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At least 109 records · Page 6

Developing an Aircraft-Based Angular Distribution Model of Solar Reflection from Wildfire Smoke to Aid Satellite-Based Radiative Flux Estimation

This study examines the angular distribution of scattered solar radiation associated with wildfire smoke aerosols observed over boreal forests in Canada during the ARCTAS (Arctic Research of the Composition of the Troposphere from Aircraft and Satellites) campaign. First, it estimates smoke radiative parameters (550 nm optical depth of 3.9 and single scattering albedo of 0.90) using quasi-simultaneous multiangular and multispectral airborne measurements by the Cloud Absorption Radiometer (CAR). Next, the paper estimates the broadband top-of-atmosphere radiances that a satellite instrument such as the Clouds and the Earth’s Radiant Energy System (CERES) could have observed, given the narrowband CAR measurements made from an aircraft circling about a kilometer above the smoke layer. This estimation includes both an atmospheric correction that accounts for the atmosphere above the aircraft and a narrowband-to-broadband conversion. The angular distribution of estimated radiances is found to be substantially different than the angular model used in the operational data processing of CERES observations over the same area. This is because the CERES model is a monthly average model that was constructed using observations taken under smoke-free conditions. Finally, a sensitivity analysis shows that the estimated angular distribution remains accurate for a fairly wide range of smoke and underlying surface parameters. Overall, results from this work suggest that airborne CAR measurements can bring some substantial improvements in the accuracy of satellite-based radiative flux estimates.

Varnai, Tamas↗

Comparing Tropopause-Penetrating Convection Identifications Derived from NEXRAD and GOES over the Contiguous United States

Overshooting cloud tops (OTs) are a result of powerful updrafts that rapidly transport air from the troposphere to the lower stratosphere. Aside from the well-known relationships between strong updrafts and severe weather, the boundaries of updrafts, including the OT, are turbulent, which leads to irreversible mixing of air between the stratosphere and troposphere, altering the composition of both layers. In order to better understand the impact of OTs, knowing precisely when and where they occur is vital. Within the last decade remote-sensing observations from satellites and radars have been used to identify OTs, but the results thus far have not been entirely consistent due to challenges with accurately identifying OTs with these sensor datasets. This study compares OTs identified using NEXRAD reflectivity data from the GridRad dataset with an approach that uses GOES infrared (IR) data. The GridRad method estimates the altitude of echo tops directly from the radar pointing geometry, merging a combination of radars that enables products every 5 mins, with 2 km spatial and 1 km vertical grid spacing. The GOES satellite method uses spatial patterns in tropopause-relative IR brightness temperature to derive an OT likelihood. The study region covers a large part of the contiguous United States during selected active convection dates in 2017 and includes data from GOES-13/16. A large sample of OTs observed by NEXRAD and GOES-13/16 satellites are analyzed to better understand NEXRAD and IR observations of OTs, quantify agreement between the OT detection methods, and demonstrate how the 4x increase in spatial resolution from GOES-13 to GOES-16 impacts OT algorithm detection performance. The results show that for nearly time-matched scenes, with many severe storms, GOES-13 and -16 detection accuracy is quite comparable; however, some missed detections are attributed to poorer GOES-13 image resolution. It was found that GOES-13 OT regions are ~2 K warmer than GOES-16 on average, but such differences exceed 5 K for the most intense OT regions. It is found that false GOES IR-based detections are unavoidable, given that cold cloud pixels significantly colder than the tropopause from nearby or recently decayed OTs can persist within anvils for 15 minutes or more.

John W. Cooney↗

Strong Sensitivity of the Isotopic Composition of Methane to the Plausible Range of Tropospheric Chlorine

