Ratio Of Black Carbon Research Articles

Numerical Investigation on Absorption Enhancement of Black Carbon Aerosols Partially Coated With Nonabsorbing Organics

AbstractThis study numerically evaluates the effects of aerosol microphysics, including coated volume fraction of black carbon (BC), shell/core ratio, and size distribution, on the absorption enhancement (Eab) of polydisperse BC aggregates partially coated by organics, which is calculated by the exact multiple‐sphere T‐matrix method. The coated volume fraction of BC plays a substantial role in determining the absorption enhancement of partially coated BC aggregates, which typically have an Eab in the range of ~1.0–2.0 with a larger value for larger coated volume fraction of BC as the shell/core ratio, BC geometry, and size distribution are fixed. The shell/core ratio, BC geometry, and size distribution have little impact on the Eab of coated BC with small coated volume fraction of BC, while they become significant for large coated volume fraction of BC. The Eab of partially coated BC particles can be slightly less than 1.0 for the large BC in the accumulation mode exhibiting large shell/core ratio and small coated volume fraction of BC, indicating that the absorption shows even slight decrease relative to uncoated BC particles. For partially coated BC aggregates in the accumulation and coarse modes, the refractive index uncertainties of BC result in the Eab differences of less than 9% and 2%, respectively, while those of organics can induce larger variations with the maximum differences up to 22% and 18%, respectively. Our study indicates that accounting for particle coating microphysics, particularly the coated volume fraction of BC, can potentially help to understand the differences in observations of largely variable absorption enhancements over various regions.

Source Apportionment of Black Carbon Aerosol in the North Suburb of Nanjing

Based on one year real-time measurements from a seven-wavelength Aethalometer combined with an Aethalometer model, the measured aerosol absorption coefficients at different wavelengths have been used to apportion the contribution of fossil fuel and biomass burning sources to the total black carbon (BC) mass concentration in the north suburb of Nanjing. Good consistency in the relationship between the Angstrom absorption exponent(α)and the ratio of BC from biomass burning sources to total BC (BB) was obtained during this period. The α was highest in winter and lowest in summer, which indicates the change in the source of the absorbing aerosols and their relative source strength. The BC and the BC from fossil fuel (BCff) and biomass burning (BCbb) mass concentrations exhibit significant diurnal variation, with higher values during 07:00 to 09:00 (local time) and 18:00 to 21:00. The BCff was three to five times higher than the BCbb and contributes greatest to the BC mass concentrations throughout the day. Night time BC values were about a factor of 1.2 higher than day time BC values. Meanwhile, the concentration weighted trajectory (CWT) analysis indicates that the highest value of BC was concentrated in the Zhejiang, Anhui, Jiangxi, and Fujian provinces.

Century-scale high-resolution black carbon records in sediment cores from the South Yellow Sea, China

Black carbon (BC) has received increasing attention in the last 20 years because it is not only an absorbent of toxic pollutants but also a greenhouse substance, preserving fire-history records, and more importantly, acting as an indicator of biogeochemical cycles and global changes. By adopting an improved chemothermal oxidation method (WXY), this study reconstructed the century-scale high-resolution records of BC deposition from two fine-grained sediment cores collected from the Yellow Sea Cold Water Mass in the South Yellow Sea. The BC records were divided into five stages, which exhibited specific sequences with three BC peaks at approximately 1891, 1921, and 2007 AD, representing times at which the first heavy storms appeared just after the termination of long-term droughts. The significant correlation between the times of the BC peaks in the cores and heavy storms in the area of the Huanghe (Yellow) River demonstrated that BC peaks could result from markedly strengthened sedimentation due to surface runoff, which augmented the atmospheric deposition. Stable carbon isotope analysis indicated that the evident increase in carbon isotope ratios of BC in Stage 5 might have resulted from the input of weathered rock-derived graphitic carbon cardinally induced by the annual anthropogenic modulation of water-borne sediment in the Huanghe River since 2005 AD. Numerical calculations demonstrated that the input fraction of graphitic carbon was 22.97% for Stage 5, whereas no graphitic carbon entered during Stages 1 and 3. The obtained data provide new and important understanding of the source-sink history of BC in the Yellow Sea.

