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Abstract
In this paper results are presented from a simple offline assimilation system that uses radiances from the Moderate Resolution Imaging Spectroradiometer (MODIS) channels that sense atmospheric aerosols over land and ocean. The MODIS information is directly inserted into the Goddard Chemistry and Aerosol Radiation Transport model (GOCART), which simulates the following five aerosol types: dust, sea salt, black carbon, organic carbon, and sulfate. The goal is to produce three-dimensional fields of these aerosol types for radiative forcing calculations.
Products from this assimilation system are compared with ground-based measurements of aerosol optical depth (AOD) from the Aerosol Robotic Network (AERONET). Insertion of MODIS radiances draws the GOCART model closer to the AERONET AOD. However, there are still uncertainties with surface reflectivity over moderately bright surfaces and with the amount of absorbing aerosol.
Also described is the assimilation cycle. The forward model takes the aerosol information from the GOCART model and calculates radiances based on optical parameters of the aerosol type, satellite viewing angle, and the particle growth from relative humidity. Because the GOCART model is driven by previously assimilated meteorology, these forward model radiances can be directly compared with the observed MODIS level-2 radiances. The offline assimilation system simply adjusts the aerosol loading in the GOCART model so that the observed minus forward model radiances agree. Minimal change is made to the GOCART aerosol vertical distribution, size distribution, and the ratio of the five different aerosol types. The loading in the GOCART model is updated with new MODIS observations every 6 h. Since the previously assimilated meteorology provides surface wind speed, radiance sensitivity to wind speed over rough ocean is taken into account. Over land the dark target approach, also used by the MODIS–atmosphere group retrieval, is used. If the underlying land surface is deemed dark enough, the surface reflectances at the 0.47- and 0.66-μm wavelengths are constant multiples of the observed 2.13-μm reflectance. Over ocean the assimilation AOD compares well with AERONET, over land less so. The results herein are also compared with AERONET-retrieved single-scattering albedo. This research is part of an ongoing effort at NASA Goddard to integrate aerosols into the Goddard Modeling and Assimilation Office (GMAO) products.
Abstract
In this paper results are presented from a simple offline assimilation system that uses radiances from the Moderate Resolution Imaging Spectroradiometer (MODIS) channels that sense atmospheric aerosols over land and ocean. The MODIS information is directly inserted into the Goddard Chemistry and Aerosol Radiation Transport model (GOCART), which simulates the following five aerosol types: dust, sea salt, black carbon, organic carbon, and sulfate. The goal is to produce three-dimensional fields of these aerosol types for radiative forcing calculations.
Products from this assimilation system are compared with ground-based measurements of aerosol optical depth (AOD) from the Aerosol Robotic Network (AERONET). Insertion of MODIS radiances draws the GOCART model closer to the AERONET AOD. However, there are still uncertainties with surface reflectivity over moderately bright surfaces and with the amount of absorbing aerosol.
Also described is the assimilation cycle. The forward model takes the aerosol information from the GOCART model and calculates radiances based on optical parameters of the aerosol type, satellite viewing angle, and the particle growth from relative humidity. Because the GOCART model is driven by previously assimilated meteorology, these forward model radiances can be directly compared with the observed MODIS level-2 radiances. The offline assimilation system simply adjusts the aerosol loading in the GOCART model so that the observed minus forward model radiances agree. Minimal change is made to the GOCART aerosol vertical distribution, size distribution, and the ratio of the five different aerosol types. The loading in the GOCART model is updated with new MODIS observations every 6 h. Since the previously assimilated meteorology provides surface wind speed, radiance sensitivity to wind speed over rough ocean is taken into account. Over land the dark target approach, also used by the MODIS–atmosphere group retrieval, is used. If the underlying land surface is deemed dark enough, the surface reflectances at the 0.47- and 0.66-μm wavelengths are constant multiples of the observed 2.13-μm reflectance. Over ocean the assimilation AOD compares well with AERONET, over land less so. The results herein are also compared with AERONET-retrieved single-scattering albedo. This research is part of an ongoing effort at NASA Goddard to integrate aerosols into the Goddard Modeling and Assimilation Office (GMAO) products.
