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Chemical Composition of Asian Continental Outflow over the Western Pacific: Results from Transport and Chemical Evolution over the Pacific (TRACE-P)

We characterize the chemical composition of Asian continental outflow observed during the NASA Transport and Chemical Evolution over the Pacific (TRACE-P) mission during February-April 2001 in the western Pacific using data collected on the NASA DC-8 aircraft. A significant anthropogenic impact was present in the free troposphere and as far east as 150degE longitude reflecting rapid uplift and transport of continental emissions. Five-day backward trajectories were utilized to identify five principal Asian source regions of outflow: central, coastal, north-northwest(NNW), southeast (SE), and west-southwest (WSW). The maximum mixing ratios for several species, such as CO, C2Cl4, CH3Cl, and hydrocarbons, were more than a factor of 2 larger in the boundary layer of the central and coastal regions due to industrial activity in East Asia. CO was well correlated with C2H2, C2H6, C2Cl4, and CH3Cl at low altitudes in these two regions (r(sup 2) approx. 0.77-0.97). The NNW, WSW, and SE regions were impacted by anthropogenic sources above the boundary layer presumably due to the longer transport distances of air masses to the western Pacific. Frontal and convective lifting of continental emissions was most likely responsible for the high altitude outflow in these three regions. Photochemical processing was influential in each source region resulting in enhanced mixing ratios of O3, PAN, HNO3, H2O2, and CH3OOH. The air masses encountered in all five regions were composed of a complex mixture of photcrchemically aged air with more recent emissions mixed into the outflow as indicated by enhanced hydrocarbon ratios (C2H2/CO greater than or equal to 3 and C3H8/C2H6 greater than or equal to 0.2). Combustion, industrial activities, and the burning of biofuels and biomass all contributed to the chemical composition of air masses from each source region as demonstrated by the H6, SO2, and C2Cl4 were compared for the TRACE-P and PEM-West B missions. In the more northern regions, O3, CO, and SO2 were higher at low altitudes during TRACE-P. In general, mixing ratios were fairly similar between the two missions in the southern regions. A comparison between CO/CO2, CO/CH4, C2H6/C3H8, NO(x)/SO2, and NO(y)/(SO2 + nss-SO4) ratios for the five source regions and for the 2000 Asian emissions summary showed vay close agreement indicating that Asian emissions were well represented by the TRACE-P data and tbe emissions inventory.

Russo, R. S.↗

Atmospheric Trace Gas (NO2 and Ozone) Dynamics over Coastal Waters near Polluted Urban Regions

At the interface between the land, oceans, and atmosphere, coastal regions are highly dynamic environments, characterized by strong variability in both water and air quality. Variability in atmospheric composition is associated with highly variable anthropogenic emissions, as well as complex meteorological processes that influence the circulation and accumulation of atmospheric pollutants at the land-ocean interface. Assessing the spatial and temporal dynamics of atmospheric pollutants, aerosols, and absorbing trace gases in coastal areas is critical for improving modeling of coastal tropospheric air quality, developing accurate satellite retrievals of coastal ocean color and biological processes, determining impacts of atmospheric pollution on human health, and assessing the ecological implications of atmospheric pollutant deposition for coastal terrestrial and aquatic ecosystems.Here, we present new measurements of atmospheric trace gas (NO2, and ozone) dynamics across a range of estuarine and coastal waters near urban regions. Measurements were conducted from research vessels using NASA's shipboard Pandora spectrometers, as part of recent multidisciplinary, multiplatform field campaigns, including the 2016 KORUS OC/AQ field campaign in the Yellow Sea and East Sea/Sea of Japan, the 2017/2018 OLWETS field campaign in the Chesapeake Bay estuary, and the 2018 LISTOS field campaign in the Long Island Sound. Shipboard measurements over these coastal waters were integrated with measurements from a ground-based Pandora network to examine differences in air quality over the land and over the ocean. Measurements were combined with air-parcel back-trajectory simulations to determine the origin of air masses over the coastal ocean. Comparisons with satellite retrievals of atmospheric composition reveal the benefits and limitations of polar-orbit satellite observations in capturing variability in atmospheric pollution gradients over land-water boundaries.

