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We present an Arctic aerosol optical depth (AOD) climatology and trend analysis for 2003–2019 spring and summertime periods derived from a combination of multi-agency aerosol reanalyses, remote-sensing retrievals, and ground observations. This includes the U.S. Navy Aerosol Analysis and Prediction System ReAnalysis version 1 (NAAPS-RA v1), the NASA Modern-Era Retrospective Analysis for Research and Applications, version 2 (MERRA-2), and the Copernicus Atmosphere Monitoring Service ReAnalysis (CAMSRA). Spaceborne remote-sensing retrievals of AOD are considered from the Moderate Resolution Imaging Spectroradiometer (MODIS), the Multi-angle Imaging SpectroRadiometer (MISR), and the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP). Ground-based data include sun photometer data from AErosol RObotic NETwork (AERONET) sites and oceanic Maritime Aerosol Network (MAN) measurements. Aerosol reanalysis AODs and spaceborne retrievals show consistent climatological spatial patterns and trends for both spring and summer seasons over the lower Arctic (60–70∘ N). Consistent AOD trends are also found for the high Arctic (north of 70∘ N) from reanalyses. The aerosol reanalyses yield more consistent AOD results than climate models, can be verified well with AERONET, and corroborate complementary climatological and trend analysis. Speciated AODs are more variable than total AOD among the three reanalyses and a little more so for March–May (MAM) than for June–August (JJA). Black carbon (BC) AOD in the Arctic comes predominantly from biomass burning (BB) sources in both MAM and JJA, and BB overwhelms anthropogenic sources in JJA for the study period. AOD exhibits a multi-year negative MAM trend and a positive JJA trend in the Arctic during 2003–2019, due to an overall decrease in sulfate/anthropogenic pollution and a significant JJA increase in BB smoke. Interannual Arctic AOD variability is significantly large, driven by fine-mode and, specifically, BB smoke, with both smoke contribution and interannual variation larger in JJA than in MAM. It is recommended that climate models should account for BB emissions and BB interannual variabilities and trends in Arctic climate change studies.

Interactions of meteorology with wildfires in British Columbia, Canada, during August 2017 led to three major pyrocumulonimbus (pyroCb) events that resulted in the injection of large amounts of smoke aerosols and other combustion products at the local upper troposphere and lower stratosphere (UTLS). These plumes of UTLS smoke with elevated values of aerosol extinction and backscatter compared to the background state were readily tracked by multiple satellite-based instruments as they spread across the Northern Hemisphere (NH). The plumes were observed in the lower stratosphere for about 8–10 months following the fire injections, with a stratospheric aerosol e-folding time of about 5 months. To investigate the radiative impacts of these events on the Earth system, we performed a number of simulations with the Goddard Earth Observing System (GEOS) atmospheric general circulation model (AGCM). Observations from multiple remote-sensing instruments were used to calibrate the injection parameters (location, amount, composition and heights) and optical properties of the smoke aerosols in the model. The resulting simulations of three-dimensional smoke transport were evaluated for a year from the day of injections using daily observations from OMPS-LP (Ozone Mapping Profiler Suite Limb Profiler). The model-simulated rate of ascent, hemispheric spread and residence time (or e-folding time) of the smoke aerosols in the stratosphere are in close agreement with OMPS-LP observations. We found that both aerosol self-lofting and the large-scale atmospheric motion play important roles in lifting the smoke plumes from near the tropopause altitudes (∼ 12 km) to about 22–23 km into the atmosphere. Further, our estimations of the radiative impacts of the pyroCb-emitted smoke aerosols showed that the smoke caused an additional warming of the atmosphere by about 0.6–1 W/m2 (zonal mean) that persisted for about 2–3 months after the injections in regions north of 40∘ N. The surface experienced a comparable magnitude of cooling. The atmospheric warming is mainly located in the stratosphere, coincident with the location of the smoke plumes, leading to an increase in zonal mean shortwave (SW) heating rates of 0.02–0.04 K/d during September 2017.

