Biomass Burning Aerosol Emissions Research Articles

Measurement report: Assessing the impacts of emission uncertainty on aerosol optical properties and radiative forcing from biomass burning in peninsular Southeast Asia

Abstract. Despite significant advancements in improving the dataset for biomass burning (BB) emissions over the past few decades, uncertainties persist in BB aerosol emissions, impeding the accurate assessment of simulated aerosol optical properties (AOPs) and direct radiative forcing (DRF) during wildfire events in global and regional models. This study assessed AOPs (including aerosol optical depth (AOD), aerosol absorption optical depth (AAOD), and aerosol extinction coefficients (AECs)) and DRF using eight independent BB emission inventories applied to the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) during the BB period (March 2019) in peninsular Southeast Asia (PSEA), where the eight BB emission inventories were the Global Fire Emissions Database version 4.1s (GFED), Fire INventory from NCAR version 1.5 (FINN1.5), the Fire Inventory from NCAR version 2.5 MOS (MODIS fire detections; FINN2.5 MOS), the Fire Inventory from NCAR version 2.5 MOSVIS (MODIS + VIIRS fire detections; FINN2.5 MOSVIS), Global Fire Assimilation System version 1.2s (GFAS), Fire Energetics and Emissions Research version 1.0 (FEER), Quick Fire Emissions Dataset version 2.5 release 1 (QFED), and Integrated Monitoring and Modelling System for Wildland FIRES project version 2.0 (IS4FIRES), respectively. The results show that in the PSEA region, organic carbon (OC) emissions in the eight BB emission inventories differ by a factor of about 9 (0.295–2.533 Tg M−1), with 1.09 ± 0.83 Tg M−1 and a coefficient of variation (CV) of 76 %. High-concentration OC emissions occurred primarily in savanna and agricultural fires. The OC emissions from the GFED and GFAS are significantly lower than the other inventories. The OC emissions in FINN2.5 MOSVIS are approximately twice as high as those in FINN1.5. Sensitivity analysis of AOD simulated by WRF-Chem to different BB emission datasets indicated that the FINN scenarios (v1.5 and 2.5) significantly overestimate AOD compared to observation (VIIRS), while the other inventories underestimate AOD in the high-AOD (HAOD; AOD > 1) regions range from 15–22.5∘ N, 97–110∘ E. Among the eight schemes, IS4FIRES and FINN1.5 performed better in terms of AOD simulation consistency and bias in the HAOD region when compared to AERONET sites. The AAOD in WRF-Chem during the PSEA wildfire period was assessed, using satellite observations (TROPOMI) and AERONET data, and it was found that the AAOD simulated with different BB schemes did not perform as well as the AOD. The significant overestimation of AAOD by FINN (v1.5 and 2.5), FEER, and IS4FIRES schemes in the HAOD region, with the largest overestimation for FINN2.5 MOSVIS. FINN1.5 schemes performed better in representing AAOD at AERONET sites within the HAOD region. The simulated AOD and AAOD from FINN2.5 MOSVIS always show the best correlation with the observations. AECs simulated by WRF-Chem with all the eight BB schemes trends were consistent with CALIPSO in the vertical direction (0.5 to 4 km), demonstrating the efficacy of the smoke plume rise model used in WRF-Chem to simulate smoke plume heights. However, the FINN (v1.5 and 2.5) schemes overestimated AECs, while the other schemes underestimated it. In the HAOD region, BB aerosols exhibited a daytime shortwave radiative forcing of −32.60 ± 24.50 W m−2 at the surface, positive forcing (1.70 ± 1.40 W m−2) in the atmosphere, and negative forcing (−30.89 ± 23.6 W m−2) at the top of the atmosphere. Based on the analysis, FINN1.5 and IS4FIRES are recommended for accurately assessing the impact of BB on air quality and climate in the PSEA region.

Impact of regional climate patterns on the biomass burning emissions and transport over Peninsular Southeast Asia, 2000-2019

The regional climate variability in peninsular Southeast Asia (PSEA) can influence springtime biomass burning (BB) aerosol emissions and associated transport patterns. To comprehend the interannual variation of regional climate and its impact on PSEA BB, a diagnostic analysis based on the Modern-Era Retrospective Analysis for Research and Applications version 2 (MERRA-2) dataset and Moderate Resolution Imaging Spectroradiometer (MODIS) observations from 2000 to 2019 has presented. Employing principal component, composite, and correlation analyses, this study identified four climatic factors governing the emission and transport of PSEA BB aerosols: (i) a low-level anticyclone (suppressed monsoon trough) in the Bay of Bengal, (ii) the relative strength of the anticyclone over the South China Sea, (iii) the Pacific subtropical high, and (iv) low-level westerlies from PSEA to Taiwan. Additionally, BB emissions and transport significantly correlate with the El Niño-Southern Oscillation (ENSO). In the El Niño year, increased anticyclones in the Bay of Bengal and South China Sea accompanied the stronger westerlies, which enhanced BB aerosol emission and transport. The diagnostic results of this study can contribute to a better understanding and improved model simulations of aerosol-climate interactions in South and Southeast Asian monsoon regions.