Emission factors of black carbon and co-pollutants from diesel vehicles in Mexico City

Abstract. Diesel-powered vehicles are intensively used in urban areas for transporting goods and people but can substantially contribute to high emissions of black carbon (BC), organic carbon (OC), and other gaseous pollutants. Strategies aimed at controlling mobile emissions sources thus have the potential to improve air quality and help mitigate the impacts of air pollutants on climate, ecosystems, and human health. However, in developing countries there are limited data on the BC and OC emission characteristics of diesel-powered vehicles, and thus there are large uncertainties in the estimation of the emission contributions from these sources. We measured BC, OC, and other inorganic components of fine particulate matter (PM), as well as carbon monoxide (CO), nitrogen oxides (NOx), sulfur dioxide (SO2), ethane, acetylene, benzene, toluene, and C2-benzenes under real-world driving conditions for 20 diesel-powered vehicles encompassing multiple emission level technologies in Mexico City with the chasing technique using the Aerodyne mobile laboratory. Average BC emission factors ranged from 0.41–2.48 g kg−1 of fuel depending on vehicle type. The vehicles were also simultaneously measured using the cross-road remote sensing technique to obtain the emission factors of nitrogen oxide (NO), CO, total hydrocarbons, and fine PM, thus allowing for the intercomparison of the results from the two techniques. There is overall good agreement between the two techniques and both can identify high and low emitters, but substantial differences were found in some of the vehicles, probably due to the ability of the chasing technique to capture a larger diversity of driving conditions in comparison to the remote sensing technique. A comparison of the results with the US EPA MOVES2014b model showed that the model underestimates CO, OC, and selected VOC species, whereas there is better agreement for NOx and BC. Larger OC / BC ratios were found in comparison to ratios measured in California using the same technique, further demonstrating the need for using locally obtained diesel-powered vehicle emission factor database in developing countries in order to reduce the uncertainty in the emissions estimates and to improve the evaluation of the effectiveness of emissions reduction measures.

Morphology, molecular structure, and stable carbon isotopic composition of black carbon (BC) in urban topsoils.

Urban soils contain significant amounts of black carbon (BC) from biomass and fossil fuel combustion and regard to be a pool of BC. BC in urban soils has multiple effects on environmental processes in urban system, such as global climate change, air quality, and public health. Urban topsoil samples (0-10cm) were collected from Anshan, Liaoning Province, northeast China, which is one of the most important old steel industrial bases in China. The BC in urban topsoils was extracted using the density method. Their chemical composition, morphology, molecular structure, and stable carbon isotopic composition were examined using elemental analysis, scanning electron microscopy with energy-dispersive X-ray spectroscopy (SEM-EDS), Fourier transform infrared spectroscopy (FTIR), thermogravimetric analysis (TGA), X-ray diffraction (XRD), and stable carbon isotope (δ13C). Elemental analysis shows that carbon content in the BC of studied soils ranged from 64.5 to 78.4%, with the average more than 70%. The O/C atomic ratio of BC is on average 0.18. The BC particle displays different morphology, including porous spherical, irregular porous fragmentary, and blocky shapes. The porous spherical BC particles has atomic molar O/C ratio determined by SEM-EDS ranging from 0.04 to 0.37. XRD indicates that BC exists in mainly combining with mineral phases hematite (Fe2O3), kaolinite (Al2Si2O5(OH)4), quartz (SiO2), and calcite (CaCO3). The FTIR spectra of BC particles show major bands at approximately 3400cm-1 (O-H), 2920cm-1 (C=H), 1600cm-1 (C=C), 1230cm-1 (C=O), and 1070cm-1 (C=O). The stable carbon isotope (δ13C) of BC ranges from -24.48 to -23.18‰ with the average of -23.79±0.39‰. The concentration of BC in the industrial area is significantly (p<0.05) higher than that in the roadside area. The BC of industrial area is characterized by porous spherical structure, suggesting that they are mainly derived from fossil fuel combustion. Results indicated that a combination of atomic O/C ratio, porous structure, and stable carbon isotopic (δ13C) of BC could reflect effectively the origin of BC in urban topsoils. It could conclude that BC in Anshan urban topsoil was mainly from fossil fuel combustion.

