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Biomass burning aerosol impacts aspects of the atmosphere and Earth system through direct and semi-direct effects, as well as influencing air quality. Despite its importance, the representation of biomass burning aerosol is not always accurate in numerical weather prediction and climate models or reanalysis products. Using observations collected as part of the Cloud, Aerosol and Monsoon Processes Philippines Experiment (CAMP2Ex) in August through October of 2019, aerosol concentration and optical properties are evaluated within the Goddard Earth Observing System (GEOS) and its underlying aerosol module, GOCART. In the operational configuration, GEOS assimilates aerosol optical depth observations at 550 nm from AERONET and MODIS to constrain aerosol fields. Particularly for biomass burning aerosol, without the assimilation of aerosol optical depth, aerosol extinction is underestimated compared to observations collected in the Philippines region during the CAMP2Ex campaign. The assimilation process adds excessive amounts of carbon to account for the underestimated extinction, resulting in positive biases in the mass of black and organic carbon, especially within the boundary layer, relative to in situ observations from the Langley Aerosol Research Group Experiment. Counteracting this, GEOS is deficient in sulfate and nitrate aerosol just above the boundary layer. Aerosol extinction within GEOS is a function of the mass of different aerosol species, the ambient relative humidity, the assumed spectral optical properties, and particle size distribution per species. The relationship between dry and ambient extinction in GEOS reveals that hygroscopic growth is too high within the model for biomass burning aerosol. An additional concern lies in the assumed particle size distribution for GEOS, which has a single mode radius that is too small for organic carbon. Variability in the observed particle size distribution for biomass burning aerosol within a single flight also illuminates the fact that a single assumed particle size distribution is not sufficient and that for a proper representation, a more advanced aerosol module within GEOS may be necessary.

Biomass burning in southwestern Africa produces smoke plumes that are transported over the Atlantic Ocean and overlie vast regions of stratocumulus clouds. This aerosol layer contributes to direct and indirect radiative forcing of the atmosphere in this region particularly during the months of August, September, and October. There was a multi-year international campaign to study this aerosol and its interactions with clouds. Here, we report on the evolution of aerosol distributions and properties as measured by the airborne high spectral resolution lidar (HSRL-2) during the ORACLES (Observations of Aerosols above Clouds and their intEractionS) campaign in September 2016. The NASA Langley HSRL-2 instrument was flown on the NASA ER-2 aircraft for several days in September 2016. Data were aggregated at two pairs of 2∘ × 2∘ grid boxes to examine the evolution of the vertical profile of aerosol properties during transport over the ocean. Results showed that the structure of the profile of aerosol extinction and microphysical properties is maintained over a 1 to 2 d timescale. In the 3–5 km altitude range, 95 % of the aerosol extinction was contributed by particles in the 0.05–0.50 µm radius size range with the aerosol in this size range having an average effective radius of 0.16 µm. This indicates that there is essentially no scavenging or dry deposition at these altitudes. Moreover, there is very little day-to-day variation in these properties, such that time sampling as happens in such campaigns may be representative of longer periods such as monthly means. Below 3 km, there is considerable mixing with larger aerosol, most likely continental source near land. Furthermore, these measurements indicated that there was often a distinct gap between the bottom of the aerosol layer and cloud tops at the selected locations as evidenced by a layer of several hundred meters that contained relatively low aerosol extinction values above the clouds.

