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At least 145 records · Page 8

Profiles of alpha 13 C and alpha D in methane from the lower stratosphere

Methane is an important greenhouse gas of biogenic and anthropogenic origin for which global budgets are being constructed from a variety of data. One approach to the global methane budget is the use of the stable isotopes C-13 and D, and the radionuclide C-14 as tracers. The authors measured the isotopic composition of methane from various sources and in tropospheric air for a number of locations. Here, the authors report on the isotopic composition of methane from the lower stratosphere. Measurements of this concentration in the stratosphere can yield estimates for the kinetic isotope effects in the methane destruction reactions. These effects have to be known for quantitative isotopic methane budgets.

Wahlen, Martin↗

Dominant Presence of Oxygenated Organic Species in the Remote Southern Hemisphere Troposphere

Oxygenated organic species are intimately involved with the fate of nitrogen oxides (NO(sub x)) and hydrogen oxides (HO(sub x)), which are necessary for tropospheric ozone formation. A recent airborne experiment (March-April, 1999) focused over the southern hemisphere (SH) Pacific Ocean (PEM-tropics-B) provided a first opportunity for a detailed characterization of the oxygenated organic composition of the remote southern hemisphere troposphere. Three co-located multi-channel airborne instruments measured a dozen key oxygenated species (carbonyls, alcohols, organic nitrates, organic pernitrates, peroxides) along with a comprehensive suite of C2-C8 Nonmethane hydrocarbons (NMHC). These measurements reveal that in the tropical SH (0-30 deg south), oxygenated chemical abundances are extremely large and collectively are nearly five times those of NMHC. Even in the NH remote atmospheres their burden is equal to or greater than that of NMHC. The relatively uniform global distribution oxygenates (EPSILON Ox-org) is indicative of the presence of large natural and distributed sources. A global 3-D model, reflecting the present state of science, is unable to correctly simulate the atmospheric distribution and variability of several of these species.

Singh, H.↗

Particles in the lower troposphere over the High Plains of the United States. I - Size distributions, elemental compositions and morphologies

Airborne measurements of particle size distributions obtained during the spring and summer of 1975-1976 at various locations in the high plains of the U.S. are presented. The instrumentation and techniques used to collect the data are described. Particle number, surface area, and volume distribution are measured; differences in particle concentrations are investigated. Variables in particle size are related to changes in strength of ground sources of Aitken nuclei, age of the particle population, and presence or absence of rain. An accumulation mode between particles diameters of 0.1-1 micron, a coarse particle mode between particle diameters between 10-20 microns, and a nucleation mode at particle diameters less than 0.1 micron are detected. The control of the accommodation and coarse particle modes and their influence on particle concentration are studied. The elemental composition of the particles is analyzed and the morphologies are examined with an electron scanner microscope.

Hobbs, P. V.↗

Interpretation of Lidar and Satellite Data Sets Using a Global Photochemical Model

A primary goal of the NASA Tropospheric Chemistry Program (TCP) is to "contribute substantially to scientific understanding of human impacts on the global troposphere". In order to analyze global or regional trends and factors of the troposphere chemistry, for example, its oxidation capacity or composition, a continuous global/regional data coverage as well as model simulations are needed. The Global Tropospheric Experiment (GTE), a major component of the TCP, provides data vital to these questions via aircraft measurement of key trace chemical species in various remote regions of the world. Another component in NASA's effort are satellite projects for exploration of tropospheric chemistry and dynamics. A unique data product is the Tropospheric Ozone Residual (TOR) utilizing global tropospheric ozone data. Another key research tool are simulation studies of atmospheric chemistry and dynamics for the theoretical understanding of the atmosphere, the extrapolation of observed trends, and for sensitivity studies assessing a changing anthropogenic impact to air chemistry and climate. In the context with model simulations, field data derived from satellites or (airborne) field missions are needed for two purposes: 1. To initialize and validate model simulations, and 2., to interpret field data by comparison to model simulation results in order to analyze global or regional trends and deviations from standard tropospheric chemistry and transport conditions as defined by the simulations. Currently, there is neither a sufficient global data coverage available nor are existing well established global circulation models. The NASA LARC CTM model is currently not yet in a state to accomplish a sufficient tropospheric chemistry simulation, so that the current research under this cooperative agreement focuses on utilizing field data products for direct interpretation. They will be also available for model testing and a later interpretation with a finally utilized model.

