African Biomass Burning Research Articles

Evidence of a dual African and Australian biomass burning influence on the vertical distribution of aerosol and carbon monoxide over the southwest Indian Ocean basin in early 2020

Abstract. During the 2020 austral summer, the pristine atmosphere of the southwest Indian Ocean (SWIO) basin experienced significant perturbations. This study examines the variability of aerosols and carbon monoxide (CO) over this remote oceanic region and investigates the underlying processes in the upper troposphere–lower stratosphere (UT-LS). Aerosol profiles in January and February 2020 revealed a multi-layer structure in the tropical UT-LS. Numerical models – the FLEXible PARTicle dispersion model (FLEXPART) and the Modèle Isentropique de transport Mésoéchelle de l'Ozone Stratosphérique par Advection (MIMOSA) – indicated that the lower-stratospheric aerosol content was influenced by the intense and persistent stratospheric aerosol layer generated during the 2019–2020 extreme Australian bushfire events. A portion of this layer was transported eastward by prevailing easterly winds, leading to increased aerosol extinction profiles over Réunion on 27 and 28 January. Analysis of advected potential vorticity revealed isentropic transport of air masses containing Australian biomass burning aerosols from extratropical latitudes to Réunion at the 400 K isentropic level on 28 January. Interestingly, we found that biomass burning (BB) activity in eastern Africa, though weak during this season, significantly influenced (contributed up to 90 % of) the vertical distribution of CO and aerosols in the upper troposphere over the SWIO basin. Ground-based observations at Réunion confirmed the simultaneous presence of African and Australian aerosol layers. This study provides the first evidence of African BB emissions impacting the CO and aerosol distribution in the upper troposphere over the SWIO basin during the convective season.

Improved simulations of biomass burning aerosol optical properties and lifetimes in the NASA GEOS Model during the ORACLES-I campaign

Abstract. 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.

African biomass burning affects aerosol cycling over the Amazon

Smoke from vegetation fires affects air quality, atmospheric cycling, and the climate in the Amazon rain forest. A major unknown has remained the quantity of long-range transported smoke from Africa in relation to local and regional fire emissions. Here we quantify the abundance, seasonality, and properties of African smoke in central Amazonia. We show that it accounts for ~ 60% of the black carbon concentrations during the wet season and ~ 30% during the dry season. The African smoke influences aerosol-radiation interactions across the entire Amazon, with the strongest impact on the vulnerable eastern basin, a hot spot of climate and land use change. Our findings further suggest that the direct influence of African smoke has been historically relevant for soil fertilization, the carbon and water cycles, and, thus, the development of the Amazon forest ecosystem, even in the pre-industrial era.

Intercomparison of airborne and surface-based measurements during the CLARIFY, ORACLES and LASIC field experiments

Abstract. 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.

Undersizing of aged African biomass burning aerosol by an ultra-high-sensitivity aerosol spectrometer

Abstract. The ultra-high-sensitivity aerosol spectrometer (UHSAS) differs from most other optical particle spectrometers by using a high-power infrared (IR) laser to detect small particles and reduce the sizing ambiguity due to the non-monotonicity of scattering with particle size. During the NASA ORACLES project (ObseRvations of Aerosols above CLouds and their intEractionS) over the southeast Atlantic Ocean, the UHSAS clearly undersized particles in the biomass burning plume extending from southern Africa. Since the horizontal and vertical extent of the plume was vast, the NASA P-3B research aircraft often flew through a fairly uniform biomass burning plume for periods exceeding 30 min, sufficient time to explore the details of the UHSAS response by selecting single particle sizes with a differential mobility analyzer (DMA) and passing them to the UHSAS. This was essentially an in-flight calibration of the UHSAS using the particles of interest. Two modes of responses appeared. Most particles were undersized by moderate amounts, ranging from not at all for 70 nm aerosols to 15 % for 280 nm particles. Mie scattering calculations show that composition-dependent refractive index of the particles cannot explain the pattern. Heating of brown carbon or tarballs in the beam causing evaporation and shrinking of the particles is the most plausible explanation, though mis-sizing due to non-sphericity cannot be ruled out. A small fraction (10 %–30 %) of the particles were undersized by 25 % to 35 %. Those were apparently the particles containing refractory black carbon. Laboratory calibrations confirm that black carbon is drastically undersized by the UHSAS, because particles heat to their vaporization point and shrink. A simple empirical correction equation was implemented that dramatically improves agreement with DMA distributions between 100 and 500 nm. It raised the median particle diameter by 18 nm, from 163 to 181 nm, during the August 2017 deployment and by smaller amounts during deployments with less intense pollution. Calculated scattering from UHSAS size distributions increased by about 130 %, dramatically improving agreement with scattering measured by nephelometers. The correction is only valid in polluted instances; clean marine boundary layer and free troposphere aerosols behaved more like the calibration spheres. We were unable to directly test the correction between 500 and 1000 nm, though aerodynamic particle sizer (APS) data appear to show that the correction is poor at the largest diameters, which is no surprise as the composition of those particles is likely to be quite different than that of the accumulation mode. This adds to the evidence that UHSAS data must be treated cautiously whenever the aerosol may absorb infrared light. Similar corrections may be required whenever brown carbon aerosol is present.

