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NASA NTRS2012

Active Upper-atmosphere Chemistry and Dynamics from Polar Circulation Reversal on Titan

Saturn's moon Titan has a nitrogen atmosphere comparable to Earth's, with a surface pressure of 1.4 bar. Numerical models reproduce the tropospheric conditions very well but have trouble explaining the observed middle-atmosphere temperatures, composition and winds. The top of the middle-atmosphere circulation has been thought to lie at an altitude of 450 to 500 kilometres, where there is a layer of haze that appears to be separated from the main haze deck. This 'detached' haze was previously explained as being due to the colocation of peak haze production and the limit of dynamical transport by the circulation's upper branch. Herewe report a build-up of trace gases over the south pole approximately two years after observing the 2009 post-equinox circulation reversal, from which we conclude that middle-atmosphere circulation must extend to an altitude of at least 600 kilometres. The primary drivers of this circulation are summer-hemisphere heating of haze by absorption of solar radiation and winter-hemisphere cooling due to infrared emission by haze and trace gases; our results therefore imply that these effects are important well into the thermosphere (altitudes higher than 500 kilometres). This requires both active upper-atmosphere chemistry, consistent with the detection of high-complexity molecules and ions at altitudes greater than 950 kilometres, and an alternative explanation for the detached haze, such as a transition in haze particle growth from monomers to fractal structures.

Titan Atmosphere↗
NASA NTRS2008

Measurement of Atmospheric Composition from Geostationary Platforms

Satellite instruments flown since 1970 have had great success in elucidating the processes that control stratospheric ozone. In contrast, space-based data for tropospheric constituents that affect air quality and climate have only recently become available. While these datasets highlight the rapidly advancing capabilities of spacebased tropospheric sensors, they are also pointing to the limitations of sun-synchronous, low-earth orbiting (SSO/LEO) satellite platforms for making such measurements. In our talk we will highlight the science requirements for new missions and the technological and algorithmic approaches that we are developing to meet these requirements. From these studies a clear need for advanced atmospheric composition sensors has emerged that can be put on geostationary (GEO) platforms to provide 5 km horizontal resolution with 15-60 minutes repeat cycle. Such measurements have been high priority in the recently released Decadal Survey report by the US National Research Council. The need for GEO is driven not only by the science requirements to track rapidly changing pollution events but also by the need to provide altitude-resolved information about tropospheric constituents. Currently, with the exception of aerosols, it is not possible to derive profile information about lower tropospheric constituents from satellite measurements. New algorithmic approaches are being developed to obtain this information by combining UV and IR data, by monitoring the spatial and temporal structures of the constituents, and by using low-level clouds to separate boundary layer constituents from free troposphere. All these approaches require better spatial and temporal resolution than that provided by LEO sensors.

Bhartia, P. K.↗
NASA NTRS1996

Chemical Characteristics of Continental Outflow Over the Tropical South Atlantic Ocean from Brazil and Africa