Characteristics of black carbon emissions from in-use light-duty passenger vehicles

Mitigating black carbon (BC) emissions from various combustion sources has been considered an urgent policy issue to address the challenges of climate change, air pollution and health risks. Vehicles contribute considerably to total anthropogenic BC emissions and urban BC concentrations. Compared with heavy-duty diesel vehicles, there is much larger uncertainty in BC emission factors for light-duty passenger vehicles (LDPVs), in particular for gasoline LDPVs, which warrants further studies. In this study, we employed the dynamometer and the Aethalometer (AE-51) to measure second-by-second BC emissions from eight LDPVs by engine technology and driving cycle. The average BC emission factors under transient cycles (e.g., ECE-15, New European Driving Cycle, NEDC, Worldwide Harmonized Light Vehicles Test Cycle, WLTC) are 3.6–91.5 mg/km, 7.6 mg/km and 0.13–0.58 mg/km, respectively, for diesel (N = 3), gasoline direct injection (GDI) (N = 1) and gasoline port-fuel injection (PFI) engine categories (N = 4). For gasoline PFI LDPVs, the instantaneous emission profiles show a strong association of peak BC emissions with cold-start and high-speed aggressive driving. Such impacts lead to considerable BC emission contributions in cold-start periods (e.g., the first 47 s–94 s) over the entire cycle (e.g., 18–76% of the NEDC and 13–36% of the WLTC) and increased BC emission factors by 80–440% under the WLTC compared to the NEDC. For diesel BC emissions, the size distribution exhibits a typical unimodal pattern with one single peak appearing approximately from 120 to 150 nm, which is largely consistent with previous studies. Nevertheless, the average mass ratios of BC to particle mass (PM) range from 0.38 to 0.54 for three diesel samples, representing substantial impacts from both driving and engine conditions. The significant discrepancy between gasoline BC emission factors obtained from tailpipe exhaust versus ambient conditions suggest that more comparative measurements and fine-grained simulations should be designed and implemented to address this discrepancy.

A campaign for investigating aerosol optical properties during winter hazes over Shijiazhuang, China

As the capital of the most air-polluted Hebei province in China, Shijiazhuang has been suffering serious haze pollutions especially during wintertime. An integrated campaign for investigating aerosol optical properties under haze conditions over Shijiazhuang were carried out using a sunphotometer, an aethalometer and a lidar in the winter from late 2013 to early 2014. The results indicated that the haze episodes during the measurement period were severer and more frequent over Shijiazhuang than Beijing. Under heavy pollution conditions (PM2.5>150μg/m3) over Shijiazhuang, fine-mode fractions of AOD500nm were larger than 0.80 with more dispersive angstrom exponent due to hygroscopic growth. The mean values of SSA over Shijiazhuang were smaller than those over Beijing both in this study and the severe haze episodes in January 2013, suggesting that there were more fine-mode absorbing particles over Shijiazhuang. More significant spectrally-dependence of imaginary part of refractive index over Shijiazhuang implies larger relative magnitude of brown carbon (BrC) as compared to Beijing. The black carbon (BC) measurement displayed extremely high records with a larger ratio of BC to PM2.5 (12.11% in average) comparing with other cities in China. The high carbonaceous aerosols (BC and BrC) should be attributed to large amounts of coal consumption. During the hazes with high BC concentrations, the daily maximal planetary boundary layer (PBL) heights were consistently lower than 500m, implying the impacts of BC aerosols on the PBL development and hence enhance the surface haze pollution.

Characterization of black carbon in the ambient air of Agra, India: Seasonal variation and meteorological influence

This study characterizes the black carbon in Agra, India home to the Taj Mahal—and situated in the Indo-Gangetic basin. The mean black carbon concentration is 9.5 μg m−3 and, owing to excessive biomass/fossil fuel combustion and automobile emissions, the concentration varies considerably. Seasonally, the black carbon mass concentration is highest in winter, probably due to the increased fossil fuel consumption for heating and cooking, apart from a low boundary layer. The nocturnal peak rises prominently in winter, when the use of domestic heating is excessive. Meanwhile, the concentration is lowest during the monsoon season because of the turbulent atmospheric conditions and the process of washout by precipitation. The ratio of black carbon to brown carbon is less than unity during the entire study period, except in winter (December). This may be because that biomass combustion and diesel exhaust are major black carbon contributors in this region, while a higher ratio in winter may be due to the increased consumption of fossil fuel and wood for heating purposes. ANOVA reveals significant monthly variation in the concentration of black carbon; plus, it is negatively correlated with wind speed and temperature. A high black carbon mass concentration is observed at moderate (1–2 m s−1) wind speed, as compared to calm or turbulent atmospheric conditions.

