Global Black Carbon Research Articles

Responses of wildfire-induced global black carbon pollution and radiative forcing to climate change

The impacts of climate change on wildfires have been studied extensively. Along with declining emissions from fossil fuel combustion due to anthropogenic emission control, black carbon (BC) released from wildfires is expected to contribute a more significant portion to its atmospheric burden. However, from a global perspective, little is known about the BC burden and radiative forcing caused by wildfires. Here, we report the results from the long-term wildfire-induced BC concentration and direct radiative forcing (DRF) from 1981 to 2010 globally simulated by an Earth System Model using an updated wildfire BC emission inventory. We show that wildfire-induced BC concentration and DRF varied significantly spatially and temporarily, with the highest in sub-Saharan Africa, attributable to its highest level of wildfire BC emission worldwide. The temporal trends of near-surface air temperature, precipitation, and evapotranspiration and their association with wildfire-induced BC concentration are explored using the multidimensional ensemble empirical mode decomposition. A statistically significant relation between changes in climate parameters and wildfire-induced BC concentration was found for 53% of the land grid cells, explaining on average 33% of the concentration variations. The result suggests that the wildfire-induced BC DRF, with an increasing trend, would be an important contributor to climate change, especially in sub-Saharan Africa. Occurrences of wildfires in the Amazon Basin respond most strongly to climate change and play an increasingly important role in changing the global climate.

An Aerosol Optical Module With Observation‐Constrained Black Carbon Properties for Global Climate Models

AbstractAtmospheric black carbon (BC) aerosols have been long‐lasting uncertain components in environmental and climate studies. Global climate models (GCMs) potentially overestimate BC absorption efficiency due to a lack of consideration of complex BC microphysical and mixing properties. We extract multiple BC properties from observations and develop an aerosol optical module known as Advanced Black Carbon (ABC) in the framework of the Modal Aerosol Model version 4 (MAM4). The ABC module is implemented in the Community Atmosphere Model version 6 (CAM6) and evaluated by in situ and remote sensing observations. CAM6‐ABC addresses the shortcomings of CAM6‐MAM4 in terms of BC microphysical and mixing properties, particularly their size, mixing state and optical simulations. Sensitivity simulations show that the global BC absorption aerosol optical depth at 550 nm simulated by CAM6‐ABC is reduced by ∼29% compared with that in CAM6‐MAM4. The BC absorption enhancement simulated by CAM6‐ABC is reduced from ∼2.6 of the default MAM4 to ∼1.4, which is closer to the observed values (mostly less than 1.5). With improved BC absorption estimation, the biases of aerosol single‐scattering coalbedo simulations are reduced by 18%–69% compared with global Aerosol Robotic Network observations. Moreover, the globally averaged BC direct radiative effect is reduced from 0.37 to 0.28 W/m2 at the top of the atmosphere. Our new scheme alleviates the overestimation of BC absorption in GCMs by constraining BC microphysical and mixing properties when assessing aerosol radiative and climate effects, and it can be easily implemented in most modal‐based aerosol modules of climate models.

Satellite (GOSAT-2 CAI-2) retrieval and surface (ARFINET) observations of aerosol black carbon over India

Abstract. Light-absorbing black carbon (BC) aerosols strongly affect Earth's radiation budget and climate. This paper presents satellite retrieval of BC over India based on observations from the Cloud and Aerosol Imager-2 (CAI-2) on board the Greenhouse gases Observing Satellite-2 (GOSAT-2). To evaluate and validate the satellite retrievals, near-surface BC mass concentrations measured across the Aerosol Radiative Forcing over India NETwork (ARFINET) of aerosol observatories are used. Then the findings are extended to elucidate global BC features. The analysis reveals that this satellite retrieval clearly demonstrates the regional and seasonal features of BC over the Indian region, similarly to those recorded by surface observations. Validation and closure studies between the two datasets show RMSE < 1 and absolute difference below 2 µg m−3 for > 60 % of simultaneous observations, exhibiting good associations for December, January, and February (R of approximately 0.73) and March, April, and May (R approx. 0.76). Over the hotspot regions of India, satellite retrievals show a soot volume fraction of approx. 5 %, columnar single-scattering albedo of approx. 0.8, and BC column optical depth of approx. 0.1 during times of the highest BC loading, which are comparable to other in situ and satellite measurements. In terms of global spatiotemporal variation, satellite retrievals show higher BC occurring mostly in areas where biomass burning is intense. Overall, this study highlights the effectiveness of satellite retrieval of BC, which can be used effectively for the regular monitoring of BC loading attributable to vehicular, industrial, or biomass burning activities.