The chemical characteristics of air parcels over the tropical South Atlantic during September - October 1992 are summarized by analysis of aged marine and continental outflow classifications. Positive correlations between CO and CH3CL and minimal enhancements of C2CL40, and various ChloroFluoroCarbon (CFC) species in air parcels recently advected over the South Atlantic basin strongly suggest an impact on tropospheric chemistry from biomass burning on adjacent continental areas of Brazil and Africa. Comparison of the composition of aged Pacific air with aged marine air over the South Atlantic basin from 0.3 to 12.5 km altitude indicates potential accumulation of long-lived species during the local dry season. This may amount to enhancements of up to two-fold for C2H6, 30% for CO, and 10% for CH3Cl. Nitric oxide and NO(x) were significantly enhanced (up to approx. 1 part per billion by volume (ppbv)) above 10 km altitude and poorly correlated with CO and CH3Cl. In addition, median mixing ratios of NO and NO(x) were essentially identical in aged marine and continental outflow air masses. It appears that in addition to biomass burning, lightning or recycled reactive nitrogen may be an important source of NO(x) to the upper troposphere. Methane exhibited a monotonic increase with altitude from approx. 1690 to 1720 ppbv in both aged marine and continental outflow air masses. The largest mixing ratios in the upper troposphere were often anticorrelated with CO, CH3Cl, and CO2, suggesting CH, contributions from natural sources. We also argue, based on CH4/CO ratios and relationships with various hydrocarbon and CFC species, that inputs from biomass burning and the northern hemisphere are unlikely to be the dominant sources of CO, CH4 and C2H6 in aged marine air. Emissions from urban areas would seem to be necessary to account for the distribution of at least CH4 and C2H6. Over the African and South American continents an efficient mechanism of convective vertical transport coupled with large-scale circulations conveys biomass burning, urban, and natural emissions to the upper troposphere over the South Atlantic basin. Slow subsidence over the eastern South Atlantic basin may play an important role in establishing and maintaining the rather uniform vertical distribution of long-lived species over this region. The common occurrence of values greater than 1 for the ratio CH3OOH/H2O2 in the upper troposphere suggests that precipitation scavenging effectively removed highly water soluble gases (H2O2, HNO3, HCOOH, and CH3COOH) and aerosols during vertical convective transport over the continents. However, horizontal injection of biomass burning products over the South Atlantic, particularly water soluble species and aerosol particles, was frequent below 6 km altitude.

Talbot, R. W.↗
NASA NTRS2004

Analysis of the Atmospheric Distribution, Sources, and Sinks of Oxygenated Volatile Organic Chemicals Based on Measurements over the Pacific during TRACE-P

Airborne measurements of a large number of oxygenated volatile organic chemicals (OVOC) were carried out in the Pacific troposphere (0.1-12 km) in winter/spring of 2001 (24 February to 10 April). Specifically, these measurements included acetone (CH3COCH3), methylethyl ketone (CH3COC2H5, MEK), methanol (CH3OH), ethanol (C2H5OH), acetaldehyde (CH3CHO), propionaldehyde (C2H5CHO), peroxyacylnitrates (PANs) (C(sub n)H(sub 2n+1)COO2NO2), and organic nitrates (C(sub n)H(sub 2n+1)ONO2). Complementary measurements of formaldehyde (HCHO), methyl hydroperoxide (CH3OOH), and selected tracers were also available. OVOC were abundant in the clean troposphere and were greatly enhanced in the outflow regions from Asia. Background mixing ratios were typically highest in the lower troposphere and declined toward the upper troposphere and the lowermost stratosphere. Their total abundance (Summation of OVOC) was nearly twice that of nonmethane hydrocarbons (Summation of C2-C8 NMHC). Throughout the troposphere, the OH reactivity of OVOC is comparable to that of methane and far exceeds that of NMHC. A comparison of these data with western Pacific observations collected some 7 years earlier (February-March 1994) did not reveal significant differences. Mixing ratios of OVOC were strongly correlated with each other as well as with tracers of fossil and biomass/biofuel combustion. Analysis of the relative enhancement of selected OVOC with respect to CH3Cl and CO in 12 plumes originating from fires and sampled in the free troposphere (3-11 km) is used to assess their primary and secondary emissions from biomass combustion. The composition of these plumes also indicates a large shift of reactive nitrogen into the PAN reservoir thereby limiting ozone formation. A three-dimensional global model that uses state of the art chemistry and source information is used to compare measured and simulated mixing ratios of selected OVOC. While there is reasonable agreement in many cases, measured aldehyde concentrations are significantly larger than predicted. At their observed levels, acetaldehyde mixing ratios are shown to be an important source of HCHO (and HO x ) and PAN in the troposphere. On the basis of presently known chemistry, measured mixing ratios of aldehydes and PANs are mutually incompatible. We provide rough estimates of the global sources of several OVOC and conclude that collectively these are extremely large (150-500 Tg C / yr) but remain poorly quantified.

