Effects Of Biomass Burning Aerosols Research Articles

Comparing the simulated influence of biomass burning plumes on low-level clouds over the southeastern Atlantic under varying smoke conditions

Abstract. Biomass burning plumes are frequently transported over the southeast Atlantic (SEA) stratocumulus deck during the southern African fire season (June–October). The plumes bring large amounts of absorbing aerosols and enhanced moisture, which can trigger a rich set of aerosol–cloud–radiation interactions with climatic consequences that are still poorly understood. We use large-eddy simulation (LES) to explore and disentangle the individual impacts of aerosols and moisture on the underlying stratocumulus clouds, the marine boundary layer (MBL) evolution, and the stratocumulus-to-cumulus transition (SCT) for three different meteorological situations over the southeast Atlantic during August 2017. For all three cases, our LES shows that the SCT is driven by increased sea surface temperatures and cloud-top entrainment as the air is advected towards the Equator. In the LES model, aerosol indirect effects, including impacts on drizzle production, have a small influence on the modeled cloud evolution and SCT, even when aerosol concentrations are lowered to background concentrations. In contrast, local semi-direct effects, i.e., aerosol absorption of solar radiation in the MBL, cause a reduction in cloud cover that can lead to a speed-up of the SCT, in particular during the daytime and during broken cloud conditions, especially in highly polluted situations. The largest impact on the radiative budget comes from aerosol impacts on cloud albedo: the plume with absorbing aerosols produces a total average 3 d of simulations. We find that the moisture accompanying the aerosol plume produces an additional cooling effect that is about as large as the total aerosol radiative effect. Overall, there is still a large uncertainty associated with the radiative and cloud evolution effects of biomass burning aerosols. A comparison between different models in a common framework, combined with constraints from in situ observations, could help to reduce the uncertainty.

The radiative impact of biomass burning aerosols on dust emissions over Namibia and the long-range transport of smoke observed during the Aerosols, Radiation and Clouds in southern Africa (AEROCLO-sA) campaign

Abstract. The radiative effects of biomass burning aerosols (BBAs) on low-level atmospheric circulation over southern Africa are investigated on 5 September 2017 during the Aerosols, Radiation and Clouds in southern Africa (AEROCLO-sA) field campaign. This is conducted using a variety of in situ and remote sensing observations, as well as two 5 d ensemble simulations made with the Meso-NH mesoscale model, one including the direct and semi-direct radiative effects of aerosols and one in which these effects are not included. We show that the radiative impact of BBA building up over a period of 5 d in the Meso-NH simulations can lead to significantly different circulations at low and middle levels, thereby affecting dust emissions over southern Namibia and northwestern South Africa as well as the transport of BBA in a so-called “river of smoke”. While most of the regional-scale dynamics, thermodynamics and composition features are convincingly represented in the simulation with BBA radiative effects, neglecting the radiative impact of BBA leads to unrealistic representations of (i) the low-level jet (LLJ) over the plateau, which is the main low-level dynamic feature fostering dust emission, and (ii) the mid-level dynamics pertaining to the transport of BBA from the fire-prone regions in the tropics to the mid-latitudes. For instance, when the BBA radiative impacts are not included, the LLJ is too weak and not well established over night, and the developing convective planetary boundary layer (PBL) is too deep compared to observations. The deeper convective PBL over Etosha and surrounding areas is related to the enhanced anomalous upward motion caused by the eastern displacement of the river of smoke. This eastern displacement is, in turn, related to the weaker southerly African easterly jet. Both ensemble simulations provide clear evidence that the enhanced near-surface extinction coefficient values detected from observations over Etosha are related to the downward mixing of BBA in the developing convective boundary layer rather than dust being emitted as a result of the LLJ breakdown after sunrise. This study suggests that the radiative effect of BBAs needs to be taken into account to properly forecast dust emissions in Namibia.