Abstract
The Georgia Institute of Technology–Goddard Global Ozone Chemistry Aerosol Radiation and Transport (GOCART) model is used to simulate the aerosol optical thickness τ for major types of tropospheric aerosols including sulfate, dust, organic carbon (OC), black carbon (BC), and sea salt. The GOCART model uses a dust emission algorithm that quantifies the dust source as a function of the degree of topographic depression, and a biomass burning emission source that includes seasonal and interannual variability based on satellite observations. Results presented here show that on global average, dust aerosol has the highest τ at 500 nm (0.051), followed by sulfate (0.040), sea salt (0.027), OC (0.017), and BC (0.007). There are large geographical and seasonal variations of τ, controlled mainly by emission, transport, and hygroscopic properties of aerosols. The model calculated total τs at 500 nm have been compared with the satellite retrieval products from the Total Ozone Mapping Spectrometer (TOMS) over both land and ocean and from the Advanced Very High Resolution Radiometer (AVHRR) over the ocean. The model reproduces most of the prominent features in the satellite data, with an overall agreement within a factor of 2 over the aerosol source areas and outflow regions. While there are clear differences among the satellite products, a major discrepancy between the model and the satellite data is that the model shows a stronger variation of τ from source to remote regions. Quantitative comparison of model and satellite data is still difficult, due to the large uncertainties involved in deriving the τ values by both the model and satellite retrieval, and by the inconsistency in physical and optical parameters used between the model and the satellite retrieval. The comparison of monthly averaged model results with the sun photometer network [Aerosol Robotics Network (AERONET)] measurements shows that the model reproduces the seasonal variations at most of the sites, especially the places where biomass burning or dust aerosol dominates.
Abstract
The Georgia Institute of Technology–Goddard Global Ozone Chemistry Aerosol Radiation and Transport (GOCART) model is used to simulate the aerosol optical thickness τ for major types of tropospheric aerosols including sulfate, dust, organic carbon (OC), black carbon (BC), and sea salt. The GOCART model uses a dust emission algorithm that quantifies the dust source as a function of the degree of topographic depression, and a biomass burning emission source that includes seasonal and interannual variability based on satellite observations. Results presented here show that on global average, dust aerosol has the highest τ at 500 nm (0.051), followed by sulfate (0.040), sea salt (0.027), OC (0.017), and BC (0.007). There are large geographical and seasonal variations of τ, controlled mainly by emission, transport, and hygroscopic properties of aerosols. The model calculated total τs at 500 nm have been compared with the satellite retrieval products from the Total Ozone Mapping Spectrometer (TOMS) over both land and ocean and from the Advanced Very High Resolution Radiometer (AVHRR) over the ocean. The model reproduces most of the prominent features in the satellite data, with an overall agreement within a factor of 2 over the aerosol source areas and outflow regions. While there are clear differences among the satellite products, a major discrepancy between the model and the satellite data is that the model shows a stronger variation of τ from source to remote regions. Quantitative comparison of model and satellite data is still difficult, due to the large uncertainties involved in deriving the τ values by both the model and satellite retrieval, and by the inconsistency in physical and optical parameters used between the model and the satellite retrieval. The comparison of monthly averaged model results with the sun photometer network [Aerosol Robotics Network (AERONET)] measurements shows that the model reproduces the seasonal variations at most of the sites, especially the places where biomass burning or dust aerosol dominates.
Abstract
The direct effects of aerosols on global and regional climate during boreal spring are investigated based on numerical simulations with the NASA Global Modeling and Assimilation Office finite-volume general circulation model (fvGCM) with Microphyics of Clouds with the Relaxed–Arakawa Schubert Scheme (McRAS), using aerosol forcing functions derived from the Goddard Ozone Chemistry Aerosol Radiation and Transport model (GOCART).
The authors find that anomalous atmospheric heat sources induced by absorbing aerosols (dust and black carbon) excite a planetary-scale teleconnection pattern in sea level pressure, temperature, and geopotential height spanning North Africa through Eurasia to the North Pacific. Surface cooling due to direct effects of aerosols is found in the vicinity and downstream of the aerosol source regions, that is, South Asia, East Asia, and northern and western Africa. Significant atmospheric heating is found in regions with large loading of dust (over northern Africa and the Middle East) and black carbon (over Southeast Asia). Paradoxically, the most pronounced feature in aerosol-induced surface temperature is an east–west dipole anomaly with strong cooling over the Caspian Sea and warming over central and northeastern Asia, where aerosol concentrations are low. Analyses of circulation anomalies show that the dipole anomaly is a part of an atmospheric teleconnection pattern driven by atmospheric heating anomalies induced by absorbing aerosols in the source regions, but the influence was conveyed globally through barotropic energy dispersion and sustained by feedback processes associated with the regional circulations.