Isolating the effect of biomass burning aerosol emissions on 20th century hydroclimate in South America and Southeast Asia

Biomass burning is a significant source of aerosol emissions in some regions and has a considerable impact on regional climate. Earth system model simulations indicate that increased biomass burning aerosol emissions contributed to statistically significant decreases in tropical precipitation over the 20th century. In this study, we use the Community Earth System Model version 1 Large Ensemble (CESM1-LENS) experiment to evaluate the mechanisms by which biomass burning aerosol contributed to decreased tropical precipitation, with a focus on South America and Southeast Asia. We analyze the all-but-one forcing simulations in which biomass burning aerosol emissions are held constant while other forcings (e.g., greenhouse gas concentrations) vary throughout the 20th century. This allows us to isolate the influence of biomass burning aerosol on processes that contribute to decreasing precipitation, including cloud microphysics, the radiative effects of absorbing aerosol particles, and alterations in regional circulation. We also show that the 20th century reduction in precipitation identified in the CESM1-LENS historical and biomass burning experiments is consistent across Coupled Model Intercomparison Project Phase 5 models with interactive aerosol schemes and the CESM2 single-forcing experiment. Our results demonstrate that higher concentrations of biomass burning aerosol increases the quantity of cloud condensation nuclei and cloud droplets, limiting cloud droplet size and precipitation formation. Additionally, absorbing aerosols (e.g., black carbon) contribute to a warmer cloud layer, which promotes cloud evaporation, increases atmospheric stability, and alters regional circulation patterns. Corresponding convectively coupled circulation responses, particularly over the tropical Andes, contribute to further reducing the flow of moisture and moisture convergence over tropical land. These results elucidate the processes that affect the water cycle in regions prone to biomass burning and inform our understanding of how future changes in aerosol emissions may impact tropical precipitation over the 21st century.

Interannual fires as a source for subarctic summer decadal climate variability mediated by permafrost thawing

Climate model simulations run under the Coupled Model Intercomparison Project Phase 6 (CMIP6) use an inhomogeneous biomass burning aerosol (BBA) emission dataset, which exhibits pronounced interannual variability from 1997–2014 due to the infusion of satellite data. Using the Community Earth System Model version 2 Large Ensemble (CESM2-LE) with original and smoothed CMIP6 BBA forcings, we show that the CMIP6 data inhomogeneity causes spurious decadal subarctic land warming. During years with reduced aerosol concentrations, increased solar radiation can trigger abrupt subarctic permafrost thawing, increased soil water drainage, upper soil drying, and subsequent surface warming. This slow process, which is further amplified by nonlinear cloud-aerosol interactions, cannot be completely offset during years of increased aerosol fluxes, thereby reddening surface temperature spectra in response to large-amplitude interannual aerosol forcing. More generally, our CESM2 experiments identify a pathway for generating decadal variability in high latitudes, involving interannual shortwave forcing and slow nonlinear soil responses.

Internal variability and forcing influence model–satellite differences in the rate of tropical tropospheric warming

Climate-model simulations exhibit approximately two times more tropical tropospheric warming than satellite observations since 1979. The causes of this difference are not fully understood and are poorly quantified. Here, we apply machine learning to relate the patterns of surface-temperature change to the forced and unforced components of tropical tropospheric warming. This approach allows us to disentangle the forced and unforced change in the model-simulated temperature of the midtroposphere (TMT). In applying the climate-model-trained machine-learning framework to observations, we estimate that external forcing has produced a tropical TMT trend of 0.25 ± 0.08 K⋅decade-1 between 1979 and 2014, but internal variability has offset this warming by 0.07 ± 0.07 K⋅decade-1. Using the Community Earth System Model version 2 (CESM2) large ensemble, we also find that a discontinuity in the variability of prescribed biomass-burning aerosol emissions artificially enhances simulated tropical TMT change by 0.04 K⋅decade-1. The magnitude of this aerosol-forcing bias will vary across climate models, but since the latest generation of climate models all use the same emissions dataset, the bias may systematically enhance climate-model trends over the satellite era. Our results indicate that internal variability and forcing uncertainties largely explain differences in satellite-versus-model warming and are important considerations when evaluating climate models.