Aerosol Optical Properties of Extreme Global Wildfires and Estimated Radiative Forcing With GCOM‐C SGLI

AbstractTo understand the climate impact of the wildfires, it is essential to monitor the aerosol emissions from biomass burning and to estimate their optical properties and radiative forcing. This study analyzed wildfires in Brazil, Angola, Australia, California, Siberia, and South‐east Asia that occurred after 2018 using data obtained with the Second‐generation GLobal Imager (SGLI) onboard Global Change Observation Mission—Climate which is a polar‐orbit satellite launched by JAXA on 23 December 2017. We showed the SGLI‐based 4‐year variation of the aerosol optical properties, Aerosol Optical Thickness, Ångström Exponent (AE), and Single Scattering Albedo (SSA) for each region complemented with other satellite‐ and ground‐based data. From the SSA and AE relationship analyses, we confirmed that their optical properties depend on the relative humidity and type of burned vegetation, which is consistent with the previous studies. Moreover, we estimated the net incoming radiation at the top of the atmosphere during the intense fire periods to understand the impact of the direct effect of biomass burning aerosols on radiative forcing. The estimates show a significant negative radiative forcing (i.e., a cooling effect) over the ocean (−78 and −96 Wm−2in Australia and California, respectively). In contrast, small values are observed over land (∼−10 Wm−2for all six regions). Therefore, taking the regional characteristics of the optical properties and surface reflectance into account is necessary to estimate the effect on radiative forcing and future impacts of a short‐lived climate forcer from wildfires.

Acceleration of the southern African easterly jet driven by the radiative effect of biomass burning aerosols and its impact on transport during AEROCLO-sA

Abstract. The direct and semi-direct radiative effects of biomass burning aerosols (BBAs) are investigated over southern Africa and the southeastern Atlantic during the Aerosols, Radiation and Clouds in southern Africa (AEROCLO-sA) field campaign in September 2017. A reference convection-permitting simulation has been performed using the Meso-NH model with an online dust emission scheme, a strongly absorbing BBA tracer emitted using the daily Global Fire Emissions Database and online-computed backward Lagrangian trajectories. The simulation captures both the aerosol optical depth and the vertical distribution of aerosols as observed from airborne and spaceborne lidars. The occurrence of stratocumulus over the southeastern Atlantic, deep convective clouds over equatorial Africa and the large-scale circulation are all reproduced by the model. If the radiative effects of BBA are omitted in the model, we show that (i) the smoke plume is too low in altitude, (ii) the low-cloud cover is too weak, (iii) the deep convective activity is too frequent but not intense enough, (iv) the Benguela low-level jet is too strong, and (v) the southern African easterly jet is too weak. The Lagrangian analysis indicates that the radiative effect of BBA leads to the transport of BBA to higher altitudes, farther southwest and with a stronger diurnal oscillation. The higher smoke plume altitude can be explained by a combination of three factors: increased upward motion induced by the stronger southern African easterly jet, self-lofting of BBA and reduced subsidence associated with less frequent deep convective activity over western equatorial Africa.

Seasonal Characteristics, Sources and Pollution Pathways of PM10 at High Altitudes Himalayas of India

The present study represents the annual and seasonal concentration of PM10 over different sites (Darjeeling, Nainital, Mohal-Kullu) across the Himalayan region of India from July 2018 to December 2019. The collected PM10 samples were analyzed for carbonaceous aerosols [organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC), primary organic carbon (POC), secondary organic carbon (SOC)] and major trace elements to inspect their possible sources. The annual average concentrations of PM10 over Mohal-Kullu, Nainital, and Darjeeling were recorded as 57 ± 32 µg m-3, 65 ± 41 µg m-3 and 54 ± 17 µg m-3, respectively. The high OC/EC ratio and significant correlation of OC with EC and WSOC with OC indicated a significant effect of biomass burning aerosols over the study sites. Principal component analysis/absolute principal component score (PCA/APCS) resolved four major sources: crustal/soil dust (26.6%), biomass burning/fossil fuel combustion (28%), vehicular emissions (28%), and industrial emissions/coal combustion (17%). Identification of source region using the potential source contribution function (PSCF) and concentration weighted trajectories (CWT) showed that PM10 were mainly transported from the northwestern part of India (Haryana, Punjab), the northeastern region of Pakistan, the Thar Desert, and Indo-Gangetic Plain (IGP), which contributed to dust-related aerosols over the Himalayan region of India.