Alteration of the size distributions and mixing states of black carbon through transport in the boundary layer in east Asia

Abstract. Ground-based measurements of black carbon (BC) were performed near an industrial source region in the early summer of 2014 and at a remote island in Japan in the spring of 2015. Here, we report the temporal variations in the transport, size distributions, and mixing states of the BC-containing particles. These particles were characterized using a continuous soot monitoring system, a single particle soot photometer, and an aerosol chemical speciation monitor. The effects of aging on the growth of BC-containing particles were examined by comparing the ground-based observations between the near-source and remote island sites. Secondary formation of sulfate and organic aerosols strongly affected the increases in BC coating (i.e., enhancement of cloud condensation nuclei activity) with air mass aging from the source to the outflow regions. The effects of wet removal on BC microphysics were elucidated by classifying the continental outflow air masses depending on the enhancement ratios of BC to CO (ΔBC ∕ ΔCO), which were used as an indicator of the transport efficiency of BC. It was found that ΔBC ∕ ΔCO ratios were controlled mainly by the wet removal during transport in the planetary boundary layer (PBL) on the timescale of 1–2 days. The meteorological conditions and backward trajectory analyses suggested that air masses strongly affected by wet removal originated mainly from a region in southern China (20–35° N) in the spring of 2015. Removal of large and thickly coated BC-containing particles was detected in the air masses that were substantially affected by the wet removal in the PBL, as predicted by Köhler theory. The size and water solubility of BC-containing particles in the PBL can be altered by the wet removal as well as the condensation of non-BC materials.

Direct radiative effect of carbonaceous aerosols from crop residue burning during the summer harvest season in East China

Abstract. East China experiences extensive crop residue burnings in fields during harvest season. The direct radiative effect (DRE) of carbonaceous aerosols from crop residue burning in June 2013 in East China was investigated using the Weather Research and Forecasting Model coupled with Chemistry (WRF-Chem). Absorption of organic aerosol (OA) in the presence of brown carbon was considered using the parameterization of Saleh et al. (2014), in which the imaginary part of the OA refractive index is a function of wavelength and the ratio of black carbon (BC) and OA. The carbonaceous emissions from crop fires were estimated using the Moderate Resolution Imaging Spectroradiometer (MODIS) fire radiative power (FRP) product with a localized crop-burning-sourced BC-to-organic carbon (OC) ratio emission ratio of 0.27. Evaluation of the model results with in situ measurements of particulate matter with aerodynamic diameter less than 2.5 µm (PM2. 5) chemical composition, MODIS aerosol optical depth (AOD) detections and meteorological observations showed that this model was able to reproduce the magnitude, spatial variation and optical characteristics of carbonaceous aerosol pollution. The observed BC and OC peak concentrations at the site in Suixi, Anhui province, during the 2013 wheat burning season reached 55.3 µg m−3 and 157.9 µg m−3. WRF-Chem simulations reproduced these trends with a correlation coefficient of 0.74, estimating that crop residue burning contributed 86 and 90 % of peak BC and OC, respectively. The simulated hourly DRE from crop residue burning at the top of atmosphere (TOA) reached a maximum of +22.66 W m−2 at the Suixi site. On average, the simulations showed that the crop residue burning introduced a net positive DRE of +0.14 W m−2 at TOA throughout East China, with BC from this source as the main heating contributor (+0.79 W m−2). The OA DRE from crop burning (−0.22 W m−2) was a combined effect of the positive DRE of absorption (+0.21 W m−2) and a stronger negative DRE of scattering (−0.43 W m−2). Sensitivity tests showed that the DRE of OA absorption strongly depended on the imaginary part of the OA refractive index, the BC-to-OA emission ratio from crop residue burning and the assumed mixing state of the aerosol, whereby the volume mixing treatment resulted in a higher positive DRE compared to the core–shell treatment. The BC mixing state and associated absorption enhancement during BC aging processes will be investigated in detail in future research.