Tzortziou, Maria↗

Size distribution and scattering phase function of aerosol particles retrieved from sky brightness measurements

Ground-based measurements of the solar transmission and sky radiance in a horizontal plane through the Sun are taken in several geographical regions and aerosol types: dust in a desert transition zone in Israel, sulfate particles in Eastern and Western Europe, tropical aerosol in Brazil, and mixed continental/maritime aerosol in California. Stratospheric aerosol was introduced after the eruption of Mount Pinatubo in June 1991. Therefore measurements taken before the eruption are used to analyze the properties of tropospheric aerosol; measurements from 1992 are also used to detect the particle size and concentration of stratospheric aerosol. The measurements are used to retrieve the size distribution and the scattering phase function at large scattering angles of the undisturbed aerosol particles. The retrieved properties represent an average on the entire atmospheric column. A comparison between the retrieved phase function for a scattering angle of 120 deg, with phase function predicted from the retrieved size distribution, is used to test the assumption of particle homogeneity and sphericity in radiative transfer models (Mie theory). The effect was found to be small (20% +/- 15%). For the stratospheric aerosol (sulfates), as expected, the phase function was very well predicted using the Mie theory. A model with a power law distribution, based on the spectral dependence of the optical thickness, alpha, cannot estimate accurately the phase function (up to 50% error for lambda = 0.87 microns). Before the Pinatubo eruption the ratio between the volumes of sulfate and coarse particles was very well correlated with alpha. The Pinatubo stratospheric aerosol destroyed this correlation. The aerosol optical properties are compared with analysis of the size, shape, and composition of the individual particles by electron microscopy of in situ samples. The measured volume size distribution before the injection of stratospheric aerosol consistently show two modes, sulfate particles with r(sub m) less than 0.2 microns and coarse paritcles with r(sub m) greater than 0.7 microns. The 'window' in the tropospheric aerosol in this radius range was used to observe a stable stratospheric aerosol in 1992, with r(sub m) approximately 0.5 microns. A combination of such optical thickness and sky measurements can be used to assess the direct forcing and the climatic impact of aerosol. Systematic inversion for the key aerosol types (sulfates, smoke, dust, and maritime aerosol) of the size distribution and phase function can give the relationship between the aerosol physical and optical properties that can be used to compute the radiative forcing. This forcing can be validated in dedicated field experiments.

Kaufman, Y. J.↗

Observations of Greenhouse Gas Changes across Summer Frontal Boundaries in the Eastern United States

Our knowledge about synoptic-scale variations of atmospheric CO2 produced by interactions between mid-latitude cyclones and regional-scale surface fluxes remains limited by scarcity of observations. We synthesize observations of greenhouse gases (GHG) with respect to frontal passages to understand how GHG distributions change vertically and horizontally during a synoptic event. We use the airborne in-situ measurements of GHGs collected during the first Atmospheric Carbon and Transport–America (ACT) summer field campaign across three regions of the eastern US. We find that frontal structures are consistently and clearly associated with spatially coherent, significant changes in GHG composition. Warm sector CO2 mole fractions (henceforth, [CO2]) are significantly higher than those in the cold sector. The CO2 frontal differences (5-30 ppm) are largest in the atmospheric boundary layer (ABL) with smaller differences (3-5 ppm) in the free troposphere (FT). Bands of elevated CO2 (5-20 ppm enhancement compared to warm-sector mean [CO2]) repeatedly occurred in the ABL adjacent to the frontal boundary. Analyses of 84 vertical profiles reveal higher [CO2] in the FT than in the ABL in the cold-sector, the opposite pattern in the warm-sector. Average ABL-to-FT [CO2] differences are 12 ppm and -6 ppm in the warm and cold sectors, respectively. The same analysis for CH4 shows higher [CH4] in the ABL than in the FT in both warm and cold sectors with at least 30-ppb higher ABL-to-FT [CH4] differences in the warm-sector than in the cold-sector. The observational analyses presented here define new metrics for model evaluation of GHG transport.