Cloud adjustments dominate the overall negative aerosol radiative effects of biomass burning aerosols in UKESM1 climate model simulations over the south-eastern Atlantic

Abstract. 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.

Unexpected Biomass Burning Aerosol Absorption Enhancement Explained by Black Carbon Mixing State

AbstractDirect and semi‐direct radiative effects of biomass burning aerosols (BBA) from southern and central African fires are still widely debated, in particular because climate models have been unsuccessful in reproducing the low single scattering albedo in BBA over the eastern Atlantic Ocean. Using state‐of‐the‐art airborne in situ measurements and Mie scattering simulations, we demonstrate that low single scattering albedo in well‐aged BBA plumes over southern West Africa results from the presence of strongly absorbing refractory black carbon (rBC), whereas the brown carbon contribution to the BBA absorption is negligible. Coatings enhance light absorption by rBC‐containing particles by up to 210%. Our results show that accounting for the diversity in black carbon mixing state by combining internal and external configurations is needed to accurately estimate the optical properties and henceforth the shortwave direct radiative effect and heating rate of BBA over southern West Africa.

The challenge of simulating the sensitivity of the Amazonian cloud microstructure to cloud condensation nuclei number concentrations

Abstract. The realistic representation of aerosol–cloud interactions is of primary importance for accurate climate model projections. The investigation of these interactions in strongly contrasting clean and polluted atmospheric conditions in the Amazon region has been one of the motivations for several field campaigns, including the airborne “Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems–Cloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (Global Precipitation Measurement) (ACRIDICON-CHUVA)” campaign based in Manaus, Brazil, in September 2014. In this work we combine in situ and remotely sensed aerosol, cloud, and atmospheric radiation data collected during ACRIDICON-CHUVA with regional, online-coupled chemistry-transport simulations to evaluate the model's ability to represent the indirect effects of biomass burning aerosol on cloud microphysical and optical properties (droplet number concentration and effective radius). We found agreement between the modeled and observed median cloud droplet number concentration (CDNC) for low values of CDNC, i.e., low levels of pollution. In general, a linear relationship between modeled and observed CDNC with a slope of 0.3 was found, which implies a systematic underestimation of modeled CDNC when compared to measurements. Variability in cloud condensation nuclei (CCN) number concentrations was also underestimated, and cloud droplet effective radii (reff) were overestimated by the model. Modeled effective radius profiles began to saturate around 500 CCN cm−3 at cloud base, indicating an upper limit for the model sensitivity well below CCN concentrations reached during the burning season in the Amazon Basin. Additional CCN emitted from local fires did not cause a notable change in modeled cloud droplet effective radii. Finally, we also evaluate a parameterization of CDNC at cloud base using more readily available cloud microphysical properties, showing that we are able to derive CDNC at cloud base from cloud-side remote-sensing observations.

Biomass burning CCN enhance the dynamics of a mesoscale convective system over the La Plata Basin: a numerical approach

Abstract. High aerosol loadings are discharged into the atmosphere every year by biomass burning in the Amazon and central Brazil during the dry season (July–December). These particles, suspended in the atmosphere, can be carried via a low-level jet toward the La Plata Basin, one of the largest hydrographic basins in the world. Once they reach this region, the aerosols can affect mesoscale convective systems (MCSs), whose frequency is higher during the spring and summer over the basin. The present study is one of the first that seeks to understand the microphysical effects of biomass burning aerosols from the Amazon Basin on mesoscale convective systems over the La Plata Basin. We performed numerical simulations initialized with idealized cloud condensation nuclei (CCN) profiles for an MCS case observed over the La Plata Basin on 21 September 2010. The experiments reveal an important link between CCN number concentration and MCS dynamics, where stronger downdrafts were observed under higher amounts of aerosols, generating more updraft cells in response. Moreover, the simulations show higher amounts of precipitation as the CCN concentration increases. Despite the model's uncertainties and limitations, these results represent an important step toward the understanding of possible impacts on the Amazon biomass burning aerosols over neighboring regions such as the La Plata Basin.