Rapid transformation of ambient absorbing aerosols from West African biomass burning

Abstract. Seasonal biomass burning (BB) over West Africa is a globally significant source of carbonaceous particles in the atmosphere, which have important climate impacts but are poorly constrained. Here, the evolution of smoke aerosols emitted from flaming-controlled burning of agricultural waste and wooded savannah in the Senegal region was characterized over a timescale of half-day advection from the source during the MOYA-2017 (Methane Observation Yearly Assessment-2017) aircraft campaign. Plumes from such fire types are rich in black carbon (BC) emissions. Concurrent measurements of chemical composition, organic aerosol (OA) oxidation state, bulk aerosol size and BC mixing state reveal that emitted BB submicron aerosols changed dramatically with time. Various aerosol optical properties (e.g. absorption Ångström exponent – AAE – and mass absorption coefficients – MACs) also evolved with ageing. In this study, brown carbon (BrC) was a minor fractional component of the freshly emitted BB aerosols (< 0.5 h), but the increasing AAE with particle age indicates that BrC formation dominated over any loss process over the first ∼ 12 h of plume transport. Using different methods, the fractional contribution of BrC to total aerosol absorption showed an increasing trend with time and was ∼ 18 %–31 % at the optical wavelength of 405 nm after half-day transport. The generated BrC was found to be positively correlated with oxygenated and low-volatility OA, likely from the oxidation of evaporated primary OA and secondary OA formation. We found that the evolution of BrC with particle age was different in this region compared with previous BB field studies that mainly focused on emissions from smouldering fires, which have shown a high contribution from BrC at the source and BrC net loss upon ageing. This study suggests an initial stage of BrC absorption enhancement during the evolution of BB smoke. Secondary processing is the dominant contributor to BrC production in this BB region, in contrast to the primary emission of BrC previously reported in other BB studies. The total aerosol absorption normalized to BC mass (MACmeas-BC) was also enhanced with ageing due to the lensing effect of increasingly thick coatings on BC and the absorption by BrC. The effect of ageing on aerosol absorption, represented by the absorption enhancement (EAbs-MAC), was estimated over timescales of hours. MOYA-2017 provides novel field results. The comparisons between MOYA-2017 and previous field studies imply that the evolution of absorbing aerosols (BC and BrC) after emission varies with source combustion conditions. Different treatments of absorbing aerosol properties from different types of fires and their downwind evolution should be considered when modelling regional radiative forcing. These observational results will be very important for predicting climate effects of BB aerosol in regions controlled by flaming burning of agricultural waste and savannah-like biomass fuels.

A dynamical pathway bridging African biomass burning and Asian summer monsoon

The Asian summer monsoon (ASM) affects more than one-third of the world’s population due to its close connection with floods, droughts thus water resources in densely populated Asian countries. The effects of aerosols emitted in remote regions on the ASM, in contrast to local emissions, remain largely unclear. Here we demonstrate through a hierarchy of climate models that aerosol emissions from the central African wildfires could strengthen the circulation of the ASM (South Asian Monsoon in particular), increase precipitation over South Asia and reduce precipitation immediately north and south of it. The enhanced latent heating over South Asia provides a critical positive feedback to the initial strengthening of monsoon westerlies associated with wildfire-driven anomalous Rossby wave source. The atmospheric dynamical bridge discovered here effectively connects African biomass burning with hydroclimate variability over East Asia in boreal summer and offers a new source of monsoon predictability across a range of timescales.