Modeling investigation of light-absorbing aerosols in the Amazon Basin during the wet season

Abstract. We use a global chemical transport model (GEOS-Chem) to interpret observed light-absorbing aerosols in Amazonia during the wet season. Observed aerosol properties, including black carbon (BC) concentration and light absorption, at the Amazon Tall Tower Observatory (ATTO) site in the central Amazon have relatively low background levels but frequently show high peaks during the study period of January–April 2014. With daily temporal resolution for open fire emissions and modified aerosol optical properties, our model successfully captures the observed variation in fine/coarse aerosol and BC concentrations as well as aerosol light absorption and its wavelength dependence over the Amazon Basin. The source attribution in the model indicates the important influence of open fire on the observed variances of aerosol concentrations and absorption, mainly from regional sources (northern South America) and from northern Africa. The contribution of open fires from these two regions is comparable, with the latter becoming more important in the late wet season. The analysis of correlation and enhancement ratios of BC versus CO suggests transport times of &lt; 3 days for regional fires and ∼ 11 days for African plumes arriving at ATTO during the wet season. The model performance of long-range transport of African plumes is also evaluated with observations from AERONET, MODIS, and CALIOP. Simulated absorption aerosol optical depth (AAOD) averaged over the wet season is lower than 0.0015 over the central Amazon, including the ATTO site. We find that more than 50 % of total absorption at 550 nm is from BC, except for the northeastern Amazon and the Guianas, where the influence of dust becomes significant (up to 35 %). The brown carbon contribution is generally between 20 and 30 %. The distribution of absorption Ångström exponents (AAE) suggests more influence from fossil fuel combustion in the southern part of the basin (AAE ∼ 1) but more open fire and dust influence in the northern part (AAE &gt; 1.8). Uncertainty analysis shows that accounting for absorption due to secondary organic aerosol (SOA) and primary biogenic aerosol (PBA) particles could result in differences of &lt; 8 and 5–40 % in total absorption, respectively.

Joint measurements of black carbon and particle mass for heavy-duty diesel vehicles using a portable emission measurement system

The black carbon (BC) emitted from heavy-duty diesel vehicles (HDDVs) is an important source of urban atmospheric pollution and creates strong climate-forcing impacts. The emission ratio of BC to total particle mass (PM) (i.e., BC/PM ratio) is an essential variable used to estimate total BC emissions from historical PM data; however, these ratios have not been measured using portable emission measurement systems (PEMS) in order to obtain real-world measurements over a wide range of driving conditions. In this study, we developed a PEMS platform by integrating two Aethalometers and an electric low pressure impactor to realize the joint measurement of real-world BC and PM emissions for ten HDDVs in China. Test results showed that the average BC/PM ratio for five HDDVs equipped with mechanical fuel injection (MI) engines was 0.43 ± 0.06, significantly lower (P < 0.05) than another five HDDVs equipped with electronically-controlled fuel injection (EI) engines (0.56 ± 0.12). Traffic conditions also affected the BC/PM ratios with higher ratios on freeway routes than on local roads. Furthermore, higher ratios were observed for HDDVs equipped with EI engines than for the MI engines for the highway and local road routes. With an operating mode binning approach, we observed that the instantaneous BC/PM ratios of EI engine vehicles were above those of the MI engine vehicles in all operating modes except for the braking mode (i.e., Bin 0). Therefore, the complex impacts from engine technology and traffic conditions on BC/PM ratios should be carefully considered when estimating real-world BC emissions from HDDVs based on overall PM emissions data.

The colors of biomass burning aerosols in the atmosphere.