Using the Vector LInearized Discrete Ordinate Radiative Transfer (VLIDORT) code as the main driver for forward model simulations, a first-of-its-kind data assimilation scheme has been developed for assimilating Ozone Monitoring Instrument (OMI) aerosol index (AI) measurements into the Naval Aerosol Analysis and Predictive System (NAAPS). This study suggests that both root mean square error (RMSE) and absolute errors can be significantly reduced in NAAPS analyses with the use of OMI AI data assimilation when compared to values from NAAPS natural runs. Improvements in model simulations demonstrate the utility of OMI AI data assimilation for aerosol model analysis over cloudy regions and bright surfaces. However, the OMI AI data assimilation alone does not outperform aerosol data assimilation that uses passive-based aerosol optical depth (AOD) products over cloud-free skies and dark surfaces. Further, as AI assimilation requires the deployment of a fully multiple-scatter-aware radiative transfer model in the forward simulations, computational burden is an issue. Nevertheless, the newly developed modeling system contains the necessary ingredients for assimilation of radiances in the ultraviolet (UV) spectrum, and our study shows the potential of direct radiance assimilation at both UV and visible spectrums, possibly coupled with AOD assimilation, for aerosol applications in the future. Additional data streams can be added, including data from the TROPOspheric Monitoring Instrument (TROPOMI), the Ozone Mapping and Profiler Suite (OMPS), and eventually the Plankton, Aerosol, Cloud and ocean Ecosystem (PACE) mission.

North African dust reaches the southeastern United States every summer. Size-resolved dust mass measurements taken in Miami, Florida, indicate that more than one-half of the surface dust mass concentrations reside in particles with geometric diameters less than 2.1 µm, while vertical profiles of micropulse lidar depolarization ratios show dust reaching above 4 km during pronounced events. These observations are compared to the representation of dust in the Modern-Era Retrospective analysis for Research and Applications, version 2 (MERRA-2) aerosol reanalysis and closely related Goddard Earth Observing System model version 5 (GEOS-5) Forward Processing (FP) aerosol product, both of which assimilate satellite-derived aerosol optical depths using a similar protocol and inputs. These capture the day-to-day variability in aerosol optical depth well, in a comparison to an independent sun-photometer-derived aerosol optical depth dataset. Most of the modeled dust mass resides in diameters between 2 and 6 µm, in contrast to the measurements. Model-specified mass extinction efficiencies equate light extinction with approximately 3 times as much aerosol mass, in this size range, compared to the measured dust sizes. GEOS-5 FP surface-layer sea salt mass concentrations greatly exceed observed values, despite realistic winds and relative humidities. In combination, these observations help explain why, despite realistic total aerosol optical depths, (1) free-tropospheric model volume extinction coefficients are lower than those retrieved from the micro-pulse lidar, suggesting too-low model dust loadings in the free troposphere, and (2) model dust mass concentrations near the surface can be higher than those measured. The modeled vertical distribution of dust, when captured, is reasonable. Large, aspherical particles exceeding the modeled dust sizes are also occasionally present, but dust particles with diameters exceeding 10 µm contribute little to the measured total dust mass concentrations after such long-range transport. Remaining uncertainties warrant a further integrated assessment to confirm this study's interpretations.

A series of in situ measurements made by optical particle counters (OPCs) at Laramie, Wyoming, provides size-resolved stratospheric aerosol concentration data over the period 1971–2018. A subset of these data covering the period of 2008–2017 is analyzed in this study for the purpose of assessing the sensitivity of the stratospheric aerosol phase function to the aerosol size distribution (ASD) model used to fit the measurements. The two unimodal ASD models investigated are the unimodal lognormal (UMLN) and gamma distribution models, with the minimum χ2 method employed to assess how well each ASD fits the measurements. The aerosol phase function (Pa(Θ)) for each ASD is calculated using Mie theory and is compared to the Pa(Θ) derived from the Community Aerosol and Radiation Model for Atmospheres (CARMA) sectional aerosol microphysics module. Comparing the χ2 values for the fits at altitudes of 20 and 25 km shows that the UMLN distribution better represents the OPC measurements; however, the gamma distribution fits the CARMA model results better than the UMLN model when the CARMA model results are subsetted into the OPC measurement bins. Comparing phase functions derived from the UMLN distribution fit to OPC data with gamma distributions fit to CARMA model results at the location of the OPC measurements shows a satisfying agreement (±5 %) within the scattering angle range of limb sounding satellites. This uncertainty is considerably larger if the CARMA data are fit with a UMLN.

