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Aerosol hygroscopicity plays a vital role in aerosol radiative forcing. One key parameter describing hygroscopicity is the scattering enhancement factor, f (RH), defined as the ratio of the scattering coefficient at humidified relative humidity (RH) to its dry value. Here, we utilize the f (80 %) from ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) 2016 and 2018 airborne measurements to investigate the hygroscopicity of aerosols, its vertical distribution, its relationship with chemical composition, and its sensitivity to organic aerosol (OA) hygroscopicity over the southeast Atlantic (SEA) Ocean during the biomass burning (BB) season. We found that aerosol hygroscopicity remains steady above 2 km, with a mean f (80 %) of 1.40 ± 0.17. Below 2 km, aerosol hygroscopicity increases with decreasing altitude, with a mean f (80 %) of 1.51 ± 0.22, consistent with higher values of BB aerosol hygroscopicity found in the literature. The hygroscopicity parameter of OA (κOA) is retrieved from the Mie model with a mean value of 0.11 ± 0.08, which is in the middle to upper range compared to the literature. Higher OA hygroscopicity is related to aerosols that are more aged, oxidized, and present at lower altitudes. The enhanced biomass burning aerosol (BBA) hygroscopicity at lower altitudes is mainly due to a lower OA fraction, increased sulfate fraction, and greater κOA at lower altitudes. We propose a parameterization that quantifies f (RH) with chemical composition and κOA based on Mie simulation of internally mixed OA–(NH4)2SO4–BC mixtures. The good agreement between the predictions and the ORACLES measurements implies that the aerosols in the SEA during the BB season can be largely represented by the OA–(NH4)2SO4–BC internal mixture with respect to the f (RH) prediction. The sensitivity of f (RH) to κOA indicates that applying a constant κOA is only suitable when the OA fraction is low and κOA shows limited variation. However, in situations deviating these two criteria, κOA can notably impact scattering coefficients and aerosol radiative effect; therefore, accounting for κOA variability is recommended. [ABSTRACT FROM AUTHOR]

Light‐absorbing carbonaceous aerosols that dominate atmospheric aerosol warming over India remain poorly characterized. Here, we delve into UV‐visible‐IR spectral aerosol absorption properties at nine PAN‐India COALESCE network sites (Venkataraman et al., 2020, https://doi.org/10.1175/bams‐d‐19‐0030.1). Absorption properties were estimated from aerosol‐laden polytetrafluoroethylene filters using a well‐constrained technique incorporating filter‐to‐particle correction factors. The measurements revealed spatiotemporal heterogeneity in spectral intrinsic and extrinsic absorption properties. Absorption analysis at near‐UV wavelengths from carbonaceous aerosols at these regional sites revealed large near‐ultraviolet brown carbon absorption contributions from 21% to 68%—emphasizing the need to include these particles in climate models. Further, satellite‐retrieved column‐integrated absorption was dominated by surface absorption, which opens possibilities of using satellite measurements to model surface‐layer optical properties (limited to specific sites) at a higher spatial resolution. Both the satellite‐modeled and direct in‐situ absorption measurements can aid in validating and constraining climate modeling efforts that suffer from absorption underestimations and high uncertainties in radiative forcing estimates. Plain Language Summary: Particulate pollution in the atmosphere scatter and absorb incoming solar energy, thus cooling or warming Earth's atmosphere. In developing countries and especially in India, one of the most polluted regions of the world, the extent to which particles can absorb solar energy and warm the atmosphere is not well understood. Here, for the first time, we measure particle absorption simultaneously at nine ground sites across India, in diverse geographical regions with different levels and types of particulate pollution. We find that organic carbon particles exert large absorption at near‐ultraviolet wavelengths, which contain significant solar energy. These light absorbing organic carbon particles, called brown carbon, are emitted in large quantities from biomass burning (e.g., burning crop residue and cooking on wood‐fired stoves). Comparing ground measurements of absorption with satellite‐retrieved measurements that are representative of the entire atmospheric column, we find that near‐surface atmospheric particles can exert significant warming. This study highlights the need to improve climate model simulations of particulate pollution's impact on the climate by incorporating spatiotemporal surface‐level absorption measurements, including absorption by brown carbon particles. Key Points: Measurements at nine regional PAN‐India sites reveal several regions with large aerosol absorption strengthBrown carbon contributes significantly (21%–68%) to near‐ultraviolet absorption, indicating its importance in shortwave light absorptionStrong correlations observed between satellite data and surface absorption indicate future potential in modeling surface absorption [ABSTRACT FROM AUTHOR]

In order to improve aerosol representation in the NASA Goddard Earth Observing System (GEOS) model, we evaluated simulations of the transport and properties of aerosols from southern African biomass burning sources that were observed during the first deployment of the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) field campaign in September 2016. An example case study of 24 September was analyzed in detail, during which aircraft-based in situ and remote sensing observations showed the presence of a multi-layered smoke plume structure with significant vertical variation in single scattering albedo (SSA). Our baseline GEOS simulations were not able to represent the observed SSA variation or the observed organic aerosol-to-black-carbon ratio (OA : BC). Analyzing the simulated smoke age suggests that the higher-altitude, less absorbing smoke plume was younger (∼4 d), while the lower-altitude and more absorbing smoke plume was older (∼7 d). We hypothesize a chemical or microphysical loss process exists to explain the change in aerosol absorption as the smoke plume ages, and we apply a simple loss rate to the model hydrophilic biomass burning OA to simulate this process. We also utilized the ORACLES airborne observations to better constrain the simulation of aerosol optical properties, adjusting the assumed particle size, hygroscopic growth, and absorption. Our final GEOS model simulation with additional OA loss and updated optics showed better performance in simulating aerosol optical depth (AOD) and SSA compared to independent ground- and space-based retrievals for the entire month of September 2016, including the Ozone Monitoring Instrument (OMI) Aerosol Index. In terms of radiative implications of our model adjustments, the final GEOS simulation suggested a decreased atmospheric warming of about 10 % (∼2 W m -2) over the southeastern Atlantic region and above the stratocumulus cloud decks compared to the model baseline simulations. These results improve the representation of the smoke age, transport, and optical properties in Earth system models. [ABSTRACT FROM AUTHOR]

The vertical distribution of biomass burning aerosol (BBA) is important in regulating their impacts on weather and climate. The plume‐rise process affects the injection height of BBA and interacts with the air parcel lifting and cloud processes. However, these processes are not represented in most global climate models. In this study, we replaced the fixed vertical profiles of monthly BBA emissions in the Department of Energy's Energy Exascale Earth System Model version 1 (E3SMv1) with an interactive fire plume‐rise model. The vertical distribution of BBA emissions was calculated as a function of ambient thermodynamic conditions from the host E3SMv1, with distributions of fire sizes and sensible heat fluxes derived from the observations. The maximum fire radiative power (FRP) technique was used to determine the fire size. Scaling‐FRP technique is used to calculate the wildfire heat release. Daily BBA emission, superimposed with a fire diurnal cycle retrieved from the satellite observation, was included in model simulations. The model shows improved agreement with satellite retrievals and in situ measurement during the National Oceanic and Atmospheric Administration Wildfire Experiment for Cloud chemistry, Aerosol absorption, and Nitrogen campaign. The model‐observation comparison demonstrates the importance of the plume‐rise model and fire diurnal cycle assumption in determining the BBA fields. We also find that E3SMv1 with new features produces a larger carbonaceous aerosol burden, leading to 0.13 W m−2 warming at the top of atmosphere compared to the default E3SMv1. This highlights the importance of accurately representing the BBA injection height and indicates a no‐linear nature in the BBA‐induced radiative effect. Plain Language Summary: In this study, we replaced fixed vertical profiles of biomass burning aerosols (BBA) used in the default doe's Energy Exascale Earth System Model version 1 (E3SMv1) with an interactive fire plume‐rise model and fire diurnal cycle assumption. The BBA vertical profiles predicted by the model with the new features are in better agreement with the satellite observations and in situ aircraft observations compared to the default version. In addition, the inclusion of the plume‐rise model and fire diurnal assumption also lead to a warming effect as strong as 0.13 W m−2. Key Points: We incorporate an interactive fire plume‐rise model and fire diurnal cycle in the Energy Exascale Earth System Model version 1 (E3SMv1)The new features in E3SMv1 generate biomass burning aerosol vertical profiles that agree better with the observations than the default onesThe E3SMv1 with plume‐rise model and fire diurnal cycle causes a 0.13 W m−2 warming effect compared to the default one [ABSTRACT FROM AUTHOR]

As criteria pollutants from anthropogenic emissions have declined in the US in the last 2 decades, biomass burning (BB) emissions are becoming more important for urban air quality. Tracking the transported BB emissions and their impacts is challenging, especially in areas that are also burdened by anthropogenic sources like the Texas Gulf Coast. During the Corpus Christi and San Antonio (CCSA) field campaign in spring 2021, two long-range-transport BB events (BB1 and BB2) were identified. The observed patterns of an absorption Ångström exponent (AAE), a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) BB tracer (f60), equivalent black carbon (eBC), acetonitrile and carbon monoxide (CO) during BB1 and BB2 indicated differences in the mixing of transported BB plumes with local anthropogenic sources. The combined information from HYSPLIT backward-trajectory (BT) and satellite observations revealed that BB1 had mixed influence of transported smoke plumes from fires in central Mexico, the Yucatán Peninsula and the central US, whereas BB2 was influenced by fires in the central US. The estimated transport times of smoke from the Mexican fires and the central US fires to our study site were not too different (48–54 and 24–36 h, respectively), and both events appeared to have undergone similar levels of atmospheric processing, as evident in the elemental ratios of bulk organic aerosol (OA). We observed an aging trend for f44 vs. f60 and f44 vs. f43 as a function of time during BB2 but not during BB1. Positive matrix factorization (PMF) analysis of OA showed that BB1 had a mixture of organics from aged BB emissions with an anthropogenic marine signal, while the oxidized organic compounds from aged BB emissions dominated the aerosols during BB2. The size distribution of aerosol composition revealed distinct characteristics between BB1 and BB2, where BB1 was found to be externally mixed, exhibiting a combination of BB and anthropogenic marine aerosols. On the other hand, BB2 exhibited internal mixing dominated by aged BB aerosol. Our analysis from mobile and stationary measurements highlights that both CO and acetonitrile are likely impacted by local sources even during the BB events and specifically that acetonitrile cannot be used as a unique BB tracer for dilute BB plumes in an industrially influenced location. A suitable volatile organic compound (VOC) tracer would need to be emitted in high concentrations during BB, resistant to degradation during transport, unique to BB and able to be measured in the field. This study effectively demonstrates that AAE and aerosol BB tracers served as precise and effective tracers in these complex emission scenarios. Network deployment of multiwavelength photometers holds promise for enhancing our understanding of BB impacts on air quality and supporting informed decision-making for effective mitigation strategies in locations with mixed sources and influence of dilute BB plumes. To demonstrate the relevance of such an aerosol optical network, we provide evidence of the potential regional impacts of these transported BB events on urban O3 levels using measurements from the surface air quality monitoring network in Texas. [ABSTRACT FROM AUTHOR]

For the observation of the global three-dimensional distribution of aerosol composition and the evaluation of the shortwave direct radiative effect (SDRE) by aerosols, we developed a retrieval algorithm that uses observation data from the Cloud–Aerosol Lidar with Orthogonal Polarization (CALIOP) on board the Cloud–Aerosol Lidar Infrared Pathfinder Satellite Observations (CALIPSO) satellite and the Moderate Resolution Imaging Spectroradiometer (MODIS) on board Aqua. The CALIOP–MODIS retrieval optimizes the aerosol composition to both the CALIOP and MODIS observations in the daytime. Aerosols were assumed to be composed of four aerosol components: water-soluble (WS), light-absorbing (LA), dust (DS), and sea salt (SS) particles. The outputs of the CALIOP–MODIS retrieval are the vertical profiles of the extinction coefficient (αa), single-scattering albedo (ω0), asymmetry factor (g) of total aerosols (WS + LA + DS + SS), and αa of WS, LA, DS, and SS. Daytime observations of CALIOP and MODIS in 2010 were analyzed by the CALIOP–MODIS retrieval. The global means of the aerosol optical depth (τa) at 532 nm were 0.147±0.148 for total aerosols, 0.072±0.085 for WS, 0.027±0.035 for LA, 0.025±0.054 for DS, and 0.023±0.020 for SS. τa of the CALIOP–MODIS retrieval was between those of the CALIPSO and MODIS standard products and was close to the MODIS standard product. The global means of ω0 and g were 0.940±0.038 and 0.718±0.037 ; these values are in the range of those reported by previous studies. The horizontal distribution of each aerosol component was reasonable; for example, DS was large in desert regions, and LA was large in the major regions of biomass burning and anthropogenic aerosol emissions. The values of τa , ω0 , g , and fine and coarse median radii of the CALIOP–MODIS retrieval were compared with those of the AERONET products. τa at 532 and 1064 nm of the CALIOP–MODIS retrieval agreed well with the AERONET products. The ω0 , g , and fine and coarse median radii of the CALIOP–MODIS retrieval were not far from those of the AERONET products, but the variations were large, and the coefficients of determination for linear regression between them were small. In the retrieval results for 2010, the clear-sky SDRE values for total aerosols at the top and bottom of the atmosphere were -4.99±3.42 and -13.10±9.93 W m -2 , respectively, and the impact of total aerosols on the heating rate was from 0.0 to 0.5 K d -1. These results are generally similar to those of previous studies, but the SDRE at the bottom of the atmosphere is larger than that reported previously. Consequently, comparison with previous studies showed that the CALIOP–MODIS retrieval results were reasonable with respect to aerosol composition, optical properties, and the SDRE. [ABSTRACT FROM AUTHOR]