The surface temperature signature associated with the aerosol-induced teleconnection bears striking resemblance to the spatial pattern of observed long-term trend in surface temperature over Eurasia. Additionally, the boreal spring wave train pattern is similar to that reported by Fukutomi et al. associated with the boreal summer precipitation seesaw between eastern and western Siberia. The results of this study raise the possibility that global aerosol forcing during boreal spring may play an important role in spawning atmospheric teleconnections that affect regional and global climates.
Abstract
The direct effects of aerosols on global and regional climate during boreal spring are investigated based on numerical simulations with the NASA Global Modeling and Assimilation Office finite-volume general circulation model (fvGCM) with Microphyics of Clouds with the Relaxed–Arakawa Schubert Scheme (McRAS), using aerosol forcing functions derived from the Goddard Ozone Chemistry Aerosol Radiation and Transport model (GOCART).
The authors find that anomalous atmospheric heat sources induced by absorbing aerosols (dust and black carbon) excite a planetary-scale teleconnection pattern in sea level pressure, temperature, and geopotential height spanning North Africa through Eurasia to the North Pacific. Surface cooling due to direct effects of aerosols is found in the vicinity and downstream of the aerosol source regions, that is, South Asia, East Asia, and northern and western Africa. Significant atmospheric heating is found in regions with large loading of dust (over northern Africa and the Middle East) and black carbon (over Southeast Asia). Paradoxically, the most pronounced feature in aerosol-induced surface temperature is an east–west dipole anomaly with strong cooling over the Caspian Sea and warming over central and northeastern Asia, where aerosol concentrations are low. Analyses of circulation anomalies show that the dipole anomaly is a part of an atmospheric teleconnection pattern driven by atmospheric heating anomalies induced by absorbing aerosols in the source regions, but the influence was conveyed globally through barotropic energy dispersion and sustained by feedback processes associated with the regional circulations.
The surface temperature signature associated with the aerosol-induced teleconnection bears striking resemblance to the spatial pattern of observed long-term trend in surface temperature over Eurasia. Additionally, the boreal spring wave train pattern is similar to that reported by Fukutomi et al. associated with the boreal summer precipitation seesaw between eastern and western Siberia. The results of this study raise the possibility that global aerosol forcing during boreal spring may play an important role in spawning atmospheric teleconnections that affect regional and global climates.
Abstract
A Saharan air layer (SAL) event associated with a nondeveloping African easterly wave (AEW) over the main development region of the eastern Atlantic was sampled by the NASA Global Hawk aircraft on 24–25 August 2013 during the NASA Hurricane and Severe Storm Sentinel (HS3) campaign and was simulated with the NASA Unified Weather Research and Forecasting (NU-WRF) Model. Airborne, ground-based, and spaceborne measurements were used to evaluate the model performance. The microphysical and radiative effects of dust and other aerosols on the SAL structure and environment were investigated with the factor-separation method. The results indicate that relative to a simulation without dust–radiative and microphysical impacts, Saharan dust and other aerosols heated the SAL air mainly through shortwave heating by the direct aerosol–radiation (AR) effect, resulting in a warmer (up to 0.6 K) and drier (up to 5% RH reduction) SAL and maintaining the strong temperature inversion at the base of the SAL in the presence of predominant longwave cooling. Radiative heating of the dust accentuated a vertical circulation within the dust layer, in which air rose (sank) in the northern (southern) portions of the dust layer. Furthermore, above and to the south of the dust layer, both the microphysical and radiative impacts of dust tended to counter the vertical motions associated with the Hadley circulation, causing a small weakening and southward shift of convection in the intertropical convergence zone (ITCZ) and reduced anvil cloud to the north. Changes in moisture and cloud/precipitation hydrometeors were largely driven by the dust-induced changes in vertical motion. Dust strengthened the African easterly jet by up to ~1 m s−1 at the southern edge of the jet, primarily through the AR effect, and produced modest increases in vertical wind shear within and in the vicinity of the dust layer. These modulations of the SAL and AEW environment clearly contributed to the nondevelopment of this AEW.