Biomass burning aerosols mainly consist of black carbon (BC) and organic aerosols (OAs), and some of OAs are brown carbon (BrC). This study simulates the colors of BrC, BC and their mixture with scattering OAs in the ambient atmosphere by using a combination of light scattering simulations, a two-stream radiative transfer model and a RGB (Red, Green, Blue) color model. We find that both BCs and tar balls (a class of BrC) appear brownish at small particle sizes and blackish at large sizes. This is because the aerosol absorption Ångström exponent (AAE) largely controls the color and larger particles give smaller AAE values. At realistic size distributions, BCs look more blackish than tar balls, but still exhibit some brown color. However, when the absorptance of aerosol layer at green wavelength becomes larger than approximately 0.8, all biomass burning aerosols look blackish. The colors for mixture of purely scattering and absorptive carbonaceous aerosol layers in the atmosphere are also investigated. We suggest that the brownishness of biomass burning aerosols indicates the amount of BC/BrC as well as the ratio of BC to BrC.

Causes of variability in light absorption by particles in snow at sites in Idaho and Utah

AbstractA characterization of black carbon (BC) and other light‐absorbing particles in snow is presented for three mountain valley sites in Idaho in early 2014 and for one site near Vernal, Utah, in early 2013 and 2014. The focus of the study was on constraining the magnitude and drivers of variations in particulate absorbers in midlatitude U.S. seasonal snow. Mass mixing ratios of BC in newly fallen snow were similar at all three Idaho sites, with a median of 4.7 ± 4.2 ng BC per gram of snow. The median total light‐absorbing particulate mixing ratios in new snow, expressed as an equivalent mixing ratio of BC, was 18 ± 23 ng g−1. At the Utah site, which is near sources of both fossil fuel and dust, the mixing ratios of BC varied from 7 to 45 ng g−1 across seven new snowfall samples, and the BC‐equivalent mixing ratios varied from 9 to 1500 ng g−1. At all sites, dry deposition and in‐snow processes increase the mixing ratio of BC by up to an order of magnitude and increase the mixing ratio of all light‐absorbing particulates by up to 2 orders of magnitude, highlighting the importance of capturing these processes for accurately representing snow albedo in climate models. Spatial variability at a range of scales is found to be considerably smaller than the temporal variations at a given site, with implications for the representativeness of field samples used in observation/model comparisons.

Measuring the morphology and density of internally mixed black carbon with SP2 and VTDMA: new insight into the absorption enhancement of black carbon in the atmosphere

Abstract. The morphology and density of black carbon (BC) cores in internally mixed BC (In-BC) particles affect their mixing state and absorption enhancement. In this work, we developed a new method to measure the morphology and effective density of the BC cores of ambient In-BC particles using a single-particle soot photometer (SP2) and a volatility tandem differential mobility analyzer (VTDMA) during the CAREBeijing-2013 campaign from 8 to 27 July 2013 at Xianghe Observatory. This new measurement system can select size-resolved ambient In-BC particles and measure the mobility diameter and mass of the In-BC cores. The morphology and effective density of the ambient In-BC cores are then calculated. For the In-BC cores in the atmosphere, changes in their dynamic shape factor (χ) and effective density (ρeff) can be characterized as a function of the aging process (Dp∕Dc) measured by SP2 and VTDMA. During an intensive field study, the ambient In-BC cores had an average shape factor χ of ∼ 1.2 and an average density of ∼ 1.2 g cm−3, indicating that ambient In-BC cores have a near-spherical shape with an internal void of ∼ 30 %. From the measured morphology and density, the average shell ∕ core ratio and absorption enhancement (Eab) of ambient BC were estimated to be 2.1–2.7 and 1.6–1.9, respectively, for In-BC particles with sizes of 200–350 nm. When the In-BC cores were assumed to have a void-free BC sphere with a density of 1.8 g cm−3, the shell ∕ core ratio and Eab were overestimated by ∼ 13 and ∼ 17 %, respectively. The new approach developed in this work improves the calculations of the mixing state and optical properties of ambient In-BC particles by quantifying the changes in the morphology and density of ambient In-BC cores during aging.