A large part of the uncertainty in climate projections comes from poorly understood or constrained aerosol properties (e.g., particle size, composition, mixing state, aging processes) and aerosol-cloud interactions, as well as the difficulty in remotely sensing them. This is an issue especially in remote regions such as the southeast Atlantic, which exhibits large model spread due to the seasonal coexistence of extensive cloud cover and regional biomass burning smoke. Here we address these gaps by comparing the WRF-CAM5 model to multi-campaign observations (ORACLES, CLARIFY, and LASIC) of the southeastern Atlantic region in August 2017 to evaluate a broad swath of the model's aerosol properties, processes, and transport, and the degree to which aerosol interactions with clouds are captured. Building on earlier work showing strong performance in model advection and mixing, we find that biomass-burning smoke aerosol size and composition are generally well-captured in the marine free troposphere, except for a likely overprediction of dust in the accumulation mode (7–17 % modeled dust fraction which is not present in the observations). Evaluating smoke aging trends, the model shows a steady increase in aerosol mean diameter and an unchanging composition as smoke ages, deviating from the observed trends that show a rise and subsequent fall in mean diameter over 4–12 days and a decreasing OA : BC ratio beyond 3 days. Both results are likely due to missing processes in the model that remove OA from the particle phase such as photolysis and heterogeneous aerosol chemistry. The observed composition change from the free-troposphere to the marine boundary layer (MBL) is not fully captured in the model, especially the observed enhancement of sulfate from 11 % to 37 % by mean mass fraction in ORACLES, and from 11 % to 26 % in CLARIFY. This points to the importance of properly representing sulfate formation from marine dimethyl sulfide (DMS) emissions and in smoke-free parcels. Additionally, the model does not capture the occurrence of an Aitken mode during clean and medium-smoke conditions in the boundary layer, likely pointing to misrepresentation of new particle formation. The model shows a persistent overprediction of aerosols in the MBL, especially for clean conditions, that multiple pieces of evidence link to weaker aerosol removal in the modeled MBL than reality. This evidence includes the model not representing observed shifts in the aerosol size distribution towards smaller sizes, the model not capturing the relative concentrations of carbon monoxide compared to black carbon, model underprediction of heavy rain events, and little evidence of persistent biases in modeled entrainment. Average below-cloud aerosol activation fraction (NCLD/NAER) remains relatively constant in WRF-CAM5 between field campaigns (~0.65), while it decreases substantially in observations from ORACLES (~0.78) to CLARIFY (~0.5), which could be due to the model misrepresentation of clean aerosol conditions. WRF-CAM5 also overshoots an observed upper limit on liquid cloud droplet concentration around NCLD=400–500 cm-3 observed in both ORACLES and CLARIFY and also overpredicts the spread in NCLD. This could be related to the model often drastically overestimating the strength of boundary layer vertical turbulence by up to a factor of 10 and having a bimodal—rather than the observed unimodal—probability distribution of updraft turbulent kinetic energy. We expect these results to motivate similar evaluations of other modeling systems and promote model development in these critical areas to reduce uncertainties in climate simulations. [ABSTRACT FROM AUTHOR]

Aerosol over the remote southeastern Atlantic is some of the most sunlight-absorbing aerosol on the planet: the in situ free-tropospheric single-scattering albedo at the 530 nm wavelength (SSA 530nm) ranges from 0.83 to 0.89 within ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) aircraft flights from late August–September. Here we seek to explain the low SSA. The SSA depends strongly on the black carbon (BC) number fraction, which ranges from 0.15 to 0.4. Low organic aerosol (OA)-to-BC mass ratios of 8–14 and modified combustion efficiency values >0.975 point indirectly to the dry, flame-efficient combustion of primarily grass fuels, with back trajectories ending in the miombo woodlands of Angola. The youngest aerosol, aged 4–5 d since emission, occupied the top half of a 5 km thick plume sampled directly west of Angola with a vertically consistent BC:ΔCO (carbon monoxide) ratio, indicating a homogenization of the source emissions. The younger aerosol, transported more quickly off of the continent by stronger winds, overlaid older, slower-moving aerosol with a larger mean particle size and fraction of BC-containing particles. This is consistent with ongoing gas condensation and the coagulation of smaller non-BC particles upon the BC-containing particles. The particle volumes and OA:BC mass ratios of the older aerosol were smaller, attributed primarily to evaporation following fragmentation, instead of dilution or thermodynamics. The CLARIFY (CLoud–Aerosol–Radiation Interaction and Forcing: Year 2017) aircraft campaign sampled aerosols that had traveled further to reach the more remote Ascension Island. CLARIFY reported higher BC number fractions, lower OA:BC mass ratios, and lower SSA yet larger mass absorption coefficients compared to this study's. Values from one ORACLES 2017 flight, held midway to Ascension Island, are intermediate, confirming the long-range changes. Overall the data are most consistent with continuing oxidation through fragmentation releasing aerosols that subsequently enter the gas phase, reducing the OA mass, rather than evaporation through dilution or thermodynamics. The data support the following best fit: SSA 530nm=0.801+0055⋅(OA:BC) (r=0.84). The fires of southern Africa emit approximately one-third of the world's carbon; the emitted aerosols are distinct from other regional smoke emissions, and their composition needs to be represented appropriately to realistically depict regional aerosol radiative effects. [ABSTRACT FROM AUTHOR]

The eastern North Atlantic (ENA) is a region dominated by pristine marine environment and subtropical marine boundary layer clouds. Under unperturbed atmospheric conditions, the regional aerosol regime in the ENA varies seasonally due to different seasonal surface-ocean biogenic emissions, removal processes, and meteorological regimes. However, during periods when the marine boundary layer aerosol in the ENA is impacted by particles transported from continental sources, aerosol properties within the marine boundary layer change significantly, affecting the concentration of cloud condensation nuclei (CCN). Here, we investigate the impact of long-range transported continental aerosol on the regional aerosol regime in the ENA using data collected at the U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) user facility on Graciosa Island in 2017 during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) campaign. We develop an algorithm that integrates number concentrations of particles with optical particle dry diameter (Dp) between 100 and 1000 nm, single scattering albedo, and black carbon concentration to identify multiday events (with duration >24 consecutive hours) of long-range continental aerosol transport in the ENA. In 2017, we detected nine multiday events of long-range transported particles that correspond to ∼ 7.5 % of the year. For each event, we perform HYSPLIT 10 d backward trajectories analysis, and we evaluate CALIPSO aerosol products to assess, respectively, the origins and compositions of aerosol particles arriving at the ENA site. Subsequently, we group the events into three categories, (1) mixture of dust and marine aerosols, (2) mixture of marine and polluted continental aerosols from industrialized areas, and (3) biomass burning aerosol from North America and Canada, and we evaluate their influence on aerosol population and cloud condensation nuclei in terms of potential activation fraction and concentrations at supersaturation of 0.1 % and 0.2 %. The arrival of plumes dominated by the mixture of dust and marine aerosol in the ENA in the winter caused significant increases in baseline Ntot. Simultaneously, the baseline particle size modes and CCN potential activation fraction remained almost unvaried, while cloud condensation nuclei concentrations increased proportionally to Ntot. Events dominated by a mixture of marine and polluted continental aerosols in spring, fall, and winter led to a statistically significant increase in baseline Ntot , a shift towards larger particular sizes, a higher CCN potential activation fractions, and cloud condensation nuclei concentrations of >170 % and up to 240 % higher than during baseline regime. Finally, the transported aerosol plumes characterized by elevated concentration of biomass burning aerosol from continental wildfires detected in the summertime did not statistically contribute to increase baseline aerosol particle concentrations in the ENA. However, particle diameters were larger than under baseline conditions, and CCN potential activation fractions were >75 % higher. Consequentially, cloud concentration nuclei concentrations increased by ∼ 115 % during the period affected by the biomass burning events. Our results suggest that, through the year, multiday events of long-range continental aerosol transport periodically affect the ENA and represent a significant source of CCN in the marine boundary layer. Based on our analysis, in 2017, the multiday aerosol plume transport dominated by a mixture of dust and marine aerosol, a mixture of marine and polluted continental aerosols, and biomass burning aerosols caused increases in the NCCN baseline regime of, respectively, 6.6 %, 8 %, and 7.4 % at SS 0.1 % (and, respectively, 6.5 %, 8.2 %, and 7.3 % at SS 0.2 %) in the ENA. [ABSTRACT FROM AUTHOR]

Biomass burning (BB) aerosols exert a strong surface cooling effect over the southeast Atlantic (SEA) via aerosol‐radiation and aerosol‐cloud interactions. The reduction of the sea surface temperature (SST) can trigger the SST‐low cloud feedback. Whether this feedback can amplify the surface cooling effect is examined. The modeling results from the Community Earth System Model version 2 (CESM2) demonstrate that counterintuitively the cloud radiative effect (CRE) caused by the BB aerosols is weaker if SST‐low cloud feedback is considered compared to fixed‐SST simulation (−2.99 W m−2 vs. −4.79 W m−2). This is caused by (a) stronger sea breeze due to larger sea‐land temperature contrast causing less smoke transport over SEA and (b) less moisture supply from surface due to colder SST. Changes in SST also lead to counterclockwise rotation of ocean circulation anomalies. Consequently, the excess heat transport from the equator reverses the direction of SST‐cloud feedback in this region. Plain Language Summary: Biomass burning aerosols can modulate the cloud macro‐ and microphysical properties over the Southeast Atlantic and induce a strong cooling effect at the surface. As a result, sea surface temperature will decrease, which can further promote cloudiness in this region (a positive SST‐low cloud feedback). Our study demonstrates that the cooling effect caused by biomass burning aerosols is actually smaller when the SST‐low cloud feedback is considered, because of stronger sea breeze that reduces the transport of biomass burning aerosols and weaker surface moisture supply. In addition, the ocean current changes can determine the direction of this SST‐low cloud feedback. Key Points: Sea surface temperature‐low cloud feedback reduces the magnitude of the cloud radiative effect (CRE) caused by the BB aerosols over Southeast AtlanticWeaker CRE is due to stronger sea breeze and less moisture supply from the oceanThe excess heat transport associated with counterclockwise rotation of ocean circulation anomalies stops the amplification of CRE [ABSTRACT FROM AUTHOR]

We characterize the aerosol physical and optical properties of 13 transported biomass burning (BB) events. BB events included long-range influence from fires in Alaskan and Siberian boreal forests transported to Mt. Bachelor Observatory (MBO) in the free troposphere (FT) over 8– 14+ d and regional wildfires in northern California and southwestern Oregon transported to MBO in the boundary layer (BL) over 10 h to 3 d. Intensive aerosol optical properties and normalized enhancement ratios for BB events were derived from measured aerosol light scattering coefficients (σscat), aerosol light-absorbing coefficients (σabs), fine particulate matter (PM 1), and carbon monoxide (CO) measurements made from July to September 2019, with particle size distribution collected from August to September. The observations showed that the Siberian BB events had a lower scattering Ångström exponent (SAE), a higher mass scattering efficiency (MSE; Δσscat/ΔPM1), and a bimodal aerosol size distribution with a higher geometric mean diameter (Dg). We hypothesize that the larger particles and associated scattering properties were due to the transport of fine dust alongside smoke in addition to contributions from condensation of secondary aerosol, coagulation of smaller particles, and aqueous-phase processing during transport. Alaskan and Siberian boreal forest BB plumes were transported long distances in the FT and characterized by lower absorption Ångström exponent (AAE) values indicative of black carbon (BC) dominance in the radiative budget. Significantly elevated AAE values were only observed for BB events with <1 d transport, which suggests strong production of brown carbon (BrC) in these plumes but limited radiative forcing impacts outside of the immediate region. [ABSTRACT FROM AUTHOR]

The sub-micron (SM) aerosol optical depth (AOD) is an optical separation based on the fraction of particles below a specified cutoff radius of the particle size distribution (PSD) at a given particle radius. It is fundamentally different from spectrally separated FM (fine-mode) AOD. We present a simple (AOD-normalized) SM fraction versus FM fraction (SMF vs. FMF) linear equation that explains the well-recognized empirical result of SMF generally being greater than the FMF. The AERONET inversion (AERinv) products (combined inputs of spectral AOD and sky radiance) and the spectral deconvolution algorithm (SDA) products (input of AOD spectra) enable, respectively, an empirical SMF vs. FMF comparison at similar (columnar) remote sensing scales across a variety of aerosol types. SMF (AERinv-derived) vs. FMF (SDA-derived) behavior is primarily dependent on the relative truncated portion (εc) of the coarse-mode (CM) AOD associated with the cutoff portion of the CM PSD and, to a second order, the cutoff FM PSD and FM AOD (εf). The SMF vs. FMF equation largely explains the SMF vs. FMF behavior of the AERinv vs. SDA products as a function of PSD cutoff radius ("inflection point") across an ensemble of AERONET sites and aerosol types (urban-industrial, biomass burning, dust, maritime and a mixed class of Arctic aerosols). The overarching dynamic was that the linear SMF vs. FMF relation pivots clockwise about the approximate (SMF, FMF) singularity of (1, 1) in a "linearly inverse" fashion (slope and intercept of approximately 1-εc and εc) with increasing cutoff radius. SMF vs. FMF slopes and intercepts derived from AERinv and SDA retrievals confirmed the general domination of εc over εf in controlling that dynamic. A more general conclusion is the apparent confirmation that the optical impact of truncating modal (whole) PSD features can be detected by an SMF vs. FMF analysis. [ABSTRACT FROM AUTHOR]