This work focuses on the characterization of vertically resolved aerosol hygroscopicity properties and their direct radiative effects through a unique combination of ground-based and airborne remote sensing measurements during the Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) 2011 field campaign in the Baltimore–Washington DC metropolitan area. To that end, we combined aerosol measurements from a multiwavelength Raman lidar located at NASA Goddard Space Flight Center and the airborne NASA Langley High Spectral Resolution Lidar-1 (HSRL-1) lidar system. In situ measurements aboard the P-3B airplane and ground-based Aerosol Robotic Network – Distributed Regional Aerosol Gridded Observational Network (AERONET-DRAGON) served to validate and complement quantifications of aerosol hygroscopicity from lidar measurements and also to extend the study both temporally and spatially. The focus here is on 22 and 29 July 2011, which were very humid days and characterized by a stable atmosphere and increasing relative humidity with height in the planetary boundary layer (PBL). Combined lidar and radiosonde (temperature and water vapor mixing ratio) measurements allowed the retrieval of the Hänel hygroscopic growth factor which agreed with that obtained from airborne in situ measurements and also explained the significant increase of extinction and backscattering with height. Airborne measurements also confirmed aerosol hygroscopicity throughout the entire day in the PBL and identified sulfates and water-soluble organic carbon as the main species of aerosol particles. The combined Raman and HSRL-1 measurements permitted the inversion for aerosol microphysical properties revealing an increase of particle radius with altitude consistent with hygroscopic growth. Aerosol hygroscopicity pattern served as a possible explanation of aerosol optical depth increases during the day, particularly for fine-mode particles. Lidar measurements were used as input to the libRadtran radiative transfer code to obtain vertically resolved aerosol radiative effects and heating rates under dry and humid conditions, and the results reveal that aerosol hygroscopicity is responsible for larger cooling effects in the shortwave range (7–10 W m−2 depending on aerosol load) near the ground, while heating rates produced a warming of 0.12 K d−1 near the top of PBL where aerosol hygroscopic growth was highest.

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.

Satellite quantification of aerosol effects on clouds relies on aerosol optical depth (AOD) as a proxy for aerosol concentration or cloud condensation nuclei (CCN). However, the lack of error characterization of satellite-based results hampers their use for the evaluation and improvement of global climate models. We show that the use of AOD for assessing aerosol–cloud interactions (ACIs) is inadequate over vast oceanic areas in the subtropics. Instead, we postulate that a more physical approach that consists of matching vertically resolved aerosol data from the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) satellite at the cloud-layer height with Moderate Resolution Imaging Spectroradiometer (MODIS) Aqua cloud retrievals reduces uncertainties in satellite-based ACI estimates. Combined aerosol extinction coefficients (σ) below cloud top (σBC) from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) and cloud droplet number concentrations (Nd) from MODIS Aqua yield high correlations across a broad range of σBC values, with σBC quartile correlations ≥0.78. In contrast, CALIOP-based AOD yields correlations with MODIS Nd of 0.54–0.62 for the two lower AOD quartiles. Moreover, σBC explains 41 % of the spatial variance in MODIS Nd, whereas AOD only explains 17 %, primarily caused by the lack of spatial covariability in the eastern Pacific. Compared with σBC, near-surface σ weakly correlates in space with MODIS Nd, accounting for a 16 % variance. It is concluded that the linear regression calculated from ln(Nd)–ln(σBC) (the standard method for quantifying ACIs) is more physically meaningful than that derived from the Nd–AOD pair.

The total effect of aerosols, both directly and on cloud properties, remains the biggest source of uncertainty in anthropogenic radiative forcing on the climate. Correct characterization of intensive aerosol optical properties, particularly in conditions where absorbing aerosol is present, is a crucial factor in quantifying these effects. The southeast Atlantic Ocean (SEA), with seasonal biomass burning smoke plumes overlying and mixing with a persistent stratocumulus cloud deck, offers an excellent natural laboratory to make the observations necessary to understand the complexities of aerosol–cloud–radiation interactions. The first field deployment of the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) campaign was conducted in September of 2016 out of Walvis Bay, Namibia. Data collected during ORACLES-2016 are used to derive aerosol properties from an unprecedented number of simultaneous measurement techniques over this region. Here, we present results from six of the eight independent instruments or instrument combinations, all applied to measure or retrieve aerosol absorption and single-scattering albedo. Most but not all of the biomass burning aerosol was located in the free troposphere, in relative humidities typically ranging up to 60 %. We present the single-scattering albedo (SSA), absorbing and total aerosol optical depth (AAOD and AOD), and absorption, scattering, and extinction Ångström exponents (AAE, SAE, and EAE, respectively) for specific case studies looking at near-coincident and near-colocated measurements from multiple instruments, and SSAs for the broader campaign average over the month-long deployment. For the case studies, we find that SSA agrees within the measurement uncertainties between multiple instruments, though, over all cases, there is no strong correlation between values reported by one instrument and another. We also find that agreement between the instruments is more robust at higher aerosol loading (AOD400>0.4). The campaign-wide average and range shows differences in the values measured by each instrument. We find the ORACLES-2016 campaign-average SSA at 500 nm (SSA500) to be between 0.85 and 0.88, depending on the instrument considered (4STAR, AirMSPI, or in situ measurements), with the interquartile ranges for all instruments between 0.83 and 0.89. This is consistent with previous September values reported over the region (between 0.84 and 0.90 for SSA at 550nm). The results suggest that the differences observed in the campaign-average values may be dominated by instrument-specific spatial sampling differences and the natural physical variability in aerosol conditions over the SEA, rather than fundamental methodological differences.