Singh, H. B.↗
NASA NTRS1994

Summertime distribution of PAN and other reactive nitrogen species in the northern high-latitude atmosphere of eastern Canada

Aircraft measurements of key reactive nitrogen species (NO, NO2, HNO3, PAN, PPN, NO3(-), NO(y)), C1 to C6 hydrocarbons, acetone, O3, chemical tracers (C2Cl4, CO), and important meteorological parameters were performed over eastern Canada during July to August 1990 at altitudes between 0 and 6 km as part of an Arctic Boundary Layer Expedition (ABLE3B). In the free troposphere, PAN was found to be the single most abundant reactive nitrogen species constituting a major fraction of NO(y) and was significantly more abundant than NO(x) and HNO3. PAN and O3 were well correlated both in their fine and gross structures. Compared to data previously collected in the Arctic/subarctic atmosphere over Alaska (ABLE3A), the lower troposphere (0-4 km) over eastern Canada was found to contain larger reactive nitrogen and anthropogenic tracer concentrations. At higher altitudes (4-6 km) the atmospheric composition was in many ways similar to what was seen over Alaska and supports the view that a large-scale reservoir of PAN (and NO(y)) is present in the upper troposphere over the entire Arctic/subarctic region. The reactive nitrogen budget based on missions conducted from the North Bay site (missions 2-10) showed a small shortfall, whereas the budget for data collected from the Goose Bay operation (missions 11-19) showed essential balance. It is calculated that 15-20 ppt of the observed NO(x) may find its source from the available PAN reservoir. Meteorological considerations as well as relationships between reactive nitrogen and tracer species suggest that the atmosphere over eastern Canada during summer is greatly influenced by forest fires and transported industrial pollution.

Singh, H. B.↗
NASA NTRS1997

Comparison of Modeled Backscatter using Measured Aerosol Microphysics with Focused CW Lidar Data over Pacific

During NASA's GLObal Backscatter Experiment (GLOBE) II flight mission over the Pacific Ocean in May-June 1990, extensive aerosol backscatter data sets from two continuous wave, focused CO2 Doppler lidars and an aerosol microphysics data set from a laser optical particle counter (LOPC) were obtained. Changes in aerosol loading in various air masses with associated changes in chemical composition, from sulfuric acid and sulfates to dustlike crustal material, significantly affected aerosol backscatter, causing variation of about 3 to 4 orders of magnitude. Some of the significant backscatter features encountered in different air masses were the low backscatter in subtropical air with even lower values in the tropics near the Intertropical Convergence Zone (ITCZ), highly variable backscatter in the ITCZ, mid-tropospheric aerosol backscatter background mode, and high backscatter in an Asian dust plume off the Japanese coast. Differences in aerosol composition and backscatter for northern and southern hemisphere also were observed. Using the LOPC measurements of physical and chemical aerosol properties, we determined the complex refractive index from three different aerosol mixture models to calculate backscatter. These values provided a well-defined envelope of modeled backscatter for various atmospheric conditions, giving good agreement with the lidar data over a horizontal sampling of approximately 18000 km in the mid-troposphere.

Srivastava, Vandana↗
NASA NTRS2004

Exploring the Saturn System in the Thermal Infrared: The Composite Infrared Spectrometer

The Composite Inbred Spectrometer (CIRS) is a remote-sensing Fourier Transform Spectrometer on the Cassini orbiter that measures thermal radiation over two decades in wave number, from 10 to 1400 cm (1 mm to 7pm), with a spectral resolution that can be set from 0.5 to 20 cm. The far in portion of the spectrum (10 - 600 cm) is measured with a polarizing interferometer having thermopile detectors with a common 4-mrad field of view. The middle infrared portion is measured with a traditional Michelson interferometer having two focal planes (600 - 1100cm, 1100-1400 cm). Each focal plane is composed of a 1x10 array of HgCdTe detectors, each detector having a 0.3-mrad field of view. CIRS observations will provide three-dimensional maps of temperature, gas composition, and aerosols/condensates of the atmospheres of Titan and Saturn with good vertical and horizontal resolution, from deep in their tropospheres to high in their mesospheres. CIRS ability to observe atmospheres in the limb viewing mode (in addition to nadir) offers the opportunity to provide accurate and highly resolved vertical profiles of these atmospheric variables. The ability to observe with high-spectral resolution should facilitate the identification of new constituents. CIRS will also map the thermal and compositional properties of the surfaces of Saturn's icy satellites. It will similarly map Saturn's rings, characterizing their formation and evolution. The combination of broad spectral range, programmable spectral resolution, the small detector fields of view, and an orbiting spacecraft platform will allow CIRS to observe the Saturnian system in the thermal infrared at a level of detail not previously achieved.