Pal, Sandip↗

Water and the photochemistry of the troposphere

A discussion is presented concerning the role of water in its liquid and gaseous states in the chemistry and photochemistry of the earth's troposphere, with attention to the formation of the hydroxyl radical, oxidation chains involving the gases methane, carbon monoxide and ammonia, the atmospheric chemistry of the sulfur, hydrogen, halogen and nitrogen species, and the function of lightning as a source of tropospheric species. The phenomena of 'rainout', 'washout', and the aqueous chemistry of cloud an rain droplets and of water-covered aerosols, are noted. A section is devoted to the past and anticipated impact of anthropogenic activities on the chemistry and composition of the earth's atmosphere.

Levine, J. S.↗

Spectroscopic database

Several aspects of quantitative atmospheric spectroscopy are considered, using a classification of the molecules according to the gas amounts in the stratosphere and upper troposphere, and reviews of quantitative atmospheric high-resolution spectroscopic measurements and field measurements systems are given. Laboratory spectroscopy and spectral analysis and prediction are presented with a summary of current laboratory spectroscopy capabilities. Spectroscopic data requirements for accurate derivation of atmospheric composition are discussed, where examples are given for space-based remote sensing experiments of the atmosphere: the ATMOS (Atmospheric Trace Molecule) and UARS (Upper Atmosphere Research Satellite) experiment. A review of the basic parameters involved in the data compilations; a summary of information on line parameter compilations already in existence; and a summary of current laboratory spectroscopy studies are used to assess the data base.

Husson, N.↗

Projecting the Lasting Fate of the Hunga Tonga-Hunga Ha’apai Eruption on the Stratosphere through Connecting Measurements to Models

On 15th Jan. 2022 the submarine volcano Hunga Tonga-Hunga Ha’apai (HTHH) injected approximately 0.5 Tg of sulfur dioxide into the stratosphere, but more significantly added 150-170 Tg of water vapor to the stratospheric background (over a 10% perturbation) in a matter of several hours. The sulfur dioxide rapidly converted to sulfate aerosol and along with water vapor, was transported around the Southern Hemisphere sub-tropics into midlatitudes with some transport into the Northern Hemisphere. With a much longer lifetime than sulfate aerosol, measurable water vapor mass anomalies have persisted with only small losses over the past almost 2 years and are likely to continue above background for the remainder of the decade. Satellite measurements from limb and nadir viewing observing instruments provide the information needed to reasonably initialize the HTHH eruption in the Goddard Earth Observing System (GEOS) model using the “replay” framework coupled to the Global Modeling Initiative (GMI) stratosphere-troposphere chemical mechanism for the recent past and continue the simulations into the future with the free running chemistry climate model (CCM). Using a number of model ensemble members together with the satellite observations, we quantify how the HTHH eruption is perturbing stratospheric composition and climate and projecting the influences to come as the enhanced water vapor continues in the stratosphere with only very slow removal mechanisms. HTHH eruption provides a useful test of chemistry climate models and an opportunity for observation-based process understanding, which we will highlight.

Hunga Tonga-Hunga Ha’apai↗

Origin and evolution of planetary atmospheres

This report concerns several research tasks related to the origin and evolution of planetary atmospheres and the large-scale distribution of volatile elements in the Solar System. These tasks and their present status are as follows: (1) we have conducted an analysis of the volatility and condensation behavior of compounds of iron, aluminum, and phosphorus in the atmosphere of Venus in response to publish interpretations of the Soviet Venera probe XRF experiment data, to investigate the chemistry of volcanic gases, injection of volatiles by cometary and asteroidal impactors, and reactions in the troposphere; (2) we have completed and are now writing up our research on condensation-accretion modeling of the terrestrial planets; (3) we have laid the groundwork for a detailed study of the effects of water transport in the solar nebula on the bulk composition, oxidation state, and volatile content of preplanetary solids; (4) we have completed an extensive laboratory study of cryovolcanic materials in the outer solar system; (5) we have begun to study the impact erosion and shock alteration of the atmosphere of Mars resulting from cometary and asteroidal bombardment; and (6) we have developed a new Monte Carlo model of the cometary and asteroidal bombardment flux on the terrestrial planets, including all relevant chemical and physical processes associated with atmospheric entry and impact, to assess both the hazards posed by this bombardment to life on Earth and the degree of cross-correlation between the various phenomena (NO(x) production, explosive yield, crater production, iridium signature, etc.) that characterize this bombardment. The purpose of these investigations has been to contribute to the developing understanding of both the dynamics of long-term planetary atmosphere evolution and the short-term stability of planetary surface environments.