Impact of Biomass Burning Aerosols on the Diurnal Cycle of Convective Clouds and Precipitation Over a Tropical Island

AbstractA coupled weather‐aerosol model is used to study the effect of biomass burning aerosols on deep convection over the Borneo Island and surrounding oceans. Simulations are performed at the convection‐permitting scale (4 km) for 40 days during the boreal summer and include interactive fire emissions and the aerosol effect on radiative and microphysical processes. Intense burning occurs daily in the southern part of the island, and smoke propagates northward to regions of deep convection. The model captures well the observed diurnal cycle of precipitation and high cloud cover. Cloud microphysics and radiative aerosol impacts are considered separately. Modifications of the cloud microphysics by smoke aerosols reinforce deep convection near the central Borneo mountainous region. This reinforced convection is due to reduced shallow precipitation in the afternoon that leads to a warm planetary boundary layer anomaly at sunset enhancing deep convection at night. Aerosol absorptive properties strongly affect local and synoptic atmospheric responses. The radiative processes of moderately absorbing aerosols tend to reduce deep convection over most regions due to local surface cooling and atmosphere warming that increase the static stability. For more absorbing aerosols, however, the impact is reversed with increased nighttime convection over most regions. This is partly related to changes in the vertical water vapor divergence profiles that decrease the convergence toward Borneo for moderately absorbing aerosols and increase it for more absorbing ones. These changes in the synoptic circulation due to large‐scale aerosol perturbations are as important as local processes to explain the observed rainfall perturbation patterns.

Modeling the radiative effects of biomass burning aerosols on carbon fluxes in the Amazon region.

Every year, a dense smoke haze covers a large portion of South America originating from fires in the Amazon Basin and central parts of Brazil during the dry biomass burning season between August and October. Over a large portion of South America, the average aerosol optical depth at 550 nm exceeds 1.0 during the fire season, while the background value during the rainy season is below 0.2. Biomass burning aerosol particles increase scattering and absorption of the incident solar radiation. The regional-scale aerosol layer reduces the amount of solar energy reaching the surface, cools the near-surface air, and increases the diffuse radiation fraction over a large disturbed area of the Amazon rainforest. These factors affect the energy and CO2 fluxes at the surface. In this work, we applied a fully integrated atmospheric model to assess the impact of biomass burning aerosols in CO2 fluxes in the Amazon region during 2010. We address the effects of the attenuation of global solar radiation and the enhancement of the diffuse solar radiation flux inside the vegetation canopy. Our results indicate that biomass burning aerosols led to increases of about 27% in the gross primary productivity of Amazonia and 10% in plant respiration as well as a decline in soil respiration of 3%. Consequently, in our model Amazonia became a net carbon sink; net ecosystem exchange during September 2010 dropped from +101 to -104 TgC when the aerosol effects are considered, mainly due to the aerosol diffuse radiation effect. For the forest biome, our results point to a dominance of the diffuse radiation effect on CO2 fluxes, reaching a balance of 50-50% between the diffuse and direct aerosol effects for high aerosol loads. For C3 grasses and savanna (cerrado), as expected, the contribution of the diffuse radiation effect is much lower, tending to zero with the increase in aerosol load. Taking all biomes together, our model shows the Amazon during the dry season, in the presence of high biomass burning aerosol loads, changing from being a source to being a sink of CO2 to the atmosphere.

Impact of anomalous forest fire on aerosol radiative forcing and snow cover over Himalayan region