Satellite-based evaluation of AeroCom model bias in biomass burning regions

Abstract. Global models are widely used to simulate biomass burning aerosol (BBA). Exhaustive evaluations on model representation of aerosol distributions and properties are fundamental to assess health and climate impacts of BBA. Here we conducted a comprehensive comparison of Aerosol Comparisons between Observations and Models (AeroCom) project model simulations with satellite observations. A total of 59 runs by 18 models from three AeroCom Phase-III experiments (i.e., biomass burning emissions, CTRL16, and CTRL19) and 14 satellite products of aerosols were used in the study. Aerosol optical depth (AOD) at 550 nm was investigated during the fire season over three key fire regions reflecting different fire dynamics (i.e., deforestation-dominated Amazon, Southern Hemisphere Africa where savannas are the key source of emissions, and boreal forest burning in boreal North America). The 14 satellite products were first evaluated against AErosol RObotic NETwork (AERONET) observations, with large uncertainties found. But these uncertainties had small impacts on the model evaluation that was dominated by modeling bias. Through a comparison with Polarization and Directionality of the Earth’s Reflectances measurements with the Generalized Retrieval of Aerosol and Surface Properties algorithm (POLDER-GRASP), we found that the modeled AOD values were biased by −93 % to 152 %, with most models showing significant underestimations even for the state-of-the-art aerosol modeling techniques (i.e., CTRL19). By scaling up BBA emissions, the negative biases in modeled AOD were significantly mitigated, although it yielded only negligible improvements in the correlation between models and observations, and the spatial and temporal variations in AOD biases did not change much. For models in CTRL16 and CTRL19, the large diversity in modeled AOD was in almost equal measures caused by diversity in emissions, lifetime, and the mass extinction coefficient (MEC). We found that in the AeroCom ensemble, BBA lifetime correlated significantly with particle deposition (as expected) and in turn correlated strongly with precipitation. Additional analysis based on Cloud-Aerosol LIdar with Orthogonal Polarization (CALIOP) aerosol profiles suggested that the altitude of the aerosol layer in the current models was generally too low, which also contributed to the bias in modeled lifetime. Modeled MECs exhibited significant correlations with the Ångström exponent (AE, an indicator of particle size). Comparisons with the POLDER-GRASP-observed AE suggested that the models tended to overestimate the AE (underestimated particle size), indicating a possible underestimation of MECs in models. The hygroscopic growth in most models generally agreed with observations and might not explain the overall underestimation of modeled AOD. Our results imply that current global models contain biases in important aerosol processes for BBA (e.g., emissions, removal, and optical properties) that remain to be addressed in future research.

Comparison of the impacts due to biomass burning, anthropogenic, and biogenic aerosol emissions on the mature phase of an urban heavy precipitation event over the Pearl River Delta

The study is aimed to discuss the differences in the aerosol impacts on the precipitation in mature phase due to three different aerosol emission sources, the biomass burning emission (BB), the anthropogenic emission (AE), and the biogenic emission (BE). Four simulations were conducted using WRF-Chem version 4.1.2 on the heavy urban precipitation event over the Pearl River Delta (PRD) region, which occurred on 21 February 2019, with 0800–0900 UTC 21 February as the mature phase. The inclusion of aerosol emissions improved the simulation performance on the temporal variations of the precipitation event and the peak precipitation. BB, AE, and BE contributed to the aerosol loading by around 6.8%, 88.1%, and 5.1%, respectively; and weakened the precipitation 28.0%, 31.0%, and 14.1%, respectively. The BE impact occurred the latest during the developing phase. The weakening effect was mainly over the convective precipitation. The aerosol indirect effect of BE strengthened the stratiform precipitation. The weakened convective precipitation was contributed by the weakened cloud microphysical processes above the zero-isotherm line. The BB impact induced the smallest change in cloud microphysical latent heating and weakened the precipitation more likely via its aerosol direct effect. The AE impact was the largest in precipitation, convection, and the cloud microphysical latent heating.

Impacts of oxidizer concentration and fuel composition on near-source aerosol emissions from lignocellulosic biomass and constituent burning

Biomass burning (BB), a multi-step process including drying, devolatilization, and oxidation of volatiles and char, is a globally occurring phenomenon that is understood to produce significant quantities of aerosols that have a broad range of local and global effects on humans and the environment. Quantities and properties of BB-derived aerosols are difficult to predict due to the complex nature of BB. Near-source conditions, such as oxygen availability and fuel composition, have been identified as influential factors in the properties of aerosol emissions. This work examined the total and size-resolved number and mass aerosol emission factors from dry, pulverized lignocellulosic biomass and its major constituents under laboratory burning conditions to understand the influence of oxygen level and fuel composition on near-source aerosol production. Lignocellulosic biomass and major constituents, including hemicellulose (xylan), cellulose and lignin, were pyrolyzed and combusted in inert and oxidative environments at varying oxygen levels, and the aerosol particle emissions were characterized in terms of size and quantity at a fixed dilution temperature. Fuel mass and fuel heating rate were varied to assess the sensitivity of results to these factors. A previously developed summative model to predict near-source BB aerosol emissions was also tested. Results showed that the total number and mass aerosol emissions decreased with increased oxygen levels. Nucleation mode particles dominated the number emissions in both inert and oxidative environments, but larger aerosol sizes were observed in the oxidative environment. Aerosol particle coagulation and growth were observed at larger fuel masses, indicated by a significant decrease in the total number emission factors in both inert and oxidative environments, while the total mass emission factor only slightly decreased and increased in inert and oxidative environments, respectively. The size of aerosols formed was found to positively correlate with absolute fuel consumption rate, and the effects of oxidation through combustion chemistry and thermal feedback were explored. Good agreement between the simulated and measured number emission factors for pinewood was observed in both the inert and oxidative reaction environments over the range of tested fuel masses. Simulated and measured mass emission factors showed good agreement in the oxidative environment and poorer agreement in the inert environment. Reasons for this discrepancy were explored and the importance of constituent surrogate selection is highlighted.