Impacts of aerosols produced by biomass burning on the stratocumulus‐to‐cumulus transition in the equatorial Atlantic

AbstractThe impact of aerosols produced by biomass burning on the stratocumulus‐to‐cumulus transition (SCT) in the equatorial Atlantic is studied using satellite‐based and reanalysis data for the month of June. The month of June is highlighted because it represents monsoon onset as well as the largest sea surface temperature gradient in the summer, which is the peak season of tropical African biomass burning. Boundary layer deepening and increasing temperatures put the location of the SCT within the Gulf of Guinea. Satellite retrievals indicate that the bulk of aerosols occur near 1,500 m in altitude, either above or below the boundary layer depending on latitudinal position. Changes in smoke loading over the Gulf of Guinea due to greater transport from southern Africa leads to increases in low‐level cloud cover above cloud decks and decreases when mixed within the boundary layer. Further south, we find significant changes to temperature, cloud top height, tropospheric stability and moisture availability near maximum aerosol loading. In addition, changes in vertical velocity during dirty conditions further reinforce changes in tropospheric stability. These effects combine to shorten the SCT in space during increased aerosol loading episodes.

An overview of the ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) project: aerosol–cloud–radiation interactions in the southeast Atlantic basin

Abstract. Southern Africa produces almost a third of the Earth's biomass burning (BB) aerosol particles, yet the fate of these particles and their influence on regional and global climate is poorly understood. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) is a 5-year NASA EVS-2 (Earth Venture Suborbital-2) investigation with three intensive observation periods designed to study key atmospheric processes that determine the climate impacts of these aerosols. During the Southern Hemisphere winter and spring (June–October), aerosol particles reaching 3–5 km in altitude are transported westward over the southeast Atlantic, where they interact with one of the largest subtropical stratocumulus (Sc) cloud decks in the world. The representation of these interactions in climate models remains highly uncertain in part due to a scarcity of observational constraints on aerosol and cloud properties, as well as due to the parameterized treatment of physical processes. Three ORACLES deployments by the NASA P-3 aircraft in September 2016, August 2017, and October 2018 (totaling ∼350 science flight hours), augmented by the deployment of the NASA ER-2 aircraft for remote sensing in September 2016 (totaling ∼100 science flight hours), were intended to help fill this observational gap. ORACLES focuses on three fundamental science themes centered on the climate effects of African BB aerosols: (a) direct aerosol radiative effects, (b) effects of aerosol absorption on atmospheric circulation and clouds, and (c) aerosol–cloud microphysical interactions. This paper summarizes the ORACLES science objectives, describes the project implementation, provides an overview of the flights and measurements in each deployment, and highlights the integrative modeling efforts from cloud to global scales to address science objectives. Significant new findings on the vertical structure of BB aerosol physical and chemical properties, chemical aging, cloud condensation nuclei, rain and precipitation statistics, and aerosol indirect effects are emphasized, but their detailed descriptions are the subject of separate publications. The main purpose of this paper is to familiarize the broader scientific community with the ORACLES project and the dataset it produced.

Patchwork Earth: navigating pathways to just, thriving, and sustainable futures

Patchwork Earth: navigating pathways to just, thriving, and sustainable futures

Airborne measurements of fire emission factors for African biomass burning sampled during the MOYA campaign