The C-13 isotopic ratio of methane, δC-13 of CH4, provides additional constraints on the CH4 budget to complement the constraints from CH4 observations. The interpretation of δC-13 observations is complicated, however, by uncertainties in the methane sink. The reaction of CH4 with Cl is highly fractionating, increasing the relative abundance of 13CH4, but there is currently no consensus on the strength of the tropospheric Cl sink. Global model simulations of halogen chemistry differ strongly from one another in terms of both the magnitude of tropospheric Cl and its geographic distribution. This study explores the impact of the inter-model diversity in Cl fields on the simulated δC-13 of CH4. We use a set of GEOS global model simulations with different predicted Cl fields to test the sensitivity of the δC-13 of CH4 to the diversity of Cl output from chemical transport models. We find that δC-13 is highly sensitive to both the amount and geographic distribution of Cl. Simulations with Cl providing 0.28% or 0.66% of the total CH4 loss bracket the δC-13 observations for a fixed set of emissions. Thus, even when Cl provides only a small fraction of the total CH4 loss and has a small impact on total CH4, it provides a strong lever on δC-13. Consequently, it is possible to achieve a good representation of total CH4 using widely different Cl concentrations, but the partitioning of CH4 loss between the OH and Cl reactions leads to strong differences in isotopic composition depending on which model’s Cl field is used. Comparing multiple simulations, we find that altering the tropospheric Cl field leads to approximately a 0.5‰ increase in δ(13)CH4for each percent increase in how much CH4 is oxidized by Cl. The geographic distribution and seasonal cycle of Cl also impacts the hemispheric gradient and seasonal cycle of δC-13. The large effect of Cl on δC-13 compared to total CH4 broadens the range of CH4 source mixtures that can be reconciled with δC-13 observations. Stronger constraints on tropospheric Cl are necessary to improve estimates of CH4 sources from δC-13 observations.

Global model simulations of halogen chemistry↗

Tropospheric Chemistry

The fundamental processes that control the chemical composition and cycles of the global troposphere and how these processes and properties affect the physical behavior of the atmosphere are examined. The long-term information needs for tropospheric chemistry are: to be able to predict tropospheric responses to perturbations, both natural and anthropogenic, of these cycles, and to provide the information required for the maintenance and effective future management of the atmospheric component of our global life support system. The processes controlling global tropospheric biogeochemical cycles include: the input of trace species into the troposphere, their long-range transport and distribution as affected by the mean wind and vertical venting, their chemical transformations, including gas to particle conversion, leading to the appearance of aerosols or aqueous phase reactions inside cloud droplets, and their removal from the troposphere via wet (precipitation) and dry deposition.

Mohnen, V.↗

Lithospheric and atmospheric interaction on the planet Venus

Lithospheric and atmospheric interaction in the planet Venus are discussed. The following subject areas are covered: (1) manifestation of exogenic processes using photogeological data; (2) the chemical composition and a chemical model of the troposphere of Venus; (3) the mineral composition of surface rock on Venus; and (4) the cycles of volatile components.

Volkov, Vladislav P.↗

The United States' Next Generation of Atmospheric Composition and Coastal Ecosystem Measurements: NASA's Geostationary Coastal and Air Pollution Events (GEO-CAPE) Mission

The Geostationary Coastal and Air Pollution Events (GEO-CAPE) mission was recommended by the National Research Council's (NRC's) Earth Science Decadal Survey to measure tropospheric trace gases and aerosols and coastal ocean phytoplankton, water quality, and biogeochemistry from geostationary orbit, providing continuous observations within the field of view. To fulfill the mandate and address the challenge put forth by the NRC, two GEO-CAPE Science Working Groups (SWGs), representing the atmospheric composition and ocean color disciplines, have developed realistic science objectives using input drawn from several community workshops. The GEO-CAPE mission will take advantage of this revolutionary advance in temporal frequency for both of these disciplines. Multiple observations per day are required to explore the physical, chemical, and dynamical processes that determine tropospheric composition and air quality over spatial scales ranging from urban to continental, and over temporal scales ranging from diurnal to seasonal. Likewise, high-frequency satellite observations are critical to studying and quantifying biological, chemical, and physical processes within the coastal ocean. These observations are to be achieved from a vantage point near 95deg-100degW, providing a complete view of North America as well as the adjacent oceans. The SWGs have also endorsed the concept of phased implementation using commercial satellites to reduce mission risk and cost. GEO-CAPE will join the global constellation of geostationary atmospheric chemistry and coastal ocean color sensors planned to be in orbit in the 2020 time frame.

Atmospheric composition↗

Interoperable Map Services with Performance Tuning for Earth Science Data through API-Tiles and Dynamic API-Styles

NASA’s Goddard Earth Sciences Data and Information Services Center (GES DISC) provides access to a wide range of global climate data from various satellite missions and models. However, the visualization and analysis of these data can be challenging due to their large volume, complex structure, and diverse formats. This study presents the implementation of interoperable map services (API-Maps) with performance tuning using API-Tiles and dynamic API-Styles. API-Maps is a standard for defining and exposing map services through RESTful (representational state transfer) APIs (application programming interfaces). API-Tiles is a technique for generating and delivering map tiles on demand from any data source. API-Styles is a method for dynamically applying styles to map tiles based on user preferences or data attributes. The use of API-Tiles and dynamic API-Styles enhances the performance and scalability of the map services, allowing for smooth and interactive visualization of large datasets. Two types of Earth Science data sources from the NASA GES DISC are used in the experiment: regularly gridded data, such as Global Precipitation Measurement (GPM) precipitation data, and low processing level data, such as low-level data of atmospheric composite measurements from the TROPOspheric Monitoring Instrument (TROPOMI) mission. Re-gridding of swath data (low level data - e.g. Level 2) of atmospheric composites (e.g. TROPOMI products, such as nitrogen dioxide, ozone and aerosol optical depth) is applied to enable the Web-based, interoperable, tiled, and styled mapping (rendering) services of such data. The results demonstrate the effectiveness of the proposed approach in providing fast and efficient access to Earth science data through interoperable map services.