Zenker, Thomas↗

NASA GEOS Composition Forecast Modeling System GEOS-CF v1.0: Stratospheric Composition

The NASA Goddard Earth Observing System (GEOS) Composition Forecast (GEOS-29CF) provides recent estimates and five-day forecasts of atmospheric composition to the public in near-real time. To do this, the GEOS Earth system model is coupled with the GEOS-Chem tropospheric-stratospheric unified chemistry extension (UCX) to represent composition from the surface to the top of the GEOS atmosphere (0.01 hPa). The GEOS-CF system is described, including updates made to the GEOS-Chem UCX mechanism within GEOS-CF for improved representation of stratospheric chemistry. Comparisons are made against balloon, lidar and satellite observations for stratospheric composition, including measurements of ozone (O3) and important nitrogen and chlorine species related to stratospheric O3recovery. The GEOS-CF nudges the stratospheric O3towards the GEOS Forward Processing (GEOS FP) assimilated O3product; as a result the stratospheric O3in the GEOS-CF historical estimate agrees well with observations. During abnormal dynamical and chemical environments such as the 2020 polar vortexes, the GEOS-CF O3forecasts are more realistic than GEOS FP O3forecasts because of the inclusion of the complex GEOS-Chem UCX stratospheric chemistry. Overall, the spatial patterns of the GEOS-CF simulated concentrations of stratospheric composition agree well with satellite observations. However, there are notable biases – such as low NOx and HNO3 in the polar regions and generally low HCl throughout the stratosphere – and future improvements to the chemistry mechanism and emissions are discussed. GEOS-CF is a new tool for the research community and instrument teams observing trace gases in the stratosphere and troposphere, providing near-real-time three-dimensional gridded information on atmospheric composition.

GEOS-CF↗

LEOMAC: A Future 'Global Atmospheric Composition Mission' (CACM) Concept

Resolution of important outstanding questions in air quality, climate change and ozone layer stability demands global observations of multiple chemical species with high horizontal and vertical resolution from the boundary layer to the stratopause. We present a mission concept that delivers the needed atmospheric composition observations, along with cloud ice and water vapor data needed for improvements in climate and weather forecasting models. The mission comprises ultraviolet and infrared nadir and microwave limb viewing instruments observing wide swaths each orbit. We review the scientific goals of the mission and the measurement capabilities this concept will deliver. We describe how precessing orbits offer significant improvements in temporal resolution and diurnal coverage compared to sun-synchronous orbits. Such improvements are needed to quantify the impact of critical 'fast processes' such as deep convection on the composition and radiative properties of the upper troposphere, a region where water vapor and ozone are strong but poorly understood greenhouse gases. This concept can serve as the 'Global Atmospheric Composition Mission' (GACM) recently recommended by the National Academy of Sciences decadal survey as one of 17 priority earth science missions for the coming decade.