Flasar, F. M.↗
NASA NTRS2022

GMAO Office Note No. 17 (Version 1.3) File Specification for GEOS-CF Products

The NASA Global Earth Observing System (GEOS) model has been expanded to provide global near-real-time forecasts of atmospheric composition at a horizontal resolution of 0.25 degrees (about 25 km). This GEOS Composition Forecast (GEOS-CF) system combines the GEOS weather analysis and forecasting system with the state-of-the-science GEOS-Chem chemistry module (Bey et al., 2001; Keller et al., 2014; Long et al., 2015) to provide detailed chemical analysis of a wide range of air pollutants including ozone, carbon monoxide, nitrogen oxides, and fine particulate matter (PM2.5). Full model description and evaluation of the GEOS-CF tropospheric simulation and forecast skill is given in Keller et al. (2021). For evaluation of GEOS-CF stratospheric composition see Knowland et al. (2021).

GEOS-CF↗
NASA NTRS1977

Global atmospheric sampling program

Automated instruments were installed on a commercial B-747 aircraft, during the program, to obtain baseline data and to monitor key atmospheric constituents associated with emissions of aircraft engines in order to determine if aircraft are contributing to pollution of the upper atmosphere. Data thus acquired on a global basis over the commercial air routes for 5 to 10 years will be analyzed. Ozone measurements in the 29,000 to 45,000 foot altitude were expanded over what has been available from ozonesondes. Limited aerosol composition measurements from filter samples show low levels of sulfates and nitrates in the upper troposphere. Recently installed instruments for measurement of carbon monoxide and condensation nuclei are beginning to return data.

Lezberg, E. A.↗
NASA NTRS1987

Orbital atmospheric physics and dynamics

There are two ways of modeling the upper atmosphere. One is the empirical model that makes use of experimental data on means and excursions from the mean and fits the data in a self-consistent manner. The other approach is to deal directly with the physical processes. This is difficult since what is happening is extremely complex. Data measured using an interferometer to give Doppler shifts of airglow lines showed 300 to 800 m/sec winds with a complex structure in the upper region of the thermosphere at high latitudes. Ionospheric electric fields, strongly influenced by interaction with the solar wind, drive the ionized component and large neutral winds result due to momentum transfer between the charged particles and the neutrals. Frictional heating results from movement of ions through the neutrals, which also influences the compositional structure. These are examples of the complex interactions involved. The NCAR General Circulation Model (tropospheric) was adapted for use at thermospheric altitudes: the Thermospheric General Circulation Model (TGCM). The model makes use partly of primitive equations and partly of empirical data for some quantities such as electron density, magnetic field, and ion drift.