The Pacific Northwest pyrocumulonimbus Event (PNE) took place in British Columbia during the nighttime hours between the 12th and 13th of August 2017. Several pyroconvective clouds erupted in this occasion, and released in the upper troposphere/lower stratosphere unprecedented amounts of carbonaceous aerosols (300 ktn). The stratospheric aerosol plume persisted in the stratosphere for several months, while gradually rising up to 22 km and dispersing around the entire northern hemisphere. In this study, we use the Goddard Earth Observing System Atmospheric General Circulation Model (GEOS AGCM) to study the pertubations that the aerosol plume from the PNE event induced on the stratospheric meteorology. Our simulations include the radiative interactions of aerosols, so that their impacts on temperatures and winds are explicitly simulated . In this work, we show how the presence of the carbonaceous aerosols from the PNE event triggers the formation and maintenance of a synoptic scale stratospheric anticyclone. We follow this disturbance considering the potential vorticity anomaly and the brown carbon aerosol loading and we describe its dynamical structure and evolution in time. The analysis presented here shows that the simulated anticyclone undergoes daily expansion-compression cycles governed by the radiative heating, which are directly related to the vertical motion of the plume, and that the aerosol radiative heating is essential in maintaining the anticyclone itself.

We present an Arctic aerosol optical depth (AOD) climatology and trend analysis for 2003–2019 spring and summertime periods derived from a combination of multi-agency aerosol reanalyses, remote sensing retrievals, and ground observations. This includes the U.S. Navy Aerosol Analysis and Prediction System ReAnalysis version 1 (NAAPS-RA v1), the NASA Modern-Era Retrospective Analysis for Research and Applications, version 2 (MERRA-2), and the Copernicus Atmosphere Monitoring Service ReAnalysis (CAMSRA). Space-borne remote sensing retrievals of AOD are considered from the Moderate Resolution Imaging Spectroradiometer (MODIS), the Multi-angle Imaging SpectroRadiometer (MISR), and Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP). Ground-based data include sun photometer data from Aerosol Robotic Network (AERONET) sites and oceanic Maritime Aerosol Network (MAN) measurements. Aerosol reanalysis AODs and space-borne retrievals show consistent climatological spatial patterns and trends for both spring and summer seasons over the sub-Arctic (60–70° N). Consistent signs in the AOD trend are also found for the high Arctic (north of 70° N) from reanalyses. The aerosol reanalyses yield more consistent AOD results than climate models, verify well with AERONET, and corroborate complementary climatological and trend analysis. Speciated AODs are more variable than total AOD among the three reanalyses, and a little more so for March–May (MAM) than for June–August (JJA). Black Carbon (BC) AOD in the Arctic comes predominantly from biomass burning sources in both MAM and JJA, and biomass burning overwhelms anthropogenic sources in JJA for the study period. AOD exhibits a negative trend in the Arctic in MAM, and a positive trend in JJA during 2003–2019, due to an overall decrease in sulfate/anthropogenic pollutions, and a significant increase in biomass burning smoke in JJA. Interannual Arctic AOD variability is significantly large, driven by fine-mode, and specifically, biomass burning (BB) smoke, though more so in JJA than in MAM. Extreme AOD events during spring and summer in the Arctic, defined as AOD greater than the 95th percentile value, are mainly attributed to BB smoke transport events. Extreme AOD cases tend to occur later in the season (i.e., July and August, in the latter decade rather than spreading over April–August in the early decade during 2003–2019) corresponding to a shift to a later time in extreme boreal BB activities.

