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At least 433 records · Page 24

The Relative Importance of Random Error and Observation Frequency in Detecting Trends in Upper Tropospheric Water Vapor

Recent published work assessed the amount of time to detect trends in atmospheric water vapor over the coming century. We address the same question and conclude that under the most optimistic scenarios and assuming perfect data (i.e., observations with no measurement uncertainty) the time to detect trends will be at least 12 years at approximately 200 hPa in the upper troposphere. Our times to detect trends are therefore shorter than those recently reported and this difference is affected by data sources used, method of processing the data, geographic location and pressure level in the atmosphere where the analyses were performed. We then consider the question of how instrumental uncertainty plays into the assessment of time to detect trends. We conclude that due to the high natural variability in atmospheric water vapor, the amount of time to detect trends in the upper troposphere is relatively insensitive to instrumental random uncertainty and that it is much more important to increase the frequency of measurement than to decrease the random error in the measurement. This is put in the context of international networks such as the Global Climate Observing System (GCOS) Reference Upper-Air Network (GRUAN) and the Network for the Detection of Atmospheric Composition Change (NDACC) that are tasked with developing time series of climate quality water vapor data.

Whiteman, David N.↗

NASA's High-Resolution GEOS Forecasting and Reanalysis Products: Support for TOLNet

Stratospheric intrusions (SIs) the introduction of ozone-rich stratospheric air into the troposphere – have been the interest of decades of research for their link with surface ozone air quality exceedances, especially at the high elevations in the western USA in springtime; however, the impact of SIs in the remaining seasons and over the rest of the USA is less clear. We can expect MERRA-2 to realistically represent both atmospheric dynamics and composition. The operational GEOS weather forecasting system, GEOS-FP, has a similar ozone observing system to MERRA-2, while NASA's new global high-resolution air quality forecast system, GEOS-CF, combines the operational GEOS weather forecasting model with the state-of-the-science GEOS-Chem chemistry module (version 12), simulating a wide range of additional air pollutants and tracers which strengthens this detailed analysis of the intrusions and the sources for the high ozone concentrations. Using a multitude of observational datasets, including lidar, air craft, ozonesondes and air quality monitoring surface sites, in combination with the GEOS forecast and reanalysis products, we aim to provide the public with tools which are available in near-real time to enhance their capability to identify the impact of stratospheric air on surface ozone concentrations separate from anthropogenic sources. In particular, improved understanding of the connections between large-scale climate variability and local-scale dynamically-driven air quality events may support improved seasonal prediction of SI events.

Knowland, K. Emma↗

Oxygenated Organic Chemicals in the Pacific Troposphere: Distribution, Sources and Chemistry

Airborne measurements of a large number of oxygenated organic chemicals (Oxorgs) were carried out in the Pacific troposphere (0.1-12 km) in the Spring of 2001 (Feb. 24-April 10). Specifically these measuremen ts included acetone, methylethyl ketone (MEK), methanol, ethanol, ace taldehyde, propionaldehyde, PANS, and organic nitrates. Complementary measurements of formaldehyde, organic peroxides, and tracers were al so available. Ox-orgs were abundant in the clean troposphere and were greatly enhanced in the outflow regions from Asia. Their mixing ratios were typically highest in the lower troposphere and declined toward s the upper troposphere and the lowermost stratosphere. Their total a bundance (Ox-orgs) significantly exceeded that of NMHC (C2-C8 NMHC). A comparison of these data with observations collected some seven yea rs earlier (Feb.-March, 1994), did not reveal any significant changes . Throughout the troposphere mixing ratios of Ox-orgs were strongly c orrelated with each other as well as with tracers of fossil and bioma sshiof'uel combustion. Analysis of the relative enhancement of selected Oxorgs with respect to CH3Cl and CO in twelve sampled plumes, origi nating from fires, is used to assess their primary and secondary sour ces from biomass combustion. The composition of these plumes also ind icates a large shift of reactive nitrogen into the PAN reservoir ther eby limiting ozone formation. The Harvard 3-D photochemical model, th at uses state of the art chemistry and source information, is used to compare simulated and observed mixing ratios of selected species. A 1 -D model is used to explore the chemistry of aldehydes. These results will be presented.