Roble, Raymond↗
NASA NTRS2019

Constraining the Earth System with EOS-Aura Observations

NASA's Goddard Earth Observing System (GEOS) model and data assimilation system is a flexible, modular global system that is used for applications that range from weather prediction to climate analysis. Resolving scales ranging from a few kilometers to several tens of kilometers, with scale-aware parametrization settings, the GEOS system offers NASA scientists and their partners a flexible system that is attuned to bringing in observations from all components of the Earth System. The GEOS system thus serves as a tool that enhances the value to NASA of observations from individual instruments, by bringing them into context with the full suite of "operational" observations and other research datasets. This presentation will emphasize how the GEOS system has been used to extend the value of observations from EOS-Aura, in conjunction with other NASA and non-NASA observations. One example is atmospheric ozone from the OMI and MLS instruments, that has been used extensively in GEOS systems for both weather (GEOS-FP) and the MERRA-2 reanalysis. The presentation will emphasize the value of these ozone datasets for studying long-term changes of ozone since 2004 and will discuss prospects of continuing such analyses in the post-Aura era. A new configuration of GEOS, the Composition Forecasting (CF) system has recently gone in to production: this uses a full troposphere-stratosphere chemistry mechanism (GEOS-Chem) to analyze and predict global constituent distributions, including surface air quality. While constituent observations are not yet assimilated into GEOS-CF, EOS-Aura data are used substantially to evaluate the system and plans are in place to introduce assimilation at a later stage. Examples from GEOS-CF will be shown to illustrate the value of EOS-Aura observations. Discussions will focus on the likely value of long-term analyses of EOS-Aura observations in context of understanding potential impacts on the health of humans and the biosphere, including the importance of sustaining long-term, global observing systems such as that pioneered by EOS-Aura.

Pawson, Steven↗
NASA NTRS2021

Assessment of Tropospheric Concentrations of NO2 from the TROPOMI/Sentinel-5 Precursor for the Estimation of Long-Term Exposure to Surface NO2 over South Korea

Since April 2018, the TROPOspheric Monitoring Instrument (TROPOMI) has provided data on tropospheric NO2 column concentrations (CTROPOMI) with unprecedented spatial resolution. This study aims to assess the capability of TROPOMI to acquire high spatial resolution data regarding surface NO2 mixing ratios. In general, the instrument effectively detected major and moderate sources of NO2 over South Korea with a clear weekday–weekend distinction. We compared the CTROPOMI with surface NO2 mixing ratio measurements from an extensive ground-based network over South Korea operated by the Korean Ministry of Environment (SKME; more than 570 sites), for 2019. Spatiotemporally collocated CTROPOMI and SKME showed a moderate correlation (correlation coefficient, r = 0.67), whereas their annual mean values at each site showed a higher correlation (r = 0.84). The CTROPOMI and SKME were well correlated around the Seoul metropolitan area, where significant amounts of NO2 prevailed throughout the year, whereas they showed lower correlation at rural sites. We converted the tropospheric NO2 from TROPOMI to the surface mixing ratio (STROPOMI) using the EAC4 (ECMWF Atmospheric Composition Reanalysis 4) profile shape, for quantitative comparison with the SKME. The estimated STROPOMI generally underestimated the in-situ value obtained, SKME (slope = 0.64), as reported in previous studies.

TROPOMI↗
NASA NTRS2012

Operational Use of the AIRS Total Column Ozone Retrievals Along with the RGB Air Mass Product as Part of the GOES-R Proving Ground

The National Oceanic and Atmospheric Administration (NOAA) National Centers for Environmental Prediction (NCEP) Hydrometeorological Prediction Center (HPC) and Ocean Prediction Center (OPC) provide short-term and medium-range forecast guidance of heavy precipitation, strong winds, and other features often associated with mid-latitude cyclones over both land and ocean. As a result, detection of factors that lead to rapid cyclogenesis and high wind events is key to improving forecast skill. One phenomenon that has been identified with these events is the stratospheric intrusion that occurs near tropopause folds. This allows for deep mixing near the top of the atmosphere where dry air high in ozone concentrations and potential vorticity descends (sometimes rapidly) deep into the mid-troposphere. Observations from satellites can aid in detection of these stratospheric air intrusions (SAI) regions. Specifically, multispectral composite imagery assign a variety of satellite spectral bands to the red, green, and blue (RGB) color components of imagery pixels and result in color combinations that can assist in the detection of dry stratospheric air associated with PV advection, which in turn may alert forecasters to the possibility of a rapidly strengthening storm system. Single channel or RGB satellite imagery lacks quantitative information about atmospheric moisture unless the sampled brightness temperatures or other data are converted to estimates of moisture via a retrieval process. Thus, complementary satellite observations are needed to capture a complete picture of a developing storm system. Here, total column ozone retrievals derived from a hyperspectral sounder are used to confirm the extent and magnitude of SAIs. Total ozone is a good proxy for defining locations and intensity of SAIs and has been used in studies evaluating that phenomenon (e.g. Tian et al. 2007, Knox and Schmidt 2005). Steep gradients in values of total ozone seen by satellites have been linked to stratosphere-troposphere exchange (WMO, 1985).