Lewis, John S.↗

SUCCESS Evidence for Cirrus Cloud Ice Nucleation Mechanisms

During the SUCCESS mission, several measurements were made which should improve our understanding of ice nucleation processes in cirrus clouds. Temperature and water vapor concentration were made with a variety of instruments on the NASA DC-8. These observations should provide accurate upper tropospheric humidities. In particular, we will evaluate what humidities are required for ice nucleation. Preliminary results suggest that substantial supersaturations frequently exist in the upper troposphere. The leading-edge region of wave-clouds (where ice nucleation occurs) was sampled extensively at temperatures near -40 and -60C. These observations should give precise information about conditions required for ice nucleation. In addition, we will relate the observed aerosol composition and size distributions to the ice formation observed to evaluate the role of soot or mineral particles on ice nucleation. As an alternative technique for determining what particles act as ice nuclei, numerous samples of aerosols inside ice crystals were taken. In some cases, large numbers of aerosols were detected in each crystal, indicating that efficient scavenging occurred. Analysis of aerosols in ice crystals when only one particle per crystal was detected should help with the ice nucleation issue. Direct measurements of the ice nucleating activity of ambient aerosols drawn into airborne cloud chambers were also made. Finally, measurements of aerosols and ice crystals in contrails should indicate whether aircraft exhaust soot particles are effective ice nuclei.

Jensen, Eric↗

The Tropospheric Emission Spectrometer: From Discovery Mission to Earth System Sounding

The Tropospheric Emission Spectrometer (TES) was launched aboard the Aura spacecraft in 2004 and decommissioned in February 2018. Over more than a decade of observations, TES has shown the potential of high-resolution Fourier Transform Spectrometer (FTS) measurements to alter our understanding of atmospheric composition and its relationship to the Earth System. We survey some of the major contributions TES has made to understanding air quality, chemistry-climate interactions, atmospheric hydrology, and carbon cycle science. We then show how innovations in retrieval methods pioneered by the TES team are now being applied to multi-spectral, multi-instrument records, establishing a new paradigm for composition measurements into the future.

Bowman, Kevin W.↗

Exploring Oxidation in the Remote Free Troposphere: Insights From Atmospheric Tomography (ATom)

Earth's atmosphere oxidizes the greenhouse gas methane and other gases, thus determining their lifetimes and oxidation products. Much of this oxidation occurs in the remote, relatively clean free troposphere above the planetary boundary layer, where the oxidation chemistry is thought to be much simpler and better understood than it is in urban regions or forests. The NASA airborne Atmospheric Tomography study (ATom) was designed to produce cross sections of the detailed atmospheric composition in the remote atmosphere over the Pacific and Atlantic Oceans during four seasons. As part of the extensive ATom data set, measurements of the atmosphere's primary oxidant, hydroxyl (OH), and hydroperoxyl (HO2) are compared to a photochemical box model to test the oxidation chemistry. Generally, observed and modeled median OH and HO2 agree to within combined uncertainties at the 2σ confidence level, which is ~±40%. For some seasons, this agreement is within ~±20% below 6-km altitude. While this test finds no significant differences, OH observations increasingly exceeded modeled values at altitudes above 8 km, becoming ~35% greater, which is near the combined uncertainties. Measurement uncertainty and possible unknown measurement errors complicate tests for unknown chemistry or incorrect reaction rate coefficients that would substantially affect the OH and HO2 abundances. Future analysis of detailed comparisons may yield additional discrepancies that are masked in the median values.