Seasonal transition of Black carbon aerosols over Qinghai-Tibet Plateau: Simulations with WRF-Chem

Black carbon (BC) particles over the Qinghai-Tibet Plateau (Q-TP), whether suspended in the air or deposited on snow, can affect snow melt and accelerate glacier retreat. Since BC over the Q-TP may originate from different regions, it is necessary to understand the transport mechanism of BC and then provide concentrations and spatial-temporal distributions of BC over Q-TP, in order to study its radiative and climatic effects. In this study, Weather Research and Forecasting model with Chemistry (WRF-Chem), with MIX emission inventory (a mosaic Asian anthropogenic emission inventory for the MICS-Asia and the HTAP projects), was used to study the BC transport from South Asia, one of the major BC source regions, to Q-TP in April (pre-monsoon season), July (summer monsoon season) and December (winter monsoon season). The model's ability to simulate the BC transport from South Asia to the Q-TP was firstly evaluate using various reanalysis data, including 2 m temperature, precipitation, 10 m wind speed and direction and BC concentration at surface. The simulated meteorological fields and seasonal distribution and variation of BC are generally in good agreement with reanalysis data. The model showed good performance in simulating transport of BC as well. Our study showed that during pre-monsoon season, BC aerosols accumulated in the foothills of the Himalayas and were transported to southern Q-TP and even Southeast Asia via dry and wet deposition and westerly winds below 200hpa. Although the cyclonic airflow, which was favorable to transport, prevailed in South Asia, slight BC aerosols would be transported to Q-TP through wet deposition due to the efficient wet scavenging by abundant precipitation during summer monsoon season. During winter monsoon season, the prevailing westerly winds at 500hpa would transport BC aerosols from South Asia to Q-TP by dry deposition. A sensitivity simulation using PKU emission inventory (Peking University's global BC emission inventory) was then conducted to investigate the impact of different emission inventory on the modeling results. It is shown that the simulations using the different BC emission inventories overall did not have significant impacts on spatial distributions of surface concentration and column burden during three studies seasons. However, the simulated BC concentrations and burden based on PKU were overall higher than that based on MIX, that is, main differences were found in the southern part of Q-TP (i.e. adjacent to South Asia), especially during pre-monsoon and winter monsoon seasons. The differences of mean BC surface concentration ranging from 0.1 to 1 μg/m3, and burden ranging from 0.1 to 1 mg/m2 due to both higher dry and wet deposition (0.1–2 μg/m2/s for dry deposition flux, and 0.1–3 μg/m2/s for wet deposition flux) during pre-monsoon. During winter monsoon seasons, relatively large differences (0–3 μg/m3 for concentration, and 0–2 mg/m2 for burden, and 0.1–3 μg/m2/s for dry deposition flux) were found in southern Q-TP.

Sediment records of black carbon variations over the last two centuries in North China

Reconstructing historical black carbon (BC) variations based on sedimentary records are significant for understanding long-term BC emissions, tracing sources, and establishing effective strategies for pollution control. By comparing BC profiles between four lake sediment cores, historical BC variations were reconstructed on the southeastern Mongolian Plateau in North China. Except one, the other three records show close fluxes and similar temporal trends of soot, indicating their repetitiveness on revealing historical variations at a regional scale. Unlike soot, char and BC in these records, derived mainly from local sources, reflected the occurrence of natural fires and human activities near the lakes. Before the ∼1940s, these records showed no well-established anthropogenic BC signals except some occasional natural-related increases. This was different from the global BC increased since the Industrial Revolution, indicating a negligible influence of transboundary BC on the region. Anthropogenic BC in the region had increased since the 1940s–1950s ascribed to emissions from Inner Mongolia and nearby provinces. The increases were moderate in the 1950s–1970s, corresponded with the initial development of industry after the founding of the P.R. China. The most pronounced BC increases occurred in 1980s–2016, commensurate with rapid socio-economic development after the Reform and Opening-up in 1978. Different from model estimations on Chinese BC emissions, our records show unexpected BC increases in recent two decades caused by pollutant emission rises in this undeveloped region. This suggests that BC emissions in relatively small cities and rural areas in China were likely underestimated and their role on national BC cycling needs to be reassessed.