Forest fires are very common in tropical region during February–May months and are known to have significant impact on ecosystem dynamics. Moreover, aerosols emitted from these burning activities significantly modulate the Earth's radiation budget. In present study, we investigated the anomalous forest fire events and their impact on atmospheric radiation budget and glaciated snow cover over the Himalayan region. We used multiple dataset derived from satellites [Moderate Resolution Spectroradiometer (MODIS) and Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO)] and reanalysis models [Global Fire Assimilation System (GFAS), Second Modern-Era Retrospective analysis for Research and Application (MERRA-2) and ERA-interim] to evaluate the effect of biomass burning aerosols on radiation budget. April 2016 is associated with anomalous fire activities over lower Himalayan region in the last fourteen years (2003–2016). The model estimated organic carbon (OC) and black carbon (BC) emission reaches up to ∼3 × 104 and ∼2 × 103 μg/m2/day, respectively during the biomass burning period of April 2016. The meteorological data analysis accompanied with CALIOP aerosol vertical profile shows that these carbonaceous aerosols could reach up to ∼5–7 km altitude and could be transported towards glaciated region of upper Himalayas. The large amount of BC/OC from biomass burning significantly modulates the atmospheric radiation budget. The estimated columnar heating rate shows that these carbonaceous aerosols could heat up the atmosphere by ∼0.04–0.06 K/day in April-2016 with respect to non-burning period (2015). The glaciated snow cover fractions are found to be decreasing by ∼5–20% in 2016 as compared to long term mean (2003–2016). The combined analyses of various climatic factors, fires and associated BC emissions show that the observed snow cover decrease could be results of increased surface/atmospheric temperature due to combined effect of large scale climatic changes and BC absorption. Our results suggest that biomass burning can have significant effects on the Himalayan region, particularly in view of its importance in hydrological cycle and ecosystem.

Deriving aerosol hygroscopic mixing state from size-resolved CCN activity and HR-ToF-AMS measurements

The ability of a particle to uptake water and form a cloud droplet depends on its hygroscopicity. To understand its impact on cloud properties and ultimately radiative forcing, knowledge of chemically-resolved mixing state information or the one based on hygroscopic growth is crucial. Typically, global models assume either pure internal or external mixing state which might not be true for all conditions and sampling locations. To investigate into this, the current study employed an indirect approach to infer the probable mixing state. The hygroscopic parameters derived from κ-Kohler theory using size-resolved CCN measurements (κCCN) and bulk/size-resolved aerosol mass spectrometer (AMS) measurements (κAMS) were compared. The accumulation mode particles were found to be more hygroscopic (κCCN = 0.24) than Aitken mode (κCCN = 0.13), perhaps due to increased ratio of inorganic to organic mass fraction. The activation diameter calculated from size-resolved CCN activity measurements at 5 different supersaturation (SS) levels varied in the range of 115 nm–42 nm with κCCN = 0.13–0.23 (avg = 0.18 ± 0.10 (±1σ)). Further, κAMS>κCCN was observed possibly due to the fact that organic and inorganic mass present in the Aitken mode was not correctly represented by bulk chemical composition and size-resolved fractional contribution of oxidized OA was not accurately accounted. Better correlation of organic fraction (forg) and κCCN at lower SS explained this behaviour. The decrease in κCCN with the time of the day was more pronounced at lower SS because of the relative mass reduction of soluble inorganic species by ∼17%.Despite the large differences between κ measured from two approaches, less over-prediction (up to 18%) between measured and predicted CCN concentration suggested lower impact of chemical composition and mixing state at higher SS. However, at lower SS, presences of externally mixed CCN-inactive aerosols lead to CCN over-prediction reflecting the significance of aerosol mixing state information. Further examination of the effect of biomass burning aerosols (∼35% in least oxidized biomass burning organic aerosol (BBOA-2 fraction) on hygroscopicity and CCN activity showed increase in the concentration of all AMS measured species (except NH4+ and SO42−), less O:C ratio, and organic mass fraction (forg) peak shift to lower diameter range caused ∼13% change in critical diameter (Da) and ∼40% change in κCCN. Increased deviation of ∼100% between κCCN and κAMS due to sudden influx of internally mixed BBOA caused suppressed hygroscopic growth. This study finally suggests the assumption of pure internally mixed aerosol does not completely hold true for this anthropogenically polluted site.