atmosphere's primary oxidant, hydroxyl (OH), and h↗

Impact of dry intrusion events on the composition and mixing state of particles during the winter Aerosol and Cloud Experiment in the Eastern North Atlantic (ACE-ENA)

Abstract. Long-range transport of continental emissions has a far-reaching influence over remote regions, resulting in substantial change in the size, morphology, and composition of the local aerosol population and cloud condensation nuclei (CCN) budget. Here, we investigate the physicochemical properties of atmospheric particles collected on board a research aircraft flown over the Azores during the winter 2018 Aerosol and Cloud Experiment in the Eastern North Atlantic (ACE-ENA) campaign. Particles were collected within the marine boundary layer (MBL) and free troposphere (FT) after long-range atmospheric transport episodes facilitated by dry intrusion (DI) events. Chemical and physical properties of individual particles were investigated using complementary capabilities of computer-controlled scanning electron microscopy and X-ray spectromicroscopy to probe particle external and internal mixing state characteristics. Furthermore, real-time measurements of aerosol size distribution, cloud condensation nuclei (CCN) concentration, and back-trajectory calculations were utilized to help bring into context the findings from offline spectromicroscopy analysis. While carbonaceous particles were found to be the dominant particle type in the region, changes in the percent contribution of organics across the particle population (i.e., external mixing) shifted from 68 % to 43 % in the MBL and from 92 % to 46 % in FT samples during DI events. This change in carbonaceous contribution is counterbalanced by the increase in inorganics from 32 % to 57 % in the MBL and 8 % to 55 % in FT. The quantification of the organic volume fraction (OVF) of individual particles derived from X-ray spectromicroscopy, which relates to the multi-component internal composition of individual particles, showed a factor of 2.06 ± 0.16 and 1.11 ± 0.04 increase in the MBL and FT, respectively, among DI samples. We show that supplying particle OVF into the κ-Köhler equation can be used as a good approximation of field-measured in situ CCN concentrations. We also report changes in the κ values in the MBL from κMBL, non-DI=0.48 to κMBL, DI=0.41, while changes in the FT result in κFT, non-DI=0.36 to κFT, DI=0.33, which is consistent with enhancements in OVF followed by the DI episodes. Our observations suggest that entrainment of particles from long-range continental sources alters the mixing state population and CCN properties of aerosol in the region. The work presented here provides field observation data that can inform atmospheric models that simulate sources and particle composition in the eastern North Atlantic.

54 ENVIRONMENTAL SCIENCES↗

M2-SCREAM: A Stratospheric Composition Reanalysis of Aura MLS

Stratospheric composition and transport patterns are changing because of increasing greenhouse gas concentrations and declining levels of ozone depleting substances. Superimposed on forced trends are: dynamical variability at a range of time scales and unforeseen perturbations such as those resulting from injections of volcanic material and smoke from PyroCb events. Chemical reanalyses can be powerful tools for studying the composition of the stratosphere and disentangling forced responses from internal variability. This presentation introduces a new chemical reanalysis of stratospheric constituents developed and produced at NASA’s Global Modeling and Assimilation Office (GMAO) using the recently developed GMAO Constituent Data Assimilation System. Called the MERRA-2 Stratospheric Composition Reanalysis with Aura MLS (M2-SCREAM), this reanalysis consists of assimilated global three-dimensional fields of stratospheric ozone, water vapor, hydrogen chloride (HCl), nitric acid (HNO3) and nitrous oxide (N2O) mixing ratios and covers the period since the beginning of MLS observations in September 2004 to the present. M2-SCREAM assimilates version 4.2 MLS profiles of the five constituents alongside total ozone column from the Ozone Monitoring Instrument. The dynamics and tropospheric water vapor are constrained by assimilated meteorological fields from MERRA-2. The assimilated constituent fields and meteorology are provided to users at a 50-km horizontal resolution and a three-hourly frequency. Monthly analysis uncertainties and flags are also provided to the users. M2-SCREAM is an accurate and dynamically consistent high-resolution data record of the five constituents, all of which are of primary importance to stratospheric chemistry and transport studies. We will present a description of M2-SCREAM and selected results of a process-based evaluation of this product using independent data. As an illustration, we will discuss the perturbation to stratospheric composition from the eruption of Hunga Tonga–Hunga Ha'apai in January 2022 as seen in the reanalysis. We will also propose potential scientific applications of M2-SCREAM and outline plans for an upcoming comprehensive composition reanalysis that is being developed at NASA GMAO.