chemistry↗

Linkages Between Ozone-depleting Substances, Tropospheric Oxidation and Aerosols

Coupling between the stratosphere and the troposphere allows changes in stratospheric ozone abundances to affect tropospheric chemistry. Large-scale effects from such changes on chemically produced tropospheric aerosols have not been systematically examined in past studies. We use a composition-climate model to investigate potential past and future impacts of changes in stratospheric ozone depleting substances (ODS) on tropospheric oxidants and sulfate aerosols. In most experiments, we find significant responses in tropospheric photolysis and oxidants, with small but significant effects on methane radiative forcing. The response of sulfate aerosols is sizeable when examining the effect of increasing future nitrous oxide (N2O) emissions. We also find that without the regulation of chlorofluorocarbons (CFCs) through the Montreal Protocol, sulfate aerosols could have increased by 2050 by a comparable amount to the decreases predicted due to relatively stringent sulfur emissions controls. The individual historical radiative forcings of CFCs and N2O through their indirect effects on methane (−22.6mW/sq. m for CFCs and −6.7mW/sq. m for N2O) and sulfate aerosols (−3.0mW/sq. m for CFCs and +6.5mW/sq. m for N2O when considering the direct aerosol effect) discussed here are non-negligible when compared to known historical ODS forcing. Our results stress the importance of accounting for stratosphere-troposphere, gas-aerosol and composition-climate interactions when investigating the effects of changing emissions on atmospheric composition and climate.

troposphere↗

Implementation of Cloud Retrievals for Tropospheric Emission Spectrometer (TES) Atmospheric Retrievals: Part 1. Description and Characterization of Errors on Trace Gas Retrievals

We develop an approach to estimate and characterize trace gas retrievals in the presence of clouds in high spectral measurements of upwelling radiance in the infrared spectral region (650-2260/cm). The radiance contribution of clouds is parameterized in terms of a set of frequency-dependent nonscattering optical depths and a cloud height. These cloud parameters are retrieved jointly with surface temperature, emissivity, atmospheric temperature, and trace gases such as ozone from spectral data. We demonstrate the application of this approach using data from the Tropospheric Emission Spectrometer (TES) and test data simulated with a scattering radiative transfer model. We show the value of this approach in that it results in accurate estimates of errors for trace gas retrievals, and the retrieved values improve over the initial guess for a wide range of cloud conditions. Comparisons are made between TES retrievals of ozone, temperature, and water to model fields from the Global Modeling and Assimilation Office (GMAO), temperature retrievals from the Atmospheric Infrared Sounder (AIRS), tropospheric ozone columns from the Goddard Earth Observing System (GEOS) GEOS-Chem, and ozone retrievals from the Total Ozone Mapping Spectrometer (TOMS). In each of these cases, this cloud retrieval approach does not introduce observable biases into TES retrievals.

aerosols↗

Carbon Isotope Biogeochemistry of Methane from Anoxic Sediments

The isotopic composition of naturally occurring methane was used to constrain the tropospheric budget of that radiatively active gas. Numerous studies have shown that the isotopic composition is not constant, even for a specific source, and may vary temporally and spatially. The objective was to develop a process-level model that reproduced the seasonal variations in the C-13/C-12 composition of methane observed at the coastal site, Cape Lookout Bight, NC. Details of the mass balance are provided. Experiments and models designed to determine what factors incluence C-13/C-12 ratio of dissolved CO2 are reported. All the factors described were combined in a model that faithfully reproduces the seasonal C-13/C-12 variations observed at Cape Lookout. The model is described.

Blair, Neal E.↗

On the Feasibility of Studying Shortwave Aerosol Radiative Forcing of Climate Using Dual-Wavelength Aerosol Backscatter Lidar

The current low confidence in the estimates of aerosol-induced perturbations of Earth's radiation balance is caused by the highly non-uniform compositional, spatial and temporal distributions of tropospheric aerosols on a global scale owing to their heterogeneous sources and short lifetimes. Nevertheless, recent studies have shown that the inclusion of aerosol effects in climate model calculations can improve agreement with observed spatial and temporal temperature distributions. In light of the short lifetimes of aerosols, determination of their global distribution with space-borne sensors seems to be a necessary approach. Until recently, satellite measurements of tropospheric aerosols have been approximate and did not provide the full set of information required to determine their radiative effects. With the advent of active aerosol remote sensing from space (e.g., PICASSO-CENA), the applicability fo lidar-derived aerosol 180 deg -backscatter data to radiative flux calculations and hence studies of aerosol effects on climate needs to be investigated.