The NOAA/NASA Fire Influence on Regional to Global Environments and Air Quality (FIREX‐AQ) experiment was a multi‐agency, inter‐disciplinary research effort to: (a) obtain detailed measurements of trace gas and aerosol emissions from wildfires and prescribed fires using aircraft, satellites and ground‐based instruments, (b) make extensive suborbital remote sensing measurements of fire dynamics, (c) assess local, regional, and global modeling of fires, and (d) strengthen connections to observables on the ground such as fuels and fuel consumption and satellite products such as burned area and fire radiative power. From Boise, ID western wildfires were studied with the NASA DC‐8 and two NOAA Twin Otter aircraft. The high‐altitude NASA ER‐2 was deployed from Palmdale, CA to observe some of these fires in conjunction with satellite overpasses and the other aircraft. Further research was conducted on three mobile laboratories and ground sites, and 17 different modeling forecast and analyses products for fire, fuels and air quality and climate implications. From Salina, KS the DC‐8 investigated 87 smaller fires in the Southeast with remote and in‐situ data collection. Sampling by all platforms was designed to measure emissions of trace gases and aerosols with multiple transects to capture the chemical transformation of these emissions and perform remote sensing observations of fire and smoke plumes under day and night conditions. The emissions were linked to fuels consumed and fire radiative power using orbital and suborbital remote sensing observations collected during overflights of the fires and smoke plumes and ground sampling of fuels. Plain Language Summary: The NOAA/NASA Fire Influence on Regional to Global Environments and Air Quality (FIREX‐AQ) experiment was aimed at understanding how fuel and fire conditions at the point of emission influence the chemistry of smoke, what conditions and processes control the rise of smoke plumes, what happens to smoke as it is distributed in the atmosphere, and how chemical transformation of smoke impacts air quality, weather, and climate downwind. Lessons learned from FIREX‐AQ will also be used to assess and improve the effectiveness of satellites for estimating the emissions from wildfires and prescribed burns and to reduce uncertainties associated with modeling and forecasting of smoke. Here we present an overview of the FIREX‐AQ effort, its motivation and design, with detailed descriptions of the measurements and analyses carried out, their connections to FIREX‐AQ science goals, and the early findings of this exceptionally broad effort to understand fire and its many impacts on the atmosphere. Key Points: This work is an overview of the NOAA/NASA Fire Influence on Regional to Global Environments and Air Quality (FIREX‐AQ) field experimentFIREX‐AQ investigated biomass burning emissions and chemistry and smoke transportFIREX‐AQ was a multi‐platform mission that also utilized fire modeling and satellite detections and validation [ABSTRACT FROM AUTHOR]

Data are presented from intercomparisons between two research aircraft, the FAAM BAe-146 and the NASA Lockheed P3, and between the BAe-146 and the surface-based DOE (Department of Energy) ARM (Atmospheric Radiation Measurement) Mobile Facility at Ascension Island (8 ∘ S, 14.5 ∘ W; a remote island in the mid-Atlantic). These took place from 17 August to 5 September 2017, during the African biomass burning (BB) season. The primary motivation was to give confidence in the use of data from multiple platforms with which to evaluate numerical climate models. The three platforms were involved in the CLouds–Aerosol–Radiation Interaction and Forcing for Year 2017 (CLARIFY-2017), ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES), and Layered Atlantic Smoke and Interactions with Clouds (LASIC) field experiments. Comparisons from flight segments on 6 d where the BAe-146 flew alongside the ARM facility on Ascension Island are presented, along with comparisons from the wing-tip-to-wing-tip flight of the P3 and BAe-146 on 18 August 2017. The intercomparison flight sampled a relatively clean atmosphere overlying a moderately polluted boundary layer, while the six fly-bys of the ARM site sampled both clean and polluted conditions 2–4 km upwind. We compare and validate characterisations of aerosol physical, chemical and optical properties as well as atmospheric radiation and cloud microphysics between platforms. We assess the performance of measurement instrumentation in the field, under conditions where sampling conditions are not as tightly controlled as in laboratory measurements where calibrations are performed. Solar radiation measurements compared well enough to permit radiative closure studies. Optical absorption coefficient measurements from all three platforms were within uncertainty limits, although absolute magnitudes were too low (<10 Mm -1) to fully support a comparison of the absorption Ångström exponents. Aerosol optical absorption measurements from airborne platforms were more comparable than aircraft-to-ground observations. Scattering coefficient observations compared adequately between airborne platforms, but agreement with ground-based measurements was worse, potentially caused by small differences in sampling conditions or actual aerosol population differences over land. Chemical composition measurements followed a similar pattern, with better comparisons between the airborne platforms. Thermodynamics, aerosol and cloud microphysical properties generally agreed given uncertainties. [ABSTRACT FROM AUTHOR]

By analyzing observations and simulations from the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem), we investigated instant and delayed responses of large-scale atmospheric circulations and precipitation to biomass burning (BB) aerosols over the Indochina Peninsula (ICP) in the peak emission of March. The results show that the BB aerosols inhibit precipitation over the ICP in March and promote precipitation from early April to mid April. Specifically, the March BB aerosols over the ICP can induce mid- to lower-tropospheric heating and planetary boundary layer cooling to enhance local atmospheric stability; meanwhile, the perturbation heating can trigger an anomalous low in the lower troposphere to moisten the mid troposphere. However, the convection suppression due to the stabilized atmosphere dominates over the favorable water-vapor condition induced by large-scale circulation responses, leading to overall reduced precipitation over the ICP in March. For the delayed effect, the anomalous low can provide more water vapor as the monsoon advances in early April, although it becomes much weaker without BB aerosols' strong heating. On the other hand, the convective instability above 850 hPa is enhanced by more water vapor, resulting in enhanced precipitation over the ICP, northern South China Sea, and southern China. Thereafter, the condensational latent heating gradually takes over from the BB aerosol radiative heating, acting as the main driver for maintaining the anomalous circulation and thus the delayed effect in mid April. [ABSTRACT FROM AUTHOR]

Monitoring and modeling aerosol particle life cycle in Southeast Asia (SEA) is challenged by high cloud cover, complex meteorology, and the wide range of aerosol species, sources, and transformations found throughout the region. Satellite observations are limited, and there are few in situ observations of aerosol extinction profiles, aerosol properties, and environmental conditions. Therefore, accurate aerosol model outputs are crucial for the region. This work evaluates the Navy Aerosol Analysis and Prediction System Reanalysis (NAAPS-RA) aerosol optical thickness (AOT) and light extinction products using airborne aerosol and meteorological measurements from the Cloud, Aerosol, and Monsoon Processes Philippines Experiment (CAMP 2 Ex) conducted in 2019 during the SEA southwest monsoon biomass burning season. Modeled AOTs and extinction coefficients are compared to those retrieved with a high spectral resolution lidar (HSRL-2). Agreement between simulated and retrieved AOT (R2= 0.78, relative bias =- 5 %, normalized root mean square error (NRMSE) = 48 %) and aerosol extinction coefficients (R2= 0.80, 0.81, and 0.42; relative bias = 3 %, -6 %, and -7 %; NRMSE = 47 %, 53 %, and 118 % for altitudes between 40–500, 500–1500, and >1500 m, respectively) is quite good considering the challenging environment and few opportunities for assimilations of AOT from satellites during the campaign. Modeled relative humidities (RHs) are negatively biased at all altitudes (absolute bias =-5 %, -8 %, and -3 % for altitudes <500 500–1500 and >1500 m, respectively), motivating interest in the role of RH errors in AOT and extinction simulations. Interestingly, NAAPS-RA AOT and extinction agreement with the HSRL-2 does not change significantly (i.e., NRMSE values do not all decrease) when RHs from dropsondes are substituted into the model, yet biases all move in a positive direction. Further exploration suggests changes in modeled extinction are more sensitive to the actual magnitude of both the extinction coefficients and the dropsonde RHs being substituted into the model as opposed to the absolute differences between simulated and measured RHs. Finally, four case studies examine how model errors in RH and the hygroscopic growth parameter, γ , affect simulations of extinction in the mixed layer (ML). We find NAAPS-RA overestimates the hygroscopicity of (i) smoke particles from biomass burning in the Maritime Continent (MC) and (ii) anthropogenic emissions transported from East Asia. This work mainly provides insight into the relationship between errors in modeled RH and simulations of AOT and extinction in a humid and tropical environment influenced by a myriad of meteorological conditions and particle types. These results can be interpreted and addressed by the modeling community as part of the effort to better understand, quantify, and forecast atmospheric conditions in SEA. [ABSTRACT FROM AUTHOR]

With the advent of spaceborne spectroradiometers in a geostationary constellation, measuring high spectral resolution ultraviolet–visible (UV-VIS) and selected near-/shortwave-infrared (NIR/SWIR) radiances can enable the probing of the life cycle of key atmospheric trace gases and aerosols at higher temporal resolutions over the globe. The UV-VIS measurements are important for retrieving several key trace gases (e.g., O 3 , SO 2 , NO 2 , and HCHO) and particularly for deriving aerosol characteristics (e.g., aerosol absorption and vertical profile). This study examines the merit of simultaneous retrievals of trace gases and aerosols using a ground-based spectroradiometer covering the UV-NIR to monitor their physicochemical processes and to obtain reliable aerosol information for various applications. During the 2019 pre-monsoon season over northern Thailand, we deployed a ground-based SMART–s (Spectral Measurements for Atmospheric Radiative Transfer–spectroradiometer) instrument, which is an extended-range Pandora with reliable radiometric calibration in the 330–820 nm range, to retrieve remotely sensed chemical and aerosol properties for the first time near biomass burning sources. The high spectral resolution (∼ 1.0 nm full width half maximum with ∼ 3.7 × oversampling) of sun and sky measurements from SMART–s provides several key trace gases (e.g., O 3 , NO 2 , and H 2 O) and aerosol properties covering the UV where significant light absorption occurs by the carbonaceous particles. During the measurement period, highly correlated total column amounts of NO 2 and aerosol optical thickness (τaer) retrieved from SMART–s (correlation coefficient, R=0.74) indicated their common emissions from biomass burning events. The SMART–s retrievals of the spectral single scattering albedo (ω0) of smoke aerosols showed an abrupt decrease in the UV, which is an important parameter dictating photochemical processes in the atmosphere. The values of ω0 and column precipitable water vapor (H 2 O) gradually increase with the mixing of biomass burning smoke particles and higher water vapor concentrations when approaching the monsoon season. The retrieved ω0 and weighted mean radius of fine-mode aerosols from SMART–s showed positive correlations with the H 2 O (R=0.81 for ω0 at 330 nm and 0.56 for the volume-weighted mean radius), whereas the real part of the refractive index of fine-mode aerosol (nf) showed negative correlations (R=-0.61 at 330 nm), which suggest that aerosol aging processes including hygroscopic growth (e.g., humidification and cloud processing) can be a major factor affecting the temporal trends of aerosol optical properties. Retrieved nf and ω0 were closer to those of the water droplet (i.e., nf of about 1.33 and ω0 of about 1.0) under lower amounts of NO 2 during the measurement period; considering that the NO 2 amounts in the smoke may indicate the aging of the plume after emission due to its short lifetime, the tendency is also consistent with active hygroscopic processes of the aerosols over this area. Retrieved UV aerosol properties from SMART–s generally support the assumed smoke aerosol models (i.e., the spectral shape of aerosol absorption) used in NASA's current satellite algorithms, and their spectral ω0 retrievals from ground and satellites showed good agreements (R = 0.73–0.79). However, temporal and spectral variabilities in the aerosol absorption properties in the UV emphasize the importance of a realistic optical model of aerosols for further improvements in satellite retrievals. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

The study presents a climatology of aerosol composition concentrations obtained by a recently developed algorithm approach, namely the Generalized Retrieval of Atmosphere and Surface Properties (GRASP)/Component. It is applied to the whole archive of observations from the POLarization and Directionality of the Earth's Reflectances (POLDER-3). The conceptual specifics of the GRASP/Component approach is in the direct retrieval of aerosol speciation (component fraction) without intermediate retrievals of aerosol optical characteristics. Although a global validation of the derived aerosol component product is challenging, the results obtained are in line with general knowledge about aerosol types in different regions. In addition, we compare the GRASP-derived black carbon (BC) and dust components with those of the Modern-Era Retrospective Analysis for Research and Applications, version 2 (MERRA-2) product. Quite a reasonable general agreement was found between the spatial and temporal distribution of the species provided by GRASP and MERRA-2. The differences, however, appeared in regions known for strong biomass burning and dust emissions; the reasons for the discrepancies are discussed. The other derived components, such as concentrations of absorbing (BC, brown carbon (BrC), iron-oxide content in mineral dust) and scattering (ammonium sulfate and nitrate, organic carbon, non-absorbing dust) aerosols, represent scarce but imperative information for validation and potential adjustment of chemical transport models. The aerosol optical properties (e.g., aerosol optical depth (AOD), Ångström exponent (AE), single-scattering albedo (SSA), fine- and coarse-mode aerosol optical depth (AODF AND AODC)) derived from GRASP/Component were found to agree well with the Aerosol Robotic Network (AERONET) ground reference data, and were fully consistent with the previous GRASP Optimized, High Precision (HP) and Models retrieval versions applied to POLDER-3 data. Thus, the presented extensive climatology product provides an opportunity for understanding variabilities and trends in global and regional distributions of aerosol species. The climatology of the aerosol components obtained in addition to the aerosol optical properties provides additional valuable, qualitatively new insight about aerosol distributions and, therefore, demonstrates advantages of multi-angular polarimetric (MAP) satellite observations as the next frontier for aerosol inversion from advanced satellite observations. The extensive satellite-based aerosol component dataset is expected to be useful for improving global aerosol emissions and component-resolved radiative forcing estimations. The GRASP/Component products are publicly available (https://www.grasp-open.com/products/ , last access: 15 March 2022) and the dataset used in the current study is registered under 10.5281/zenodo.6395384 (Li et al., 2022b). [ABSTRACT FROM AUTHOR]