Abstract. Airborne sampling of methane (CH4), carbon dioxide (CO2), carbon monoxide (CO), and nitrous oxide (N2O) mole fractions was conducted during field campaigns targeting fires over Senegal in February and March 2017 and Uganda in January 2019. The majority of fire plumes sampled were close to or directly over burning vegetation, with the exception of two longer-range flights over the West African Atlantic seaboard (100–300 km from source), where the continental outflow of biomass burning emissions from a wider area of West Africa was sampled. Fire emission factors (EFs) and modified combustion efficiencies (MCEs) were estimated from the enhancements in measured mole fractions. For the Senegalese fires, mean EFs and corresponding uncertainties in units of gram per kilogram of dry fuel were 1.8±0.19 for CH4, 1633±171.4 for CO2, and 67±7.4 for CO, with a mean MCE of 0.94±0.005. For the Ugandan fires, mean EFs were 3.1±0.35 for CH4, 1610±169.7 for CO2, and 78±8.9 for CO, with a mean modified combustion efficiency of 0.93±0.004. A mean N2O EF of 0.08±0.002 g kg−1 is also reported for one flight over Uganda; issues with temperature control of the instrument optical bench prevented N2O EFs from being obtained for other flights over Uganda. This study has provided new datasets of African biomass burning EFs and MCEs for two distinct study regions, in which both have been studied little by aircraft measurement previously. These results highlight the important intracontinental variability of biomass burning trace gas emissions and can be used to better constrain future biomass burning emission budgets. More generally, these results highlight the importance of regional and fuel-type variability when attempting to spatially scale biomass burning emissions. Further work to constrain EFs at more local scales and for more specific (and quantifiable) fuel types will serve to improve global estimates of biomass burning emissions of climate-relevant gases.

Characterisation of African biomass burning plumes and impacts on the atmospheric composition over the south-west Indian Ocean

Abstract. We present an investigation of biomass burning (BB) plumes originating from Africa and Madagascar based on measurements of a suite of volatile organic compounds (VOCs), carbon monoxide (CO), ozone (O3) and nitrogen dioxide (NO2) obtained during the dry season of 2018 and 2019 at the high-altitude Maïdo observatory (21.1∘ S, 55.4∘ E, 2160 ma.s.l.), located on the remote island of La Réunion in the south-west Indian Ocean (SWIO). Biomass burning plume episodes were identified from increased acetonitrile (CH3CN) mixing ratios. Enhancement ratios (EnRs) – relative to CO – were calculated from in situ measurements for CH3CN, acetone (CH3COCH3), formic acid (HCOOH), acetic acid (CH3COOH), benzene (C6H6), methanol (CH3OH) and O3. We compared the EnRs to emission ratios (ERs) – relative to CO – reported in the literature in order to estimate loss or production of these compounds during transport. For CH3CN and CH3COOH, the calculated EnRs are similar to the ERs. For C6H6 and CH3OH, the EnR is lower than the ER, indicating a net sink of these compounds which was found to be in line with the expected atmospheric lifetime. For CH3COCH3 and HCOOH, the calculated EnRs are larger than the ERs. The discrepancy reaches an order of magnitude for HCOOH (18–34 pptv ppbv−1 compared to 1.8–4.5 pptv ppbv−1). This points to significant secondary production of HCOOH during transport. The Copernicus Atmospheric Monitoring Service (CAMS) global model simulations reproduce the temporal variation of CO mixing ratios well at the observatory but underestimate O3 and NO2 mixing ratios in the plumes by on average 16 ppbv and 60 pptv respectively. This discrepancy between modelled and measured O3 mixing ratios was attributed to (i) large uncertainties in VOC and NOx (NO+NO2) emissions due to BB in CAMS and (ii) misrepresentation of NOx recycling in the model during transport. Finally, transport of pyrogenically emitted CO is calculated with FLEXPART in order to (i) determine the mean plume age during the intrusions at the observatory and (ii) estimate the impact of BB on the pristine marine boundary layer (MBL). By multiplying the excess CO in the MBL with inferred EnRs at the observatory, we calculated the expected impact of BB on CH3CN, CH3COCH3, CH3OH and C6H6 concentrations in the MBL. These excesses constitute increases of ∼20 %–150 % compared to background measurements in the SWIO MBL reported in the literature.

Comparison of south-east Atlantic aerosol direct radiative effect over clouds from SCIAMACHY, POLDER and OMI–MODIS

Abstract. 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.