Folmer, Michael↗
NASA NTRSDate not supplied

Distribution and Sources of Tropospheric Aerosols Over the Western North Atlantic During ACTIVATE (February-March 2020)

The Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) is a five-year (2019-2023) NASA Earth-Venture Suborbital-3 (EVS-3) mission to robustly characterize aerosol-cloud-meteorology interactions during February-June, with a focus on marine boundary layer clouds. This characterization requires understanding of aerosol composition, distribution, transport pathways, and sources. Here we use the GEOS-Chem chemical transport model driven by the MERRA-2 reanalysis to simulate tropospheric carbon monoxide (CO) and aerosols over the western North Atlantic Ocean (WNAO) during the first field deployment of ACTIVATE (February-March 2020). CO is used as a tracer to diagnose transport pathways for continental pollution outflow to the WNAO. The aerosol simulation represents all major aerosols including sulfate-nitrate-ammonium (SNA), mineral dust, sea salt, black and organic carbon aerosols. Model-simulated mixing ratios of SNA and organic carbon are compared with aircraft observations. We show that intensive aerosol mass measurements in the lower troposphere over the North American outflow region during ACTIVATE provide strong constraints on model aerosol wet scavenging. Comparisons of model aerosol extinctions with the airborne High Spectral Resolution Lidar-2 (HSRL-2) measurements indicate that the model generally captures continental outflow of aerosols and enhanced extinctions associated with sea salt. Simulated aerosol optical depths (AODs) and extinction vertical profiles are also compared with satellite retrievals from MODIS/Aqua and CALIOP/CALIPSO, respectively. CALIOP sometimes observes enhanced aerosol extinction at altitudes between ~1.5km and ~2.0km south of 32°N. The model reproduces this enhancement and attributes it to coarse-mode sea salt associated with high relative humidity. The relative contributions of continental and oceanic sources to the aerosol loading, AOD, and their distributions over the study domain will also be discussed.

aerosols↗
NASA NTRS1985

A survey of major east coast snowstorms, 1960-1983. Part 2: Case studies of eighteen storms

Snowfall, surface and upper air charts, and available satellite images are presented for eighteen major East Coast snowstorms that occurred between 1960 and 1983. The charts and descriptions of key fields are provided so that students, weather forecasters, and researchers alike can visualize how a large sample of major winter cyclones form and intensify. Although there are noted similarities in certain aspects of the surface and upper tropospheric development of the storms, significant case-to-case variability precludes the ability to effectively composite these weather systems.

Kocin, P. J.↗
NASA NTRS2004

Airborne In Situ and Ground-based Polarimetric Radar Measurements of Tropical Convection in Support of CRYSTAL-FACE

This report describes the work performed by the University of North Dakota (UND) under NASA Grant NAG5-11509, titled Airborne In Situ and Ground-based Polarimetric Radar Measurements of Tropical Convection in Support of CRYSTAL-FACE. This work focused on the collection of data by two key platforms: the UND Citation II research aircraft and the NASA NPOL radar system. The CRYSTAL-FACE (C-F) mission addresses several key issues from the NASA Earth System Enterprise, including the variability of water in the atmosphere, the forcing provided by tropical cirrus and the response of the Earth system to this forcing. In situ measurements and radar observations of tropical convection, cirrus clouds and their environment are core elements of C-F. One of the primary issues that C-F is addressing is the relationship of tropical cirrus anvils to precipitating deep convection. The in situ measurements from C-F are being used to validate remote sensing of Earth-Atmosphere properties, increase our knowledge of upper tropospheric water vapor and its distribution, and increase our knowledge of tropical cirrus cloud morphology and composition. Radar measurements, especially polarimetric diversity observations available fiom the NASA NPOL radar, are providing essential information about the initiation, modulation, and dissipation of convective cores and the generation of associated anvils in tropical convection. Specifically, NPOL radar measurements contain information about convective intensity and its vertical structure for comparison with thermodynamic and kinematic environmental measurements observed from soundings. Because of the polarimetric diversity of MOL, statistics on bulk microphysical properties can be retrieved and compared to the other characteristics of convection and associated cirrus anvils. In summary, the central objectives of this proposal were to deploy the UND Citation research aircraft as an in situ sensing platform for this mission and to provide collaborative analyses of the recorded data and to deploy the NPOL radar to observe the characteristics of cirrus and parent convection.