Singh, Hanwant B.↗

Next-Generation Aura/OMI NO2 and SO2 Products

The measurement of both SO2 and NO2 gases are recognized as an essential component of atmospheric composition missions. We describe current capabilities and limitations of the operational Aura/OMI NO2 and SO2 data that have been used by a large number of researchers. Analyses of the data and validation studies have brought to light a number of areas in which these products can be expanded and improved. Major improvements for new NASA standard (SP) NO2 product include more accurate tropospheric and stratospheric column amounts, along with much improved error estimates and diagnostics. Our approach uses a monthly NO2 climatology based on the NASA Global Modeling Initiative (GMI) chemistry-transport model and takes advantage of OMI data from cloudy scenes to find clean areas where the contribution from the trap NO2 column is relatively small. We then use a new filtering, interpolation and smoothing techniques for separating the stratospheric and tropospheric components of NO2, minimizing the influence of a priori information. The new algorithm greatly improves the structure of stratospheric features relative to the original SP. For the next-generation OMI SO2 product we plan to implement operationally the offline iterative spectral fitting (ISF) algorithm and re-process the OMI Level-2 SO2 dataset using a priori SO2 and aerosol profiles, clouds, and surface reflectivity appropriate for observation conditions. This will improve the ability to detect and quantify weak tropospheric SO2 loadings. The new algorithm is validated using aircraft in-situ data during field campaigns in China (2005 and 2008) and in Maryland (Frostburg, 2010 and DISCOVER-AQ in July 2011). The height of the SO2 plumes will also be estimated for high SO2 loading cases (e.g., volcanic eruptions). The same SO2 algorithm will be applied to the data from OMPS sensor to be launched on NPP satellite later this year. The next-generation NO2 and SO2 products will provide critical information (e.g., averaging kernels) for evaluation of chemistry-transport models, for data assimilation, and to impose top-down constraints on the SO2 and NO2 emission sources.

Krotkov, Nickolay↗

The Abundances of Methane and Ortho/Para Hydrogen in Uranus and Neptune: Implications of New Laboratory 4-0 H(sub 2) Quadrapole Line Parameters

The tropospheric methane molar fraction (f(sub ch4,t)) and the ortho/para hydrogen ratio are derived for Uranus and Neptune based on new determinations of spectroscopic parameters for key hydrogen features as reported by Ferguson et al. (1993, J. Mol. Spec 160, 315-325). For each planet, the relatively weak laboratory linestrengths (approximately 30% and 15% less than the theoretical 4-0 S(0) and S(1) linestrengths, respectively) results, when compared to analyses adopting theoretical values, in a ~30% decrease in the tropospheric methane ratio and a comparable increase in the pressure level of the optically-thick cloudtop marking the bottom of the visible atmosphere (P(sub cld)).

Uranus atmosphere; Neptune atmosphere; abundances ↗

An Assessment of Our Ability to Model the Upper Troposphere and Lower Stratosphere in Interactive Climate Models

The physics of the upper troposphere is dominated by the different phases of water, while the lower stratosphere is governed by the presence of ozone. The tropopause may be regarded as the layer which separates the regions where stratospheric and tropospheric processes dominate the physics, but it is clearly not a smooth transition level. Modelling this region in comprehensive climate models is complicated, partly because of the constraints inherent in numerical methods (such as the finite resolution used in models) and partly because of our incomplete knowledge of the physical and chemical interactions which occur (such as the phase transitions of water and the composition of aerosols). However, studies of stratospheric impacts on climate change clearly require the tropopause region to be modelled with a high degree of accuracy. This paper will examine how well we can currently model the structure and dynamics of the tropopause region; this includes some comparisons of the simulated atmospheric composition with observational estimates of these species, some studies of discrepancies between forecasts and observations in the Data Assimilation System of the Data Assimilation office, and inferences for sparsely observed quantities. The analysis will focus on meteorological quantities, physical forcing mechanisms, and the transport and interactions of trace species.