Size-resolved aerosol emissions from lignocellulosic biomass and biomass constituent pyrolysis under variable dilution temperatures

Biomass burning events produce significant amounts of particulate matter which influence global radiative forcing, decrease air quality and visibility, and have negative health impacts. The quantity, size distribution, and volatility of biomass burning aerosol emissions are influenced by the combustion mode and ensuing dilution process of the emissions mixing into ambient air. This work examined the emissions from lignocellulosic biomass and its major constituents under laboratory pyrolysis conditions to understand biomass composition and dilution temperature influences on aerosol formation. The major constituents of lignocellulosic biomass, hemicellulose (xylan), cellulose and lignin, were pyrolyzed and the resultant aerosol emissions were characterized in terms of size-resolved number and mass emission factors under variable dilution temperatures. The aerosol emissions formed from biomass constituents were then compared to those of pine and corn stover, and a summative model for predicting characteristics of biomass burning emissions from the behavior of individual constituents was assessed. Results showed a significant influence of dilution temperature on particle size, number, and distribution, with the nucleation mode of particle formation dominating. The summative model performed well in predicting particle number formation from lignocellulosic biomass, but highlighted the effect of uncertainty on predicting particle mass formation.

Biomass combustion produces ice-active minerals in biomass-burning aerosol and bottom ash

Ice nucleation and the resulting cloud glaciation are significant atmospheric processes that affect the evolution of clouds and their properties including radiative forcing and precipitation, yet the sources and properties of atmospheric ice nucleants are poorly constrained. Heterogeneous ice nucleation caused by ice-nucleating particles (INPs) enables cloud glaciation at temperatures above the homogeneous freezing regime that starts near -35 °C. Biomass burning is a significant global source of atmospheric particles and a highly variable and poorly understood source of INPs. The nature of these INPs and how they relate to the fuel composition and its combustion are critical gaps in our understanding of the effects of biomass burning on the environment and climate. Here we show that the combustion process transforms inorganic elements naturally present in the biomass (not soil or dust) to form potentially ice-active minerals in both the bottom ash and emitted aerosol particles. These particles possess ice-nucleation activities high enough to be relevant to mixed-phase clouds and are active over a wide temperature range, nucleating ice at up to -13 °C. Certain inorganic elements can thus serve as indicators to predict the production of ice nucleants from the fuel. Combustion-derived minerals are an important but understudied source of INPs in natural biomass-burning aerosol emissions in addition to lofted primary soil and dust particles. These discoveries and insights should advance the realistic incorporation of biomass-burning INPs into atmospheric cloud and climate models. These mineral components produced in biomass-burning aerosol should also be studied in relation to other atmospheric chemistry processes, such as facilitating multiphase chemical reactions and nutrient availability.

Six global biomass burning emission datasets: intercomparison and application in one global aerosol model

Abstract. Aerosols from biomass burning (BB) emissions are poorly constrained in global and regional models, resulting in a high level of uncertainty in understanding their impacts. In this study, we compared six BB aerosol emission datasets for 2008 globally as well as in 14 regions. The six BB emission datasets are (1) GFED3.1 (Global Fire Emissions Database version 3.1), (2) GFED4s (GFED version 4 with small fires), (3) FINN1.5 (FIre INventory from NCAR version 1.5), (4) GFAS1.2 (Global Fire Assimilation System version 1.2), (5) FEER1.0 (Fire Energetics and Emissions Research version 1.0), and (6) QFED2.4 (Quick Fire Emissions Dataset version 2.4). The global total emission amounts from these six BB emission datasets differed by a factor of 3.8, ranging from 13.76 to 51.93 Tg for organic carbon and from 1.65 to 5.54 Tg for black carbon. In most of the regions, QFED2.4 and FEER1.0, which are based on satellite observations of fire radiative power (FRP) and constrained by aerosol optical depth (AOD) data from the Moderate Resolution Imaging Spectroradiometer (MODIS), yielded higher BB aerosol emissions than the rest by a factor of 2–4. By comparison, the BB aerosol emissions estimated from GFED4s and GFED3.1, which are based on satellite burned-area data, without AOD constraints, were at the low end of the range. In order to examine the sensitivity of model-simulated AOD to the different BB emission datasets, we ingested these six BB emission datasets separately into the same global model, the NASA Goddard Earth Observing System (GEOS) model, and compared the simulated AOD with observed AOD from the AErosol RObotic NETwork (AERONET) and the Multiangle Imaging SpectroRadiometer (MISR) in the 14 regions during 2008. In Southern Hemisphere Africa (SHAF) and South America (SHSA), where aerosols tend to be clearly dominated by smoke in September, the simulated AOD values were underestimated in almost all experiments compared to MISR, except for the QFED2.4 run in SHSA. The model-simulated AOD values based on FEER1.0 and QFED2.4 were the closest to the corresponding AERONET data, being, respectively, about 73 % and 100 % of the AERONET observed AOD at Alta Floresta in SHSA and about 49 % and 46 % at Mongu in SHAF. The simulated AOD based on the other four BB emission datasets accounted for only ∼50 % of the AERONET AOD at Alta Floresta and ∼20 % at Mongu. Overall, during the biomass burning peak seasons, at most of the selected AERONET sites in each region, the AOD values simulated with QFED2.4 were the highest and closest to AERONET and MISR observations, followed closely by FEER1.0. However, the QFED2.4 run tends to overestimate AOD in the region of SHSA, and the QFED2.4 BB emission dataset is tuned with the GEOS model. In contrast, the FEER1.0 BB emission dataset is derived in a more model-independent fashion and is more physically based since its emission coefficients are independently derived at each grid box. Therefore, we recommend the FEER1.0 BB emission dataset for aerosol-focused hindcast experiments in the two biomass-burning-dominated regions in the Southern Hemisphere, SHAF, and SHSA (as well as in other regions but with lower confidence). The differences between these six BB emission datasets are attributable to the approaches and input data used to derive BB emissions, such as whether AOD from satellite observations is used as a constraint, whether the approaches to parameterize the fire activities are based on burned area, FRP, or active fire count, and which set of emission factors is chosen.