Redemann, Jens↗

Relationships Between Variability in the Stratospheric Polar Vortex, Upper Tropospheric Jets, Tropopauses, and UTLS Ozone

The impacts of stratospheric polar vortex variations on upper troposphere / lower stratosphere (UTLS) circulation and composition are not well understood. We use stratospheric polar vortex geometry / strength diagnostics combined with characterisation of tropopauses and UTLS jets to show links between stratospheric polar vortex variability and regional variations in UTLS jet and tropopause characteristics. Polar vortex diagnostics are from Characterization and Analysis of Vortex Evolution using Algorithms for Region Tracking (CAVE-ART), while UTLS diagnostics are from JEt and Tropopause Products for Analysis and Characterization (JETPAC). We will present results showing UTLS jet and tropopause characteristics for strong and weak stratospheric vortex states (defined using vortex-focused metrics that are less dependent on geometry and position than commonly used diagnostics), as well as regional variations in correlations between CAVE-ART and JETPAC diagnostics. Furthermore, we will focus on preliminary results extending the stratospheric vortex, UTLS jet, and tropopause relationships to assess their impacts on regional ozone variations diagnosed from the M2-SCREAM (MERRA-2 Stratospheric Composition Reanalysis of Aura Microwave Limb Sounder) composition reanalysis.

Gloria Manney↗

Explosive east coast cyclogenesis over the west-central North Atlantic Ocean - A composite study derived from ECMWF operational analyses

This paper describes the observational aspects of explosive east-coast cyclogenesis using composites constructed from the daily global analyses generated and archived by ECMWF. An explosively deepening storm or bomb is defined as an extratropical cyclone whose mean sea-level pressure falls at least 1 mb/h for 24 h. The ECMWF data sets are used to examine the three-dimensional kinematic and thermodynamic structure of bombs over the entire depth of the troposphere. The evolution and structure of the composite bomb is diagnosed using a moving coordinate system consisting of a box with dimensions of 35 x 35 deg of latitude-longitude. The results reveal that explosive cyclogenesis is a baroclinic phenomenon in which the rapid development in the presence of strong upper tropospheric forcing is most likely enhanced by a highly destabilized lower troposphere.

Manobianco, John↗

How Do UTLS Jet and Tropopause Dynamics Influence Ozone Variability? Investigations Supporting the SPARC OCTAV-UTLS Activity

Understanding changes in UTLS ozone is exceptionally challenging because of large spatial and temporal variability and because of the difficulty of satellite measurements in the UTLS. It is also exceptionally important: for example, to understand climate impacts of radiatively active substances and to understand physical and biological effects of pollution transport and stratosphere-troposphere exchange (STE). Multi-decadal global observations of UTLS ozone are now available from numerous satellite platforms, as well as local and regional observations from aircraft, balloons, and lidar. The upper tropospheric (UT) jets and tropopauses are important drivers of composition variability in the UTLS, acting as transport barriers and controlling STE and long-range transport. We report here on investigations of relationships between extratropical UTLS ozone variability and dynamical diagnostics of mixing / transport barriers, Rossby Wave breaking, and stratosphere-troposphere exchange. We will view these relationships in the context of ozone mapped into dynamical coordinates with respect to the UTLS jets and / or the tropopause. This work will help provide direction for analyses within the Stratosphere-troposphere Processes And their Role in Climate (SPARC) Observed Composition Trends and Variability in the UTLS (OCTAV-UTLS) activity, which aims to use dynamical coordinate mapping to help detect and attribute observed UTLS composition trends, and to project future data needs to better quantify those trends. The work we report on here will focus on satellite ozone observations (primarily from the Aura Microwave Limb Sounder, additionally from ACE-FTS and OSIRIS) and assimilated ozone and dynamical fields (from multiple reanalyses); we will also provide some examples of comparisons with aircraft and balloon observations.