Pawson, Steven↗

Convective Transport to the Upper Troposphere and Lower Stratosphere Over the Asian Summer Monsoon as Observed During the 2022 ACCLIP Airborne Campaign

Deep convection in the Asian summer monsoon (ASM) rapidly transports boundary layer pollutants including ozone-depleting substances into the upper troposphere and lower stratosphere (UTLS). The confinement of the seasonal anticyclonic circulation in the UTLS over Asia initially traps the pollutants near the tropopause level, but air masses are subsequently transported throughout the global stratosphere and impact Earth’s climate. Characterizing the transport pathways and processes of these pollutants are critical for identifying source regions and quantifying regional contributions to global stratospheric concentrations. The Asian summer monsoon Chemical and Climate Impact Project (ACCLIP) was conducted in summer 2022 using two high-altitude aircraft (NSF NCAR Gulfstream V and the NASA WB-57) to obtain UTLS chemical composition and aerosol distribution for characterizing the impact of the ASM on global chemistry and climate. Backward trajectories from ACCLIP flight tracks were traced through time-varying, satellite-derived global convective cloud top altitude fields to investigate the convective air mass origins of the sampled air parcels. Analyses reveal that air masses lofted by convection within the ASM (South Asian summer monsoon) and near the edge of the of the ASM anticyclone (East Asian summer monsoon) contributed to the airborne observations. In this study, we present a summary of the transport statistics of UTLS air masses sampled during ACCLIP and discuss the implications of these results on our understanding of the role of ASM in global constituent transport.

Convective↗

Meridional Variations of C2H2 and C2H6 in Jupiter's Atmosphere from Cassini CIRS Infrared Spectra

Hydrocarbons such as acetylene (C2H2) and ethane (C2H6) are important tracers in Jupiter's atmosphere, constraining our models of the chemical and dynamical processes. However, our knowledge of the vertical and meridional variations of their abundances has remained sparse. During the flyby of the Cassini spacecraft in December 2000, the Composite Infrared Spectrometer (CIRS) instrument was used to map the spatial variation of emissions from 10-1400 cm(sup -1) (1000-7 microns). In this paper we analyze a zonally-averaged set of CIRS spectra taken at the highest (0.5 cm(sup -1)) resolution, to infer atmospheric temperatures in the stratosphere at 0.5-20 mbar via the v4 band of CH4, and in the troposphere at 150-400 mbar, via the H2 absorption at 600-800 cm(sup -1). Simultaneously, we retrieve the abundances of C2H2 and C2H6 via the v5 and vg bands respectively. Tropospheric absorption and stratospheric emission are highly anti-correlated at the CIRS resolution, introducing a non-uniqueness into the retrievals, such that vertical gradient and column abundance cannot both be found without additional constraints. Assuming profile gradients from photochemical calculations, we show that the column abundance of C2H2 decreases sharply towards the poles by a factor approximately 4, while C2H6 is unchanged in the north and increasing in the south, by a factor approximately 1.8. An explanation for the meridional trends is proposed in terms of a combination of photochemistry and dynamics. Poleward, the decreasing UV flux is predicted to decrease the abundances of C2H2 and C2H6 by factors 2.7 and 3.5 respectively at a latitude 70 deg. However, the lifetime of C2H6 in the stratosphere (5 x 10(exp 9)) is much longer than the dynamical timescale for meridional motions inferred from SL-9 debris (5 x 10(exp 8 s)), and therefore the constant or rising abundance towards high latitudes likely indicates that meridional mixing dominates over photochemical effects. For C2H2, the opposite occurs, with the relatively short photochemical lifetime (3 x 10(exp 7 s)), compared to meridional mixing times, ensuring that the expected photochemical trends are visible.