Estimation of black carbon emissions from Siberian fires using satellite observations of absorption and extinction optical depths

Abstract. Black carbon (BC) emissions from open biomass burning (BB) are known to have a considerable impact on the radiative budget of the atmosphere at both global and regional scales; however, these emissions are poorly constrained in models by atmospheric observations, especially in remote regions. Here, we investigate the feasibility of constraining BC emissions from BB using satellite observations of the aerosol absorption optical depth (AAOD) and the aerosol extinction optical depth (AOD) retrieved from OMI (Ozone Monitoring Instrument) and MODIS (Moderate Resolution Imaging Spectroradiometer) measurements, respectively. We consider the case of Siberian BB BC emissions, which have the strong potential to impact the Arctic climate system. Using aerosol remote sensing data collected at Siberian sites of the AErosol RObotic NETwork (AERONET) along with the results of the fourth Fire Lab at Missoula Experiment (FLAME-4), we establish an empirical parameterization relating the ratio of the elemental carbon (EC) and organic carbon (OC) contents in BB aerosol to the ratio of AAOD and AOD at the wavelengths of the satellite observations. Applying this parameterization to the BC and OC column amounts simulated using the CHIMERE chemistry transport model, we optimize the parameters of the BB emission model based on MODIS measurements of the fire radiative power (FRP); we then obtain top-down optimized estimates of the total monthly BB BC amounts emitted from intense Siberian fires that occurred from May to September 2012. The top-down estimates are compared to the corresponding values obtained using the Global Fire Emissions Database (GFED4) and the Fire Emission Inventory–northern Eurasia (FEI-NE). Our simulations using the optimized BB aerosol emissions are verified against AAOD and AOD data that were withheld from the estimation procedure. The simulations are further evaluated against in situ EC and OC measurements at the Zotino Tall Tower Observatory (ZOTTO) and also against aircraft aerosol measurement data collected in the framework of the Airborne Extensive Regional Observations in SIBeria (YAK-AEROSIB) experiments. We conclude that our BC and OC emission estimates, considered with their confidence intervals, are consistent with the ensemble of the measurement data analyzed in this study. Siberian fires are found to emit 0.41±0.14 Tg of BC over the whole 5-month period considered; this estimate is a factor of 2 larger and a factor of 1.5 smaller than the corresponding estimates based on the GFED4 (0.20 Tg) and FEI-NE (0.61 Tg) data, respectively. Our estimates of monthly BC emissions are also found to be larger than the BC amounts calculated using the GFED4 data and smaller than those calculated using the FEI-NE data for any of the 5 months. Particularly large positive differences of our monthly BC emission estimates with respect to the GFED4 data are found in May and September. This finding indicates that the GFED4 database is likely to strongly underestimate BC emissions from agricultural burns and grass fires in Siberia. All of these differences have important implications for climate change in the Arctic, as it is found that about a quarter of the huge BB BC mass emitted in Siberia during the fire season of 2012 was transported across the polar circle into the Arctic. Overall, the results of our analysis indicate that a combination of the available satellite observations of AAOD and AOD can provide the necessary constraints on BB BC emissions.