The black carbon cycle and its role in the Earth system

Black carbon (BC) is produced by incomplete combustion of biomass by wildfires and burning of fossil fuels. BC is environmentally persistent over centuries to millennia, sequestering carbon in marine and terrestrial environments. However, its production, storage and dynamics, and therefore its role in the broader carbon cycling during global change, are poorly understood. In this Review, we discuss BC cycling across the land-to-ocean continuum. Wildfires are the main source of BC, producing 128 ± 84 teragrams per year. Negative climate–BC feedbacks could arise as wildfire increases with anthropogenic warming, producing more BC, which in turn will sequester carbon, but the magnitude of these effects are unknown. Most BC is stored in terrestrial systems with some transported to the ocean via rivers and the atmosphere. However, the oceanic BC budget is not balanced, with known BC removal fluxes exceeding BC inputs. We demonstrate these observed inconsistencies using a simple ocean box model, which highlights key areas of future research. Measurements of BC mineralization and export rates along the land-to-ocean continuum and quantification of previously unexplored sources of oceanic BC are needed to close the global BC budget. Black carbon is produced by wildfire and fossil fuel burning, and persists in the environment over centuries to millennia. This Review describes black carbon sources and budgets, discusses its transport along the land-to-ocean continuum and highlights its enigmatic cycling in the ocean.

A Review of Progress in Constraining Global Black Carbon Climate Effects

A Review of Progress in Constraining Global Black Carbon Climate Effects

Acute effects of black carbon on mortality in nine megacities of China, 2008-2016: a time-stratified case-crossover study.

Black carbon (BC) may have more adverse effects on human health than other constituents of PM2.5. The daily mean concentrations of BC in China are much higher than those in developed countries and are estimated to account for more than a quarter of global anthropogenic BC emissions. However, reports on the health effects of BC in China have been limited. Thus, a time-stratified case-crossover study was conducted to evaluate the impacts of BC on daily mortality risk in nine Chinese megacities from 2008-2016. Our results show that for all-cause mortality, when compared to the interquartile range (IQR) of BC concentration increased, odds ratios (ORs) were in the range of 1.01-1.06 (95% CIs: 0.99-1.10). For cardiovascular mortality, ORs were in the range of 1.02-1.07 (95% CIs: 1.003-1.12), and for respiratory mortality, ORs were in the range of 1.01-1.15 (95% CIs: 1.00-1.18). The effects of BC in the nine cities were robust after adjusting for PM2.5, or even became more prominent. Furthermore, BC had stronger effects in spring and winter in northern cities, whereas in mid-latitude cities, BC had stronger effects in the warm seasons. In southern cities, BC had stronger effects in the cool and dry seasons. Our findings support an association between residential exposure to BC and mortality and thus provide further evidence that BC negatively impacts human health and is helpful for decision-making.

Urban residential energy switching in China between 1980 and 2014 prevents 2.2 million premature deaths

Urban residential energy switching in China between 1980 and 2014 prevents 2.2 million premature deaths

Responses of Arctic black carbon and surface temperature to multi-region emission reductions: a Hemispheric Transport of Air Pollution Phase 2 (HTAP2) ensemble modeling study

Abstract. Black carbon (BC) emissions play an important role in regional climate change in the Arctic. It is necessary to pay attention to the impact of long-range transport from regions outside the Arctic as BC emissions from local sources in the Arctic were relatively small. The task force Hemispheric Transport of Air Pollution Phase 2 (HTAP2) set up a series of simulation scenarios to investigate the response of BC in a given region to different source regions. This study investigated the responses of Arctic BC concentrations and surface temperature to 20 % anthropogenic emission reductions from six regions in 2010 within the framework of HTAP2 based on ensemble modeling results. Emission reductions from East Asia (EAS) had the most (monthly contributions: 0.2–1.5 ng m−3) significant impact on the Arctic near-surface BC concentrations, while the monthly contributions from Europe (EUR), Middle East (MDE), North America (NAM), Russia–Belarus–Ukraine (RBU), and South Asia (SAS) were 0.2–1.0, 0.001–0.01, 0.1–0.3, 0.1–0.7, and 0.0–0.2 ng m−3, respectively. The responses of the vertical profiles of the Arctic BC to the six regions were found to be different due to multiple transport pathways. Emission reductions from NAM, RBU, EUR, and EAS mainly influenced the BC concentrations in the low troposphere of the Arctic, while most of the BC in the upper troposphere of the Arctic derived from SAS. The response of the Arctic BC to emission reductions in six source regions became less significant with the increase in the latitude. The benefit of BC emission reductions in terms of slowing down surface warming in the Arctic was evaluated by using absolute regional temperature change potential (ARTP). Compared to the response of global temperature to BC emission reductions, the response of Arctic temperature was substantially more sensitive, highlighting the need for curbing global BC emissions.