Geographic Information System↗

Large-Scale Tropospheric Transport in the Chemistry-Climate Model Initiative (CCMI) Simulations

Understanding and modeling the large-scale transport of trace gases and aerosols is important for interpreting past (and projecting future) changes in atmospheric composition. Here we show that there are large differences in the global-scale atmospheric transport properties among the models participating in the IGAC SPARC Chemistry–Climate Model Initiative (CCMI). Specifically, we find up to 40% differences in the transport timescales connecting the Northern Hemisphere (NH) midlatitude surface to the Arctic and to Southern Hemisphere high latitudes, where the mean age ranges between 1.7 and 2.6 years. We show that these differences are related to large differences in vertical transport among the simulations, in particular to differences in parameterized convection over the oceans. While stronger convection over NH midlatitudes is associated with slower transport to the Arctic, stronger convection in the tropics and subtropics is associated with faster interhemispheric transport. We also show that the differences among simulations constrained with fields derived from the same reanalysis products are as large as (and in some cases larger than) the differences among free-running simulations, most likely due to larger differences in parameterized convection. Our results indicate that care must be taken when using simulations constrained with analyzed winds to interpret the influence of meteorology on tropospheric composition.

Orbe, Clara↗

Modeling and Observations of the Response of Tropical Tropospheric Ozone to ENSO

The El Nino-Southern Oscillation (ENSO) is the dominant mode of tropical variability on interannual time scales. ENSO appears to extend its influence into the chemical composition of the tropical troposphere, Recent results have revealed an ENSO induced wave-1 anomaly in observed tropical tropospheric column ozone, This results in a dipole over the western and eastern tropical Pacific, whereby differencing the two regions produces an ozone anomaly with an extremely high correlation to the Nino 3.4 Index. We have successfully reproduced this result using the Goddard Earth Observing System Version 5 (GEOS-5) general circulation model coupled to a comprehensive stratospheric and tropospheric chemical mechanism forced with observed sea surface temperatures over the past 25 years, An examination of the modeled ozone field reveals the vertical contributions of tropospheric ozone to the column over the western and eastern Pacific region, We will show targeted comparisons with SHADOZ ozonesondes over these regions to provide insight into the vertical structure. Also, comparisons with NASA's Aura satellite Microwave Limb Sounder (MLS) and Tropospheric Emissions Spectrometer (TES) instruments and other appropriate data sets will be shown. In addition, the water vapor response to ENSO will be compared to help illuminate its role relative to dynamics in impacting ozone concentrations. These results indicate that the tropospheric ozone response to ENSO is potentially a very useful chemistry-climate diagnostic and should be considered in future modeling assessments.

Oman, L. D.↗

ATMOS Stratospheric Deuterated Water and Implications for Troposphere-Stratosphere Transport

The isotopic composition of stratospheric water vapor is used as a tracer for the convective history of air injected into the stratosphere. Stratospheric profiles of HDO, H 2 O,CH 3 D, and CH 4 fro the ATMOS instrument, obtained over four missions from 1985-1994, are used to determine the initial deuterium-to-hydrogen ration of water vapor entering the stratosphere. We find that the initial DeltaD of stratospheric water is - 680 ± 80 (68 percent loss of deuterium), consistent with extrapolations from previous measurements at higher altitudes.

stratospheric↗

The Response of Tropospheric Ozone to ENSO in Observations and a Chemistry-Climate Simulation

The El Nino-Southern Oscillation (ENSO) is the dominant mode of tropical variability on interannual time scales. ENSO appears to extend its influence into the chemical composition of the tropical troposphere. Recent results have revealed an ENSO induced wave-l anomaly in observed tropical tropospheric column ozone. This results in a dipole over the western and eastern tropical Pacific, whereby differencing the two regions produces an ozone anomaly with an extremely high correlation to the Nino 3.4 Index. We have successfully reproduced this result using the Goddard Earth Observing System Version 5 (GEOS-5) general circulation model coupled to a comprehensive stratospheric and tropospheric chemical mechanism forced with observed sea surface temperatures over the past 25 years. An examination of the modeled ozone field reveals the vertical contributions of tropospheric ozone to the column over the western and eastern Pacific region. We will show targeted comparisons with observations from NASA's Aura satellite Microwave Limb Sounder (MLS), and the Tropospheric Emissions Spectrometer (TES) to provide insight into the vertical structure of ozone changes. The tropospheric ozone response to ENSO could be a useful chemistry-climate model evaluation tool and should be considered in future modeling assessments.