OMI tropospheric NO<sub>2</sub> air mass factors over South America: effects of biomass burning aerosols

Abstract. Biomass burning is an important and uncertain source of aerosols and NOx (NO + NO2) to the atmosphere. Satellite observations of tropospheric NO2 are essential for characterizing this emissions source, but inaccuracies in the retrieval of NO2 tropospheric columns due to the radiative effects of aerosols, especially light-absorbing carbonaceous aerosols, are not well understood. It has been shown that the O2–O2 effective cloud fraction and pressure retrieval is sensitive to aerosol optical and physical properties, including aerosol optical depth (AOD). Aerosols implicitly influence the tropospheric air mass factor (AMF) calculations used in the NO2 retrieval through the effective cloud parameters used in the independent pixel approximation. In this work, we explicitly account for the effects of biomass burning aerosols in the Ozone Monitoring Instrument (OMI) tropospheric NO2 AMF calculation for cloud-free scenes. We do so by including collocated aerosol extinction vertical profile observations from the CALIOP instrument, and aerosol optical depth (AOD) and single scattering albedo (SSA) retrieved by the OMI near-UV aerosol algorithm (OMAERUV) in the DISAMAR radiative transfer model. Tropospheric AMFs calculated with DISAMAR were benchmarked against AMFs reported in the Dutch OMI NO2 (DOMINO) retrieval; the mean and standard deviation of the difference was 0.6 ± 8 %. Averaged over three successive South American biomass burning seasons (2006–2008), the spatial correlation in the 500 nm AOD retrieved by OMI and the 532 nm AOD retrieved by CALIOP was 0.6, and 68 % of the daily OMAERUV AOD observations were within 30 % of the CALIOP observations. Overall, tropospheric AMFs calculated with observed aerosol parameters were on average 10 % higher than AMFs calculated with effective cloud parameters. For effective cloud radiance fractions less than 30 %, or effective cloud pressures greater than 800 hPa, the difference between tropospheric AMFs based on implicit and explicit aerosol parameters is on average 6 and 3 %, respectively, which was the case for the majority of the pixels considered in our study; 70 % had cloud radiance fraction below 30 %, and 50 % had effective cloud pressure greater than 800 hPa. Pixels with effective cloud radiance fraction greater than 30 % or effective cloud pressure less than 800 hPa corresponded with stronger shielding in the implicit aerosol correction approach because the assumption of an opaque effective cloud underestimates the altitude-resolved AMF; tropospheric AMFs were on average 30–50 % larger when aerosol parameters were included, and for individual pixels tropospheric AMFs can differ by more than a factor of 2. The observation-based approach to correcting tropospheric AMF calculations for aerosol effects presented in this paper depicts a promising strategy for a globally consistent aerosol correction scheme for clear-sky pixels.

The Role of Clouds in Modulating Global Aerosol Direct Radiative Effects in Spaceborne Active Observations and the Community Earth System Model

Abstract Observational benchmarks of global and regional aerosol direct radiative effects, over all surfaces and all sky conditions, are generated using CloudSat’s new multisensor radiative fluxes and heating rates product. Improving upon previous techniques, the approach leverages the capability of CloudSat and CALIPSO to retrieve vertically resolved estimates of cloud and aerosol properties required for complete and accurate assessment of aerosol direct effects under all conditions. The global annually averaged aerosol direct radiative effect is estimated to be −1.9 W m−2 with an uncertainty range of ±0.6 W m−2, which is in better agreement with previously published estimates from global models than previous satellite-based estimates. Detailed comparisons against a fully coupled simulation of the Community Earth System Model, however, reveal that this agreement on the global annual mean masks large regional discrepancies between modeled and observed estimates of aerosol direct effects. A series of regional analyses demonstrate that, in addition to previously documented biases in simulated aerosol distributions, the magnitude and sign of these discrepancies are often related to model biases in the geographic and seasonal distribution of clouds. A low bias in stratocumulus cloud cover over the southeastern Pacific, for example, leads to an overestimate of the radiative effects of marine aerosols in the region. Likewise, errors in the seasonal cycle of low clouds in the southeastern Atlantic distort the radiative effects of biomass burning aerosols from southern Africa. These findings indicate that accurate assessment of aerosol direct effects requires models to correctly represent not only the source, strength, and optical properties of aerosols, but their relative proximity to clouds as well.