Estimates of the direct radiative effect (DRE) from absorbing smoke aerosols over the southeast Atlantic Ocean (SAO) require simulation of the microphysical and optical properties of stratocumulus clouds as well as of the altitude and shortwave (SW) optical properties of biomass burning aerosols (BBAs). In this study, we take advantage of the large number of observations acquired during the ObseRvations of Aerosols above Clouds and their intEractionS (ORACLES-2016) and Layered Atlantic Smoke Interactions with Clouds (LASIC) projects during September 2016 and compare them with datasets from the ALADIN-Climate (Aire Limitée Adaptation dynamique Développement InterNational) regional model. The model provides a good representation of the liquid water path but the low cloud fraction is underestimated compared to satellite data. The modeled total-column smoke aerosol optical depth (AOD) and above-cloud AOD are consistent (∼0.7 over continental sources and ∼0.3 over the SAO at 550 nm) with the Modern-Era Retrospective analysis for Research and Applications version 2 (MERRA-2), Ozone Monitoring Instrument (OMI) or Moderate Resolution Imaging Spectroradiometer (MODIS) data. The simulations indicate smoke transport over the SAO occurs mainly between 2 and 4 km, consistent with surface and aircraft lidar observations. The BBA single scattering albedo is slightly overestimated compared to the Aerosol Robotic Network (AERONET) and more significantly when compared to Ascension Island surface observations. The difference could be due to the absence of internal mixing treatment in the ALADIN-Climate model. The SSA overestimate leads to an underestimation of the simulated SW radiative heating compared to ORACLES data. ALADIN-Climate simulates a positive (monthly mean) SW DRE of about +6 W m−2 over the SAO (20∘ S–10∘ N and 10∘ W–20∘ E) at the top of the atmosphere and in all-sky conditions. Over the continent, the presence of BBA is shown to significantly decrease the net surface SW flux, through direct and semi-direct effects, which is compensated by a decrease (monthly mean) in sensible heat fluxes (−25 W m−2) and surface land temperature (−1.5 ∘C) over Angola, Zambia and the Democratic Republic of the Congo, notably. The surface cooling and the lower tropospheric heating decrease the continental planetary boundary layer height by about ∼200 m.

The Global Fire Assimilation System (GFAS) assimilates fire radiative power (FRP) observations from satellite-based sensors to produce daily estimates of biomass burning emissions. It has been extended to include information about injection heights derived from fire observations and meteorological information from the operational weather forecasts of ECMWF. Injection heights are provided by two distinct methods: the Integrated Monitoring and Modelling System for wildland fires (IS4FIRES) parameterisation and the one-dimensional plume rise model (PRM). A global database of daily biomass burning emissions and injection heights at 0.1° resolution has been produced for 2003–2015 and is continuously extended in near-real time with the operational GFAS service of the Copernicus Atmospheric Monitoring Service (CAMS). In this study, the two injection height data sets were compared with the new MPHP2 (MISR Plume Height Project 2) satellite-based plume height retrievals. The IS4FIRES parameterisation showed a better overall agreement than the observations, while the PRM was better at capturing the variability of injection heights. The performance of both parameterisations is also dependent on the type of vegetation. Furthermore, the use of biomass burning emission heights from GFAS in atmospheric composition forecasts was assessed in two case studies: the South AMerican Biomass Burning Analysis (SAMBBA) campaign which took place in September 2012 in Brazil, and a series of large fire events in the western USA in August 2013. For these case studies, forecasts of biomass burning aerosol species by the Composition Integrated Forecasting System (C-IFS) of CAMS were found to better reproduce the observed vertical distribution when using PRM injection heights from GFAS compared to aerosols emissions being prescribed at the surface. The globally available GFAS injection heights introduced and evaluated in this study provide a comprehensive data set for future fire and atmospheric composition modelling studies.