The inorganic fraction of fine particles affects numerous physicochemical processes in the atmosphere. However, there is large uncertainty in its burden and composition due to limited global measurements. Here, we present observations from eleven different aircraft campaigns from around the globe and investigate how aerosol pH and ammonium balance change from polluted to remote regions, such as over the oceans. Both parameters show increasing acidity with remoteness, at all altitudes, with pH decreasing from about 3 to about −1 and ammonium balance decreasing from almost 1 to nearly 0. We compare these observations against nine widely used chemical transport models and find that the simulations show more scatter (generally R2

The June 21, 2019 eruption of the Raikoke volcano (Kuril Islands, Russia, 48°N, 153°E) produced significant amounts of volcanic aerosols (sulfate and ash) and sulfur dioxide (SO2) gas that penetrated into the lower stratosphere. The dispersed SO2 and sulfate aerosols in the stratosphere were still detectable by multiple satellite sensors for three months after the eruption. For this study of SO2 and aerosol clouds we use data obtained from two of the Ozone Mapping Profiler Suite (OMPS) sensors on the Suomi National Polar-orbiting Partnership (SNPP) satellite: total column SO2 from the Nadir Mapper (NM) and aerosol extinction profiles from the Limb Profiler (LP) as well as other satellite data sets. The LP standard aerosol extinction product at 674 nm has been re-processed with an adjustment correcting for limb viewing geometry effects. It was shown that the amount of SO2 decreases with a characteristic period of 8–18 days and the peak of sulfate aerosol recorded at a wavelength of 674 nm lags the initial peak of SO2 by 1.5 months. Using satellite observations and a trajectory model, we examined the dynamics of unusual atmospheric feature that was observed, a stratospheric coherent circular cloud (CCC) of SO2 and aerosol from July 18 to September 22, 2019.

This study characterizes a massive African dust intrusion into the Caribbean Basin and southern U.S. in June 2020, which is nicknamed the Godzilla dust plume, using a comprehensive set of satellite and ground-based observations (including MODIS, CALIOP, SEVIRI, AERONET, and EPA Air Quality network) and the NASA GEOS global aerosol transport model. The MODIS data record registered this massive dust intrusion event as the most intense episode over the past two decades. During this event, the aerosol optical depth observed by AERONET and MODIS peaked at 3.5 off the coast of West Africa and 1.8 in the Caribbean Basin. CALIOP observations show that the top of dust plume reached altitudes of 6–8 km in West Africa and descended to about 4 km altitude over the Caribbean Basin and 2 km over the U.S. Gulf coast. The dust plume degraded the air quality in Puerto Rico to the hazardous level, with maximum daily PM10 concentration of 453 μg m−3 recorded on June 23. The dust intrusion into the U.S. raised the PM2.5 concentration on June 27 to a level exceeding the EPA air quality standard in about 40 % of the stations in the southern U.S. Satellite observations reveal that dust emissions from convection-generated haboobs and other sources in West Africa were large albeit not extreme on a daily basis. However, the anomalous strength and northern shift of the North Atlantic Subtropical High (NASH) together with the Azores low formed a closed circulation pattern that allowed for accumulation of the dust near the African coast for about four days. When the NASH was weakened and wandered back to south, the dust outflow region was dominated by a strong African Easterly Jet that rapidly transported the accumulated dust from the coastal region toward the Caribbean Basin, resulting in the record-breaking African dust intrusion. In comparison to satellite observations, the GEOS model well reproduced the MODIS observed tracks of the meandering dust plume as it was carried by the wind systems. However, the model substantially underestimated dust emissions from haboobs and did not lift up enough dust to the middle troposphere for ensuing long-range transport. Consequently, the model largely missed the satellite-observed elevated dust plume along the cross-ocean track and underestimated the dust intrusion into the Caribbean Basin by a factor of more than 4. Modeling improvements need to focus on developing more realistic representations of moist convection, haboobs, and the vertical transport of dust.

