is a critical component of PSC heterogeneous chemistry. In a related application of this work, the inefficiency of chlorine injection into the stratosphere during major volcanic eruptions was explained on the basis of nucleation of sulfuric acid aerosols in rising volcanic plumes leading to the formation of supercooled water droplets on these aerosols, which efficiently scavenges HCl via precipitation.

Turco, Richard P.↗

A Melting Layer Model for Passive/Active Microwave Remote Sensing Applications: Model Formulation and Comparison with Observations - Part 1

In this study, a 1-D steady-state microphysical model which describes the vertical distribution of melting precipitation particles is developed. The model is driven by the ice-phase precipitation distributions just above the freezing level at applicable gridpoints of "parent" 3-D cloud-resolving model (CRM) simulations. It extends these simulations by providing the number density and meltwater fraction of each particle in finely separated size categories through the melting layer. The depth of the modeled melting layer is primarily determined by the initial material density of the ice-phase precipitation. The radiative properties of melting precipitation at microwave frequencies are calculated based upon different methods for describing the dielectric properties of mixed phase particles. Particle absorption and scattering efficiencies at the Tropical Rainfall Measuring Mission Microwave Imager frequencies (10.65 to 85.5 GHz) are enhanced greatly for relatively small (approx. 0.1) meltwater fractions. The relatively large number of partially-melted particles just below the freezing level in stratiform regions leads to significant microwave absorption, well-exceeding the absorption by rain at the base of the melting layer. Calculated precipitation backscatter efficiencies at the Precipitation Radar frequency (13.8 GHz) increase in proportion to the particle meltwater fraction, leading to a "bright-band" of enhanced radar reflectivities in agreement with previous studies. The radiative properties of the melting layer are determined by the choice of dielectric models and the initial water contents and material densities of the "seeding" ice-phase precipitation particles. Simulated melting layer profiles based upon snow described by the Fabry-Szyrmer core-shell dielectric model and graupel described by the Maxwell-Garnett water matrix dielectric model lead to reasonable agreement with radar-derived melting layer optical depth distributions. Moreover, control profiles that do not contain mixed-phase precipitation particles yield optical depths that are systematically lower than those observed. Therefore, the use of the melting layer model to extend 3-D CRM simulations appears justified, at least until more realistic spectral methods for describing melting precipitation in high-resolution, 3-D CRM's are implemented.

Olson, William S.↗

GEWEX Cloud System Study (GCSS) Working Group on Cirrus Cloud Systems (WG2)

Status, progress and plans will be given for current GCSS (GEWEX Cloud System Study) WG2 (Working Group on Cirrus Cloud Systems) projects, including: (a) the Idealized Cirrus Model Comparison Project, (b) the Cirrus Parcel Model Comparison Project (Phase 2), and (c) the developing Hurricane Nora extended outflow model case study project. Past results will be summarized and plans for the upcoming year described. Issues and strategies will be discussed. Prospects for developing improved cloud parameterizations derived from results of GCSS WG2 projects will be assessed. Plans for NASA's CRYSTAL-FACE (Cirrus Regional Study of Tropical Anvils and Layers - Florida Area Cirrus Experiment) potential opportunities for use of those data for WG2 model simulations (future projects) will be briefly described.

Starr, David↗

Warm Rain Processes Over the Tropical Oceans and Implications on Climate Change

In this talk, we will first show results from TRMM regarding the characteristics of warm rains over the tropical oceans, and the dependence of rate of warm rain production on sea surface temperature. Results lead to the hypothesis that warm rain production efficiency, i.e., autoconversion, may be increased in a warm climate. We use the GEOS-II GCM to test this hypothesis. Our modeling results show that in a climate with increased rate of autoconversion, the total rain amount is increased, with warm rain contributing to a larger portion of the increase. The abundant rainout of warm precipitation at middle to low levels causes a reduction of high cloud cover due to the depletion of water available for ice-phase rain production. As a result, more isolated, but more intense penetrative convection develops. Results also show that increased autoconversion reduces the convective adjustment time scale tends, implying a faster recycling of atmospheric water. Most interestingly, the increased low level heating associated with warm rain leads to more energetic Madden and Julian oscillations in the tropics, with well-defined eastward propagation. While reducing the autoconversion leads to an abundant mix of westward and eastward tropical disturbance on daily to weekly time scales. The causes of the sensitivity of the dynamical regimes to the microphysics parameterization in the GCM will be discussed.

Lau, William K. M.↗

A Search for PAHs in Astrophysical Environments

We present the results of a dedicated search for the spectral signatures in the visible range of neutral polycyclic aromatic hydrocarbons (PAHs) in astronomical observations representing various astrophysical environments, probing a total column of line of sight material corresponding to Av=50. Laboratory measurements of PAHs in simulated astrophysical conditions are now available (see contribution of Salama et al.) which provide for the first time the exact wavelengths for the spectral features of these molecules, as well as detailed information on the intrinsic line profiles and oscillator strengths. These measurements therefore allow a direct comparison to astronomical observations and an estimate of, or upper limit to, the abundance of individual PAHs in space. As the column densities for individual PAHs in interstellar or circumstellar lines of sight are expected to be very low, such a comparison and analysis requires astronomical observations at very high signal to noise. We present such a data set here for lines of sight representing diffuse clouds and circumstellar environments of carbon stars, and their comparison with gas phase spectra of a representative set of free, cold PAHs.