From June to October, southern Africa produces one-third of the global biomass burning (BB) emissions by widespread fires. BB aerosols are transported westward over the south-eastern Atlantic with the mid-tropospheric winds, resulting in significant radiative effects. Ascension Island (ASI) is located midway between Africa and South America. From June 2016 to October 2017, a 17-month in situ observation campaign on ASI found a low single-scattering albedo (SSA) as well as a high mass absorption cross-section of black carbon (MAC BC), demonstrating the strong absorbing marine boundary layer in the south-eastern Atlantic. Here we investigate the monthly variations of critical optical properties of BB aerosols, i.e. SSA and MAC BC , during the BB seasons and the driving factors behind these variations. Both SSA and MAC BC increase from June to August and decrease in September and October. The average SSA during the BB seasons is 0.81 at 529 nm wavelength, with the highest mean ∼ 0.85 in October and the lowest ∼ 0.78 in August. The absorption enhancement (Eabs) derived from the MAC BC shows similar trends with SSA, with the average during the whole of the BB seasons at ∼ 1.96 and ∼ 2.07 in 2016 and 2017, respectively. As the Eabs is higher than the ∼ 1.5 commonly adopted value by climate models, this result suggests the marine boundary layer in the south-eastern Atlantic is more absorbing than model simulations. We find the enhanced ratio of BC to CO (ΔBC/ΔCO , equal to BC/ΔCO as the BC background concentration is considered to be 0) is well correlated with SSA and MAC BC , providing a simple way to estimate the aerosol optical characteristics in the south-eastern Atlantic. The exponential function we proposed can approximate SSA and MAC BC with BC/ΔCO , and when BC/ΔCO is small it can capture the rapid growth of SSA as BC/ΔCO decreases. BC/ΔCO is influenced by combustion conditions and aerosol scavenging. From the analysis of the location of BB, the primary source fuel, the water content in the fuel, combined with the mean cloud cover and precipitation in the transport areas of the BB plume, we conclude that the increase in BC/ΔCO from June to August is likely to be caused by burning becoming more flaming. The reduction in the water content of fuels may be responsible for the change in the burning conditions from June to August. The decrease in BC/ΔCO in September and October may be caused by two factors, one being a lower proportion of flaming conditions, possibly associated with a decrease in mean surface wind speed in the burning area, and the other being an increase in precipitation in the BB transport pathway, leading to enhanced aerosol scavenging, which ultimately results in an increase in SSA and MAC BC. [ABSTRACT FROM AUTHOR]

During the summer of 2018, the upward-pointing Wyoming Cloud Lidar (WCL) was deployed on board the University of Wyoming King Air (UWKA) research aircraft for the Biomass Burning Flux Measurements of Trace Gases and Aerosols (BB-FLUX) field campaign. This paper describes the generation of calibrated attenuated backscatter coefficients and aerosol extinction coefficients from the WCL measurements. The retrieved aerosol extinction coefficients at the flight level strongly correlate (correlation coefficient, rr > 0.8) with in situ aerosol concentration and carbon monoxide (CO) concentration, providing a first-order estimate for converting WCL extinction coefficients into vertically resolved CO and aerosol concentration within wildfire smoke plumes. The integrated CO column concentrations from the WCL data in nonextinguished profiles also correlate (rr = 0.7) with column measurements by the University of Colorado Airborne Solar Occultation Flux instrument, indicating the validity of WCL-derived extinction coefficients. During BB-FLUX, the UWKA sampled smoke plumes from more than 20 wildfires during 35 flights over the western United States. Seventy percent of flight time was spent below 3 km above ground level (AGL) altitude, although the UWKA ascended up to 6 km AGL to sample the top of some deep smoke plumes. The upward-pointing WCL observed a nearly equal amount of thin and dense smoke below 2 km and above 5 km due to the flight purpose of targeted fresh fire smoke. Between 2 and 5 km, where most of the wildfire smoke resided, the WCL observed slightly more thin smoke than dense smoke due to smoke spreading. Extinction coefficients in dense smoke were 2–10 times stronger, and dense smoke tended to have larger depolarization ratio, associated with irregular aerosol particles. [ABSTRACT FROM AUTHOR]

The Atlantic Tradewind Ocean‐Atmosphere Mesoscale Campaign (ATOMIC) took place from 7 January to 11 July 2020 in the tropical North Atlantic between the east coast of Barbados and the Northwest Tropical Atlantic Station (NTAS) mooring. Measurements of aerosol chemical, microphysical, optical, and cloud‐nucleating properties were made during boreal winter onboard the NOAA RV Ronald H. Brown from 7 January to 13 February 2020. Observed aerosol properties indicate there were distinct periods when the aerosol was typical of clean marine conditions (particle number concentrations <400 cm−3, light absorption levels <1 Mm−1, and 222Rn concentrations <500 mBq m−3) and when there were intrusions of dust mixed to varying degrees with biomass burning aerosol. In comparison to the long‐term dust record at the Barbados Atmospheric Chemistry Observatory, the fraction of samples collected during ATOMIC with dust concentrations greater than 20 μg m−3 exceeded all years of the Barbados January to February record with the exception of 1983. The degree of mixing of the dust with biomass burning aerosol was modulated by the location of the North Atlantic subtropical high. A high located to the west of Africa led to a more northerly transport route and more dust‐like (MDL) aerosol arriving at the ship. A location of the high further to the east over northern Africa led to a more southerly transport route and more biomass burning aerosol mixed with the dust. Properties for the marine, MDL, and mixed dust and biomass burning aerosol are presented. Key Points: The frequency of episodic dust events was higher during ATOMIC than normal for the Caribbean in January and FebruaryRelative amounts of dust and biomass burning aerosol were modulated by the location of the North Atlantic subtropical highCloud Condensation Nuclei concentrations were highest when dust was mixed with biomass [ABSTRACT FROM AUTHOR]

Black carbon aerosols are the second largest contributor to global warming while also being linked to respiratory and cardiovascular disease. These particles are generally found in smoke plumes originating from biomass burning and fossil fuel combustion. They are also heavily concentrated in smoke plumes originating from oil fires, exhibiting the largest ratio of black carbon to organic carbon. In this study, we identified and analysed oil smoke plumes derived from 30 major industrial events within a 12-year timeframe. To our knowledge, this is the first study of its kind that utilized a synergetic approach based on satellite remote sensing techniques. Satellite data offer access to these events, which, as seen in this study, are mainly located in war-prone or hazardous areas. This study focuses on the use of MODIS (Moderate Resolution Imaging Spectroradiometer) and CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations) products regarding these types of aerosol while also highlighting their intrinsic limitations. By using data from both MODIS instruments on board Terra and Aqua satellites, we addressed the temporal evolution of the smoke plume while assessing lidar-specific properties and plume elevation using CALIPSO data. The analysis method in this study was developed to better differentiate between oil smoke aerosols and the local atmospheric scene. We present several aerosol properties in the form of plume-specific averaged values. We believe that MODIS values are a conservative estimation of plume aerosol optical depth (AOD) since MODIS algorithms rely on general aerosol models and various atmospheric conditions within the look-up tables, which do not reflect the highly absorbing nature of these smoke plumes. Based on this study we conclude that the MODIS land algorithms are not yet suited for retrieving aerosol properties for these types of smoke plumes due to the strong absorbing properties of these aerosols. CALIPSO retrievals rely heavily on the type of lidar solutions showing discrepancy between constrained and unconstrained retrievals. Smoke plumes identified within a larger aerosol layer were treated as unconstrained retrievals and resulted in conservative AOD estimates. Conversely, smoke plumes surrounded by clear air were identified as opaque aerosol layers and resulted in higher lidar ratios and AOD values. Measured lidar ratios and particulate depolarization ratios showed values similar to the upper ranges of biomass burning smoke. Results agree with studies that utilized ground-based retrievals, in particular for Ångström exponent (AE) and effective radius (Reff) values. MODIS and CALIPSO retrieval algorithms disagree on AOD ranges, for the most part, due to the extreme light-absorbing nature of these types of aerosols. We believe that these types of studies are a strong indicator for the need of improved aerosol models and retrieval algorithms. [ABSTRACT FROM AUTHOR]

Biomass burning smoke is advected over the southeastern Atlantic Ocean between July and October of each year. This smoke plume overlies and mixes into a region of persistent low marine clouds. Model calculations of climate forcing by this plume vary significantly in both magnitude and sign. NASA EVS-2 (Earth Venture Suborbital-2) ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) had deployments for field campaigns off the west coast of Africa in 3 consecutive years (September 2016, August 2017, and October 2018) with the goal of better characterizing this plume as a function of the monthly evolution by measuring the parameters necessary to calculate the direct aerosol radiative effect. Here, this dataset and satellite retrievals of cloud properties are used to test the representation of the smoke plume and the underlying cloud layer in two regional models (WRF-CAM5 and CNRM-ALADIN) and two global models (GEOS and UM-UKCA). The focus is on the comparisons of those aerosol and cloud properties that are the primary determinants of the direct aerosol radiative effect and on the vertical distribution of the plume and its properties. The representativeness of the observations to monthly averages are tested for each field campaign, with the sampled mean aerosol light extinction generally found to be within 20 % of the monthly mean at plume altitudes. When compared to the observations, in all models, the simulated plume is too vertically diffuse and has smaller vertical gradients, and in two of the models (GEOS and UM-UKCA), the plume core is displaced lower than in the observations. Plume carbon monoxide, black carbon, and organic aerosol masses indicate underestimates in modeled plume concentrations, leading, in general, to underestimates in mid-visible aerosol extinction and optical depth. Biases in mid-visible single scatter albedo are both positive and negative across the models. Observed vertical gradients in single scatter albedo are not captured by the models, but the models do capture the coarse temporal evolution, correctly simulating higher values in October (2018) than in August (2017) and September (2016). Uncertainties in the measured absorption Ångstrom exponent were large but propagate into a negligible (<4 %) uncertainty in integrated solar absorption by the aerosol and, therefore, in the aerosol direct radiative effect. Model biases in cloud fraction, and, therefore, the scene albedo below the plume, vary significantly across the four models. The optical thickness of clouds is, on average, well simulated in the WRF-CAM5 and ALADIN models in the stratocumulus region and is underestimated in the GEOS model; UM-UKCA simulates cloud optical thickness that is significantly too high. Overall, the study demonstrates the utility of repeated, semi-random sampling across multiple years that can give insights into model biases and how these biases affect modeled climate forcing. The combined impact of these aerosol and cloud biases on the direct aerosol radiative effect (DARE) is estimated using a first-order approximation for a subset of five comparison grid boxes. A significant finding is that the observed grid box average aerosol and cloud properties yield a positive (warming) aerosol direct radiative effect for all five grid boxes, whereas DARE using the grid-box-averaged modeled properties ranges from much larger positive values to small, negative values. It is shown quantitatively how model biases can offset each other, so that model improvements that reduce biases in only one property (e.g., single scatter albedo but not cloud fraction) would lead to even greater biases in DARE. Across the models, biases in aerosol extinction and in cloud fraction and optical depth contribute the largest biases in DARE, with aerosol single scatter albedo also making a significant contribution. [ABSTRACT FROM AUTHOR]

Aerosol heating due to shortwave absorption has implications for local atmospheric stability and regional dynamics. The derivation of heating rate profiles from space-based observations is challenging because it requires the vertical profile of relevant properties such as the aerosol extinction coefficient and single-scattering albedo (SSA). In the southeastern Atlantic, this challenge is amplified by the presence of stratocumulus clouds below the biomass burning plume advected from Africa, since the cloud properties affect the magnitude of the aerosol heating aloft, which may in turn lead to changes in the cloud properties and life cycle. The combination of spaceborne lidar data with passive imagers shows promise for future derivations of heating rate profiles and curtains, but new algorithms require careful testing with data from aircraft experiments where measurements of radiation, aerosol, and cloud parameters are better colocated and readily available. In this study, we derive heating rate profiles and vertical cross sections (curtains) from aircraft measurements during the NASA ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) project in the southeastern Atlantic. Spectrally resolved irradiance measurements and the derived column absorption allow for the separation of total heating rates into aerosol and gas (primarily water vapor) absorption. The nine cases we analyzed capture some of the co-variability of heating rate profiles and their primary drivers, leading to the development of a new concept: the heating rate efficiency (HRE; the heating rate per unit aerosol extinction). HRE, which accounts for the overall aerosol loading as well as vertical distribution of the aerosol layer, varies little with altitude as opposed to the standard heating rate. The large case-to-case variability for ORACLES is significantly reduced after converting from heating rate to HRE, allowing us to quantify its dependence on SSA, cloud albedo, and solar zenith angle. [ABSTRACT FROM AUTHOR]