Oman, L. D.↗

Cloud chemistry on Jupiter

Chemical equilibrium models used currently to interpret observations of Jupiter are reexamined using new data defining thermal profiles, which are substantially different from those used in the previous models. A model is developed for the chemical reactions controlling the composition of the upper troposphere on Jupiter, specifically the cloud-forming region from 10 bar to 0.1 bar, which includes, for the first time, the effects of aqueous chemistry on the composition and the vertical distribution of many measurable species in the atmosphere, identifying the factors influencing their abundances above the H2O cloud. The thermodynamic data for potential condensates on Jupiter, i.e., NH3(s), NH4SH(s), (NH4)2S(s), and H2S(s), are reexamined, recognizing the lack of data on sulfides for the temperature range of interest on Jupiter. Vertical profiles of mixing ratios for CO2, H2S, NH3, and H2, obtained for several assumed bulk abundances with respect to solar, are presented.

Carlson, Barbara E.↗

Asian Influence Over the Western North Pacific during the Fall Season: Inferences from Lead 210, Soluble Ionic Species and Ozone

Aerosol samples collected over the western Pacific during the NASA/Global Tropospheric Experiment Pacific Exploratory Mission (PEM-West A) expedition (September - October 1991) revealed mean Pb-210 concentrations in the free troposphere in the 5-10 fCi m(exp -3) STP range. Most soluble ionic aerosol-associated species were near detection limits [much less than 40 parts per trillion by volume (pptv)] in these same samples. The altitude distribution of O3 near Asia closely resembled that of Pb-210, while no relationship was found between the concentrations of O3 and Be-7. Free tropospheric air over the western Pacific was depleted in soluble aerosol-associated species but enriched in Pb-210 and O3, indicative of deep wet convection over the Asian continent. The influence of Asian air on the composition of the free troposphere over the western Pacific was evident on most of the PEM-West A flights. However, evidence of continental influence was largely restricted to those species that are relatively insoluble (or have insoluble precursors), hence escape scavenging during vertical transport from the boundary layer into the free troposphere by wet convective activity.

Dibb, J. E.↗

Modeling of Isotope Fractionation in Stratospheric CO2, N2O, CH4, and O3: Investigations of Stratospheric Chemistry and Transport, Stratosphere-Troposphere Exchange, and Their Influence on Global Isotope Budgets

We investigated the isotopic fractionation of CH4 and hydrogen (H2) in the stratosphere by incorporating isotope-specific rate coefficients into the Lawrence Livermore National Laboratory (LLNL) 2D model and comparing the model results with new observations from the NASA ER-2 aircraft (funded through a separate task under the Upper Atmosphere Research Program). The model results reveal that fractionation which occurs in the stratosphere has a significant influence on isotope compositions in the free troposphere, an important point which had previously been ignored, unrecognized or unquantified for many long-lived trace gases, including CH4 and H2 which we have focused our efforts on to date. Our analyses of the model results and new isotope observations have also been used to test how well the kinetic isotope effects are known, at least to within the uncertainties in model chemistry and transport. Overall, these results represent an important step forward in our understanding of isotope fractionation in the atmosphere and demonstrate that stratospheric isotope fractionation cannot be ignored in modeling studies which use isotope observations in the troposphere to infer the global budgets of CH4 (an important greenhouse gas) and of H2 (a gas whose atmospheric budget must be better quantified, particularly before a large human perturbation from fuel cell use is realized). Our analyses of model results and observations from the NASA ER-2 aircraft are briefly summarized separately below for CH4, H2, and H2O and for the contribution of these modeling studies to date to our understanding of isotope fractionation for N2O, CO2, and O3 as well.