Abstract
A Saharan air layer (SAL) event associated with a nondeveloping African easterly wave (AEW) over the main development region of the eastern Atlantic was sampled by the NASA Global Hawk aircraft on 24–25 August 2013 during the NASA Hurricane and Severe Storm Sentinel (HS3) campaign and was simulated with the NASA Unified Weather Research and Forecasting (NU-WRF) Model. Airborne, ground-based, and spaceborne measurements were used to evaluate the model performance. The microphysical and radiative effects of dust and other aerosols on the SAL structure and environment were investigated with the factor-separation method. The results indicate that relative to a simulation without dust–radiative and microphysical impacts, Saharan dust and other aerosols heated the SAL air mainly through shortwave heating by the direct aerosol–radiation (AR) effect, resulting in a warmer (up to 0.6 K) and drier (up to 5% RH reduction) SAL and maintaining the strong temperature inversion at the base of the SAL in the presence of predominant longwave cooling. Radiative heating of the dust accentuated a vertical circulation within the dust layer, in which air rose (sank) in the northern (southern) portions of the dust layer. Furthermore, above and to the south of the dust layer, both the microphysical and radiative impacts of dust tended to counter the vertical motions associated with the Hadley circulation, causing a small weakening and southward shift of convection in the intertropical convergence zone (ITCZ) and reduced anvil cloud to the north. Changes in moisture and cloud/precipitation hydrometeors were largely driven by the dust-induced changes in vertical motion. Dust strengthened the African easterly jet by up to ~1 m s−1 at the southern edge of the jet, primarily through the AR effect, and produced modest increases in vertical wind shear within and in the vicinity of the dust layer. These modulations of the SAL and AEW environment clearly contributed to the nondevelopment of this AEW.
Abstract
The determination of an accurate quantitative understanding of the role of tropospheric aerosols in the earth's radiation budget is extremely important because forcing by anthropogenic aerosols presently represents one of the most uncertain aspects of climate models. Here the authors present a systematic comparison of three different analyses of satellite-retrieved aerosol optical depth based on the Advanced Very High Resolution Radiometer (AVHRR)-measured radiances with optical depths derived from six different models. Also compared are the model-derived clear-sky reflected shortwave radiation with satellite-measured reflectivities derived from the Earth Radiation Budget Experiment (ERBE) satellite.
The three different satellite-derived optical depths differ by between −0.10 and 0.07 optical depth units in comparison to the average of the three analyses depending on latitude and month, but the general features of the retrievals are similar. The models differ by between −0.09 and +0.16 optical depth units from the average of the models. Differences between the average of the models and the average of the satellite analyses range over −0.11 to +0.05 optical depth units. These differences are significant since the annual average clear-sky radiative forcing associated with the difference between the average of the models and the average of the satellite analyses ranges between −3.9 and 0.7 W m−2 depending on latitude and is −1.7 W m−2 on a global average annual basis. Variations in the source strengths of dimethylsulfide-derived aerosols and sea salt aerosols can explain differences between the models, and between the models and satellite retrievals of up to 0.2 optical depth units.
The comparison of model-generated reflected shortwave radiation and ERBE-measured shortwave radiation is similar in character as a function of latitude to the analysis of modeled and satellite-retrieved optical depths, but the differences between the modeled clear-sky reflected flux and the ERBE clear-sky reflected flux is generally larger than that inferred from the difference between the models and the AVHRR optical depths, especially at high latitudes. The difference between the mean of the models and the ERBE-analyzed clear-sky flux is 1.6 W m−2.
The overall comparison indicates that the model-generated aerosol optical depth is systematically lower than that inferred from measurements between the latitudes of 10° and 30°S. It is not likely that the shortfall is due to small values of the sea salt optical depth because increases in this component would create modeled optical depths that are larger than those from satellites in the region north of 30°N and near 50°S. Instead, the source strengths for DMS and biomass aerosols in the models may be too low. Firm conclusions, however, will require better retrieval procedures for the satellites, including better cloud screening procedures, further improvement of the model's treatment of aerosol transport and removal, and a better determination of aerosol source strengths.