Aerosol absorption is a key property to assess the radiative impacts of aerosols on climate at both global and regional scales. The aerosol physico-chemical and optical properties remain not sufficiently constrained in climate models, with difficulties to properly represent both the aerosol load and their absorption properties in clear and cloudy scenes, especially for absorbing biomass burning aerosols (BBA). In this study we focus on biomass burning (BB) particle plumes transported above clouds over the southeast Atlantic (SEA) region off the southwest coast of Africa, in order to improve the representation of their physico-chemical and absorption properties. The methodology is based on aerosol regional numerical simulations from the WRF-Chem coupled meteorology–chemistry model combined with a detailed inventory of BB emissions and various sets of innovative aerosol remote sensing observations, both in clear and cloudy skies from the POLDER-3/PARASOL space sensor. Current literature indicates that some organic aerosol compounds (OC), called brown carbon (BrOC), primarily emitted by biomass combustion absorb the ultraviolet-blue radiation more efficiently than pure black carbon (BC). We exploit this specificity by comparing the spectral dependence of the aerosol single scattering albedo (SSA) derived from the POLDER-3 satellite observations in the 443–1020 nm wavelength range with the SSA simulated for different proportions of BC, OC and BrOC at the source level, considering the homogeneous internal mixing state of particles. These numerical simulation experiments are based on two main constraints: maintaining a realistic aerosol optical depth both in clear and above cloudy scenes and a realistic BC/OC mass ratio. Modelling experiments are presented and discussed to link the chemical composition with the absorption properties of BBA and to provide estimates of the relative proportions of black, organic and brown carbon in the African BBA plumes transported over the SEA region for July 2008. The absorbing fraction of organic aerosols in the BBA plumes, i.e. BrOC, is estimated at 2 % to 3 %. The simulated mean SSA are 0.81 (565 nm) and 0.84 (550 nm) in clear and above cloudy scenes respectively, in good agreement with those retrieved by POLDER-3 (0.85±0.05 at 565 nm in clear sky and at 550 nm above clouds) for the studied period. [ABSTRACT FROM AUTHOR]

In situ measurements of aerosol microphysical, chemical, and optical properties were made during global-scale flights from 2016–2018 as part of the Atmospheric Tomography Mission (ATom). The NASA DC-8 aircraft flew from ∼ 84 ∘ N to ∼ 86 ∘ S latitude over the Pacific, Atlantic, Arctic, and Southern oceans while profiling nearly continuously between altitudes of ∼ 160 m and ∼ 12 km. These global circuits were made once each season. Particle size distributions measured in the aircraft cabin at dry conditions and with an underwing probe at ambient conditions were combined with bulk and single-particle composition observations and measurements of water vapor, pressure, and temperature to estimate aerosol hygroscopicity and hygroscopic growth factors and calculate size distributions at ambient relative humidity. These reconstructed, composition-resolved ambient size distributions were used to estimate intensive and extensive aerosol properties, including single-scatter albedo, the asymmetry parameter, extinction, absorption, Ångström exponents, and aerosol optical depth (AOD) at several wavelengths, as well as cloud condensation nuclei (CCN) concentrations at fixed supersaturations and lognormal fits to four modes. Dry extinction and absorption were compared with direct in situ measurements, and AOD derived from the extinction profiles was compared with remotely sensed AOD measurements from the ground-based Aerosol Robotic Network (AERONET); this comparison showed no substantial bias. The purpose of this work is to describe the methodology by which ambient aerosol properties are estimated from the in situ measurements, provide statistical descriptions of the aerosol characteristics of different remote air mass types, examine the contributions to AOD from different aerosol types in different air masses, and provide an entry point to the ATom aerosol database. The contributions of different aerosol types (dust, sea salt, biomass burning, etc.) to AOD generally align with expectations based on location of the profiles relative to continental sources of aerosols, with sea salt and aerosol water dominating the column extinction in most remote environments and dust and biomass burning (BB) particles contributing substantially to AOD, especially downwind of the African continent. Contributions of dust and BB aerosols to AOD were also significant in the free troposphere over the North Pacific. Comparisons of lognormally fitted size distribution parameters to values in the Optical Properties of Aerosols and Clouds (OPAC) database commonly used in global models show significant differences in the mean diameters and standard deviations for accumulation-mode particles and coarse-mode dust. In contrast, comparisons of lognormal parameters derived from the ATom data with previously published shipborne measurements in the remote marine boundary layer show general agreement. The dataset resulting from this work can be used to improve global-scale representation of climate-relevant aerosol properties in remote air masses through comparison with output from global models and assumptions used in retrievals of aerosol properties from both ground-based and satellite remote sensing. [ABSTRACT FROM AUTHOR]

The Sierra Nevada Lidar aerOsol Profiling Experiment I and II (SLOPE I and II) campaigns were intended to determine the vertical structure of aerosols by remote sensing instruments and test the various retrieval schemes for obtaining aerosol microphysical and optical properties with in situ measurements. The SLOPE I and II campaigns were developed during the summers of 2016 and 2017, respectively, combining active and passive remote sensing with in situ measurements at stations belonging to the AGORA observatory (Andalusian Global ObseRvatory of the Atmosphere) in the Granada area (Spain). In this work, we use the in situ measurements of these campaigns to evaluate aerosol properties retrieved by the GRASP code (Generalized Retrieval of Atmosphere and Surface Properties) combining lidar and sun–sky photometer measurements. We show an overview of aerosol properties retrieved by GRASP during the SLOPE I and II campaigns. In addition, we evaluate the GRASP retrievals of total aerosol volume concentration (discerning between fine and coarse modes), extinction and scattering coefficients, and for the first time we present an evaluation of the absorption coefficient. The statistical analysis of aerosol optical and microphysical properties, both column-integrated and vertically resolved, from May to July 2016 and 2017 shows a large variability in aerosol load and types. The results show a strong predominance of desert dust particles due to North African intrusions. The vertically resolved analysis denotes a decay of the atmospheric aerosols with an altitude up to 5 km a.s.l. Finally, desert dust and biomass burning events were chosen to show the high potential of GRASP to retrieve vertical profiles of aerosol properties (e.g. absorption coefficient and single scattering albedo) for different aerosol types. The aerosol properties retrieved by GRASP show good agreement with simultaneous in situ measurements (nephelometer, aethalometer, scanning mobility particle sizer, and aerodynamic particle sizer) performed at the Sierra Nevada Station (SNS) in Granada. In general, GRASP overestimates the in situ data at the SNS with a mean difference lower than 6 µ m 3 cm -3 for volume concentration, and 11 and 2 Mm -1 for the scattering and absorption coefficients. On the other hand, the comparison of GRASP with airborne measurements also shows an overestimation with mean absolute differences of 14 ± 10 and 1.2 ± 1.2 Mm -1 for the scattering and absorption coefficients, showing a better agreement for the absorption (scattering) coefficient with higher (lower) aerosol optical depth. The potential of GRASP shown in this study will contribute to enhancing the representativeness of the aerosol vertical distribution and provide information for satellite and global model evaluation. [ABSTRACT FROM AUTHOR]

The southeast Atlantic has expansive aerosol plumes overlying clouds for a third of each year. Aerosol optical depths (AODs) were measured from the airborne Sun photometer and lidar during the 2016 NASA ObseRvations of Aerosols above CLouds and their intEractionS field campaign. We compare these measurements with one another and with collocated Moderate Resolution Imaging Spectroradiometer (MODIS) observations at native spatial resolutions using <15‐min and 3‐h temporal collocation criteria. We find better statistical relationships for the <15‐min temporal resolution, indicating that AODs in the southeast Atlantic commonly vary below three‐hourly temporal scales over MODIS spatial resolutions. We also use the airborne Solar Spectral Flux Radiometer (SSFR) to conduct the first comprehensive evaluation of attenuation‐corrected below‐aerosol cloud optical depths (CODs) from MODIS and the Spinning Enhanced Visible and Infrared Imager (SEVIRI). MODIS COD retrievals improve their agreement with the SSFR when accounting for overlying aerosol attenuation whereas SEVIRI CODs are mostly underestimated. Plain Language Summary: Aerosols are suspended particles in the atmosphere that affect the Earth's regional and global climate both by absorbing and scattering solar light and through their interaction with clouds. Hotspots of aerosols above clouds are present in some parts of the world, yet aerosol products from satellites are largely unavailable in cloudy conditions in part because of large uncertainties at estimating aerosol properties above bright backgrounds such as clouds. In 2016, two research aircraft from the National Aeronautics and Space Administration flew over the southeast Atlantic Ocean, a region with significant biomass burning aerosol (from agricultural fires) and a large oceanic cloud deck, to measure the properties of each. We use the aircraft data to evaluate satellite estimates of liquid cloud thicknesses and aerosol amounts above clouds. We then confirm that changes in aerosols and clouds over time affect the accuracy of satellite measurements. This information is crucial for refining satellite measurements and improving our understanding of how aerosols and clouds affect Earth's climate. Key Points: We conduct the first comprehensive spatiotemporal evaluation of satellite‐derived optical properties of clouds underlying absorbing aerosolsCloud optical depths from satellite retrievals agree better with aircraft data when accounting for overlying aerosol attenuationAerosol loadings in the southeast Atlantic commonly vary below three‐hourly temporal scales over the spatial scale of satellite retrievals [ABSTRACT FROM AUTHOR]

Marine stratocumulus cloud properties over the Southeast Atlantic Ocean are impacted by contact between above-cloud biomass burning aerosols and cloud tops. Different vertical separations (0 to 2000 m) between the aerosol layer and cloud tops were observed on six research flights in September 2016 during the NASA ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) field campaign. There were 30 contact profiles, where an aerosol layer with aerosol concentration (Na) > 500 cm-3 was within 100 m of cloud tops, and 41 separated profiles, where the aerosol layer with Na > 500 cm-3 was located more than 100 m above cloud tops. For contact profiles, the average cloud droplet concentration (Nc) in the cloud layer was up to 68 cm-3 higher, the effective radius (Re) up to 1.3 µm lower, and the liquid water content (LWC) within 0.01 gm-3 compared to separated profiles. Free-tropospheric humidity was higher in the presence of biomass burning aerosols, and contact profiles had a smaller decrease in humidity (and positive buoyancy) across cloud tops with higher median above-cloud Na (895 cm-3) compared to separated profiles (30 cm-3). Due to droplet evaporation from entrainment mixing of warm, dry free-tropospheric air into the clouds, the median Nc and LWC for contact profiles decreased with height by 21 and 9 % in the top 20 % of the cloud layer. The impact of droplet evaporation was stronger during separated profiles as a greater decrease in humidity (and negative buoyancy) across cloud tops led to greater decreases in median Nc (30 %) and LWC (16 %) near cloud tops. Below-cloud Na was sampled during 61 profiles, and most contact profiles (20 out of 28) were within high- Na (> 350 cm-3) boundary layers, while most separated profiles (22 out of 33) were within low- Na (< 350 cm-3) boundary layers. Although the differences in below-cloud Na were statistically insignificant, contact profiles within low- Na boundary layers had up to 34.9 cm-3 higher Nc compared to separated profiles. This is consistent with a weaker impact of droplet evaporation in the presence of biomass burning aerosols within 100 m above cloud tops. For contact profiles within high- Na boundary layers, the presence of biomass burning aerosols led to higher below-cloud Na (up to 70.5 cm-3) and additional droplet nucleation above the cloud base along with weaker droplet evaporation. Consequently, the contact profiles in high- Na boundary layers had up to 88.4 cm-3 higher Nc compared to separated profiles. These results motivate investigations of aerosol–cloud–precipitation interactions over the Southeast Atlantic since the changes in Nc and Re induced by the presence of above-cloud biomass burning aerosols are likely to impact precipitation rates, liquid water path, and cloud fraction, and modulate closed-to-open-cell transitions. [ABSTRACT FROM AUTHOR]

The tropical Northwest Pacific (TNWP) is a receptor for pollution sources throughout Asia and is highly susceptible to climate change, making it imperative to understand long-range transport in this complex aerosol-meteorological environment. Measurements from the NASA Cloud, Aerosol, and Monsoon Processes Philippines Experiment (CAMP 2 Ex; 24 August to 5 October 2019) and back trajectories from the National Oceanic and Atmospheric Administration Hybrid Single Particle Lagrangian Integrated Trajectory Model (HYSPLIT) were used to examine transport into the TNWP from the Maritime Continent (MC), peninsular Southeast Asia (PSEA), East Asia (EA), and the West Pacific (WP). A mid-campaign monsoon shift on 20 September 2019 led to distinct transport patterns between the southwest monsoon (SWM; before 20 September) and monsoon transition (MT; after 20 September). During the SWM, long-range transport was a function of southwesterly winds and cyclones over the South China Sea. Low- (high-) altitude air generally came from MC (PSEA), implying distinct aerosol processing related to convection and perhaps wind shear. The MT saw transport from EA and WP, driven by Pacific northeasterly winds, continental anticyclones, and cyclones over the East China Sea. Composition of transported air differed by emission source and accumulated precipitation along trajectories (APT). MC air was characterized by biomass burning tracers while major components of EA air pointed to Asian outflow and secondary formation. Convective scavenging of PSEA air was evidenced by considerable vertical differences between aerosol species but not trace gases, as well as notably higher APT and smaller particles than other regions. Finally, we observed a possible wet scavenging mechanism acting on MC air aloft that was not strictly linked to precipitation. These results are important for understanding the transport and processing of air masses with further implications for modeling aerosol lifecycles and guiding international policymaking to public health and climate, particularly during the SWM and MT. [ABSTRACT FROM AUTHOR]