Salama, F.↗

Visualizing Airborne and Satellite Imagery

Remote sensing is a process able to provide information about Earth to better understand Earth's processes and assist in monitoring Earth's resources. The Cloud Absorption Radiometer (CAR) is one remote sensing instrument dedicated to the cause of collecting data on anthropogenic influences on Earth as well as assisting scientists in understanding land-surface and atmospheric interactions. Landsat is a satellite program dedicated to collecting repetitive coverage of the continental Earth surfaces in seven regions of the electromagnetic spectrum. Combining these two aircraft and satellite remote sensing instruments will provide a detailed and comprehensive data collection able to provide influential information and improve predictions of changes in the future. This project acquired, interpreted, and created composite images from satellite data acquired from Landsat 4-5 Thematic Mapper (TM) and Landsat 7 Enhanced Thematic Mapper plus (ETM+). Landsat images were processed for areas covered by CAR during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCT AS), Cloud and Land Surface Interaction Campaign (CLASIC), Intercontinental Chemical Transport Experiment-Phase B (INTEXB), and Southern African Regional Science Initiative (SAFARI) 2000 missions. The acquisition of Landsat data will provide supplemental information to assist in visualizing and interpreting airborne and satellite imagery.

Bierwirth, Victoria A.↗

Aerosol Comparisons Between Observations and Models: AeroCom and ABC

I will represent the AeroCom community to the Atmospheric Brown Cloud (ABC) workshop. I will summarize the activities and results from AeroCom Phase I activities in the past 8 years and introduce the new results and activities in the current AeroCom Phase II. We hope to coordinate some activities with the ABC community to share model output and data access for model evaluations, comparisons, and assessment.

Chin, Mian↗

Vertical Profile of Cloud Optical Parameters Derived from Airborne Measurements Above, Inside and Below Clouds

Past strategies for retrieving cloud optical properties from remote sensing assumed significant limits for desired parameters such as semi-infinite optical thickness, single scattering albedo equaling unity (non-absorbing scattering), absence of spectral dependence of the optical thickness, etc., and only one optical parameter could be retrieved (either optical thickness or single scattering albedo). Here, we demonstrate a new method based on asymptotic theory for thick atmospheres, and the presence of a diffusion domain within the clouds that does not put restrictions and makes it possible to get two or even three optical parameters (optical thickness, single scattering albedo and phase function asymmetry parameter) for every wavelength independently. We applied this method to measurements of angular distribution of solar radiation above, inside and below clouds, obtained with NASA's Cloud Absorption Radiometer (CAR) over two cases of marine stratocumulus clouds; first case, offshore of Namibia and the second case, offshore of California. The observational and retrieval errors are accounted for by regularization, which allows stable and smooth solutions. Results show good potential for parameterization of the shortwave radiative properties (reflection, transmission, radiative divergence and heating rate) of water clouds.

airborne observations↗

IONIZATION IN ATMOSPHERES OF BROWN DWARFS AND EXTRASOLAR PLANETS. II. DUST-INDUCED COLLISIONAL IONIZATION

Observations have shown that continuous radio emission and also sporadic H{alpha} and X-ray emission are prominent in singular, low-mass objects later than spectral class M. These activity signatures are interpreted as being caused by coupling of an ionized atmosphere to the stellar magnetic field. What remains a puzzle, however, is the mechanism by which such a cool atmosphere can produce the necessary level of ionization. At these low temperatures, thermal gas processes are insufficient, but the formation of clouds sets in. Cloud particles can act as seeds for electron avalanches in streamers that ionize the ambient gas, and can lead to lightning and indirectly to magnetic field coupling, a combination of processes also expected for protoplanetary disks. However, the precondition is that the cloud particles are charged. We use results from DRIFT-PHOENIX model atmospheres to investigate collisional processes that can lead to the ionization of dust grains inside clouds. We show that ionization by turbulence-induced dust-dust collisions is the most efficient kinetic process. The efficiency is highest in the inner cloud where particles grow quickly and, hence, the dust-to-gas ratio is high. Dust-dust collisions alone are not sufficient to improve the magnetic coupling of the atmosphere inside the cloud layers, but the charges supplied either on grains or within the gas phase as separated electrons can trigger secondary nonlinear processes. Cosmic rays are likely to increase the global level of ionization, but their influence decreases if a strong, large-scale magnetic field is present as on brown dwarfs. We suggest that although thermal gas ionization declines in objects across the fully convective boundary, dust charging by collisional processes can play an important role in the lowest mass objects. The onset of atmospheric dust may therefore correlate with the anomalous X-ray and radio emission in atmospheres that are cool, but charged more than expected by pure thermal ionization.

79 ASTRONOMY AND ASTROPHYSICS↗