The effect of South American biomass burning aerosol emissions on the regional climate

Abstract. The impact of biomass burning aerosol (BBA) on the regional climate in South America is assessed using 30-year simulations with a global atmosphere-only configuration of the Met Office Unified Model. We compare two simulations of high and low emissions of biomass burning aerosol based on realistic interannual variability. The aerosol scheme in the model has hygroscopic growth and optical properties for BBA informed by recent observations, including those from the recent South American Biomass Burning Analysis (SAMBBA) intensive aircraft observations made during September 2012. We find that the difference in the September (peak biomass emissions month) BBA optical depth between a simulation with high emissions and a simulation with low emissions corresponds well to the difference in the BBA emissions between the two simulations, with a 71.6 % reduction from high to low emissions for both the BBA emissions and the BB AOD in the region with maximum emissions (defined by a box of extent 5–25∘ S, 40–70∘ W, used for calculating mean values given below). The cloud cover at all altitudes in the region of greatest BBA difference is reduced as a result of the semi-direct effect, by heating of the atmosphere by the BBA and changes in the atmospheric stability and surface fluxes. Within the BBA layer the cloud is reduced by burn-off, while the higher cloud changes appear to be responding to stability changes. The boundary layer is reduced in height and stabilized by increased BBA, resulting in reduced deep convection and reduced cloud cover at heights of 9–14 km, above the layer of BBA. Despite the decrease in cloud fraction, September downwelling clear-sky and all-sky shortwave radiation at the surface is reduced for higher emissions by 13.77 ± 0.39 W m−2 (clear-sky) and 7.37 ± 2.29 W m−2 (all-sky), whilst the upwelling shortwave radiation at the top of atmosphere is increased in clear sky by 3.32 ± 0.09 W m−2, but decreased by -1.36±1.67 W m−2 when cloud changes are included. Shortwave heating rates increase in the aerosol layer by 18 % in the high emissions case. The mean surface temperature is reduced by 0.14 ± 0.24 ∘C and mean precipitation is reduced by 14.5 % in the peak biomass region due to both changes in cloud cover and cloud microphysical properties. If the increase in BBA occurs in a particularly dry year, the resulting reduction in precipitation may exacerbate the drought. The position of the South Atlantic high pressure is slightly altered by the presence of increased BBA, and the strength of the southward low-level jet to the east of the Andes is increased. There is some evidence that some impacts of increased BBA persist through the transition into the monsoon, particularly in precipitation, but the differences are only statistically significant in some small regions in November. This study therefore provides an insight into how variability in deforestation, realized through variability in biomass burning emissions, may contribute to the South American climate, and consequently on the possible impacts of future changes in BBA emissions.

Biomass burning emissions in north Australia during the early dry season: an overview of the 2014 SAFIRED campaign

Abstract. The SAFIRED (Savannah Fires in the Early Dry Season) campaign took place from 29 May until 30 June 2014 at the Australian Tropical Atmospheric Research Station (ATARS) in the Northern Territory, Australia. The purpose of this campaign was to investigate emissions from fires in the early dry season in northern Australia. Measurements were made of biomass burning aerosols, volatile organic compounds, polycyclic aromatic carbons, greenhouse gases, radon, speciated atmospheric mercury and trace metals. Aspects of the biomass burning aerosol emissions investigated included; emission factors of various species, physical and chemical aerosol properties, aerosol aging, micronutrient supply to the ocean, nucleation, and aerosol water uptake. Over the course of the month-long campaign, biomass burning signals were prevalent and emissions from several large single burning events were observed at ATARS.Biomass burning emissions dominated the gas and aerosol concentrations in this region. Dry season fires are extremely frequent and widespread across the northern region of Australia, which suggests that the measured aerosol and gaseous emissions at ATARS are likely representative of signals across the entire region of north Australia. Air mass forward trajectories show that these biomass burning emissions are carried north-west over the Timor Sea and could influence the atmosphere over Indonesia and the tropical atmosphere over the Indian Ocean. Here we present characteristics of the biomass burning observed at the sampling site and provide an overview of the more specific outcomes of the SAFIRED campaign.

Four-dimensional variational inversion of black carbon emissions during ARCTAS-CARB with WRFDA-Chem

Abstract. Biomass burning emissions of atmospheric aerosols, including black carbon, are growing due to increased global drought, and comprise a large source of uncertainty in regional climate and air quality studies. We develop and apply new incremental four-dimensional variational (4D-Var) capabilities in WRFDA-Chem to find optimal spatially and temporally distributed biomass burning (BB) and anthropogenic black carbon (BC) aerosol emissions. The constraints are provided by aircraft BC concentrations from the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites in collaboration with the California Air Resources Board (ARCTAS-CARB) field campaign and surface BC concentrations from the Interagency Monitoring of PROtected Visual Environment (IMPROVE) network on 22, 23, and 24 June 2008. We consider three BB inventories, including Fire INventory from NCAR (FINN) v1.0 and v1.5 and Quick Fire Emissions Database (QFED) v2.4r8. On 22 June, aircraft observations are able to reduce the spread between a customized QFED inventory and FINNv1.0 from a factor of 3. 5 ( × 3. 5) to only × 2. 1. On 23 and 24 June, the spread is reduced from × 3. 4 to × 1. 4. The posterior corrections to emissions are heterogeneous in time and space, and exhibit similar spatial patterns of sign for both inventories. The posterior diurnal BB patterns indicate that multiple daily emission peaks might be warranted in specific regions of California. The US EPA's 2005 National Emissions Inventory (NEI05) is used as the anthropogenic prior. On 23 and 24 June, the coastal California posterior is reduced by × 2, where highway sources dominate, while inland sources are increased near Barstow by × 5. Relative BB emission variances are reduced from the prior by up to 35 % in grid cells close to aircraft flight paths and by up to 60 % for fires near surface measurements. Anthropogenic variance reduction is as high as 40 % and is similarly limited to sources close to observations. We find that the 22 June aircraft observations are able to constrain approximately 14 degrees of freedom of signal (DOF), while surface and aircraft observations together on 23/24 June constrain 23 DOF. Improving hourly- to daily-scale concentration predictions of BC and other aerosols during BB events will require more comprehensive and/or targeted measurements and a more complete accounting of sources of error besides the emissions.

