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At least 127 records · Page 7

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↗

A Tropospheric Emission Spectrometer HDO/H2O Retrieval Simulator for Climate Models

Retrievals of the isotopic composition of water vapor from the Aura Tropospheric Emission Spectrometer (TES) have unique value in constraining moist processes in climate models. Accurate comparison between simulated and retrieved values requires that model profiles that would be poorly retrieved are excluded, and that an instrument operator be applied to the remaining profiles. Typically, this is done by sampling model output at satellite measurement points and using the quality flags and averaging kernels from individual retrievals at specific places and times. This approach is not reliable when the model meteorological conditions influencing retrieval sensitivity are different from those observed by the instrument at short time scales, which will be the case for free-running climate simulations. In this study, we describe an alternative, categorical approach to applying the instrument operator, implemented within the NASA GISS ModelE general circulation model. Retrieval quality and averaging kernel structure are predicted empirically from model conditions, rather than obtained from collocated satellite observations. This approach can be used for arbitrary model configurations, and requires no agreement between satellite-retrieved and model meteorology at short time scales. To test this approach, nudged simUlations were conducted using both the retrieval-based and categorical operators. Cloud cover, surface temperature and free-tropospheric moisture content were the most important predictors of retrieval quality and averaging kernel structure. There was good agreement between the D fields after applying the retrieval-based and more detailed categorical operators, with increases of up to 30 over the ocean and decreases of up to 40 over land relative to the raw model fields. The categorical operator performed better over the ocean than over land, and requires further refinement for use outside of the tropics. After applying the TES operator, ModelE had D biases of 8 over ocean and 34 over land compared to TES D, which were less than the biases using raw model D fields.

Field, R. D.↗

Planetary atmospheres program

Non-solar compositional models of the troposphere of Jupiter, halide cloud condensation and volatile element inventories on Venus, and shock-wave processing of interstellar cloud materials are discussed.

Source record↗

Titan Science with the James Webb Space Telescope

The James Webb Space Telescope (JWST), scheduled for launch in 2018, is the successor to the Hubble Space Telescope (HST) but with a signicantly larger aperture (6.5 m) and advanced instrumentation focusing on infrared science (0.6-28.0 microns). In this paper, we examine the potential for scientic investigation of Titan using JWST, primarily with three of the four instruments: NIRSpec, NIRCam, and MIRI, noting that science with NIRISS will be complementary. Five core scientic themes are identied: (1) surface (2) tropospheric clouds (3) tropospheric gases (4) stratospheric composition, and (5) stratospheric hazes. We discuss each theme in depth, including the scientic purpose, capabilities, and limitations of the instrument suite and suggested observing schemes. We pay particular attention to saturation, which is a problem for all three instruments, but may be alleviated for NIRCam through use of selecting small sub-arrays of the detectorssufcient to encompass Titan, but with signicantly faster readout times. We nd that JWST has very signicant potential for advancing Titan science, with a spectral resolution exceeding the Cassini instrument suite at near-infrared wavelengths and a spatial resolution exceeding HST at the same wavelengths. In particular, JWST will be valuable for time-domain monitoring of Titan, given a ve- to ten-year expected lifetime for the observatory, for example, monitoring the seasonal appearance of clouds. JWST observations in the post-Cassini period will complement those of other large facilities such as HST, ALMA, SOFIA, and next-generation ground-based telescopes (TMT, GMT, EELT).