Updated Global Black Carbon Emissions from 1960 to 2017: Improvements, Trends, and Drivers.

Accurate estimation of black carbon (BC) emissions is essential for assessing the health and climate impact of this pollutant. Past emission inventories were associated with high uncertainty due to data limitations, and recent information has provided a unique updating opportunity. Moreover, understanding the drivers that cause temporal emission changes is of research value. Here, we update the global BC emission estimates using new data on the activities and emission factors (EFs). The new inventory covers 73 detailed sources at 0.1° × 0.1° spatial resolution and monthly temporal resolution from 1960 to 2017. The estimated annual emissions were 32% higher than the average of several previous inventories, which was primarily due to field-measured EFs for residential stoves and differentiated EFs for motor vehicles. In addition, the updated emissions show an inverse U-shaped temporal trend, which was mainly driven by the interaction between the positive effects of population growth, per capita energy consumption, and vehicle fleet and the negative effects of residential energy switching, stove upgrading, phasing out of beehive coke ovens, and reduced EFs for vehicles and industrial processes. Urbanization caused a significant increase in urban emissions accompanied by a more significant decline in rural emissions.

The Direct Radiative Forcing Impact of Agriculture‐Emitted Black Carbon Associated With India's Green Revolution

AbstractBiomass burning contributes considerably to black carbon (BC) emissions in South Asia, but such emissions have not been linked with the Green Revolution (GR) which has enabled substantial crop production growth in South Asian countries, India in particular. Here, we use an Earth system model to quantify climate change through the direct radiative forcing (DRF) by agriculture‐emitted BC associated with the GR in India. We show that the BC DRF in India has increased significantly since the GR, especially during the post‐GR period. The estimated BC DRF in India rose from +0.197 W/m2 in 1961 to +0.805 W/m2 in 2011; this represents a fourfold increase in DRF since the onset of the GR. The contribution of BC DRF by India's intensive agriculture to the global BC forcing also increased from 2.6% to 4.4% during the GR. Our results reveal that increasing BC emissions associated with the GR raises the importance of emission mitigation from agriculture source.

Black Carbon Contributes Substantially to Allochthonous Carbon Storage in Deltaic Vegetated Coastal Habitats

Vegetated coastal habitats (VCHs) rank among the most intense carbon sinks in natural ecosystems, playing an important role in the global carbon cycle. A significant part of the organic carbon (OC) they store may be allochthonous OC that has been sequestered elsewhere. Yet, the compositions of allochthonous OC are largely unknown. Here, we present concentrations and carbon isotopic (13C and 14C) compositions and accumulation rates of carbon in the VCHs from major temperate-subtropical deltas of China: Yellow, Yangtze, and Pearl river deltas. We find that black carbon (BC) amounts to 9-25% of OC across sites. Temperate VCHs exhibit lower BC contents but higher BC contributions than subtropical VCHs. This seemingly counterintuitive result can be explained by increased accumulation of long-term, stable, allochthonous OC in temperate VCHs. BC in temperate VCHs contains 1.5-2 times more fossil BC than that in subtropical VCHs in the 1 m depth soil, which is likely influenced by atmospheric input and the aging effect. We estimate an accumulation rate of BC in China's VCHs of 33.1 ± 14.5 g m-2 year-1, acting as a hotspot for BC burial. These results point to a substantial and hitherto unquantified contribution of BC components to blue carbon storage, as well as the VCHs to global BC storage. Preservation of this old-aged, stable OC implies an important ecosystem service of the VCHs for climate change mitigation.