Abstract
The determination of an accurate quantitative understanding of the role of tropospheric aerosols in the earth's radiation budget is extremely important because forcing by anthropogenic aerosols presently represents one of the most uncertain aspects of climate models. Here the authors present a systematic comparison of three different analyses of satellite-retrieved aerosol optical depth based on the Advanced Very High Resolution Radiometer (AVHRR)-measured radiances with optical depths derived from six different models. Also compared are the model-derived clear-sky reflected shortwave radiation with satellite-measured reflectivities derived from the Earth Radiation Budget Experiment (ERBE) satellite.
The three different satellite-derived optical depths differ by between −0.10 and 0.07 optical depth units in comparison to the average of the three analyses depending on latitude and month, but the general features of the retrievals are similar. The models differ by between −0.09 and +0.16 optical depth units from the average of the models. Differences between the average of the models and the average of the satellite analyses range over −0.11 to +0.05 optical depth units. These differences are significant since the annual average clear-sky radiative forcing associated with the difference between the average of the models and the average of the satellite analyses ranges between −3.9 and 0.7 W m−2 depending on latitude and is −1.7 W m−2 on a global average annual basis. Variations in the source strengths of dimethylsulfide-derived aerosols and sea salt aerosols can explain differences between the models, and between the models and satellite retrievals of up to 0.2 optical depth units.
The comparison of model-generated reflected shortwave radiation and ERBE-measured shortwave radiation is similar in character as a function of latitude to the analysis of modeled and satellite-retrieved optical depths, but the differences between the modeled clear-sky reflected flux and the ERBE clear-sky reflected flux is generally larger than that inferred from the difference between the models and the AVHRR optical depths, especially at high latitudes. The difference between the mean of the models and the ERBE-analyzed clear-sky flux is 1.6 W m−2.
The overall comparison indicates that the model-generated aerosol optical depth is systematically lower than that inferred from measurements between the latitudes of 10° and 30°S. It is not likely that the shortfall is due to small values of the sea salt optical depth because increases in this component would create modeled optical depths that are larger than those from satellites in the region north of 30°N and near 50°S. Instead, the source strengths for DMS and biomass aerosols in the models may be too low. Firm conclusions, however, will require better retrieval procedures for the satellites, including better cloud screening procedures, further improvement of the model's treatment of aerosol transport and removal, and a better determination of aerosol source strengths.
This document outlines a practical strategy for achieving an observationally based quantification of direct climate forcing by anthropogenic aerosols. The strategy involves a four-step program for shifting the current assumption-laden estimates to an increasingly empirical basis using satellite observations coordinated with suborbital remote and in situ measurements and with chemical transport models. Conceptually, the problem is framed as a need for complete global mapping of four parameters: clear-sky aerosol optical depth f f, radiative efficiency per unit optical depth δ, fine-mode fraction of optical depth f f, and the anthropogenic fraction of the fine mode f af . The first three parameters can be retrieved from satellites, but correlative, suborbital measurements are required for quantifying the aerosol properties that control E, for validating the retrieval of f f, and for partitioning fine-mode δ between natural and anthropogenic components. The satellite focus is on the “A-Train,” a constellation of six spacecraft that will fly in formation from about 2005 to 2008. Key satellite instruments for this report are the Moderate Resolution Imaging Spectroradiometer (MODIS) and Clouds and the Earth's Radiant Energy System (CERES) radiometers on Aqua, the Ozone Monitoring Instrument (OMI) radiometer on Aura, the Polarization and Directionality of Earth's Reflectances (POLDER) polarimeter on the Polarization and Anistropy of Reflectances for Atmospheric Sciences Coupled with Observations from a Lidar (PARASOL), and the Cloud and Aerosol Lider with Orthogonal Polarization (CALIOP) lidar on the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO). This strategy is offered as an initial framework—subject to improvement over time—for scientists around the world to participate in the A-Train opportunity. It is a specific implementation of the Progressive Aerosol Retrieval and Assimilation Global Observing Network (PARAGON) program, presented earlier in this journal, which identified the integration of diverse data as the central challenge to progress in quantifying global-scale aerosol effects. By designing a strategy around this need for integration, we develop recommendations for both satellite data interpretation and correlative suborbital activities that represent, in many respects, departures from current practice.