MERRA-2↗

Atmospheric Tar Balls: Particles from Biomass and Biofuel Burning

Tar balls are amorphous, carbonaceous spherules that occur in the tropospheric aerosol as a result of biomass and biofuel burning. They form a distinct group of particles with diameters typically between 30 and 500 nm and readily identifiable with electron microscopy. Their lack of a turbostratic microstructure distinguishes them from soot, and their morphology and composition (approximately 90 mol% carbon) renders them distinct from other carbonaceous particles. Tar balls are particularly abundant in slightly aged (minutes to hours old) biomass smoke, indicating that they likely form by gas-to-particle conversion within smoke plumes. The material of tar balls is initially hygroscopic; however, the particles become largely insoluble as a result of free radical polymerization of their organic molecules. Consequently, tar balls are primarily externally mixed with other particle types, and they do not appreciably increase in size during aging. When tar balls coagulate with water-bearing particles, their material may partly dissolve and no longer be recognizable as distinct particles. Tar balls may contain organic compounds that absorb sunlight. They are an important, previously unrecognized type of carbonaceous (organic) atmospheric particle.

Posfai, Mihaly↗

Aerosol Abundances and Optical Characteristics in the Pacific Basin Free Troposphere

During NASA's Global Backscatter Experiment (GLOBE) mission flights in November 1989 and May 1990, a DC-8 research aircraft probed the Pacific Basin free troposphere for about 90 flight hours in each month between +72 and -62 degrees latitude, +130 and -120 degrees longitude, and up to 39,000 feet pressure altitudes. Aerosols were sampled continuously in situ by optical particle counters to measure concentration and particle size, and during 48 10-min intervals during each mission by wire impactors for concentration, size, composition, phase and shape analyses. The optical particle counters cover a particle diameter range between 0.3 and 20 microns; wire impactors extend the range down to 0.03 microns. Results of particle number, size, shape, together with the assumption of a refractive index corresponding to (NH4)2SO4 to account for the prevalence of aerosol sulfur, were utilized in a Mie algorithm to calculate aerosol extinction and backscatter for a range of wavelengths (0.385 less than lambda less than 10.64 microns). Computations for 22 randomly selected size distributions yield coefficients of extinction E(0.525) = (2.03 +/- 1.20) x 10(exp -4) km(exp -1) and backscatter beta(0.525) = (6.45 +/- 3.49) x 10(exp -6) km(exp -1) sr(exp -1) in the visible, and E(10.64) = (8.13 +/- 6.47) x 10(exp -6) km(exp -1) and beta(10.64) = (9.98 +/- 10.69) x 10(exp -8) km(exp -1) sr(exp -1) in the infrared, respectively. Large particles (D greater than 0.3 microns) contribute two-thirds to the total extinction in the visible (lambda = 0.525 microns), and almost 100% in the infrared (lambda = 10.64 microns). These results have been used to define an IR optical aerosol climatology of the Pacific Basin free troposphere, from which it follows that the infrared backscatter coefficient at lambda = 9.25 microns wavelength fluctuates between 5.0 x 10(exp -10) and 2.0 x 10(exp -7) km(exp -1) sr(exp -1) with a modal value 2.0 x 10(exp -8) km(exp -1) sr(exp -1).

Pueschel, R. F.↗

Meteorological context for fall experiments including distributions of water vapor, ozone, and carbon monoxide

Meteorological contexts for the NASA GTE/CITE 1 fall 1983 flight series are presented and discussed. The large-scale wind, cold cloud, and moisture patterns are illustrated by composite diagrams based on the National Oceanic and Atmospheric Administration 700-, 500-, and 250-mbar analyses and the GOES-West broadband and 6.7-micron (water vapor) infrared photographs. Detailed flight path diagrams are included for seven maritime flights and one continental flight in the free troposphere and boundary layer. For three flights from Hickam Field, in Honolulu, HI, to the Intertropical Convergence Zone, vertical profiles of temperature, dew/frost point departures, wind velocity, and ozone, and carbon monoxide mixing ratios are also presented and discussed. Excellent agreement is demonstrated between the in situ and remote measurements. In particular, the predictive and diagnostic value of the 6.7-micron water vapor photographs is demonstrated.