Improved Simulations of Global Black Carbon Distributions by Modifying Wet Scavenging Processes in Convective and Mixed‐Phase Clouds

AbstractIn‐cloud wet scavenging dominates the wet removal of aerosols in the atmosphere, but is not well represented in climate models. Aircraft measurements of black carbon (BC) concentrations suggest that models commonly overestimate BC concentrations in the upper troposphere of the tropics by more than one order of magnitude but underestimate BC burdens in polar latitudes. In this study, we improved the in‐cloud wet scavenging parameterizations for convective clouds and mixed‐phase clouds to better characterize BC abundances in the remote atmosphere (remote oceans and polar regions) with a global model, CAM5‐ATRAS2. The modified wet scavenging processes in the model achieved a more realistic simulation of BC concentrations over both the tropics and the Arctic. The new, unified scheme for vertical transport and wet removal during deep convection generally reproduced the observed low mixing ratios (about 0.1 ng kg−1) of BC in the middle and upper troposphere over the tropics, and the Wegener–Bergeron–Findeisen process (WBF) lowered the wet removal efficiency of BC from mixed‐phase clouds and consequently increased BC burdens in the Arctic by about a factor of 2. The BC direct radiative forcings increased by 20% globally (from 0.26 to 0.31 W m−2), and more importantly by a factor of 2 in the Arctic (from 0.09 to 0.18 W m−2). Our results indicated that good agreement between modeled and observed BC concentrations could be obtained in the remote atmosphere without requiring the relatively short global BC lifetime (∼4 days) suggested by previous studies.

Particulate and Dissolved Black Carbon in Coastal China Seas: Spatiotemporal Variations, Dynamics, and Potential Implications.

Elaborating the spatiotemporal variations and dynamic mechanisms of black carbon (BC) in coastal seas, the geographically pivotal intermediate zones that link the terrestrial and open oceanic ecosystems, will contribute significantly to refine the regional and global BC geochemistry. In this study, we implemented a large spatial-scale and multiseason and -layer seawater sampling campaign in high BC emission influenced coastal China seas (Bohai Sea and Northern Yellow Sea) and quantified the thermal/optical reflectance-based particulate BC (PBC) and benzene polycarboxylic acids-based dissolved BC (DBC). We found that the climate and its associated hydrological effects (including the intensive resuspension and coastal current transport) largely regulate both PBC and DBC spatiotemporal variations and dynamics. In combination with previous work on upstream rivers and downstream open ocean, a significant and continuous decrease in the DBC aromatic condensation was observed along the river-to-ocean continuum, probably due to the increment of the photochemical degradation during the waterborne transport. Based on our DBC methodological development, i.e., the determination and subsequent inclusion of the nitrated BC molecular markers, the magnitudes of the current global DBC fluxes and pools were updated. After the update, the DBC fluxes from atmospheric deposition and riverine delivery were estimated at rates of 4.3 and 66.3 Tg yr-1, respectively, and the global oceanic DBC pool was approximately 36 Gt. This update will greatly assist in constructing a more robust regional and global DBC and BC cycling and budgets.

Distinct responses of Asian summer monsoon to black carbon aerosols and greenhouse gases

Abstract. Black carbon (BC) aerosols emitted from natural and anthropogenic sources induce positive radiative forcing and global warming, which in turn significantly affect the Asian summer monsoon (ASM). However, many aspects of the BC effect on the ASM remain elusive and largely inconsistent among previous studies, which is strongly dependent on different low-level thermal feedbacks over the Asian continent and the surrounding ocean. This study examines the response of the ASM to BC forcing in comparison with the effect of doubled greenhouse gases (GHGs) by analyzing the Precipitation Driver Response Model Intercomparison Project (PDRMIP) simulations under an extremely high BC level (10 times modern global BC emissions or concentrations, labeled BC×10) from nine global climate models (GCMs). The results show that although BC and GHGs both enhance the ASM precipitation minus evaporation (P−E; a 13.6 % increase for BC forcing and 12.1 % for GHGs from the nine-model ensemble, respectively), there exists a much larger uncertainty in changes in ASM P−E induced by BC than by GHGs. The summer P−E is increased by 7.7 % to 15.3 % due to these two forcings over three subregions, including East Asian, South Asian and western North Pacific monsoon regions. Further analysis of moisture budget reveals distinct mechanisms controlling the increases in ASM P−E induced by BC and GHGs. The change in ASM P−E by BC is dominated by the dynamic effect due to the enhanced large-scale monsoon circulation, whereas the GHG-induced change is dominated by the thermodynamic effect through increasing atmospheric water vapor. Radiative forcing of BC significantly increases the upper-level atmospheric temperature over the Asian region to enhance the upper-level meridional land–sea thermal gradient (MLOTG), resulting in a northward shift of the upper-level subtropical westerly jet and an enhancement of the low-level monsoon circulation, whereas radiative forcing of GHGs significantly increases the tropical upper-level temperature, which reduces the upper-level MLOTG and suppresses the low-level monsoonal circulation. Hence, our results indicate a different mechanism of BC climate effects under the extremely high BC level: that BC forcing significantly enhances the upper-level atmospheric temperature over the Asian region, determining ASM changes, instead of low-level thermal feedbacks as indicated by previous studies.