Formaldehyde (HCHO) column data from satellites are widely used as a proxy for emissions of volatile organic compounds (VOCs), but validation of the data has been extremely limited. Here we use highly accurate HCHO aircraft observations from the NASA SEAC4RS (Studies of Emissions, Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys) campaign over the southeast US in August–September 2013 to validate and intercompare six retrievals of HCHO columns from four different satellite instruments (OMI, GOME2A, GOME2B and OMPS; for clarification of these and other abbreviations used in the paper, please refer to Appendix A) and three different research groups. The GEOS-Chem chemical transport model is used as a common intercomparison platform. All retrievals feature a HCHO maximum over Arkansas and Louisiana, consistent with the aircraft observations and reflecting high emissions of biogenic isoprene. The retrievals are also interconsistent in their spatial variability over the southeast US (r = 0.4–0.8 on a 0.5° × 0.5° grid) and in their day-to-day variability (r = 0.5–0.8). However, all retrievals are biased low in the mean by 20–51 %, which would lead to corresponding bias in estimates of isoprene emissions from the satellite data. The smallest bias is for OMI-BIRA, which has high corrected slant columns relative to the other retrievals and low scattering weights in its air mass factor (AMF) calculation. OMI-BIRA has systematic error in its assumed vertical HCHO shape profiles for the AMF calculation, and correcting this would eliminate its bias relative to the SEAC4RS data. Our results support the use of satellite HCHO data as a quantitative proxy for isoprene emission after correction of the low mean bias. There is no evident pattern in the bias, suggesting that a uniform correction factor may be applied to the data until better understanding is achieved.

The performance of the Weather Research and Forecasting regional model with chemistry (WRF-Chem) in simulating the spatial and temporal variations in aerosol mass, composition, and size over California is quantified using the extensive meteorological, trace gas, and aerosol measurements collected during the California Nexus of Air Quality and Climate Experiment (CalNex) and the Carbonaceous Aerosol and Radiative Effects Study (CARES) conducted during May and June of 2010. The overall objective of the field campaigns was to obtain data needed to better understand processes that affect both climate and air quality, including emission assessments, transport and chemical aging of aerosols, aerosol radiative effects. Simulations were performed that examined the sensitivity of aerosol concentrations to anthropogenic emissions and to long-range transport of aerosols into the domain obtained from a global model. The configuration of WRF-Chem used in this study is shown to reproduce the overall synoptic conditions, thermally driven circulations, and boundary layer structure observed in region that controls the transport and mixing of trace gases and aerosols. Reducing the default emissions inventory by 50% led to an overall improvement in many simulated trace gases and black carbon aerosol at most sites and along most aircraft flight paths; however, simulated organic aerosol was closer to observed when there were no adjustments to the primary organic aerosol emissions. We found that sulfate was better simulated over northern California whereas nitrate was better simulated over southern California. While the overall spatial and temporal variability of aerosols and their precursors were simulated reasonably well, we show cases where the local transport of some aerosol plumes were either too slow or too fast, which adversely affects the statistics quantifying the differences between observed and simulated quantities. Comparisons with lidar and in situ measurements indicate that long-range transport of aerosols from the global model was likely too high in the free troposphere even though their concentrations were relatively low. This bias led to an over-prediction in aerosol optical depth by as much as a factor of 2 that offset the under-predictions of boundary-layer extinction resulting primarily from local emissions. Lowering the boundary conditions of aerosol concentrations by 50% greatly reduced the bias in simulated aerosol optical depth for all regions of California. This study shows that quantifying regional-scale variations in aerosol radiative forcing and determining the relative role of emissions from local and distant sources is challenging during `clean' conditions and that a wide array of measurements are needed to ensure model predictions are correct for the right reasons. In this regard, the combined CalNex and CARES data sets are an ideal test bed that can be used to evaluate aerosol models in great detail and develop improved treatments for aerosol processes.