The representations of clouds, aerosols, and cloud–aerosol–radiation impacts remain some of the largest uncertainties in climate change, limiting our ability to accurately reconstruct past climate and predict future climate. The south-east Atlantic is a region where high atmospheric aerosol loadings and semi-permanent stratocumulus clouds are co-located, providing an optimum region for studying the full range of aerosol–radiation and aerosol–cloud interactions and their perturbations of the Earth's radiation budget. While satellite measurements have provided some useful insights into aerosol–radiation and aerosol–cloud interactions over the region, these observations do not have the spatial and temporal resolution, nor the required level of precision to allow for a process-level assessment. Detailed measurements from high spatial and temporal resolution airborne atmospheric measurements in the region are very sparse, limiting their use in assessing the performance of aerosol modelling in numerical weather prediction and climate models. CLARIFY-2017 was a major consortium programme consisting of five principal UK universities with project partners from the UK Met Office and European- and USA-based universities and research centres involved in the complementary ORACLES, LASIC, and AEROCLO-sA projects. The aims of CLARIFY-2017 were fourfold: (1) to improve the representation and reduce uncertainty in model estimates of the direct, semi-direct, and indirect radiative effect of absorbing biomass burning aerosols; (2) to improve our knowledge and representation of the processes determining stratocumulus cloud microphysical and radiative properties and their transition to cumulus regimes; (3) to challenge, validate, and improve satellite retrievals of cloud and aerosol properties and their radiative impacts; (4) to improve the impacts of aerosols in weather and climate numerical models. This paper describes the modelling and measurement strategies central to the CLARIFY-2017 deployment of the FAAM BAe146 instrumented aircraft campaign, summarizes the flight objectives and flight patterns, and highlights some key results from our initial analyses. [ABSTRACT FROM AUTHOR]

The south-eastern Atlantic Ocean (SEA) is semi-permanently covered by one of the most extensive stratocumulus cloud decks on the planet and experiences about one-third of the global biomass burning emissions from the southern Africa savannah region during the fire season. To get a better understanding of the impact of these biomass burning aerosols on clouds and the radiation balance over the SEA, the latest generation of the UK Earth System Model (UKESM1) is employed. Measurements from the CLARIFY and ORACLES flight campaigns are used to evaluate the model, demonstrating that the model has good skill in reproducing the biomass burning plume. To investigate the underlying mechanisms in detail, the effects of biomass burning aerosols on the clouds are decomposed into radiative effects (via absorption and scattering) and microphysical effects (via perturbation of cloud condensation nuclei – CCN – and cloud microphysical processes). July–August means are used to characterize aerosols, clouds, and the radiation balance during the fire season. Results show that around 65 % of CCN at 0.2 % supersaturation in the SEA can be attributed to biomass burning. The absorption effect of biomass burning aerosols is the most significant on clouds and radiation. Near the continent, it increases the supersaturation diagnosed by the activation scheme, while further from the continent it reduces the altitude of the supersaturation. As a result, the cloud droplet number concentration responds with a similar pattern to the absorption effect of biomass burning aerosols. The microphysical effect, however, decreases the supersaturation and increases the cloud droplet concentration over the ocean, although this change is relatively small. The liquid water path is also significantly increased over the SEA (mainly caused by the absorption effect of biomass burning aerosols) when biomass burning aerosols are above the stratocumulus cloud deck. The microphysical pathways lead to a slight increase in the liquid water path over the ocean. These changes in cloud properties indicate the significant role of biomass burning aerosols for clouds in this region. Among the effects of biomass burning aerosols on the radiation balance, the semi-direct radiative effects (rapid adjustments induced by the radiative effects of biomass burning aerosols) have a dominant cooling impact over the SEA, which offset the warming direct radiative effect (radiative forcing from biomass burning aerosol–radiation interactions) and lead to an overall net cooling radiative effect in the SEA. However, the magnitude and the sign of the semi-direct effects are sensitive to the relative location of biomass burning aerosols and clouds, reflecting the critical task of the accurate modelling of the biomass burning plume and clouds in this region. [ABSTRACT FROM AUTHOR]

Proven by multiple theoretical and practical studies, multi-angular spectral polarimetry is ideal for comprehensive retrieval of properties of aerosols. Furthermore, a large number of advanced space polarimeters have been launched recently or planned to be deployed in the coming few years (Dubovik et al., 2019). Nevertheless, at present, practical utilization of aerosol products from polarimetry is rather limited, due to the relatively small number of polarimetric compared to photometric observations, as well as challenges in making full use of the extensive information content available in these complex observations. Indeed, while in recent years several new algorithms have been developed to provide enhanced aerosol retrievals from satellite polarimetry, the practical value of available aerosol products from polarimeters yet remains to be proven. In this regard, this paper presents the analysis of aerosol products obtained by the Generalized Retrieval of Atmosphere and Surface Properties (GRASP) algorithm from POLDER/PARASOL observations. After about a decade of development, GRASP has been adapted for operational processing of polarimetric satellite observations and several aerosol products from POLDER/PARASOL observations have been released. These updated PARASOL/GRASP products are publicly available (e.g., http://www.icare.univ-lille.fr , last access: 16 October 2018, http://www.grasp-open.com/products/ , last access: 28 March 2020); the dataset used in the current study is registered under 10.5281/zenodo.3887265 (Chen et al., 2020). The objective of this study is to comprehensively evaluate the GRASP aerosol products obtained from POLDER/PARASOL observations. First, the validation of the entire 2005–2013 archive was conducted by comparing to ground-based Aerosol Robotic Network (AERONET) data. The subjects of the validation are spectral aerosol optical depth (AOD), aerosol absorption optical depth (AAOD) and single-scattering albedo (SSA) at six wavelengths, as well as Ångström exponent (AE), fine-mode AOD (AODF) and coarse-mode AOD (AODC) interpolated to the reference wavelength 550 nm. Second, an inter-comparison of PARASOL/GRASP products with the PARASOL/Operational, MODIS Dark Target (DT), Deep Blue (DB) and Multi-Angle Implementation of Atmospheric Correction (MAIAC) aerosol products for the year 2008 was performed. Over land both satellite data validations and inter-comparisons were conducted separately for different surface types, discriminated by bins of normalized difference vegetation index (NDVI): < 0.2, 0.2 ≤ and < 0.4, 0.4 ≤ and < 0.6, and ≥ 0.6. Three PARASOL/GRASP products were analyzed: GRASP/HP ("High Precision"), Optimized and Models. These different products are consistent but were obtained using different assumptions in aerosol modeling with different accuracies of atmospheric radiative transfer (RT) calculations. Specifically, when using GRASP/HP or Optimized there is direct retrieval of the aerosol size distribution and spectral complex index of refraction. When using GRASP/Models, the aerosol is approximated by a mixture of several prescribed aerosol components, each with their own fixed size distribution and optical properties, and only the concentrations of those components are retrieved. GRASP/HP employs the most accurate RT calculations, while GRASP/Optimized and GRASP/Models are optimized to achieve the best trade-off between accuracy and speed. In all these three options, the underlying surface reflectance is retrieved simultaneously with the aerosol properties, and the radiative transfer calculations are performed "online" during the retrieval. All validation results obtained for the full archive of PARASOL/GRASP products show solid quality of retrieved aerosol characteristics. The GRASP/Models retrievals, however, provided the most solid AOD products, e.g., AOD (550 nm) is unbiased and has the highest correlation (R ∼ 0.92) and the highest fraction of retrievals (∼ 55.3 %) satisfying the accuracy requirements of the Global Climate Observing System (GCOS) when compared to AERONET observations. GRASP/HP and GRASP/Optimized AOD products show a non-negligible positive bias (∼ 0.07) when AOD is low (< 0.2). On the other hand, the detailed aerosol microphysical characteristics (AE, AODF, AODC, SSA, etc.) provided by GRASP/HP and GRASP/Optimized correlate generally better with AERONET than do the results of GRASP/Models. Overall, GRASP/HP processing demonstrates the high quality of microphysical characteristics retrieval versus AERONET. Evidently, the GRASP/Models approach is more adapted for retrieval of total AOD, while the detailed aerosol microphysical properties are limited when a mixture of aerosol models with fixed optical properties are used. The results of a comparative analysis of PARASOL/GRASP and MODIS products showed that, based on validation against AERONET, the PARASOL/GRASP AOD (550 nm) product is of similar and sometimes of higher quality compared to the MODIS products. All AOD retrievals are more accurate and in good agreement over ocean. Over land, especially over bright surfaces, the retrieval quality degrades and the differences in total AOD products increase. The detailed aerosol characteristics, such as AE, AODF and AODC from PARASOL/GRASP, are generally more reliable, especially over land. The global inter-comparisons of PARASOL/GRASP versus MODIS showed rather robust agreement, though some patterns and tendencies were observed. Over ocean, PARASOL/Models and MODIS/DT AOD agree well with the correlation coefficient of 0.92. Over land, the correlation between PARASOL/Models and the different MODIS products is lower, ranging from 0.76 to 0.85. There is no significant global offset; though over bright surfaces MODIS products tend to show higher values compared to PARASOL/Models when AOD is low and smaller values for moderate and high AODs. Seasonal AOD means suggest that PARASOL/GRASP products show more biomass burning aerosol loading in central Africa and dust over the Taklamakan Desert, but less AOD in the northern Sahara. It is noticeable also that the correlation for the data over AERONET sites are somewhat higher, suggesting that the retrieval assumptions generally work better over AERONET sites than over the rest of the globe. One of the potential reasons may be that MODIS retrievals, in general, rely more on AERONET climatology than GRASP retrievals. Overall, the analysis shows that the quality of AOD retrieval from multi-angular polarimetric observations like POLDER is at least comparable to that of single-viewing MODIS-like imagers. At the same time, the multi-angular polarimetric observations provide more information on other aerosol properties (e.g., spectral AODF, AODC, AE), as well as additional parameters such as AAOD and SSA. [ABSTRACT FROM AUTHOR]

Atmospheric high-viscosity organic particles (HVOPs) were observed in samples of ambient aerosols collected in April and May 2016 in the Southern Great Plains of the United States. These particles were apportioned as either airborne soil organic particles (ASOPs) or tar balls (TBs) from biomass burning based on spetro-microscopic imaging and assessments of meteorological records of smoke and precipitation data. Regardless of their apportionment, the number fractions of HVOPs were positively correlated (R2=0.85) with increased values of absorption Ångström exponent (AAE) measured in situ for ambient aerosol at the site. Extending this correlation to 100 % HVOPs yields an AAE of 2.6, similar to previous literature reports of the class of light-absorbing organic particles known as brown carbon (BrC). One out of the three samples investigated had a significant number of ASOPs, while the other two samples contained TBs. Although there are chemical similarities between ASOPs and TBs, they can be distinguished based on composition inferred from near-edge absorption X-ray fine structure (NEXAFS) spectroscopy. ASOPs were distinguished from TBs based on their average -COOH/C=C and -COOH/COH peak ratios, with ASOPs having lower ratios. NEXAFS spectra of filtered soil organic brine particles nebulized from field samples of standing water deposited after rain were consistent with ASOPs when laboratory particles were generated by bubble bursting at the air–organic brine interface. However, particles generated by nebulizing the bulk volume of soil organic brine had a particle composition different from ASOPs. These observations are consistent with the raindrop generation mechanism responsible for ASOP emissions in the area of study. In contrast, nebulized samples carry with them higher fractions of soil inorganics dissolved in the bulk volume of soil brine, which are not aerosolized by the raindrop mechanism. Our results support the bubble bursting mechanism of particle generation during rainfall resulting in the ejection of soil organics into the atmosphere. In addition, our results show that ASOPs may only be atmospherically relevant during times when suitable emission conditions are met. [ABSTRACT FROM AUTHOR]

The AErosol RObotic NETwork (AERONET) is the most developed ground-based network for aerosol remote sensing and has been playing a significant role not only in monitoring air quality for protecting human health but also in assessing the radiative budget of our planet Earth. In this paper, we report the direct-Sun and inversion products, comprising of spectral variation of aerosol optical depth (AOD), associated Ångström exponent (AE), fine- and coarse-mode aerosol fractions, aerosol size distribution (ASD), refractive index (RI), asymmetry parameter (AP), single scattering albedo (SSA), aerosol radiative forcing (ARF) and columnar concentration of gas constituents such as water vapor (H2O), obtained from a Cimel Sun–sky radiometer, functioning in Pune, India, under the AERONET program since October 2004. These long-term measurements carried out from 2005 to 2015 could serve as an urban aerosol optical long-term average or climatology. The AOD long-term variations at all wavelengths, considered in the study, exhibited an increasing trend, implying year-to-year enhancement in aerosol loading. The mean seasonal variations in AOD from cloud-free days indicated greater values during the monsoon season, revealing dominance of hygroscopic aerosol particles over the station. Contribution by different aerosol types to AOD has also been deduced and discussed, and dominance of a mixed type of aerosols (44.85 %) found, followed by combination of biomass burning and urban industrial aerosols (22.57 %) compared to other types of aerosols during the study period. The long-term datasets, derived aerosol and trace gas products play a significant role in understanding aerosol climate forcing, trends and evaluation of regional air pollution and validation of aerosol transport models over the study region. [ABSTRACT FROM AUTHOR]

An accurate measurement of the optical properties of aerosol is critical for quantifying the effect of aerosol on climate. Uncertainties persist and results of measurements vary significantly. Biomass burning (BB) aerosol has been extensively studied through both field and laboratory environments for North American fuels to understand the changes in optical and chemical properties as a function of aging. There is a need for a wider sampling of fuels from different regions of the world for laboratory studies. This work represents the first such study of the optical and chemical properties of wood fuel samples commonly used for domestic purposes in east Africa. In general, combustion temperature or modified combustion efficiency (MCE) plays a major role in the optical properties of the emitted aerosol. For fuels combusted with MCE of 0.974±0.015 , which is referred to as flaming-dominated combustion, the single-scattering albedo (SSA) values were in the range of 0.287 to 0.439, while for fuels combusted with MCE of 0.878±0.008 , which is referred to as smoldering-dominated combustion, the SSA values were in the range of 0.66 to 0.769. There is a clear but very small dependence of SSA on fuel type. A significant increase in the scattering and extinction cross section (with no significant change in absorption cross section) was observed, indicating the occurrence of chemistry, even during dark aging for smoldering-dominated combustion. This fact cannot be explained by heterogeneous oxidation in the particle phase, and we hypothesize that secondary organic aerosol formation is potentially happening during dark aging. After 12 h of photochemical aging, BB aerosol becomes highly scattering with SSA values above 0.9, which can be attributed to oxidation in the chamber. Aging studies of aerosol from flaming-dominated combustion were inconclusive due to the very low aerosol number concentration. We also attempted to simulate polluted urban environments by injecting volatile organic compounds (VOCs) and BB aerosol into the chamber, but no distinct difference was observed when compared to photochemical aging in the absence of VOCs. [ABSTRACT FROM AUTHOR]