Downward cloud venting of the central African biomass burning plume during the West Africa summer monsoon

Abstract. Between June and September large amounts of biomass burning aerosol are released into the atmosphere from agricultural fires in central and southern Africa. Recent studies have suggested that this plume is carried westward over the Atlantic Ocean at altitudes between 2 and 4 km and then northward with the monsoon flow at low levels to increase the atmospheric aerosol load over coastal cities in southern West Africa (SWA), thereby exacerbating air pollution problems. However, the processes by which these fire emissions are transported into the planetary boundary layer (PBL) are still unclear. One potential factor is the large-scale subsidence related to the southern branch of the monsoon Hadley cell over the tropical Atlantic. Here we use convection-permitting model simulations with COSMO-ART to investigate for the first time the contribution of downward mixing induced by clouds, a process we refer to as downward cloud venting in contrast to the more common process of upward transport from a polluted PBL. Based on a monthly climatology, model simulations compare satisfactory with wind fields from reanalysis data, cloud observations, and satellite-retrieved carbon monoxide (CO) mixing ratio. For a case study on 2 July 2016, modelled clouds and rainfall show overall good agreement with Spinning Enhanced Visible and InfraRed Imager (SEVIRI) cloud products and Global Precipitation Measurement Integrated Multi-satellitE Retrievals (GPM-IMERG) rainfall estimates. However, there is a tendency for the model to produce too much clouds and rainfall over the Gulf of Guinea. Using the CO dispersion as an indicator for the biomass burning plume, we identify individual mixing events south of the coast of Côte d'Ivoire due to midlevel convective clouds injecting parts of the biomass burning plume into the PBL. Idealized tracer experiments suggest that around 15 % of the CO mass from the 2–4 km layer is mixed below 1 km within 2 d over the Gulf of Guinea and that the magnitude of the cloud venting is modulated by the underlying sea surface temperatures. There is even stronger vertical mixing when the biomass burning plume reaches land due to daytime heating and a deeper PBL. In that case, the long-range-transported biomass burning plume is mixed with local anthropogenic emissions. Future work should provide more robust statistics on the downward cloud venting effect over the Gulf of Guinea and include aspects of aerosol deposition.

Influx of African biomass burning aerosol during the Amazonian dry season through layered transatlantic transport of black carbon-rich smoke

Abstract. Black carbon (BC) aerosols influence the Earth's atmosphere and climate, but their microphysical properties, spatiotemporal distribution, and long-range transport are not well constrained. This study presents airborne observations of the transatlantic transport of BC-rich African biomass burning (BB) smoke into the Amazon Basin using a Single Particle Soot Photometer (SP2) as well as several complementary techniques. We base our results on observations of aerosols and trace gases off the Brazilian coast onboard the HALO (High Altitude and LOng range) research aircraft during the ACRIDICON-CHUVA campaign in September 2014. During flight AC19 over land and ocean at the northeastern coastline of the Amazon Basin, we observed a BC-rich layer at ∼3.5 km altitude with a vertical extension of ∼0.3 km. Backward trajectories suggest that fires in African grasslands, savannas, and shrublands were the main source of this pollution layer and that the observed BB smoke had undergone more than 10 d of atmospheric transport and aging over the South Atlantic before reaching the Amazon Basin. The aged smoke is characterized by a dominant accumulation mode, centered at about 130 nm, with a particle concentration of Nacc=850±330 cm−3. The rBC particles account for ∼15 % of the submicrometer aerosol mass and ∼40 % of the total aerosol number concentration. This corresponds to a mass concentration range from 0.5 to 2 µg m−3 (1st to 99th percentiles) and a number concentration range from 90 to 530 cm−3. Along with rBC, high cCO (150±30 ppb) and cO3 (56±9 ppb) mixing ratios support the biomass burning origin and pronounced photochemical aging of this layer. Upon reaching the Amazon Basin, it started to broaden and to subside, due to convective mixing and entrainment of the BB aerosol into the boundary layer. Satellite observations show that the transatlantic transport of pollution layers is a frequently occurring process, seasonally peaking in August/September. By analyzing the aircraft observations together with the long-term data from the Amazon Tall Tower Observatory (ATTO), we found that the transatlantic transport of African BB smoke layers has a strong impact on the northern and central Amazonian aerosol population during the BB-influenced season (July to December). In fact, the early BB season (July to September) in this part of the Amazon appears to be dominated by African smoke, whereas the later BB season (October to December) appears to be dominated by South American fires. This dichotomy is reflected in pronounced changes in aerosol optical properties such as the single scattering albedo (increasing from 0.85 in August to 0.90 in November) and the BC-to-CO enhancement ratio (decreasing from 11 to 6 ng m−3 ppb−1). Our results suggest that, despite the high fraction of BC particles, the African BB aerosol acts as efficient cloud condensation nuclei (CCN), with potentially important implications for aerosol–cloud interactions and the hydrological cycle in the Amazon.