Probing into the aging dynamics of biomass burning aerosol by using satellite measurements of aerosol optical depth and carbon monoxide

Abstract. Carbonaceous aerosol released into the atmosphere from open biomass burning (BB) is known to undergo considerable chemical and physical transformations (aging). However, there is substantial controversy about the nature and observable effects of these transformations. A shortage of consistent observational evidence on BB aerosol aging processes under different environmental conditions and at various temporal scales hinders development of their adequate representations in chemistry transport models (CTMs). In this study, we obtain insights into the BB aerosol dynamics by using available satellite measurements of aerosol optical depth (AOD) and carbon monoxide (CO). The basic concept of our method is to consider AOD as a function of the BB aerosol photochemical age (that is, the time period characterizing the exposure of BB aerosol emissions to atmospheric oxidation reactions) predicted by means of model tracers. We evaluate the AOD enhancement ratio (ER) defined as the ratio of optical depth of actual BB aerosol with respect to that of a modeled aerosol tracer that is assumed to originate from the same fires as the real BB aerosol but that is not affected by any aging processes. To limit possible effects of model transport errors, the AOD measurements are normalized to CO column amounts that are also retrieved from satellite measurements. The method is applied to the analysis of the meso- and synoptic-scale evolution of aerosol in smoke plumes from major wildfires that occurred in Siberia in summer 2012. AOD and CO retrievals from MODIS and IASI measurements, respectively, are used in combination with simulations performed with the CHIMERE CTM. The analysis indicates that aging processes strongly affected the evolution of BB aerosol in the situation considered, especially in dense plumes (with spatial average PM2. 5 concentration exceeding 100 µg m−3). For such plumes, the ER is found to increase almost 2-fold on the scale of ∼ 10 h of daytime aerosol evolution (after a few first hours of the evolution that are not resolved in our analysis). The robustness of this finding is corroborated by sensitivity tests and Monte Carlo experiments. Furthermore, a simulation using the volatility basis set framework suggests that a large part of the increase in the ER can be explained by atmospheric processing of semi-volatile organic compounds. Our results are consistent with findings of a number of earlier studies reporting considerable underestimation of AOD by CTMs in which BB aerosol aging processes have either been disregarded or simulated in a highly simplified way. In general, this study demonstrates the feasibility of using satellite measurements of AOD in biomass burning plumes in combination with aerosol tracer simulations for the investigation of BB aerosol evolution and validation of BB aerosol aging schemes in atmospheric models.

Aerosol climate change effects on land ecosystem services.

A coupled global aerosol-carbon-climate model is applied to assess the impacts of aerosol physical climate change on the land ecosystem services gross primary productivity (GPP) and net primary productivity (NPP) in the 1996-2005 period. Aerosol impacts are quantified on an annual mean basis relative to the hypothetical aerosol-free world in 1996-2005, the global climate state in the absence of the historical rise in aerosol pollution. We examine the separate and combined roles of fast feedbacks associated with the land and slow feedbacks associated with the ocean. We consider all fossil fuel, biofuel and biomass burning aerosol emission sources as anthropogenic. The effective radiative forcing for aerosol-radiation interactions is -0.44 W m-2 and aerosol-cloud interactions is -1.64 W m-2. Aerosols cool and dry the global climate system by -0.8 °C and -0.08 mm per day relative to the aerosol-free world. Without aerosol pollution, human-induced global warming since the preindustrial would have already exceeded the 1.5 °C aspirational limit set in the Paris Agreement by the 1996-2005 decade. Aerosol climate impacts on the global average land ecosystem services are small due to large opposite sign effects in the tropical and boreal biomes. Aerosol slow feedbacks associated with the ocean strongly dominate impacts in the Amazon and North American Boreal. Aerosol cooling of the Amazon by -1.2 °C drives NPP increases of 8% or +0.76 ± 0.61 PgC per year, a 5-10 times larger impact than estimates of diffuse radiation fertilization by biomass burning aerosol in this region. The North American Boreal suffers GPP and NPP decreases of 35% due to aerosol-induced cooling and drying (-1.6 °C, -0.14 mm per day). Aerosol-land feedbacks play a larger role in the eastern US and Central Africa. Our study identifies an eco-climate teleconnection in the polluted earth system: the rise of the northern hemisphere mid-latitude reflective aerosol pollution layer causes long range cooling that protects Amazon NPP by 8% and suppresses boreal NPP by 35%.