Nixon, C. A.↗

Evidence for subsidence in the 1989 Arctic winter stratosphere from airborne infrared composition measurements

Simultaneous measurements of the stratospheric burdens of CO2, HCN, N2O, CH4, OCS, CF2Cl2, CFCl3, CHF2Cl and HF were made by the Jet propulsion Laboratory MkIV interferometer on board the NASA DC-8 aircraft during January and early February 1989 as part of the Airborne Arctic Stratosphere Experiment. Data were acquired on 11 flights at altitudes of up to 12 km over a geographic region covering the NE Atlantic Ocean, Iceland and Greenland. The results obtained show large variations in the burdens of these tracers due to the effects of transport. The tropospheric source gas burdens were reduced inside the polar vortex, suggesting that the air had subsided with respect to the surrounding midlatitude air. Increased HF burdens inside the vortex support this interpretation. The results obtained from the different tracers are highly consistent with each other and indicate that in the 15- to 20-km altitude range inside the vortex, surfaces of constant volume mixing ratio were located some 5-6 km lower in absolute altitude than outside the vortex. The results also indicate that the magnitude of this subsidence increases with altitude. These conclusions are consistent with other measurements.

Toon, G. C.↗

Aerosol Chemical Composition in Asian Continental Outflow during the TRACE-P Campaign: Comparison with PEM-West B

Aerosol associated soluble ions and the radionuclide tracers (7)Be and (210)Pb were quantified in 414 filter samples collected in spring 2001 from the DC-8 during the Transport and Chemical Evolution over the Pacific (TRACE-P) campaign. Binning the data into near Asia (flights from Hong Kong and Japan) and remote Pacific (all other flights) revealed large enhancements of NO3(-), SO4(-), C2O4(-), NH4(+), K(+), Mg2(+), and Ca2(+) near Asia. The boundary layer and lower troposphere were most strongly influenced by continental outflow, and the largest enhancements were seen in Ca2(+) (a dust tracer) and NO3(-) (reflecting uptake of HNO3 onto the dust). Comparing the TRACE P near Asia bin with earlier results from the same region during PEM-West B (in 1994) shows at least twofold enhancements during TRACE P in most of the ions listed above. Calcium and NO3(-) were most enhanced in this comparison as well (more than sevenfold higher in the boundary layer and threefold higher in the lower troposphere). Independent estimation of Asian emissions of gaseous precursors of the aerosol-associated ions suggest only small changes between the two missions, and precipitation fields do not suggest any significant difference in the efficiency of the primary sink, precipitation scavenging. It thus appears that with the possible exception of dust, the enhancements of aerosol-associated species during TRACE P cannot be explained by stronger sources or weaker sinks. We argue that the enhancements largely reflect the fact that TRACE P focused on characterizing Asian outflow, and thus the DC-8 was more frequently flown into regions that were influenced by well-organized flow off the continent.

Dibb, Jack E.↗

Scattering and Absorption by Nonspherical Particles in Planetary Atmospheres

The atmospheres of Mars, the giant planets, and Titan all support populations of nonspherical particles. Analyses of observations of these atmospheres therefore rely on an understanding of the optical properties of nonspherical particles. We can glean information on particle size and composition from the wavelength dependence of the optical depth and from the shape of the forward peak of the scattering phase function. Additional information comes from polarization measurements which have been especially fruitful for Titan's haze. The Mars atmosphere contains mineral dust particles with effective radii near 1.6 micro meters, and water ice particles with radii between about 1 and 4 micro meters. The uppermost tropospheric hazes in Jupiter and Saturn are composed of ice crystals of ammonia, water and possibly traces of ammonium hydrosulfide, Methane ice and hydrogen sulfide ice are present in the atmospheres of Uranus and Neptune. Size estimation for these hazes in the giant planets is difficult, and even the expected spectral signatures are elusive, Titan's haze is both forward scattering and strongly polarized - a combination which points toward a fractal aggregate struc1.ure of 10 - 100 or more organic monomers whose radius is about 0.06 micro meters. Polar stratospheric hazes on Jupiter and Saturn also display this characteristic.