Even though desert dust is the most abundant aerosol by mass in Earth's atmosphere, the relative contributions of the world's major source regions to the global dust cycle remain poorly constrained. This problem hinders accounting for the potentially large impact of regional differences in dust properties on clouds, the Earth's energy balance, and terrestrial and marine biogeochemical cycles. Here, we constrain the contribution of each of the world's main dust source regions to the global dust cycle. We use an analytical framework that integrates an ensemble of global aerosol model simulations with observationally informed constraints on the dust size distribution, extinction efficiency, and regional dust aerosol optical depth (DAOD). We obtain a dataset that constrains the relative contribution of nine major source regions to size-resolved dust emission, atmospheric loading, DAOD, concentration, and deposition flux. We find that the 22–29 Tg (1 standard error range) global loading of dust with a geometric diameter up to 20 µm is partitioned as follows: North African source regions contribute ∼ 50 % (11–15 Tg), Asian source regions contribute ∼ 40 % (8–13 Tg), and North American and Southern Hemisphere regions contribute ∼ 10 % (1.8–3.2 Tg). These results suggest that current models on average overestimate the contribution of North African sources to atmospheric dust loading at ∼ 65 %, while underestimating the contribution of Asian dust at ∼ 30 %. Our results further show that each source region's dust loading peaks in local spring and summer, which is partially driven by increased dust lifetime in those seasons. We also quantify the dust deposition flux to the Amazon rainforest to be ∼ 10 Tg yr−1, which is a factor of 2–3 less than inferred from satellite data by previous work that likely overestimated dust deposition by underestimating the dust mass extinction efficiency. The data obtained in this paper can be used to obtain improved constraints on dust impacts on clouds, climate, biogeochemical cycles, and other parts of the Earth system.

Interactions of meteorology with wildfires in British Columbia, Canada during August 2017 led to three major pyrocumulonimbus (pyroCb) events that resulted in the injection of large amounts of smoke aerosols and other combustion products at the local upper troposphere and lower stratosphere (UTLS). These plumes of UTLS smoke with elevated values of aerosol extinction and backscatter compared to the background state were readily tracked by multiple satellite-based instruments as they spread across the Northern Hemisphere (NH). The plumes resided in the lower stratosphere for about 8–10 months following the fire injections. To investigate the radiative impacts of these events on the Earth system, we performed a number of simulations with the Goddard Earth Observing System (GEOS) atmospheric general circulation model (AGCM). Observations from multiple remote-sensing instruments were used to calibrate the injection parameters (location, amount, composition, and heights) and optical properties of the smoke aerosols in the model. The resulting simulations of three-dimensional smoke transport were evaluated for a year from the day of injections using daily observations from OMPS-LP (Ozone Mapping Profiler Suite Limb Profiler). The model simulated rate of ascent, hemispheric spread, and residence time of the smoke aerosols in the stratosphere are in close agreement with OMPS-LP observations. We found that both aerosol self-lofting and the large-scale atmospheric motion play important roles in lifting the smoke plumes from near the tropopause altitudes (~12 km) to about 22–23 km into the atmosphere. Further, our estimations of the radiative impacts of the pyroCb-emitted smoke aerosols showed that the smoke caused additional warming of the atmosphere by about 0.6–1 W/m2 (zonal mean) that persisted for about 2–3 months after the injections in regions north of 40° N. The surface experienced a comparable magnitude of cooling. The atmospheric warming is mainly located in the stratosphere, coincident with the location of the smoke plumes, leading to an increase in zonal mean shortwave (SW) heating rates of 0.02–0.04 K/day during September 2017.

Using the Vector LInearized Discrete Ordinate Radiative Transfer (VLIDORT) code as the main driver for forward model simulations, a first-of-its-kind data assimilation scheme has been developed for assimilating Ozone Monitoring Instrument (OMI) aerosol index (AI) measurements into the Naval Aerosol Analysis and Predictive System (NAAPS). This study suggests both RMSE and absolute errors can be significantly reduced in NAAPS analyses with the use of OMI AI data assimilation, when compared to values from NAAPS natural runs. Improvements in model simulations demonstrate the utility of OMI AI data assimilation for improving the accuracy of aerosol model analysis over cloudy regions and bright surfaces. However, the OMI AI data assimilation alone does not out-perform aerosol data assimilation that uses passive-based aerosol optical depth (AOD) products over cloud free skies and dark surfaces. Further, as AI assimilation requires the deployment of a fully-multiple-scatter-aware radiative transfer model in the forward simulations, computational burden is an issue. Nevertheless, the newly-developed modeling system contains the necessary ingredients for assimilation of radiances in the ultra-violet (UV) spectrum, and our study shows the potential of direct radiance assimilation at both UV and visible spectrums, possibly coupled with AOD assimilation, for aerosol applications in the future. Additional data streams can be added, including data from TROPOspheric Monitoring Instrument (TROPOMI), Ozone Mapping and Profiler Suite (OMPS) and eventually with the Plankton, Aerosol, Cloud and ocean Ecosystem (PACE) mission.