Evaluation of biomass burning aerosols in the HadGEM3 climate model with observations from the SAMBBA field campaign

Abstract. We present observations of biomass burning aerosol from the South American Biomass Burning Analysis (SAMBBA) and other measurement campaigns, and use these to evaluate the representation of biomass burning aerosol properties and processes in a state-of-the-art climate model. The evaluation includes detailed comparisons with aircraft and ground data, along with remote sensing observations from MODIS and AERONET. We demonstrate several improvements to aerosol properties following the implementation of the Global Model for Aerosol Processes (GLOMAP-mode) modal aerosol scheme in the HadGEM3 climate model. This predicts the particle size distribution, composition, and optical properties, giving increased accuracy in the representation of aerosol properties and physical–chemical processes over the Coupled Large-scale Aerosol Scheme for Simulations in Climate Models (CLASSIC) bulk aerosol scheme previously used in HadGEM2. Although both models give similar regional distributions of carbonaceous aerosol mass and aerosol optical depth (AOD), GLOMAP-mode is better able to capture the observed size distribution, single scattering albedo, and Ångström exponent across different tropical biomass burning source regions. Both aerosol schemes overestimate the uptake of water compared to recent observations, CLASSIC more so than GLOMAP-mode, leading to a likely overestimation of aerosol scattering, AOD, and single scattering albedo at high relative humidity. Observed aerosol vertical distributions were well captured when biomass burning aerosol emissions were injected uniformly from the surface to 3 km. Finally, good agreement between observed and modelled AOD was gained only after scaling up GFED3 emissions by a factor of 1.6 for CLASSIC and 2.0 for GLOMAP-mode. We attribute this difference in scaling factor mainly to different assumptions for the water uptake and growth of aerosol mass during ageing via oxidation and condensation of organics. We also note that similar agreement with observed AOD could have been achieved with lower scaling factors if the ratio of organic carbon to primary organic matter was increased in the models toward the upper range of observed values. Improved knowledge from measurements is required to reduce uncertainties in emission ratios for black carbon and organic carbon, and the ratio of organic carbon to primary organic matter for primary emissions from biomass burning.

Local biomass burning is a dominant cause of the observed precipitation reduction in southern Africa.

Observations indicate a precipitation decline over large parts of southern Africa since the 1950s. Concurrently, atmospheric concentrations of greenhouse gases and aerosols have increased due to anthropogenic activities. Here we show that local black carbon and organic carbon aerosol emissions from biomass burning activities are a main cause of the observed decline in southern African dry season precipitation over the last century. Near the main biomass burning regions, global and regional modelling indicates precipitation decreases of 20–30%, with large spatial variability. Increasing global CO2 concentrations further contribute to precipitation reductions, somewhat less in magnitude but covering a larger area. Whereas precipitation changes from increased CO2 are driven by large-scale circulation changes, the increase in biomass burning aerosols causes local drying of the atmosphere. This study illustrates that reducing local biomass burning aerosol emissions may be a useful way to mitigate reduced rainfall in the region.

The role of semi-volatile organic compounds in the mesoscale evolution of biomass burning aerosol: a modeling case study of the 2010 mega-fire event in Russia

Abstract. Chemistry transport models (CTMs) are an indispensable tool for studying and predicting atmospheric and climate effects associated with carbonaceous aerosol from open biomass burning (BB); this type of aerosol is known to contribute significantly to both global radiative forcing and to episodes of air pollution in regions affected by wildfires. Improving model performance requires systematic comparison of simulation results with measurements of BB aerosol and elucidation of possible reasons for discrepancies between them, which, by default, are frequently attributed in the literature to uncertainties in emission data. Based on published laboratory data on the atmospheric evolution of BB aerosol and using the volatility basis set (VBS) framework for organic aerosol modeling, we examined the importance of taking gas-particle partitioning and oxidation of semi-volatile organic compounds (SVOCs) into account in simulations of the mesoscale evolution of smoke plumes from intense wildfires that occurred in western Russia in 2010. Biomass burning emissions of primary aerosol components were constrained with PM10 and CO data from the air pollution monitoring network in the Moscow region. The results of the simulations performed with the CHIMERE CTM were evaluated by considering, in particular, the ratio of smoke-related enhancements in PM10 and CO concentrations (ΔPM10 and ΔCO) measured in Finland (in the city of Kuopio), nearly 1000 km downstream of the fire emission sources. It is found that while the simulations based on a "conventional" approach to BB aerosol modeling (disregarding oxidation of SVOCs and assuming organic aerosol material to be non-volatile) strongly underestimated values of ΔPM10/ΔCO observed in Kuopio (by a factor of 2), employing the "advanced" representation of atmospheric processing of organic aerosol material resulted in bringing the simulations to a much closer agreement with the ground measurements. Furthermore, taking gas-particle partitioning and oxidation of SVOCs into account is found to result in a major improvement of the agreement of simulations and satellite measurements of aerosol optical depth, as well as in considerable changes in predicted aerosol composition and top-down BB aerosol emission estimates derived from AOD measurements.