Nixon, Conor A.↗

Reanalysis Activities at the NASA Global Modeling and Assimilation Office

This talk presents an overview of recent reanalysis activities at the NASA Global Modeling and Assimilation Office (GMAO) as part of a multi-faceted strategy towards an Integrated Earth System retrospective analysis, coupling components of the atmosphere, ocean, chemistry, land, and ice. While elements of the atmosphere-ocean coupled Goddard Earth Observing System (GEOS) model and data assimilation are being actively developed, a suite of reanalysis products is designed to provide further understanding of key aspects of Earth system coupling in a reanalysis context: The baseline atmospheric reanalysis, the GEOS Retrospective analysis for the early 21st Century (GEOS-R21C), features recent advances in the GEOS model and data assimilation, and targets the NASA’s Earth Observing System EOS and post-EOS satellite observations; GEOS-IT, a user-tailored low-resolution atmospheric reanalysis, serves as a second baseline to the NASA Instrument Teams for validation and calibration and drives a one-way coupled ocean reanalysis, GEOSIT-Ocean; PolarMERRA, a high-resolution downscaled product for the polar regions, focuses on improving the representation of polar atmospheric processes with an assessment of current cryospheric biases, and targeted improvements to surface sea ice and glacier conditions; Finally, R21C-Chem, an off-line atmospheric chemistry and composition reanalysis, includes both tropospheric and stratospheric trace gases. The diversity of these reanalysis activities presents unique opportunities for collaborations cross-teams/institutions, with new commercial data partners, and with end-user groups. This talk will discuss these opportunities and explore leveraging the lessons learned along the way on key drivers in Earth system interactions as we converge towards the next generation of the Modern-Era Retrospective analysis for Research and Applications (MERRA) suite.

Amal El Akkraoui↗

Transport and Mixing in the Stratosphere and Troposphere

Long-term changes in the composition of the atmosphere are known to have significant effects on atmospheric chemistry and stratospheric ozone. Increasing levels of greenhouse gases have the potential to change the global climate in the middle and upper atmospheres, as well as in the troposphere. Volcanic eruptions, El Nino events, and other natural variations can also cause changes in atmospheric composition and climate. Whether the causes are natural or manmade, changes in the global climate system can have impacts on human society. In order to understand and predict the consequences of these changes, and of control measures such as the Montreal Protocol, it is necessary to understand the complex interactions between radiation, chemistry, and dynamics in the atmosphere. Much of the uncertainty in our understanding of atmospheric processes comes from an incomplete understanding of atmospheric transport. A complete and self-consistent model of transport requires not only an understanding of trace-species transport, but also the transport of dynamically active quantities such as heat and potential vorticity. Therefore, the goal of the proposed research is to better understand large-scale transport and mixing processes in the middle atmosphere and troposphere.

Bowman, Kenneth P.↗

Strat-trop exchange

Exchange between the stratosphere and troposphere is important to the chemical composition of both regions. The export of ozone from the stratosphere provides the troposphere with a means of initiating photochemistry. The precursor molecules originating from the planetary surface provide the stratosphere with its chemical feedstock from which the ozone-controlling HO(x), NO(x), and Cl(x) photochemistries are driven. The tropopause is defined both statistically and in a local, synoptic sense by the value P(sub theta) = .000016 K sq m/kg/s, taken from an objective analysis of 8 years of zonal, temporal mean cross sections of potential temperature, wind and potential vorticity.

Tuck, A. F.↗

Response of the global climate to changes in atmospheric chemical composition due to fossil fuel burning

Tropospheric ozone and methane might increase in the future as the result of increasing anthropogenic emissions of CO, NOx and CH4 due to fossil fuel burning. Since O3 and CH4 are both greenhouse gases, increases in their concentrations could augment global warming due to larger future amounts of atmospheric CO2. To test this possible climatic impact, a zonal energy-balance climate model has been combined with a vertically-averaged tropospheric chemical model. The latter model includes all relevant chemical reactions which affect species derived from H2O, O2, CH4 and NOx. The climate model correspondingly incorporates changes in the infrared heating of the surface-troposphere system resulting from chemically induced changes in tropospheric ozone and methane. This coupled climate-chemical model indicates that global climate is sensitive to changes in emissions of CO, NOx and CH4, and that future increases in these emissions could enhance global warming due to increasing atmospheric CO2.