Rapid changes in biomass burning aerosols by atmospheric oxidation

Primary and secondary aerosol particles originating from biomass burning contribute significantly to the atmospheric aerosol budget and thereby to both direct and indirect radiative forcing. Based on detailed measurements of a large number of biomass burning plumes of variable age in southern Africa, we show that the size distribution, chemical composition, single-scattering albedo, and hygroscopicity of biomass burning particles change considerably during the first 2–4 h of their atmospheric transport. These changes, driven by atmospheric oxidation and subsequent secondary aerosol formation, may reach a factor of 6 for the aerosol scattering coefficient and a factor >10 for the cloud condensation nuclei concentration. Since the observed changes take place over the spatial and temporal scales that are neither covered by emission inventories nor captured by large-scale model simulations, the findings reported here point out a significant gap in our understanding on the climatic effects of biomass burning aerosols.

Spatial variability of the direct radiative forcing of biomass burning aerosols and the effects of land use change in Amazonia

Abstract. This paper addresses the Amazonian shortwave radiative budget over cloud-free conditions after considering three aspects of deforestation: (i) the emission of aerosols from biomass burning due to forest fires; (ii) changes in surface albedo after deforestation; and (iii) modifications in the column water vapour amount over deforested areas. Simultaneous Clouds and the Earth's Radiant Energy System (CERES) shortwave fluxes and aerosol optical depth (AOD) retrievals from the Moderate Resolution Imaging SpectroRadiometer (MODIS) were analysed during the peak of the biomass burning seasons (August and September) from 2000 to 2009. A discrete-ordinate radiative transfer (DISORT) code was used to extend instantaneous remote sensing radiative forcing assessments into 24-h averages. The mean direct radiative forcing of aerosols at the top of the atmosphere (TOA) during the biomass burning season for the 10-yr studied period was −5.6 ± 1.7 W m−2. Furthermore, the spatial distribution of the direct radiative forcing of aerosols over Amazonia was obtained for the biomass burning season of each year. It was observed that for high AOD (larger than 1 at 550 nm) the maximum daily direct aerosol radiative forcing at the TOA may be as high as −20 W m−2 locally. The surface reflectance plays a major role in the aerosol direct radiative effect. The study of the effects of biomass burning aerosols over different surface types shows that the direct radiative forcing is systematically more negative over forest than over savannah-like covered areas. Values of −15.7 ± 2.4 W m−2τ550 nm and −9.3 ± 1.7 W m−2τ550 nm were calculated for the mean daily aerosol forcing efficiencies over forest and savannah-like vegetation respectively. The overall mean annual land use change radiative forcing due to deforestation over the state of Rondônia, Brazil, was determined as −7.3 ± 0.9 W m−2. Biomass burning aerosols impact the radiative budget for approximately two months per year, whereas the surface albedo impact is observed throughout the year. Because of this difference, the estimated impact in the Amazonian annual radiative budget due to surface albedo-change is approximately 6 times higher than the impact due to aerosol emissions. The influence of atmospheric water vapour content in the radiative budget was also studied using AERONET column water vapour. It was observed that column water vapour is on average smaller by about 0.35 cm (around 10% of the total column water vapour) over deforested areas compared to forested areas. Our results indicate that this drying contributes to an increase in the shortwave radiative forcing, which varies from 0.4 W m−2 to 1.2 W m−2 depending on the column water vapour content before deforestation. The large radiative forcing values presented in this study point out that deforestation could have strong implications in convection, cloud development and the ratio of direct to diffuse radiation, which impacts carbon uptake by the forest.