A La Niña‐Like Climate Response to South African Biomass Burning Aerosol in CESM Simulations

AbstractThe 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.

Remote biomass burning dominates southern West African air pollution during the monsoon

Abstract. Vast stretches of agricultural land in southern and central Africa are burnt between June and September each year, which releases large quantities of aerosol into the atmosphere. The resulting smoke plumes are carried west over the Atlantic Ocean at altitudes between 2 and 4 km. As only limited observational data in West Africa have existed until now, whether this pollution has an impact at lower altitudes has remained unclear. The Dynamics-aerosol-chemistry-cloud interactions in West Africa (DACCIWA) aircraft campaign took place in southern West Africa during June and July 2016, with the aim of observing gas and aerosol properties in the region in order to assess anthropogenic and other influences on the atmosphere. Results presented here show that a significant mass of aged accumulation mode aerosol was present in the southern West African monsoon layer, over both the ocean and the continent. A median dry aerosol concentration of 6.2 µg m−3 (standard temperature and pressure, STP) was observed over the Atlantic Ocean upwind of the major cities, with an interquartile range from 5.3 to 8.0 µg m−3. This concentration increased to a median of 11.1 µg m−3 (8.6 to 15.7 µg m−3) in the immediate outflow from cities. In the continental air mass away from the cities, the median aerosol loading was 7.5 µg m−3 (5.9 to 10.5 µg m−3). The accumulation mode aerosol population over land displayed similar chemical properties to the upstream population, which implies that upstream aerosol is a significant source of aerosol pollution over the continent. The upstream aerosol is found to have most likely originated from central and southern African biomass burning. This demonstrates that biomass burning plumes are being advected northwards, after being entrained into the monsoon layer over the eastern tropical Atlantic Ocean. It is shown observationally for the first time that they contribute up to 80 % to the regional aerosol loading in the monsoon layer over southern West Africa. Results from the COSMO-ART (Consortium for Small-scale Modeling – Aerosol and Reactive Trace gases) and GEOS-Chem models support this conclusion, showing that observed aerosol concentrations over the northern Atlantic Ocean can only be reproduced when the contribution of transported biomass burning aerosol is taken into account. As a result, the large and growing emissions from the coastal cities are overlaid on an already substantial aerosol background. Simulations using COSMO-ART show that cloud droplet number concentrations can increase by up to 27 % as a result of transported biomass burning aerosol. On a regional scale this renders cloud properties and precipitation less sensitive to future increases in anthropogenic emissions. In addition, such high background loadings will lead to greater pollution exposure for the large and growing population in southern West Africa. These results emphasise the importance of including aerosol from across country borders in the development of air pollution policies and interventions in regions such as West Africa.

African biomass burning is a substantial source of phosphorus deposition to the Amazon, Tropical Atlantic Ocean, and Southern Ocean

The deposition of phosphorus (P) from African dust is believed to play an important role in bolstering primary productivity in the Amazon Basin and Tropical Atlantic Ocean (TAO), leading to sequestration of carbon dioxide. However, there are few measurements of African dust in South America that can robustly test this hypothesis and even fewer measurements of soluble P, which is readily available for stimulating primary production in the ocean. To test this hypothesis, we measured total and soluble P in long-range transported aerosols collected in Cayenne, French Guiana, a TAO coastal site located at the northeastern edge of the Amazon. Our measurements confirm that in boreal spring when African dust transport is greatest, dust supplies the majority of P, of which 5% is soluble. In boreal fall, when dust transport is at an annual minimum, we measured unexpectedly high concentrations of soluble P, which we show is associated with the transport of biomass burning (BB) from southern Africa. Integrating our results into a chemical transport model, we show that African BB supplies up to half of the P deposited annually to the Amazon from transported African aerosol. This observational study links P-rich BB aerosols from Africa to enhanced P deposition in the Amazon. Contrary to current thought, we also show that African BB is a more important source of soluble P than dust to the TAO and oceans in the Southern Hemisphere and may be more important for marine productivity, particularly in boreal summer and fall.