We present the first study of the weekly cycles (WCs) of chemically speciated and size‐resolved particulate matter (PM) in Metro Manila, Philippines, a coastal megacity located within a highly complex meteorological environment that is subject to both anthropogenic and natural sources. To measure PM, Micro‐Orifice Uniform Deposit Impactors (MOUDIs) were deployed in Metro Manila from August 2018 to October 2019 and samples were analyzed for ionic and elemental species, including black carbon (BC). The WC in Metro Manila varied remarkably across seasons, linked to shifts in meteorology, transport, and aerosol source. Identified aerosol sources were traffic, local and regional burning, dust, sea salt, and secondary aerosol formation. Direct emissions induced a late workweek peak, while secondary aerosol formation led to a weekend peak in response to precursor buildup mainly from traffic. Seasonal analysis revealed that local burning from solid waste management and agricultural fires induced a strong WC peak while regional burning emissions from the Maritime Continent (MC) and possibly the Asian continent elevated seasonal baseline concentrations of the WC. BC showed a seasonally persistent WC, consistent in magnitude, weekly peak timing, and particle size. The dominant submicrometer WC and the contribution of BC across seasons have important ramifications on public health and policymaking, which are also discussed. As many of the observed WC patterns are undetectable when using only bulk PM, this study demonstrates that a seasonal, size‐resolved, and chemically speciated characterization is required to more fully understand the driving mechanisms governing WCs. Key Points: Significant variability was observed in the weekly cycle of particulate matter (particle size and composition) as a function of seasonSubmicrometer aerosol peak timing indicates that secondary formation increases in response to precursor buildup, inducing a weekend peakBlack carbon showed a seasonally persistent weekly cycle, consistent in magnitude, weekly peak timing, and particle size [ABSTRACT FROM AUTHOR]

The direct radiative effect (DRE) of aerosols above clouds has been found to be significant over the south-east Atlantic Ocean during the African biomass burning season due to elevated smoke layers absorbing radiation above the cloud deck. So far, global climate models have been unsuccessful in reproducing the high DRE values measured by various satellite instruments. Meanwhile, the radiative effects by aerosols have been identified as the largest source of uncertainty in global climate models. In this paper, three independent satellite datasets of DRE during the biomass burning season in 2006 are compared to constrain the south-east Atlantic radiation budget. The DRE of aerosols above clouds is derived from the spectrometer SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY), the polarimeter Polarization and Directionality of the Earth's Reflectances (POLDER), and collocated measurements by the spectrometer Ozone Monitoring Instrument (OMI) and the imager Moderate Resolution Imaging Spectroradiometer (MODIS). All three datasets confirm the high DRE values during the biomass season, underlining the relevance of local aerosol effects. Differences between the instruments can be attributed mainly to sampling issues. When these are accounted for, the remaining differences can be explained by a higher cloud optical thickness (COT) derived from POLDER compared to the other instruments and a neglect of aerosol optical thickness (AOT) at shortwave infrared (SWIR) wavelengths in the method used for SCIAMACHY and OMI–MODIS. The higher COT from POLDER by itself can explain the difference found in DRE between POLDER and the other instruments. The AOT underestimation is mainly evident at high values of the aerosol DRE and accounts for about a third of the difference between POLDER and OMI–MODIS DRE. The datasets from POLDER and OMI–MODIS effectively provide lower and upper bounds for the aerosol DRE over clouds over the south-east Atlantic, which can be used to challenge global circulation models (GCMs). Comparisons of model and satellite datasets should also account for sampling issues. The complementary DRE retrievals from OMI–MODIS and POLDER may benefit from upcoming satellite missions that combine spectrometer and polarimeter measurements. [ABSTRACT FROM AUTHOR]

Among the various measurement approaches to quantify the light absorption coefficient (Babs), filter-based absorption photometers are dominant in monitoring networks around the globe. Numerous correction algorithms have been introduced to minimize the artifacts due to the presence of the filter in these instruments. However, from our recent studies conducted during the Fire Influence on Regional and Global Environments Experiment (FIREX) laboratory campaign, corrected filter-based Babs remains biased high by roughly a factor of 2.5 when compared to a reference value using a photoacoustic instrument for biomass burning emissions. Similar overestimations of Babs from filter-based instruments exist when implementing the algorithms on 6 months of ambient data from the Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) user facility from 2013 (factor of roughly 3). In both datasets, we observed an apparent dependency on single-scattering albedo (SSA) and the absorption Ångström exponent (AAE) in the agreement between Babs based on existing correction factors and the reference Babs. Consequently, we developed a new correction approach that is applicable to any filter-based absorption photometer that includes light transmission from the filter-based instrument as well as the derived AAE and SSA. For the FIREX and SGP datasets, our algorithm results in good agreement between all corrected filter-based Babs values from different filter-based instruments and the reference (slopes ≈1 and R2≈0.98 for biomass burning aerosols and slopes ≈1.05 and R2≈0.65 for ambient aerosols). Moreover, for both the corrected Babs and the derived optical properties (SSA and AAE), our new algorithms work better or at least as well as the two common correction algorithms applied to a particle soot absorption photometer (PSAP). The uncertainty of the new correction algorithm is estimated to be ∼10 %, considering the measurement uncertainties of the operated instruments. Therefore, our correction algorithm is applicable to any filter-based absorption photometer and has the potential to "standardize" reported results across any filter-based instrument. [ABSTRACT FROM AUTHOR]

This work presents synergistic satellite, airborne and surface-based observations of a pocket of open cells (POC) in the remote south-east Atlantic. The observations were obtained over and upwind of Ascension Island during the CLouds and Aerosol Radiative Impacts and Forcing (CLARIFY) and the Layered Smoke Interacting with Clouds (LASIC) field experiments. A novel aspect of this case study is that an extensive free-tropospheric biomass burning aerosol plume that had been transported from the African continent was observed to be in contact with the boundary layer inversion over the POC and the surrounding closed cellular cloud regime. The in situ measurements show marked contrasts in the boundary layer thermodynamic structure, cloud properties, precipitation and aerosol conditions between the open cells and surrounding overcast cloud field. The data demonstrate that the overlying biomass burning aerosol was mixing down into the boundary layer in the stratocumulus cloud downwind of the POC, with elevated carbon monoxide, black carbon mass loadings and accumulation-mode aerosol concentrations measured beneath the trade-wind inversion. The stratocumulus cloud in this region was moderately polluted and exhibited very little precipitation falling below cloud base. A rapid transition to actively precipitating cumulus clouds and detrained stratiform remnants in the form of thin quiescent veil clouds was observed across the boundary into and deep within the POC. The subcloud layer in the POC was much cleaner than that in the stratocumulus region. The clouds in the POC formed within an ultra-clean layer (accumulation-mode aerosol concentrations of approximately a few cm-3) in the upper region of the boundary layer, which was likely to have been formed via efficient collision–coalescence and sedimentation processes. Enhanced Aitken-mode aerosol concentrations were also observed intermittently in this ultra-clean layer, suggesting that new particle formation was taking place. Across the boundary layer inversion and immediately above the ultra-clean layer, accumulation-mode aerosol concentrations were ∼ 1000 cm-3. Importantly, the air mass in the POC showed no evidence of elevated carbon monoxide over and above typical background conditions at this location and time of year. As carbon monoxide is a good tracer for biomass burning aerosol that is not readily removed by cloud processing and precipitation, it demonstrates that the open cellular convection in the POC is not able to entrain large quantities of the free-tropospheric aerosol that was sitting directly on top of the boundary layer inversion. This suggests that the structure of the mesoscale cellular convection may play an important role in regulating the transport of aerosol from the free troposphere down into the marine boundary layer. We then develop a climatology of open cellular cloud conditions in the south-east Atlantic from 19 years of September Moderate Resolution Imaging Spectroradiometer (MODIS) Terra imagery. This shows that the maxima in open cell frequency (> 0.25) occurs far offshore and in a region where subsiding biomass burning aerosol plumes may often come into contact with the underlying boundary layer cloud. If the results from the observational case study applied more broadly, then the apparent low susceptibility of open cells to free-tropospheric intrusions of additional cloud condensation nuclei could have some important consequences for aerosol–cloud interactions in the region. [ABSTRACT FROM AUTHOR]

The climate response to atmospheric aerosols, including their effects on dominant modes of climate variability like El Niño–Southern Oscillation (ENSO), remains highly uncertain. This is due to several sources of uncertainty, including aerosol emission, transport, removal, vertical distribution, and radiative properties. Here, we conduct coupled ocean‐atmosphere simulations with two versions of the Community Earth System Model (CESM) driven by semiempirical fine‐mode aerosol direct radiative effects without dust and sea salt. Aerosol atmospheric heating off the west coast of Africa—most of which is due to biomass burning—leads to a significant atmospheric dynamical response, including localized ascent and upper‐level divergence. Coupled Model Intercomparison Project version 6 (CMIP6) biomass burning simulations support this response. Moreover, CESM shows that the anomalous aerosol heating in the Atlantic triggers an atmospheric teleconnection to the tropical Pacific, including strengthening of the Walker circulation. The easterly trade winds accelerate, and through coupled ocean‐atmosphere processes and the Bjerknes feedback, a La Niña‐like response develops. Observations also support a relationship between south African biomass burning emissions and ENSO, with La Niña events preceding strong south African biomass burning in boreal fall. Our simulations suggest a possible two‐way feedback between ENSO and south African biomass burning, with La Niña promoting more biomass burning emissions, which may then strengthen the developing La Niña. Key Points: South African biomass burning aerosol locally warms the atmosphereThis heating drives local ascent and divergence, triggering a teleconnection to the PacificThe Pacific Walker circulation strengthens, and a La Niña‐like response develops [ABSTRACT FROM AUTHOR]

Black carbon (BC) aerosols have been widely recognized as a vital climate forcer in the atmosphere. Amplification of light absorption can occur due to coatings on BC during atmospheric aging, an effect that remains uncertain in accessing the radiative forcing of BC. Existing studies on the absorption enhancement factor (Eabs) have poor coverage on both seasonal and diurnal scales. In this study, we applied a recently developed minimum R squared (MRS) method, which can cover both seasonal and diurnal scales, for Eabs quantification. Using field measurement data in Guangzhou, the aims of this study are to explore (1) the temporal dynamics of BC optical properties at seasonal (wet season, 31 July–10 September; dry season, 15 November 2017–15 January 2018) and diel scales (1 h time resolution) in the typical urban environment and (2) the influencing factors on Eabs temporal variability. Mass absorption efficiency at 520 nm by primary aerosols (MAE p520) determined by the MRS method exhibited a strong seasonality (8.6 m 2 g -1 in the wet season and 16.8 m 2 g -1 in the dry season). Eabs520 was higher in the wet season (1.51±0.50) and lower in the dry season (1.29±0.28). Absorption Ångström exponent (AAE 470–660) in the dry season (1.46±0.12) was higher than that in the wet season (1.37±0.10). Collective evidence showed that the active biomass burning (BB) in the dry season effectively altered the optical properties of BC, leading to elevated MAE, MAE p and AAE in the dry season compared to those in the wet season. Diurnal Eabs520 was positively correlated with AAE 470–660 (R2=0.71) and negatively correlated with the AE33 aerosol loading compensation parameter (k) (R2=0.74) in the wet season, but these correlations were significantly weaker in the dry season, which may be related to the impact of BB. This result suggests that during the wet season, the lensing effect was more likely dominating the AAE diurnal variability rather than the contribution from brown carbon (BrC). Secondary processing can affect Eabs diurnal dynamics. The Eabs520 exhibited a clear dependency on the ratio of secondary organic carbon to organic carbon (SOC/OC), confirming the contribution of secondary organic aerosols to Eabs ; Eabs520 correlated well with nitrate and showed a clear dependence on temperature. This new finding implies that gas–particle partitioning of semivolatile compounds may potentially play an important role in steering the diurnal fluctuation of Eabs520. In the dry season, the diurnal variability in Eabs520 was associated with photochemical aging as evidenced by the good correlation (R2= 0.69) between oxidant concentrations (Ox=O3+NO2) and Eabs520. [ABSTRACT FROM AUTHOR]