Boering, Kristie A.↗

Atmospheric Composition Change: Climate-Chemistry Interactions

Chemically active climate compounds are either primary compounds such as methane (CH4), removed by oxidation in the atmosphere, or secondary compounds such as ozone (O3), sulfate and organic aerosols, formed and removed in the atmosphere. Man-induced climate-chemistry interaction is a two-way process: Emissions of pollutants change the atmospheric composition contributing to climate change through the aforementioned climate components, and climate change, through changes in temperature, dynamics, the hydrological cycle, atmospheric stability, and biosphere-atmosphere interactions, affects the atmospheric composition and oxidation processes in the troposphere. Here we present progress in our understanding of processes of importance for climate-chemistry interactions, and their contributions to changes in atmospheric composition and climate forcing. A key factor is the oxidation potential involving compounds such as O3 and the hydroxyl radical (OH). Reported studies represent both current and future changes. Reported results include new estimates of radiative forcing based on extensive model studies of chemically active climate compounds such as O3, and of particles inducing both direct and indirect effects. Through EU projects such as ACCENT, QUANTIFY, and the AEROCOM project, extensive studies on regional and sector-wise differences in the impact on atmospheric distribution are performed. Studies have shown that land-based emissions have a different effect on climate than ship and aircraft emissions, and different measures are needed to reduce the climate impact. Several areas where climate change can affect the tropospheric oxidation process and the chemical composition are identified. This can take place through enhanced stratospheric-tropospheric exchange of ozone, more frequent periods with stable conditions favouring pollution build up over industrial areas, enhanced temperature-induced biogenic emissions, methane releases from permafrost thawing, and enhanced concentration through reduced biospheric uptake. During the last 510 years, new observational data have been made available and used for model validation and the study of atmospheric processes. Although there are significant uncertainties in the modelling of composition changes, access to new observational data has improved modelling capability. Emission scenarios for the coming decades have a large uncertainty range, in particular with respect to regional trends, leading to a significant uncertainty range in estimated regional composition changes and climate impact.

Atmosphere climate chemistry↗

Atmospheric CH4, CO and OH from 1860 to 1985

Studies have shown that atmospheric methane, CO and the gaseous OH radical are interdependent: if CH4, CO or OH is perturbed, background concentrations of the other two constituents are affected. Perturbations to OH alter photooxidation rates of numerous natural and anthropogenic trace gases and affect lifetimes of those species that pass from the earth's surface to the free troposphere and stratosphere. It is now known that global atmospheric methane concentrations are increasing; less definite data suggest that carbon monoxide is also increasing. Even before the measurements reported in nine literature references, modeling studies of CH4-CO-OH coupling had led to predictions (Chameides, Liu and Ciceronne, 1977; Sze, 1977; and Hameed, Pinto and Stewart 1979) of future increases of CH4 and CO. A photochemical model is used to look backwards in time by simulating the trace-gas composition of the unpolluted troposphere at the start of the industrial era (taken as 1860) and at intervals up to 1985. It is found that the OH concentration in the background troposphere has decreased significantly and O3 has increased due to increases of CH4 and CO; calculated changes depend on temporal trends of NOx (NOx = NO + NO2), for which no historical data are available. The calculations allow recent trace-gas trends affecting background chemistry and climate to be viewed in a longer-term context.

Thompson, A. M.↗

Long-Term Changes in Lower Tropospheric Baseline Ozone Concentrations:

Two recent papers have quantified long-term ozone (O3) changes observed at northernmidlatitude sites that are believed to represent baseline (here understood as representative of continental to hemispheric scales) conditions. Three chemistry-climate models (NCAR CAM-chem, GFDL-CM3, and GISS-E2-R) have calculated retrospective tropospheric O3 concentrations as part of the Atmospheric Chemistry and Climate Model Intercomparison Project and Coupled Model Intercomparison Project Phase 5 model intercomparisons. We present an approach for quantitative comparisons of model results with measurements for seasonally averaged O3 concentrations. There is considerable qualitative agreement between the measurements and the models, but there are also substantial and consistent quantitative disagreements. Most notably, models (1) overestimate absolute O3 mixing ratios, on average by approximately 5 to 17 ppbv in the year 2000, (2) capture only approximately 50% of O3 changes observed over the past five to six decades, and little of observed seasonal differences, and (3) capture approximately 25 to 45% of the rate of change of the long-term changes. These disagreements are significant enough to indicate that only limited confidence can be placed on estimates of present-day radiative forcing of tropospheric O3 derived from modeled historic concentration changes and on predicted future O3 concentrations. Evidently our understanding of tropospheric O3, or the incorporation of chemistry and transport processes into current chemical climate models, is incomplete. Modeled O3 trends approximately parallel estimated trends in anthropogenic emissions of NO(sub x), an important O3 precursor, while measured O3 changes increase more rapidly than these emission estimates.

atmospheric composition↗