nonsperical particles↗

Radiative Forcing Due to Enhancements in Tropospheric Ozone and Carbonaceous Aerosols Caused by Asian Fires During Spring 2008

Simulations of tropospheric ozone and carbonaceous aerosol distributions, conducted with the Real-time Air Quality Modeling System (RAQMS), are used to study the effects of major outbreaks of fires that occurred in three regions of Asia, namely Thailand, Kazakhstan, and Siberia, during spring 2008. RAQMS is a global scale meteorological and chemical modeling system. Results from these simulations, averaged over April 2008, indicate that tropospheric ozone column increases by more than 10 Dobson units (DU) near the Thailand region, and by lesser amounts in the other regions due to the fires. Widespread increases in the optical depths of organic and black carbon aerosols are also noted. We have used an off-line radiative transfer model to evaluate the direct radiative forcing due to the fire-induced changes in atmospheric composition. For clear sky, the monthly averaged radiative forcing at the top of the atmosphere (TOA) is mostly negative with peak values less than -12 W/sq m occurring near the fire regions. The negative forcing represents the increased outgoing shortwave radiation caused by scattering due to carbonaceous aerosols. At high latitudes, the radiative forcing is positive due to the presence of absorbing aerosols over regions of high surface albedo. Regions of positive forcing at TOA are more pronounced under total sky conditions. The monthly averaged radiative forcing at the surface is mostly negative, and peak values of less than -30 W/sq m occur near the fire regions. Persistently large negative forcing at the surface could alter the surface energy budget and potentially weaken the hydrological cycle.

Natarajan, Murali↗

Constraining Venus Cloud Habitability: Earth's Aerobiosphere as an Analogue Environment

The potential habitability of Venus's cloud and haze layers has been debated for decades, with interest fueled by observations including disequilibria in atmospheric chemistry, strongly UV-absorbing particles, and (most recently) a controversial phosphine detection. Venus cloud temperature and pressure are clement by Earth standards; however, the calculated high acid activity and low water activity may exceed the limits of Earth biochemistry, based on observed life in extreme environments. A significant challenge in understanding Venus's habitability is the lack of an appropriate terrestrial analogue environment. Life has not been found in hydrothermal systems approaching Venus aerosol acidities, but these systems also contain high levels of other harsh solutes. Earth's stratospheric sulfate layer is a partial match in terms of acidity, desiccation, size, and isolation from the surface, but the few samples returned from these altitudes have yielded only sparse, inactive cells. Earth's tropospheric cloud droplets have an active microbial presence, but are larger and far more water-rich than Venus aerosols; tropospheric times aloft are also similar to microbial generation times, making Earth's aerobiosphere dependent on continuous surface replenishment. Direct detection of potential biosignatures from a single transect is challenging; Earth's cloud microbiota yields 102 - 108 viable cells per mL, equivalent to one per 103 - 109 particles, with highly dynamic and heterogeneous distribution. The most important in situ measurement for Venus cloud habitability is detailed aerosol composition: confirmation of acid and water activity, presence of potentially bioavailable nutrients and energy, and potential presence of organic matter. Modeling Venus cloud aerosol residence time in comparison to periodic influxes of water and photochemical energy, and thus the ability of an ecosystem to maintain itself over time, would also address a significant habitability constraint particular to aerobiospheres.