This document outlines a practical strategy for achieving an observationally based quantification of direct climate forcing by anthropogenic aerosols. The strategy involves a four-step program for shifting the current assumption-laden estimates to an increasingly empirical basis using satellite observations coordinated with suborbital remote and in situ measurements and with chemical transport models. Conceptually, the problem is framed as a need for complete global mapping of four parameters: clear-sky aerosol optical depth f f, radiative efficiency per unit optical depth δ, fine-mode fraction of optical depth f f, and the anthropogenic fraction of the fine mode f af . The first three parameters can be retrieved from satellites, but correlative, suborbital measurements are required for quantifying the aerosol properties that control E, for validating the retrieval of f f, and for partitioning fine-mode δ between natural and anthropogenic components. The satellite focus is on the “A-Train,” a constellation of six spacecraft that will fly in formation from about 2005 to 2008. Key satellite instruments for this report are the Moderate Resolution Imaging Spectroradiometer (MODIS) and Clouds and the Earth's Radiant Energy System (CERES) radiometers on Aqua, the Ozone Monitoring Instrument (OMI) radiometer on Aura, the Polarization and Directionality of Earth's Reflectances (POLDER) polarimeter on the Polarization and Anistropy of Reflectances for Atmospheric Sciences Coupled with Observations from a Lidar (PARASOL), and the Cloud and Aerosol Lider with Orthogonal Polarization (CALIOP) lidar on the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO). This strategy is offered as an initial framework—subject to improvement over time—for scientists around the world to participate in the A-Train opportunity. It is a specific implementation of the Progressive Aerosol Retrieval and Assimilation Global Observing Network (PARAGON) program, presented earlier in this journal, which identified the integration of diverse data as the central challenge to progress in quantifying global-scale aerosol effects. By designing a strategy around this need for integration, we develop recommendations for both satellite data interpretation and correlative suborbital activities that represent, in many respects, departures from current practice.
Abstract
This article provides an overview of the NASA Atmospheric Tomography (ATom) mission and a summary of selected scientific findings to date. ATom was an airborne measurements and modeling campaign aimed at characterizing the composition and chemistry of the troposphere over the most remote regions of the Pacific, Southern, Atlantic, and Arctic Oceans, and examining the impact of anthropogenic and natural emissions on a global scale. These remote regions dominate global chemical reactivity and are exceptionally important for global air quality and climate. ATom data provide the in situ measurements needed to understand the range of chemical species and their reactions, and to test satellite remote sensing observations and global models over large regions of the remote atmosphere. Lack of data in these regions, particularly over the oceans, has limited our understanding of how atmospheric composition is changing in response to shifting anthropogenic emissions and physical climate change. ATom was designed as a global-scale tomographic sampling mission with extensive geographic and seasonal coverage, tropospheric vertical profiling, and detailed speciation of reactive compounds and pollution tracers. ATom flew the NASA DC-8 research aircraft over four seasons to collect a comprehensive suite of measurements of gases, aerosols, and radical species from the remote troposphere and lower stratosphere on four global circuits from 2016 to 2018. Flights maintained near-continuous vertical profiling of 0.15–13-km altitudes on long meridional transects of the Pacific and Atlantic Ocean basins. Analysis and modeling of ATom data have led to the significant early findings highlighted here.
Abstract
This article provides an overview of the NASA Atmospheric Tomography (ATom) mission and a summary of selected scientific findings to date. ATom was an airborne measurements and modeling campaign aimed at characterizing the composition and chemistry of the troposphere over the most remote regions of the Pacific, Southern, Atlantic, and Arctic Oceans, and examining the impact of anthropogenic and natural emissions on a global scale. These remote regions dominate global chemical reactivity and are exceptionally important for global air quality and climate. ATom data provide the in situ measurements needed to understand the range of chemical species and their reactions, and to test satellite remote sensing observations and global models over large regions of the remote atmosphere. Lack of data in these regions, particularly over the oceans, has limited our understanding of how atmospheric composition is changing in response to shifting anthropogenic emissions and physical climate change. ATom was designed as a global-scale tomographic sampling mission with extensive geographic and seasonal coverage, tropospheric vertical profiling, and detailed speciation of reactive compounds and pollution tracers. ATom flew the NASA DC-8 research aircraft over four seasons to collect a comprehensive suite of measurements of gases, aerosols, and radical species from the remote troposphere and lower stratosphere on four global circuits from 2016 to 2018. Flights maintained near-continuous vertical profiling of 0.15–13-km altitudes on long meridional transects of the Pacific and Atlantic Ocean basins. Analysis and modeling of ATom data have led to the significant early findings highlighted here.