Previous studies have noted a relationship between African dust and Atlantic tropical cyclone (TC) activity. However, due to the limitations of past dust analyses, the strength of this relationship remains uncertain. The emergence of aerosol reanalyses, including the Navy Aerosol Analysis and Prediction System (NAAPS) aerosol optical depth (AOD) reanalysis, NASA Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2), and ECMWF Copernicus Atmosphere Monitoring Service reanalysis (CAMSRA), enables an investigation of the relationship between African dust and TC activity over the tropical Atlantic and Caribbean in a consistent temporal and spatial manner for 2003–2018. Although June–July–August (JJA) 550 nm dust AOD (DAOD) from all three reanalysis products correlates significantly over the tropical Atlantic and Caribbean, the difference in DAOD magnitude between products can be as large as 60 % over the Caribbean and 20 % over the tropical North Atlantic. Based on the three individual reanalyses, we have created an aerosol multi-reanalysis consensus (MRC). The MRC presents overall better root mean square error over the tropical Atlantic and Caribbean compared to individual reanalyses when verified with ground-based AErosol RObotic NETwork (AERONET) AOD measurements. Each of the three individual reanalyses and the MRC have significant negative correlations between JJA Caribbean DAOD and seasonal Atlantic accumulated cyclone energy (ACE), while the correlation between JJA tropical North Atlantic DAOD and seasonal ACE is weaker. Possible reasons for this regional difference are provided. A composite analysis of 3 high-JJA-Caribbean-DAOD years versus 3 low-JJA-Caribbean-DAOD years reveals large differences in overall Atlantic TC activity. We also show that JJA Caribbean DAOD is significantly correlated with large-scale fields associated with variability in interannual Atlantic TC activity including zonal wind shear, mid-level moisture, and sea surface temperature (SST), as well as the El Niño–Southern Oscillation (ENSO) and the Atlantic Meridional Mode (AMM), implying confounding effects of these factors on the dust–TC relationship. We find that seasonal Atlantic DAOD and the AMM, the leading mode of coupled Atlantic variability, are inversely related and intertwined in the dust–TC relationship. Overall, DAOD in both the tropical Atlantic and Caribbean is negatively correlated with Atlantic hurricane frequency and intensity, with stronger correlations in the Caribbean than farther east in the tropical North Atlantic.

The spatial distribution and properties of submicron organic aerosol (OA) are among the key sources of uncertainty in our understanding of aerosol effects on climate. Uncertainties are particularly large over remote regions of the free troposphere and Southern Ocean, where very few data have been available and where OA predictions from AeroCom Phase II global models span 2 to 3 orders of magnitude, greatly exceeding the model spread over source regions. The (nearly) pole-to-pole vertical distribution of non-refractory aerosols was measured with an aerosol mass spectrometer onboard the NASA DC-8 aircraft as part of the Atmospheric Tomography (ATom) mission during the Northern Hemisphere summer (August 2016) and winter (February 2017). This study presents the first extensive characterization of OA mass concentrations and their level of oxidation in the remote atmosphere. OA and sulfate are the major contributors by mass to submicron aerosols in the remote troposphere, together with sea salt in the marine boundary layer. Sulfate was dominant in the lower stratosphere. OA concentrations have a strong seasonal and zonal variability, with the highest levels measured in the lower troposphere in the summer and over the regions influenced by biomass burning from Africa (up to 10 µg sm−3). Lower concentrations (∼0.1–0.3 µg sm−3) are observed in the northern middle and high latitudes and very low concentrations ( µg sm−3) in the southern middle and high latitudes. The ATom dataset is used to evaluate predictions of eight current global chemistry models that implement a variety of commonly used representations of OA sources and chemistry, as well as of the AeroCom-II ensemble. The current model ensemble captures the average vertical and spatial distribution of measured OA concentrations, and the spread of the individual models remains within a factor of 5. These results are significantly improved over the AeroCom-II model ensemble, which shows large overestimations over these regions. However, some of the improved agreement with observations occurs for the wrong reasons, as models have the tendency to greatly overestimate the primary OA fraction and underestimate the secondary fraction. Measured OA in the remote free troposphere is highly oxygenated, with organic aerosol to organic carbon (OA ∕ OC) ratios of ∼2.2–2.8, and is 30 %–60 % more oxygenated than in current models, which can lead to significant errors in OA concentrations. The model–measurement comparisons presented here support the concept of a more dynamic OA system as proposed by Hodzic et al. (2016), with enhanced removal of primary OA and a stronger production of secondary OA in global models needed to provide better agreement with observations.