Manney, Gloria L.↗

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

Until recently, the stable isotopic composition of chemically and datively important stratospheric species, such as ozone (O3), carbon dioxide (CO2), nitrous oxide (N2O), and methane (CH4), was largely unexplored, despite indications from the few measurements available and theoretical studies that global-scale isotopic variations will provide a unique tool for quantifying rates of global-scale mass transport into, within, and out of the stratosphere and for understanding the mechanisms of chemical reactions involved in ozone production. The number and geographical extent of observations are beginning to increase rapidly, however, as access to the stratosphere, both directly and by remote-sensing, has increased over the last 10 years and as new analytical techniques have been developed that make global-scale isotope measurements by whole-air sampling more feasible. The objective of this study, begun in April 1999, is to incorporate into the Livermore 2D model the likely photochemical fractionation processes that determine the isotopic compositions of stratospheric CO2, N2O, CH4, and O3, and to use the model results and new observations from NASA field campaigns in 1996 and 1997 to investigate stratospheric chemistry and mass transport. Additionally, since isotopic signatures from the stratosphere are transferred to the troposphere by downward transport at middle and high latitudes, the isotopic compositions may also serve as sensitive tracers of stratosphere-totroposphere transport. Comparisons of model results with stratospheric and upper tropospheric observations from these campaigns, as well as with ground-based observations from new NOAA and NSF-sponsored studies, will help determine whether the magnitudes of the stratospheric fractionation processes are large enough to use as global-scale tracers of transport into the troposphere and, if so, will be used to help constrain the degree of coupling between the troposphere and the stratosphere.

Boering, Kristie A.↗

The Origin and Evolution of Saturn's 2011-2012 Stratospheric Vortex

The planet-encircling springtime storm in Saturn's troposphere (December 2010-July 2011, Fletcher, L.N. et al. [2011]. Science 332, 1413-1414; Sánchez-Lavega, A. et al. [2011]. Nature 475, 71-74; Fischer, G. et al. [2011]. Nature 475, 75-77) produced dramatic perturbations to stratospheric temperatures, winds and composition at mbar pressures that persisted long after the tropospheric disturbance had abated. Thermal infrared (IR) spectroscopy from the Cassini Composite Infrared Spectrometer (CIRS), supported by ground-based IR imaging from the VISIR instrument on the Very Large Telescope and the MIRSI instrument on NASA's IRTF, is used to track the evolution of a large, hot stratospheric anticyclone between January 2011 and March 2012. 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 35degN (B1 and B2) between January-April 2011, moving westward with different zonal velocities, B1 residing directly above the convective tropospheric storm head; (II) the merging of the warm airmasses to form the large single 'stratospheric beacon' near 40degN (B0) between April and June 2011, disassociated from the storm head and at a higher pressure (2 mbar) than the original beacons, a downward shift of 1.4 scale heights (approximately 85 km) post-merger; and (III) the mature phase characterised by slow cooling (0.11 +/- 0.01 K/day) and longitudinal shrinkage of the anticyclone since July 2011. Peak temperatures of 221.6 +/- 1.4 K at 2 mbar were measured on May 5th 2011 immediately after the merger, some 80 K warmer than the quiescent surroundings. From July 2011 to the time of writing, B0 remained as a long-lived stable stratospheric phenomenon at 2 mbar, moving west with a near-constant velocity of 2.70 +/- 0.04 deg/day (24.5 +/- 0.4 m/s at 40degN relative to System III longitudes). No perturbations to visible clouds and hazes were detected during this period. With no direct tracers of motion in the stratosphere, we use thermal windshear calculations to estimate clockwise peripheral velocities of 200-400 m/s at 2 mbar around B0. The peripheral velocities of the two original airmasses were smaller (70-140 m/s). In August 2011, the size of the vortex as defined by the peripheral collar was 65deg longitude (50,000 km in diameter) and 25deg latitude. Stratospheric acetylene (C2H2) was uniformly enhanced by a factor of three within the vortex, whereas ethane (C2H6) remained unaffected. The passage of B0 generated a new band of warm stratospheric emission at 0.5 mbar at its northern edge, and there are hints of warm stratospheric structures associated with the beacons at higher altitudes (p < 0.1 mbar) than can be reliably observed by CIRS nadir spectroscopy. Analysis of the zonal windshear suggests that Rossby wave perturbations from the convective storm could have propagated vertically into the stratosphere at this point in Saturn's seasonal cycle, one possible source of energy for the formation of these stratospheric anticyclones.