The contribution of black carbon to global ice nucleating particle concentrations relevant to mixed-phase clouds

Black carbon (BC) aerosol plays an important role in the Earth's climate system because it absorbs solar radiation and therefore potentially warms the climate; however, BC can also act as a seed for cloud particles, which may offset much of its warming potential. If BC acts as an ice nucleating particle (INP), BC could affect the lifetime, albedo, and radiative properties of clouds containing both supercooled liquid water droplets and ice particles (mixed-phase clouds). Over 40% of global BC emissions are from biomass burning; however, the ability of biomass burning BC to act as an INP in mixed-phase cloud conditions is almost entirely unconstrained. To provide these observational constraints, we measured the contribution of BC to INP concentrations ([INP]) in real-world prescribed burns and wildfires. We found that BC contributes, at most, 10% to [INP] during these burns. From this, we developed a parameterization for biomass burning BC and combined it with a BC parameterization previously used for fossil fuel emissions. Applying these parameterizations to global model output, we find that the contribution of BC to potential [INP] relevant to mixed-phase clouds is ∼5% on a global average.

Effects of black carbon mitigation on Arctic climate

Abstract. We use the ECHAM-HAMMOZ aerosol-climate model to assess the effects of black carbon (BC) mitigation measures on Arctic climate. To this end we constructed several mitigation scenarios that implement all currently existing legislation and then implement further reductions of BC in a successively increasing global area, starting from the eight member states of the Arctic Council, expanding to its active observer states, then to all observer states, and finally to the entire globe. These scenarios also account for the reduction of the co-emitted organic carbon (OC) and sulfate (SU). We find that, even though the additional BC emission reductions in the member states of the Arctic Council are small, the resulting reductions in Arctic BC mass burdens can be substantial, especially in the lower troposphere close to the surface. This in turn means that reducing BC emissions only in the Arctic Council member states can reduce BC deposition in the Arctic by about 30 % compared to the current legislation, which is about 60 % of what could be achieved if emissions were reduced globally. Emission reductions further south affect Arctic BC concentrations at higher altitudes and thus only have small additional effects on BC deposition in the Arctic. The direct radiative forcing scales fairly well with the total amount of BC emission reduction, independent of the location of the emission source, with a maximum direct radiative forcing in the Arctic of about −0.4 W m−2 for a global BC emission reduction. On the other hand, the Arctic effective radiative forcing due to the BC emission reductions, which accounts for aerosol–cloud interactions, is small compared to the direct aerosol radiative forcing. This happens because BC- and OC-containing particles can act as cloud condensation nuclei, which affects cloud reflectivity and lifetime and counteracts the direct radiative forcing of BC. Additionally, the effective radiative forcing is accompanied by very large uncertainties that originate from the strong natural variability of meteorology, cloud cover, and surface albedo in the Arctic. We further used the TM5-FASST model to assess the benefits of the aerosol emission reductions for human health. We found that a full implementation in all Arctic Council member and observer states could reduce the annual global number of premature deaths by 329 000 by the year 2030, which amounts to 9 % of the total global premature deaths due to particulate matter.