Cloud condensation nuclei activity of fresh primary and aged biomass burning aerosol

Abstract. We quantify the hygroscopic properties of particles freshly emitted from biomass burning and after several hours of photochemical aging in a smog chamber. Values of the hygroscopicity parameter, κ, were calculated from cloud condensation nuclei (CCN) measurements of emissions from combustion of 12 biomass fuels commonly burned in North American wildfires. Prior to photochemical aging, the κ of the fresh primary aerosol varied widely, between 0.06 (weakly hygroscopic) and 0.6 (highly hygroscopic). The hygroscopicity of the primary aerosol was positively correlated with the inorganic mass fraction of the particles. Photochemical processing reduced the range of κ values to between 0.08 and 0.3. The changes in κ were driven by the photochemical production of secondary organic aerosol (SOA). SOA also contributed to growth of particles formed during nucleation events. Analysis of the nucleation mode particles enabled the first direct quantification of the hygroscopicity parameter κ for biomass burning SOA, which was on average 0.11, similar to values observed for biogenic SOA. Although initial CCN activity of biomass burning aerosol emissions are highly variable, after a few hours of photochemical processing κ converges to a value of 0.2 ± 0.1. Therefore, photochemical aging reduces the variability of biomass burning CCN κ, which should simplify analysis of the potential effects of biomass burning aerosol on climate.

Regional simulations of deep convection and biomass burning over South America: 2. Biomass burning aerosol effects on clouds and precipitation

[1] A fully coupled meteorology-chemistry-aerosol mesoscale model (WRF-Chem) is used to simulate a multiday biomass burning event in the dry season of South America. The effects of biomass burning aerosols on clouds and precipitation are described at both 36 km and 4 km horizontal resolutions. The dominant effect of the aerosols is to reduce the diurnal amplitude of convection by decreasing clouds and precipitation in the afternoon but increasing them at night, with the afternoon decrease greater than the nighttime increase on the daily mean. On average, the decrease of surface precipitation is about 5% (3%) and the amplitude of diurnal cycle is reduced by about 11% (5%) in the 36 km (4 km) simulations. Such a modulation of clouds and precipitation is primarily contributed by the aerosol radiative effect, i.e., their ability to scatter and absorb solar radiation. The aerosol microphysical effect as cloud condensation nuclei tends to act oppositely to the aerosol radiative effect but with a smaller magnitude, especially in the simulations at 36 km horizontal resolution. The 4 km resolution runs exhibit similar behaviors to the 36 km simulations, with a slightly stronger role of the aerosol microphysical effect relative to the aerosol radiative effect. We find another important effect of biomass burning aerosols. When uplifted into the upper troposphere by deep convection, they can significantly warm the upper troposphere through their local radiative heating effect and result in significant moistening in the upper troposphere, potentially affecting the water vapor transport from the troposphere to the stratosphere.

Direct and semidirect aerosol effects of southern African biomass burning aerosol

[1] Direct and semidirect radiative effects of biomass burning aerosols from southern African fires during July–October are investigated using 20 year runs of the Community Atmospheric Model (CAM) coupled to a slab ocean model. Aerosol optical depth is constrained using observations in clear skies from Moderate Resolution Imaging Spectroradiometer (MODIS) and for aerosol layers above clouds from Cloud Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO). Over the ocean, where the aerosol layers are primarily located above cloud, negative top of atmosphere (TOA) semidirect radiative effects associated with increased low cloud cover dominate over a weaker positive all-sky direct radiative effect (DRE). In contrast, over the land where the aerosols are often below or within cloud layers, reductions in cloud liquid water path (LWP) lead to a positive semidirect radiative effect that dominates over a near-zero DRE. Over the ocean, the cloud response can be understood as a response to increased lower tropospheric stability (LTS) which is caused both by radiative heating in overlying layers and surface cooling in response to direct aerosol forcing. The marine cloud changes are robust to changes in the cloud parameterization (removal of the hard-wired dependence of clouds on LTS), suggesting that they are physically realistic. Over land, decreased LWP is consistent with weaker convection driven by increased static stability. Over the entire region the overall TOA radiative effect from the biomass burning aerosols is almost zero due to opposing effects over the land and ocean. However, the surface forcing is strongly negative, which leads to a reduction in precipitation and also a reduction in sensible heat flux. The former is primarily realized through reductions in convective precipitation on both the southern and northern flanks of the convective precipitation region spanning the equatorial rain forest and the Intertropical Convergence Zone (ITCZ) in the southern Sahel. The changes are consistent with the low-level aerosol-forced cooling pattern. The results highlight the importance of semidirect radiative effects and precipitation responses for determining the climatic effects of aerosols in the African region.