Danielsen, Edwin F.↗

Projecting the Lasting Fate of the Hunga Tonga-Hunga Ha’apai Eruption on the Stratosphere through Connecting Measurements to Models

On 15th Jan. 2022 the submarine volcano Hunga Tonga-Hunga Ha’apai (HTHH) injected approximately 0.5 Tg of sulfur dioxide into the stratosphere, but more significantly added 150-170 Tg of water vapor to the stratospheric background (over a 10% perturbation) in a matter of several hours. The sulfur dioxide rapidly converted to sulfate aerosol and along with water vapor, was transported around the Southern Hemisphere sub-tropics into midlatitudes with some transport into the Northern Hemisphere. With a much longer lifetime than sulfate aerosol, measurable water vapor anomalies are likely to persist for the remainder of the decade. Satellite measurements from limb and nadir viewing observing instruments provide the information needed to reasonably initialize the HTHH eruption in the Goddard Earth Observing System (GEOS) model using the “replay” framework coupled to the Global Modeling Initiative (GMI) stratosphere-troposphere chemical mechanism for the recent past and continue the simulations into the future with the free running chemistry climate model (CCM). Using a number of model ensemble members together with the satellite observations, we are beginning to quantify how the HTHH eruption is perturbing stratospheric composition and climate and projecting the influences to come as the enhanced water vapor continues to spread globally with only very slow removal mechanisms. We will also discuss some of the future measurement needs to understand how the atmosphere is responding to events like the HTHH eruption, large wildfires, and a changing climate.

volcano↗

Seasonal Change on Saturn from Cassini/CIRS Observations, 2004-2009

Five years of thermal infrared spectra from the Cassini Composite Infrared Spectrometer (CIRS) are analyzed to determine the response of Saturn's atmosphere to seasonal changes in insolation. Hemispheric mapping sequences at 15.0 cm-1 spectral resolution are used to retrieve the variation in the zonal mean temperatures in the stratosphere (0.5-5.0 mbar) and upper troposphere (75-800 mbar) between October 2004 (shortly after the summer solstice in the southern hemisphere) and July 2009 (shortly before the autumnal equinox). Saturn's northern mid-latitudes show signs of dramatic warming in the stratosphere (by 6-10 K) as they emerge from ring-shadow into springtime conditions, whereas southern mid-latitudes show evidence for cooling (4-6 K). The 40-K asymmetry in stratospheric temperatures between northern and southern hemispheres (at 1 mbar) slowly decreased during the timespan of the observations. Tropospheric temperatures also show temporal variations but with a smaller range, consistent with the increasing radiative time constant of the atmospheric response with increasing pressure. The tropospheric response to the insolation changes shows the largest magnitude at the locations of the broad retrograde jets. Saturn's warm south-polar stratospheric hood has cooled over the course of the mission, but remains present. Stratospheric temperatures are compared to a radiative climate model which accounts for the spatial distribution of the stratospheric coolants. The model successfully predicts the magnitude and morphology of the observed changes at most latitudes. However, the model fails at locations where strong dynamical perturbations dominate the temporal changes in the thermal field, such as the hot polar vortices and the equatorial semi-annual oscillation (Orton, G., and 27 colleagues [2008]. Nature 453, 196-198). Furthermore, observed temperatures in Saturn's ring-shadowed regions are larger than predicted by all radiative-climate models to date due to the incomplete characterization of the dynamical response to the shadow. Finally, far-infrared CIRS spectra are used to demonstrate variability of the para-hydrogen distribution over the 5-year span of the dataset, which may be related to observed changes in Saturn's tropospheric haze in the spring hemisphere.

Fletcher, Leigh N.↗