Constraining global aerosol emissions using POLDER/PARASOL satellite remote sensing observations

Abstract. We invert global black carbon (BC), organic carbon (OC) and desert dust (DD) aerosol emissions from POLDER/PARASOL spectral aerosol optical depth (AOD) and aerosol absorption optical depth (AAOD) using the GEOS-Chem inverse modeling framework. Our inverse modeling framework uses standard a priori emissions to provide a posteriori emissions that are constrained by POLDER/PARASOL AODs and AAODs. The following global emission values were retrieved for the three aerosol components: 18.4 Tg yr−1 for BC, 109.9 Tg yr−1 for OC and 731.6 Tg yr−1 for DD for the year 2010. These values show a difference of +166.7 %, +184.0 % and −42.4 %, respectively, with respect to the a priori values of emission inventories used in “standard” GEOS-Chem runs. The model simulations using a posteriori emissions (i.e., retrieved emissions) provide values of 0.119 for global mean AOD and 0.0071 for AAOD at 550 nm, which are +13.3 % and +82.1 %, respectively, higher than the AOD and AAOD obtained using the a priori values of emissions. Additionally, the a posteriori model simulation of AOD, AAOD, single scattering albedo, Ångström exponent and absorption Ångström exponent show better agreement with independent AERONET, MODIS and OMI measurements than the a priori simulation. Thus, this study suggests that using satellite-constrained global aerosol emissions in aerosol transport models can improve the accuracy of simulated global aerosol properties.

Fossil fuel combustion and biomass burning sources of global black carbon from GEOS-Chem simulation and carbon isotope measurements

Abstract. We identify sources (fossil fuel combustion versus biomass burning) of black carbon (BC) in the atmosphere and in deposition using a global 3-D chemical transport model GEOS-Chem. We validate the simulated sources against carbon isotope measurements of BC around the globe and find that the model reproduces mean biomass burning contribution (fbb; %) in various regions within a factor of 2 (except in Europe, where fbb is underestimated by 63 %). GEOS-Chem shows that contribution from biomass burning in the Northern Hemisphere (fbb: 35±14 %) is much less than that in the Southern Hemisphere (50±11 %). The largest atmospheric fbb is in Africa (64±20 %). Comparable contributions from biomass burning and fossil fuel combustion are found in southern (S) Asia (53±10 %), southeastern (SE) Asia (53±11 %), S America (47±14 %), the S Pacific (47±7 %), Australia (53±14 %) and the Antarctic (51±2 %). fbb is relatively small in eastern Asia (40±13 %), Siberia (35±8 %), the Arctic (33±6 %), Canada (31±7 %), the US (25±4 %) and Europe (19±7 %). Both observations and model results suggest that atmospheric fbb is higher in summer (59 %–78 %, varying with sub-regions) than in winter (28 %–32 %) in the Arctic, while it is higher in winter (42 %–58 %) and lower in summer (16 %–42 %) over the Himalayan–Tibetan Plateau. The seasonal variations of Atmosphericfbb are relatively flat in North America, Europe and Asia. We conducted four experiments to investigate the uncertainties associated with biofuel emissions, hygroscopicity of BC in fresh emissions, the aging rate and size-resolved wet scavenging. We find that doubling biofuel emissions for domestic heating north of 45∘ N increases fbb values in Europe in winter by ∼30 %, reducing the discrepancy between observed and modeled atmospheric fbb from −63 % to −54 %. The remaining large negative discrepancy between model and observations suggests that the biofuel emissions are probably still underestimated at high latitudes. Increasing the fraction of thickly coated hydrophilic BC from 20 % to 70 % in fresh biomass burning plumes increases the fraction of hydrophilic BC in biomass burning plumes by 0 %–20 % (varying with seasons and regions) and thereby reduces atmospheric fbb by up to 11 %. Faster aging (4 h e-folding time versus 1.15 d e-folding time) of BC in biomass burning plumes reduces atmospheric fbb by 7 % (1 %–14 %, varying with seasons and regions), with the largest reduction in remote regions, such as the Arctic, the Antarctic and the S Pacific. Using size-resolved scavenging accelerates scavenging of BC particles in both fossil fuel and biomass burning plumes, with a faster scavenging of BC in fossil fuel plumes. Thus, atmospheric fbb increases in most regions by 1 %–14 %. Overall, atmospheric fbb is determined mainly by fbb in emissions and, to a lesser extent, by atmospheric processes, such as aging and scavenging. This confirms the assumption that fbb in local emissions determines atmospheric fbb in previous studies, which compared measured atmospheric fbb directly with local fbb in bottom-up emission inventories.