Interactions of meteorology with wildfires in British Columbia, Canada during August 2017 led to several extreme pyrocumulonimbus (PyroCb) events that resulted in the injection of smoke aerosols and other combustion products into the lower stratosphere. These plumes of stratospheric smoke were observed by many satellite instruments to have elevated values of aerosol extinction and backscatter compared to the background state and were readily tracked as they spread across the Northern Hemisphere and resided in the lower stratosphere for about ten months following the fires. To investigate the radiative impacts of these events on the Earth system, we performed a number of simulations with the Goddard Earth Observing System (GEOS) global Earth system model, which includes detailed aerosol and chemistry packages coupled to the underlying model physical and dynamical cores. Retrievals of smoke aerosol properties from space-based OMPS/NPP, SAGE-III/ISS, and CALIOP/CALIPSO instruments were used to calibrate the injection location, timing, amount, and optical properties of the smoke aerosols. The resulting simulations of three-dimensional smoke transport were evaluated over a year following the injections using observations from OMPS-Limb Profiler (LP), which provides aerosol retrievals at a high temporal and vertical resolution for altitudes greater than 10 km. We found that diabatic heating due to aerosol absorption, combined with the large-scale atmospheric motions, play important roles in lifting the smoke plumes from near the tropopause altitudes to about 22 km into the atmosphere. The model was able to simulate the rate of plume ascent from lower to the middle stratosphere, hemispherical spread and residence time of the smoke aerosols in the stratosphere in close agreement with OMPS-LP. Finally, we also investigated the impact of these PyroCb emitted smoke aerosols on the stratospheric radiative forcing and the subsequent impact on temperature tendencies.

The inorganic composition of aerosol impacts numerous chemical and physical processes and properties. However, many chemical transport models show large variability in both the concentration of the inorganic aerosols and their precursors (up to 3 orders of magnitude differences) and the inorganic aerosol composition. Different models predict very different properties (e.g., aerosol liquid water concentration and aerosol acidity) and outcomes (e.g., heterogeneous uptake of gases or aerosols’ direct and indirect impacts on climate). Here, we use airborne observations from campaigns conducted around the world to investigate how the inorganic fine aerosol (PM1) composition, and one of its key parameters, aerosol acidity, changes from polluted regions (Mexico City, Los Angeles, Northeastern US, and Seoul) to remote ocean basins (the Atmospheric Tomography campaigns 1 and 2) in order to provide constraints for the chemical transport models. I find that the empirical ammonium balance with major ions (ammonium balance = mol NH4 / (2×mol SO4 + mol NO3)) rapidly decreases from ~1 at the highest inorganic PM1 concentration to 0 at the lowest inorganic PM1. The data indicate a robust trend for ammonium balance vs inorganic PM1 at all altitude levels in the troposphere, suggesting that NH3 emissions and subsequent neutralization of H2SO4 becomes negligible in the most remote (lowest inorganic PM1) regions. Further, a robust trend for PM1 pH (calculated with E-AIM) vs inorganic PM1 is observed at all levels for these campaigns, as well, decreasing from a pH of ~3 to a pH of ~ –1 from the highest to lowest inorganic PM1. The data overall implies very low NH3 (and NH4+) throughout most of the atmosphere, contrary to predictions of some models, implying different physical properties than predicted in models. We compare these trends of ammonium balance and pH vs inorganic PM1 against 9 chemical transport models (CTMs), and we find that the CTMs show large variability for both the ammonium balance and pH vs inorganic PM­1, compared to observations. Generally, we find a high bias in the ammonium balance and pH, likely due to too much NH­3 in model (possibly too high NH3 emissions over oceans or too long lifetime) and inclusion of externally mixed seasalt into the submicron pH calculation. These results overall would imply different aerosol properties in the models than observed, impacting the chemistry, optical properties, and cloud properties.