Cess, R. D.↗

Effective radiative forcing from emissions of reactive gases and aerosols - a multi-model comparison

This paper quantifies the pre-industrial (1850) to present-day (2014) effective radiative forcing (ERF) of anthropogenic emissions of NOX, volatile organic compounds (VOCs; including CO), SO2, NH3, black carbon, organic carbon, and concentrations of methane, N2O and ozone-depleting halocarbons, using CMIP6 models. Concentration and emission changes of reactive species can cause multiple changes in the composition of radiatively active species: tropospheric ozone, stratospheric ozone, stratospheric water vapour, secondary inorganic and organic aerosol, and methane. Where possible we break down the ERFs from each emitted species into the contributions from the composition changes. The ERFs are calculated for each of the models that participated in the AerChemMIP experiments as part of the CMIP6 project, where the relevant model output was available. The 1850 to 2014 multi-model mean ERFs (± standard deviations) are −1.03 ± 0.37 W/sq.m for SO2 emissions, −0.25 ± 0.09 W/sq.m for organic carbon (OC), 0.15 ± 0.17 W/sq.m for black carbon (BC) and −0.07 ± 0.01 W/sq.m for NH3. For the combined aerosols (in the piClim-aer experiment) it is −1.01 ± 0.25 W/sq.m. The multi-model means for the reactive well-mixed greenhouse gases (including any effects on ozone and aerosol chemistry) are 0.67 ± 0.17 W/sq.m for methane (CH4), 0.26 ± 0.07 W/sq.m for nitrous oxide (N2O) and 0.12 ± 0.2 W/sq.m for ozone-depleting halocarbons (HC). Emissions of the ozone precursors nitrogen oxides (NOx), volatile organic compounds and both together (O3) lead to ERFs of 0.14 ± 0.13, 0.09 ± 0.14 and 0.20 ± 0.07 W/sq.m respectively. The differences in ERFs calculated for the different models reflect differences in the complexity of their aerosol and chemistry schemes, especially in the case of methane where tropospheric chemistry captures increased forcing from ozone production.

radiative forcing↗

The Evolution and Fate of Saturn's Stratospheric Vortex: Infrared Spectroscopy from Cassini

The planet-encircling springtime storm in Saturn's troposphere (December 2010-July 2011) produced dramatic perturbations to stratospheric temperatures, winds and composition at mbar pressures that persisted long after the tropospheric disturbance had abated. Observations from the Cassini Composite Infrared Spectrometer (CIRS), supported by ground-based imaging from the VISIR instrument on the Very Large Telescope,is used to track the evolution of a large, hot stratospheric anticyclone between January 2011 and the present day. The evolutionary sequence can be divided into three phases: (I) the formation and intensification of two distinct warm airmasses near 0.5 mbar between 25 and 35N (one residing directly above the convective storm head) between January-April 2011, moving westward with different zonal velocities; (II) the merging of the warm airmasses to form the large single 'stratospheric beacon' near 40N between April and June 2011, dissociated from the storm head and at a higher pressure (2 mbar) than the original beacons; and (III) the mature phase characterized by slow cooling and longitudinal shrinkage of the anticyclone since July 2011, moving west with a near-constant velocity of 2.70+/-0.04 deg/day (-24.5+/-0.4 m/s at 40N). Peak temperatures of 220 K at 2 mbar were measured on May 5th 2011 immediately after the merger, some 80 K warmer than the quiescent surroundings. Thermal winds hear calculations in August 2011 suggest clockwise peripheral velocities of 200400 mls at 2 mbar, defining a peripheral collar with a width of 65 degrees longitude (50,000 km in diameter) and 25 degrees latitude. Stratospheric acetylene (C2H2) was uniformly enhanced by a factor of three within the vortex, whereas ethane (C2H6) remained unaffected. We will discuss the thermal and chemical characteristics of Saturn's beacon in its mature phase, and implications for stratospheric vortices on other giant planets.

Fletcher, Leigh N.↗