Absorbing aerosols play an important, but uncertain, role in the global climate. Much of this uncertainty is due to a lack of adequate aerosol measurements. While great strides have been made in observational capability in the previous years and decades, it has become increasingly apparent that this development must continue. Scanning polarimeters have been designed to help resolve this issue by making accurate, multi-spectral, multi-angle polarized observations. This work involves the use of the Research Scanning Polarimeter (RSP). The RSP was designed as the airborne prototype for the Aerosol Polarimetery Sensor (APS), which was due to be launched as part of the (ultimately failed) NASA Glory mission. Field observations with the RSP, however, have established that simultaneous retrievals of aerosol absorption and vertical distribution over bright land surfaces are quite uncertain. We test a merger of RSP and High Spectral Resolution Lidar (HSRL) data with observations of boreal forest fire smoke, collected during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS). During ARCTAS, the RSP and HSRL instruments were mounted on the same aircraft, and validation data were provided by instruments on an aircraft flying a coordinated flight pattern. We found that the lidar data did indeed improve aerosol retrievals using an optimal estimation method, although not primarily because of the contraints imposed on the aerosol vertical distribution. The more useful piece of information from the HSRL was the total column aerosol optical depth, which was used to select the initial value (optimization starting point) of the aerosol number concentration. When ground based sun photometer network climatologies of number concentration were used as an initial value, we found that roughly half of the retrievals had unrealistic sizes and imaginary indices, even though the retrieved spectral optical depths agreed within uncertainties to independent observations. The convergence to an unrealistic local minimum by the optimal estimator is related to the relatively low sensitivity to particles smaller than 0.1 (μm) at large optical thicknesses. Thus, optimization algorithms used for operational aerosol retrievals of the fine mode size distribution, when the total optical depth is large, will require initial values generated from table look-ups that exclude unrealistic size/complex index mixtures. External constraints from lidar on initial values used in the optimal estimation methods will also be valuable in reducing the likelihood of obtaining spurious retrievals.

MILAGRO (Megacity Initiative: Local And Global Research Observations) is an international collaborative project to examine the behavior and the export of atmospheric emissions from a megacity. The Mexico City Metropolitan Area (MCMA) – one of the world's largest megacities and North America's most populous city – was selected as the case study to characterize the sources, concentrations, transport, and transformation processes of the gases and fine particles emitted to the MCMA atmosphere and to evaluate the regional and global impacts of these emissions. The findings of this study are relevant to the evolution and impacts of pollution from many other megacities. The measurement phase consisted of a month-long series of carefully coordinated observations of the chemistry and physics of the atmosphere in and near Mexico City during March 2006, using a wide range of instruments at ground sites, on aircraft and satellites, and enlisting over 450 scientists from 150 institutions in 30 countries. Three ground supersites were set up to examine the evolution of the primary emitted gases and fine particles. Additional platforms in or near Mexico City included mobile vans containing scientific laboratories and mobile and stationary upward-looking lidars. Seven instrumented research aircraft provided information about the atmosphere over a large region and at various altitudes. Satellite-based instruments peered down into the atmosphere, providing even larger geographical coverage. The overall campaign was complemented by meteorological forecasting and numerical simulations, satellite observations and surface networks. Together, these research observations have provided the most comprehensive characterization of the MCMA's urban and regional atmospheric composition and chemistry that will take years to analyze and evaluate fully. In this paper we review over 120 papers resulting from the MILAGRO/INTEX-B Campaign that have been published or submitted, as well as relevant papers from the earlier MCMA-2003 Campaign, with the aim of providing a road map for the scientific community interested in understanding the emissions from a megacity such as the MCMA and their impacts on air quality and climate. This paper describes the measurements performed during MILAGRO and the results obtained on MCMA's atmospheric meteorology and dynamics, emissions of gases and fine particles, sources and concentrations of volatile organic compounds, urban and regional photochemistry, ambient particulate matter, aerosol radiative properties, urban plume characterization, and health studies. A summary of key findings from the field study is presented.