Aerosol influences on low-level clouds in the West African monsoon

Abstract. Low-level clouds (LLCs) cover a wide area of southern West Africa (SWA) during the summer monsoon months and have an important cooling effect on the regional climate. Previous studies of these clouds have focused on modelling and remote sensing via satellite. We present the first comprehensive set of in situ measurements of cloud microphysics from the region, taken during June–July 2016, as part of the DACCIWA (Dynamics–aerosol–chemistry–cloud interactions in West Africa) campaign. This novel dataset allows us to assess spatial, diurnal, and day-to-day variation in the properties of these clouds over the region. LLCs developed overnight and mean cloud cover peaked a few hundred kilometres inland around 10:00 local solar time (LST), before clouds began to dissipate and convection intensified in the afternoon. Regional variation in LLC cover was largely orographic, and no lasting impacts in cloud cover related to pollution plumes were observed downwind of major population centres. The boundary layer cloud drop number concentration (CDNC) was locally variable inland, ranging from 200 to 840 cm−3 (10th and 90th percentiles at standard temperature and pressure), but showed no systematic regional variations. Enhancements were seen in pollution plumes from the coastal cities but were not statistically significant across the region. A significant fraction of accumulation mode aerosols, and therefore cloud condensation nuclei, were from ubiquitous biomass burning smoke transported from the Southern Hemisphere. To assess the relative importance of local and transported aerosol on the cloud field, we isolated the local contribution to the aerosol population by comparing inland and offshore size and composition measurements. A parcel model sensitivity analysis showed that doubling or halving local emissions only changed the calculated cloud drop number concentration by 13 %–22 %, as the high background meant local emissions were a small fraction of total aerosol. As the population of SWA grows, local emissions are expected to rise. Biomass burning smoke transported from the Southern Hemisphere is likely to dampen any effect of these increased local emissions on cloud–aerosol interactions. An integrative analysis between local pollution and Central African biomass burning emissions must be considered when predicting anthropogenic impacts on the regional cloud field during the West African summer monsoon.

Seasonal and diurnal variability in O<sub>3</sub>, black carbon, and CO measured at the Rwanda Climate Observatory

Abstract. Air pollution is understudied in sub-Saharan Africa, resulting in a gap in the scientific understanding of emissions, atmospheric processes, and impacts of air pollutants in this region. The Rwanda Climate Observatory, a joint partnership between MIT and the government of Rwanda, has been measuring ambient concentrations of key long-lived greenhouse gases and the short-lived climate-forcing pollutants CO2, CO, CH4, black carbon (BC), and O3 with state-of-the-art instruments on the summit of Mt. Mugogo (1.586∘ S, 29.566∘ E; 2590 m above sea level) since May 2015. Rwanda is a small, mountainous, and densely populated country in equatorial East Africa, currently undergoing rapid development but still at less than 20 % urbanization. Black carbon concentrations during Rwanda's two dry seasons (December–January–February, DJF, and June–July–August, JJA), which coincide with the two regional biomass burning seasons, are higher at Mt. Mugogo than in major European cities with daily values (24 h) during the dry season of around 5 µg m−3 (daily average concentrations ranging from less than 0.1 to over 17 µg m−3 for the entire measurement period). BC baseline concentrations during biomass burning seasons are loosely correlated with fire radiative power data for the region acquired with a MODIS satellite instrument. The position and meteorology of Rwanda is such that the emissions transported from both the northern and southern African biomass burning seasons affect BC, CO, and O3 concentrations in Rwanda. Spectral aerosol absorption measured with a dual-spot Aethalometer varies seasonally due to changes in types of fuel burned and the direction of pollution transport to the site. Ozone concentrations peaked during Rwanda's dry seasons (daily measured maximum of 70 ppbv). The understanding and quantification of the percent contributions of regional and local (beyond large-scale biomass) emissions is essential to guide policy in the region. During the rainy seasons, local emitting activities (e.g., cooking, transportation, trash burning) remain steady, regional biomass burning is low, and transport distances are shorter as rainout of pollution occurs regularly. Thus, local pollution at Mugogo can be estimated during this time period and was found to account for up to 35 % of annual average BC measured. Our measurements indicate that air pollution is a current and growing problem in equatorial East Africa.