Poellot, Michael R.↗
NASA NTRS1986

The gas composition of Jupiter derived from 5 micron airborne spectroscopic observations

It is pointed out that Jupiter's 5-micron spectrum is a very diagnostic observational tool to probe the troposphere of this giant planet. A report is presented of abundance analyses of NH3, PH3, CH4, CH3D, CO, and GeH4 in the 1- to 6-bar pressure range in Jupiter's troposphere. All the considered molecules have been previously detected in ground-based, airborne, and spacecraft observations of Jupiter. The contribution made by the present study is related to a self-consistent simultaneous determination of the abundances of all of these molecules at the same physical level in Jupiter's atmosphere using one high spectral resolution dataset and a radiative transfer model. It is found that most abundances deviate significantly from expectations based upon an atmospheric model assuming solar composition and chemical equilibrium. The D/H ratio in Jupiter is comparable to that measured in the interstellar medium.

Bjoraker, G. L.↗
NASA NTRS2020

Modeling the smoky troposphere of the southeast Atlantic: a comparison to ORACLES airborne observations from September of 2016

In the southeast Atlantic, well-defined smoke plumes from Africa advect over marine boundary layer cloud decks; both are most extensive around September, when most of the smoke resides in the free troposphere. A framework is put forth for evaluating the performance of a range of global and regional atmospheric composition models against observations made during the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) airborne mission in September 2016. A strength of the comparison is a focus on the spatial distribution of a wider range of aerosol composition and optical properties than has been done previously. The sparse airborne observations are aggregated into approximately 2° grid boxes and into three vertical layers: 3–6 km, the layer from cloud top to 3 km, and the cloud-topped marine boundary layer. Simulated aerosol extensive properties suggest that the flight-day observations are reasonably representative of the regional monthly average, with systematic deviations of 30 % or less. Evaluation against observations indicates that all models have strengths and weaknesses, and there is no single model that is superior to all the others in all metrics evaluated. Whereas all six models typically place the top of the smoke layer within 0–500 m of the airborne lidar observations, the models tend to place the smoke layer bottom 300–1400 m lower than the observations. A spatial pattern emerges, in which most models underestimate the mean of most smoke quantities (black carbon, extinction, carbon monoxide) on the diagonal corridor between 16° S, 6° E, and 10° S, 0° E, in the 3–6 km layer, and overestimate them further south, closer to the coast, where less aerosol is present. Model representations of the above-cloud aerosol optical depth differ more widely. Most models overestimate the organic aerosol mass concentrations relative to those of black carbon, and with less skill, indicating model uncertainties in secondary organic aerosol processes. Regional-mean free-tropospheric model ambient single scattering albedos vary widely, between 0.83 and 0.93 compared with in situ dry measurements centered at 0.86, despite minimal impact of humidification on particulate scattering. The modeled ratios of the particulate extinction to the sum of the black carbon and organic aerosol mass concentrations (a mass extinction efficiency proxy) are typically too low and vary too little spatially, with significant inter-model differences. Most models overestimate the carbonaceous mass within the offshore boundary layer. Overall, the diversity in the model biases suggests that different model processes are responsible. The wide range of model optical properties requires further scrutiny because of their importance for radiative effect estimates.

Yohei Shinozuka↗