Venus↗

The Thermal Structure and Composition of Jupiter's Great Red Spot From JWST/MIRI

Jupiter's Great Red Spot (GRS) was mapped by the James Webb Space Telescope (JWST)/Mid-Infrared Instrument (4.9–27.9 μm) in July and August 2022. These observations took place alongside a suite of visual and infrared observations from; Hubble, JWST/NIRCam, Very Large Telescope/VISIR and amateur observers which provided both spatial and temporal context across the jovian disc. The stratospheric temperature structure retrieved using the NEMESIS software revealed a series of hot-spots above the GRS. These could be the consequence of GRS-induced wave activity. In the troposphere, the temperature structure was used to derive the thermal wind structure of the GRS vortex. These winds were only consistent with the independently determined wind field by JWST/NIRCam at 240 mbar if the altitude of the Hubble-derived winds were located around 1,200 mbar, considerably deeper than previously assumed. No enhancement in ammonia was found within the GRS but a link between elevated aerosol and phosphine abundances was observed within this region. North-south asymmetries were observed in the retrieved temperature, ammonia, phosphine and aerosol structure, consistent with the GRS tilting in the north-south direction. Finally, a small storm was captured north-west of the GRS that displayed a considerable excess in retrieved phosphine abundance, suggestive of vigorous convection. Despite this, no ammonia ice was detected in this region. The novelty of JWST required us to develop custom-made software to resolve challenges in calibration of the data. This involved the derivation of the “FLT-5” wavelength calibration solution that has subsequently been integrated into the standard calibration pipeline.

Jake Harkett↗

The CRYSTAL-FACE Mission

The Cirrus Regional Study of Tropical Anvils and Cirrus Layers - Florida Area Cirrus Experiment (CRYSTAL-FACE) was a measurement campaign designed to investigate tropical cirrus cloud physical properties and formation processes. Understanding the production of upper tropospheric cirrus clouds is essential for the successful modeling of the Earth's climate. The mission was staged in July 2002 with flights of 6 aircraft from Key West, Florida. Several aircraft were used for in situ and remote sensing of aerosols, ice crystals, meteorological fields, radiative fluxes, and gas concentrations. The NASA ER-2 and WB-57, the Proteus aircraft, owned by Northrop Grumman and operated by Scaled Composites, CIRPAS provided the DeHavilland UV-l8A, "Twin Otter" aircraft, the University of North Dakota provided a Cessna Citation II aircraft , and NSF supported the ELDORA radar onboard the Naval Research Laboratory P-3 aircraft. In this presentation, I will describe some of the flights, the conditions, and some of the results from the mission.

Newman, P.↗

Evaluating Ammonium, Nitrate and Sulfate Aerosols in 3-Dimensions

The effect aerosols have on climate and air quality is a func-on of their chemical composi-on, concentra-on and spa-al distribu-on. These parameters are controlled by emissions, heterogeneous and homogeneous chemistry, where thermodynamics plays a key role, transport, which includes stratospheric-­‐ tropospheric exchange, and deposi-onal sinks. In this work we demonstrate the effect of some of these processes on the SO4‐NH4­‐NO3 system using the GISS ModelE2 Global Circula-on Model (GCM).

Aerosols↗

Eddy mixing coefficient on Saturn

Data on the composition, thermal structure, and Lyman-alpha dayglow of Saturn, when analyzed in conjunction with photochemical models of the hydrocarbons and the atomic hydrogen production, yield the homopause value of the eddy diffusion coefficient to be approximately 100 million/sq cm per sec. The equatorial value of the eddy diffusion coefficient at the homopause of Saturn is thus found to be approximately 100 times greater than on Jupiter. The mesosphere (and presumably, troposphere) of Saturn appears to be considerably more turbulent than the upper atmosphere of Jupiter.

Atreya, S. K.↗

Cassini/CIRS capabilities for aerosol, cloud, and surface measurements

Information that should be revealed by the Cassini Composite Infrared Spectrometer (CIRS) about the aerosol, cloud, and surface properties of Titan are addressed. Limb sounding data will be used to determine aerosol abundances, scale heights, and gradients between 80 and 400 km for various latitudes. Stratospheric condensate cloud top altitudes and column abundances will be inferred as functions of latitude. A search for new species will be conducted. Thermal maps between 500 and 550/cm will be used to investigate tropospheric methane clouds and surface topography; time resolution provided by different orbits will be used to distinguish the two.

Samuelson, Robert E.↗