We study 41 d with daily median surface accumulation mode aerosol particle concentrations below 50 cm -3 (ultra-clean conditions) observed at Ascension Island (ASI; 7.9 ∘ S, 14.4 ∘ W) between June 2016 and October 2017 as part of the Layered Atlantic Smoke Interactions with Clouds (LASIC) campaign. Interestingly, these days occur during a period of great relevance for aerosol–cloud–radiation interactions, the southeast Atlantic (SEATL) biomass-burning season (approximately June–October). That means that these critical months can feature both the highest surface aerosol numbers, from smoke intrusion into the marine boundary layer, as well as the lowest. While carbon monoxide and refractory black carbon concentrations on ultra-clean days do not approach those on days with heavy smoke, they also frequently exceed background concentrations calculated in the non-burning season from December 2016 to April 2017. This is evidence that even what become ultra-clean boundary layers can make contact with and entrain from an overlying SEATL smoke layer before undergoing a process of rapid aerosol removal. Because many ultra-clean and polluted boundary layers observed at Ascension Island during the biomass burning season follow similar isobaric back trajectories, the variability in this entrainment is likely more closely tied to the variability in the overlying smoke rather than large-scale horizontal circulation through the boundary layer. Since exceptionally low accumulation mode aerosol numbers at ASI do not necessarily indicate the relative lack of other trace pollutants, this suggests the importance of regional variations in what constitutes an "ultra-clean" marine boundary layer. Finally, surface drizzle rates, frequencies and accumulation – as well as retrievals of liquid water path – all consistently tend toward higher values on ultra-clean days. This implicates enhanced coalescence scavenging in low clouds as the key driver of ultra-clean events in the southeast Atlantic marine boundary layer. These enhancements occur against and are likely mediated by the backdrop of a seasonal increase in daily mean cloud fraction and daily median liquid water path over ASI, peaking in September and October in both LASIC years. Therefore the seasonality in ultra-clean day occurrence seems directly linked to the seasonality in SEATL cloud properties. These results highlight the importance of two-way aerosol–cloud interactions in the region. [ABSTRACT FROM AUTHOR]

The southeast Atlantic (SEA) region is host to a climatologically significant biomass burning aerosol layer overlying marine stratocumulus. We present the first results of the directly measured above-cloud aerosol optical depth (ACAOD) from the recent ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) airborne field campaign during August and September 2016. In our analysis, we use data from the Spectrometers for Sky-Scanning Sun-Tracking Atmospheric Research (4STAR) instrument and found an average ACAOD of 0.32 at 501 nm (range of 0.02 to 1.04), with an average Ångström exponent (AE) above clouds of 1.71. The AE is much lower at 1.25 for the full column (including below-cloud-level aerosol, with an average of 0.36 at 501 nm and a range of 0.02 to 0.74), indicating the presence of large aerosol particles, likely marine aerosol, in the lower atmospheric column. The ACAOD is observed from 4STAR to be highest near the coast at about 12 ∘ S, whereas its variability is largest at the southern edge of the average aerosol plume, as indicated by 12 years of MODIS observations. In comparison to MODIS-derived ACAOD and long-term fine-mode plume-average AOD along a diagonal routine track extending out from the coast of Namibia, the directly measured ACAOD from 4STAR is slightly lower than the ACAOD product from MODIS. The peak ACAOD expected from MODIS AOD retrievals averaged over a long term along the routine diagonal flight track (peak of 0.5) was measured to be closer to coast in 2016 at about 1.5–4 ∘ E, with 4STAR ACAOD averages showing a peak of 0.42. When considering the full observation set over the SEA, by spatially binning each sampled AOD, we obtain a geographically representative mean ACAOD of 0.37. Vertical profiles of AOD showcase the variability in the altitude of the aerosol plume and its separation from the cloud top. We measured larger AOD at a high altitude near the coast than farther from the coast, while generally observing a larger vertical gap farther from the coast. Changes in AOD with altitude are correlated with carbon monoxide, a gas tracer of the biomass burning aerosol plume. Vertical extent of gaps between aerosol and cloud show a wide distribution, with a near-zero gap being most frequent. The gap distribution with longitude is observed to be largest at about 7 ∘ E, farther from coast than expected from previous studies. [ABSTRACT FROM AUTHOR]

The Po Valley (Italy) is a well-known air quality hotspot characterized by particulate matter (PM) levels well above the limit set by the European Air Quality Directive and by the World Health Organization, especially during the colder season. In the framework of Emilia-Romagna regional project "Supersito", the southern Po Valley submicron aerosol chemical composition was characterized by means of high-resolution aerosol mass spectroscopy (HR-AMS) with the specific aim of organic aerosol (OA) characterization and source apportionment. Eight intensive observation periods (IOPs) were carried out over 4 years (from 2011 to 2014) at two different sites (Bologna, BO, urban background, and San Pietro Capofiume, SPC, rural background), to characterize the spatial variability and seasonality of the OA sources, with a special focus on the cold season. On the multi-year basis of the study, the AMS observations show that OA accounts for averages of 45±8 % (ranging from 33 % to 58 %) and 46±7 % (ranging from 36 % to 50 %) of the total non-refractory submicron particle mass (PM 1 -NR) at the urban and rural sites, respectively. Primary organic aerosol (POA) comprises biomass burning (23±13 % of OA) and fossil fuel (12±7 %) contributions with a marked seasonality in concentration. As expected, the biomass burning contribution to POA is more significant at the rural site (urban / rural concentration ratio of 0.67), but it is also an important source of POA at the urban site during the cold season, with contributions ranging from 14 % to 38 % of the total OA mass. Secondary organic aerosol (SOA) contributes to OA mass to a much larger extent than POA at both sites throughout the year (69±16 % and 83±16 % at the urban and rural sites, respectively), with important implications for public health. Within the secondary fraction of OA, the measurements highlight the importance of biomass burning aging products during the cold season, even at the urban background site. This biomass burning SOA fraction represents 14 %–44 % of the total OA mass in the cold season, indicating that in this region a major contribution of combustion sources to PM mass is mediated by environmental conditions and atmospheric reactivity. Among the environmental factors controlling the formation of SOA in the Po Valley, the availability of liquid water in the aerosol was shown to play a key role in the cold season. We estimate that the organic fraction originating from aqueous reactions of biomass burning products ("bb-aqSOA") represents 21 % (14 %–28 %) and 25 % (14 %–35 %) of the total OA mass and 44 % (32 %–56 %) and 61 % (21 %–100 %) of the SOA mass at the urban and rural sites, respectively. [ABSTRACT FROM AUTHOR]

Emissions and long-range transport of mineral dust and combustion-related aerosol from burning fossil fuels and biomass vary from year to year, driven by the evolution of the economy and changes in meteorological conditions and environmental regulations. This study offers both satellite and model perspectives on the interannual variability and possible trends of combustion aerosol and dust in major continental outflow regions over the past 15 years (2003–2017). The decade-long record of aerosol optical depth (AOD, denoted as τ), separately for combustion aerosol (τc) and dust (τd), over global oceans is derived from the Collection 6 aerosol products of the Moderate Resolution Imaging Spectroradiometer (MODIS) onboard both Terra and Aqua. These MODIS Aqua datasets, complemented by aerosol source-tagged simulations using the Community Atmospheric Model version 5 (CAM5), are then analyzed to understand the interannual variability and potential trends of τc and τd in the major continental outflows. Both MODIS and CAM5 consistently yield a similar decreasing trend of -0.017 to -0.020 per decade for τc over the North Atlantic Ocean and the Mediterranean Sea that is attributable to reduced emissions from North America and Europe, respectively. On the contrary, both MODIS and CAM5 display an increasing trend of + 0.017 to + 0.036 per decade for τc over the tropical Indian Ocean, the Bay of Bengal, and the Arabian Sea, which reflects the influence of increased anthropogenic emissions from South Asia and the Middle East in the last 2 decades. Over the northwestern Pacific Ocean, which is often affected by East Asian emissions of pollution and dust, the MODIS retrievals show a decreasing trend of -0.021 per decade for τc and -0.012 per decade for τd , which is, however, not reproduced by the CAM5 model. In other outflow regions strongly influenced by biomass burning smoke or dust, both MODIS retrievals and CAM5 simulations show no statistically significant trends; the MODIS-observed interannual variability is usually larger than that of the CAM5 simulation. [ABSTRACT FROM AUTHOR]

This study integrates data from regional model simulations, reanalysis data set, radiosonde observations, lidar measurements, and satellite products to evaluate the direct radiative forcing effect of biomass burning and dust over East Asia. During March and April, we find an overall cooling effect of the dust of −5 to −9 W/m2. Biomass burning aerosols from Peninsular Southeast Asia exhibit a warming effect of 5–10 W/m2 over the source area, lower than that over the downwind area of 10–20 W/m2 because of significantly higher cloud coverage in South China. Dust and biomass burning aerosols are found to cool the near surface layer (0–1 km) by −0.5 and −0.3 K, respectively, and warm the upper air (1–5 km) by +0.1 and +0.2 K, respectively. In Taipei, simultaneous presences of dust and biomass burning lead to cooling of near‐surface air by −1.5 K and warming of upper air by +1 K. Plain Language Summary: Biomass burning and dust are the largest natural emission sources of atmospheric aerosol. However, no solid consensus exists regarding whether biomass burning or dust contributes to a net warming or cooling effect. This study integrates data from regional climate model simulations, reanalysis data, radiosonde observations, lidar measurements, and satellite products to evaluate the climate effects of biomass burning and dust at a regional scale over East Asia. We find prominent warming effects by biomass burning in Peninsular Southeast Asia, which is more significant over the downwind area in South China than over the emission source area. Dust exhibits cooling effects, with a few exceptions over areas covered by semipersistent snow or ice. We also reveal that under conditions in which both biomass burning and dust aerosols are present, they exhibit an overall slight warming effect. Key Points: Peninsular Southeast Asia biomass burning shows larger warming effect (10‐20 W/m2) over downwind region than over the source area (5‐10 W/m2)Dust shows a cooling effect of up to ‐9 W/m2 with a few exceptions along north and east edges of Tibet Plateau due to snow or ice coverDust and biomass burning cool the near surface air and warm the upper air, and their radiative efficiencies decrease during transport [ABSTRACT FROM AUTHOR]

Aerosols have a direct effect on the Earth's radiative budget and can also affect cloud development and lifetime, and the aerosols above clouds (AAC) are particularly associated with high uncertainties in global climate models. Therefore, it is a prerequisite to improve the description and understanding of these situations. During the austral winter, large loadings of biomass burning aerosols originating from fires in the southern African subcontinent are lifted and transported westwards, across the southeastern Atlantic Ocean. The negligible wet scavenging of these absorbing aerosols leads to a near-persistent smoke layer above one of the largest stratocumulus cloud decks on the planet. Therefore, the southeastern Atlantic region is a very important area for studying the impact of above-cloud absorbing aerosols, their radiative forcing and their possible effects on clouds. In this study we aim to analyse and quantify the effect of smoke loadings on cloud properties using a synergy of different remote sensing techniques from A-Train retrievals (methods based on the passive instruments POLDER and MODIS and the operational method of the spaceborne lidar CALIOP), collocated with ERA-Interim re-analysis meteorological profiles. To analyse the possible mechanisms of AAC effects on cloud properties, we developed a high and low aerosol loading approach, which consists in evaluating the change in radiative quantities (i.e. cloud-top cooling, heating rate vertical profiles) and cloud properties with the smoke loading. During this analysis, we account for the variation in the meteorological conditions over our sample area by selecting the months associated with one meteorological regime (June–August). The results show that the region we focus on is primarily under the energetic influence of absorbing aerosols, leading to a significant positive shortwave direct effect at the top of the atmosphere. For larger loads of AACs, clouds are optically thicker, with an increase in liquid water path of 20 g m -2 and lower cloud-top altitudes by 100 m. These results do not contradict the semi-direct effect of above-cloud aerosols, explored in previous studies. Furthermore, we observe a strong covariance between the aerosol and the water vapour loadings, which has to be accounted for. A detailed analysis of the heating rate profiles shows that within the smoke layer, the absorbing aerosols are 90 % responsible for warming the ambient air by approximately 5.7 K d -1. The accompanying water vapour, however, has a longwave effect at distance on the cloud top, reducing its cooling by approximately 4.7 K d -1 (equivalent to 7 %). We infer that this decreased cloud-top cooling in particular, in addition with the higher humidity above the clouds, might modify the cloud-top entrainment rate and its effect, leading to thicker clouds. Therefore, smoke (the combination of aerosol and water vapour) events would have the potential to modify and probably reinforce the underlaying cloud cover. [ABSTRACT FROM AUTHOR]

Aerosol models, composed of size distribution, complex refractive index, and spherical fraction, are derived from a new synergistic retrieval of airborne in situ angular scattering measurements made by the Polarized Imaging Nephelometer and absorption measurements from the Particle Soot Absorption Photometer. The data utilized include phase function (F11), degree of polarization (−F12/F11), and absorption coefficient (βabs) measured at low relative humidities during the Studies of Emissions and Atmospheric Composition, Clouds, and Climate Coupling by Regional Surveys (SEAC4RS) and Deep Convection Clouds and Chemistry (DC3) field campaigns. The Generalized Retrieval of Aerosol and Surface Properties (GRASP) is applied to these measurements to obtain summaries of particle properties that are optically consistent with the original measurements. A classification scheme is then used to categorize the corresponding retrieval results. Inversions performed on the DC3 measurements indicate the presence of a significant amount of dust‐like aerosol in the inflow of storms sampled during this campaign, with the quantity of dust present depending strongly on the underlying surface features. In the SEAC4RS data, the retrieved size distributions were found to be remarkably similar among a range of aerosol types, including urban and industrial, biogenic, and biomass burning (BB) emissions. These aerosol types were found to have average fine mode volume median radii 0.155 ≤ rvf ≤ 0.163μm and lognormal standard deviations 0.32 ≤ σf ≤ 0.36. There were, however, consistent differences between the angular scattering patterns of the BB samples and the other particle types. The GRASP retrieval predominantly attributed these differences to elevated real and imaginary refractive indices in the BB samples (m532nm≈1.55+0.007i) relative to the two other categories (m532nm≈1.51+0.004i). Key Points: Aerosol properties are obtained using a novel synergistic retrieval of in situ angular‐dependent scattering and absorption measurementsBiomass burning particles were found to have elevated real and imaginary refractive indices relative to other aerosol typesSignificant concentrations of dust‐like particles are observed in measurements made in the vicinity of convective systems [ABSTRACT FROM AUTHOR]