evolution↗

Soluble species in the Arctic summer troposphere - Acidic gases, aerosols, and precipitation

The large-scale spatial distribution from 0.15-to 6 km altitude in the North American Arctic troposphere of several soluble acidic gases and major aerosol species during the summertime is reported. The distribution is found to be compositionally consistent on a large spatial scale. The summertime troposphere is an acidic environment, with HCOOH and CH3COOH the principal acidic gases while acidic sulfate aerosols dominate the particulate phase. There appears to be a surface source of NH3 over the pack ice which may originate from decay of dead marine organisms on the ice surface, evolution from surface ocean waters in open ice leads, or release from rotting sea ice. At low altitude over the pack ice this NH34 appears to partially neutralize aerosol acidity. Over sub-Arctic tundra in southeastern Alaska, inputs of marine biogenic sulfur from the Bering Sea appear to be an important source of boundary layer aerosol SO4(2-). The rainwater acidity over the tundra is typical of remote regions.

Talbot, R. W.↗

Evaluation of the GEOS-Chem UCX Stratosphere in the GEOS Composition Forecast System

The NASA GEOS Composition Forecast (GEOS-CF) system provides 3-dimensional atmospheric composition analyses and forecasts to the public in near-real time at the high spatial resolution of 25 km. While the main focus of this new product is on tropospheric air quality information, the GEOS-Chem chemistry model (v12) used in this system includes the UCX stratospheric chemistry mechanism. Here, we describe the GEOS-CF system and provide comparisons against remote-sensed observations for stratospheric composition, including measurements of HCl, ClO, NO2, and O3. The GEOS-CF nudges the stratospheric ozone towards the GEOS Forward Processing (GEOS FP) assimilated ozone product; as a result the stratospheric ozone analysis in theGEOS-CF agrees well with observations. Additionally, with the inclusion of the GEOS-Chem UCX stratospheric chemistry mechanism in GEOS-CF, 5-day forecasts, especially during the abnormal 2020 NH polar spring, capture the chemical and dynamical changes missed by the GEOS FP system, which tends towards climatology. The GEOS-CF is a new tool for the research community providing near-real time 3-dimensional gridded information on atmospheric composition throughout the troposphere and stratosphere.

Stratosphere↗

A global average model of atmospheric aerosols for radiative transfer calculations

A global average model is proposed for the size distribution, chemical composition, and optical thickness of stratospheric and tropospheric aerosols. This aerosol model is designed to specify the input parameters to global average radiative transfer calculations which assume the atmosphere is horizontally homogeneous. The model subdivides the atmosphere at multiples of 3 km, where the surface layer extends from the ground to 3 km, the upper troposphere from 3 to 12 km, and the stratosphere from 12 to 45 km. A list of assumptions made in construction of the model is presented and discussed along with major model uncertainties. The stratospheric aerosol is modeled as a liquid mixture of 75% H2SO4 and 25% H2O, while the tropospheric aerosol consists of 60% sulfate and 40% soil particles above 3 km and of 50% sulfate, 35% soil particles, and 15% sea salt below 3 km. Implications and consistency of the model are discussed.

Toon, O. B.↗