The impact of residential combustion emissions on atmospheric aerosol, human health, and climate

Abstract. Combustion of fuels in the residential sector for cooking and heating results in the emission of aerosol and aerosol precursors impacting air quality, human health, and climate. Residential emissions are dominated by the combustion of solid fuels. We use a global aerosol microphysics model to simulate the impact of residential fuel combustion on atmospheric aerosol for the year 2000. The model underestimates black carbon (BC) and organic carbon (OC) mass concentrations observed over Asia, Eastern Europe, and Africa, with better prediction when carbonaceous emissions from the residential sector are doubled. Observed seasonal variability of BC and OC concentrations are better simulated when residential emissions include a seasonal cycle. The largest contributions of residential emissions to annual surface mean particulate matter (PM2.5) concentrations are simulated for East Asia, South Asia, and Eastern Europe. We use a concentration response function to estimate the human health impact due to long-term exposure to ambient PM2.5 from residential emissions. We estimate global annual excess adult (&gt; 30 years of age) premature mortality (due to both cardiopulmonary disease and lung cancer) to be 308 000 (113 300–497 000, 5th to 95th percentile uncertainty range) for monthly varying residential emissions and 517 000 (192 000–827 000) when residential carbonaceous emissions are doubled. Mortality due to residential emissions is greatest in Asia, with China and India accounting for 50 % of simulated global excess mortality. Using an offline radiative transfer model we estimate that residential emissions exert a global annual mean direct radiative effect between −66 and +21 mW m−2, with sensitivity to the residential emission flux and the assumed ratio of BC, OC, and SO2 emissions. Residential emissions exert a global annual mean first aerosol indirect effect of between −52 and −16 mW m−2, which is sensitive to the assumed size distribution of carbonaceous emissions. Overall, our results demonstrate that reducing residential combustion emissions would have substantial benefits for human health through reductions in ambient PM2.5 concentrations.

Quantifying sources of black carbon in western North America using observationally based analysis and an emission tagging technique in the Community Atmosphere Model

Abstract. The Community Atmosphere Model (CAM5), equipped with a technique to tag black carbon (BC) emissions by source regions and types, has been employed to establish source–receptor relationships for atmospheric BC and its deposition to snow over western North America. The CAM5 simulation was conducted with meteorological fields constrained by reanalysis for year 2013 when measurements of BC in both near-surface air and snow are available for model evaluation. We find that CAM5 has a significant low bias in predicted mixing ratios of BC in snow but only a small low bias in predicted atmospheric concentrations over northwestern USA and western Canada. Even with a strong low bias in snow mixing ratios, radiative transfer calculations show that the BC-in-snow darkening effect is substantially larger than the BC dimming effect at the surface by atmospheric BC. Local sources contribute more to near-surface atmospheric BC and to deposition than distant sources, while the latter are more important in the middle and upper troposphere where wet removal is relatively weak. Fossil fuel (FF) is the dominant source type for total column BC burden over the two regions. FF is also the dominant local source type for BC column burden, deposition, and near-surface BC, while for all distant source regions combined the contribution of biomass/biofuel (BB) is larger than FF. An observationally based positive matrix factorization (PMF) analysis of the snow-impurity chemistry is conducted to quantitatively evaluate the CAM5 BC source-type attribution. While CAM5 is qualitatively consistent with the PMF analysis with respect to partitioning of BC originating from BB and FF emissions, it significantly underestimates the relative contribution of BB. In addition to a possible low bias in BB emissions used in the simulation, the model is likely missing a significant source of snow darkening from local soil found in the observations.

Interannual variations of light‐absorbing particles in snow on Arctic sea ice

AbstractSamples of snow on sea ice were collected in springtime of the 6 years 2008–2013 in the region between Greenland, Ellesmere Island, and the North Pole (82°N –89°N, 0°W–100°W). The meltwater was passed through filters, whose spectral absorption was then measured to determine the separate contributions by black carbon (BC) and other light‐absorbing impurities. The median mixing ratio of BC across all years' samples was 4 ± 3 ng g−1, and the median fraction of absorption due to non‐BC absorbers was 36 ± 11%. Variances represent both spatial and interannual variability; there was no interannual trend in either variable. The absorption Ångström exponent, however, decreased with latitude, suggesting a transition from dominance by biomass‐burning sources in the south to an increased influence by fossil‐fuel‐burning sources in the north, consistent with earlier measurements of snow in Svalbard and at the North Pole.

Uncertainties in global aerosols and climate effects due to biofuel emissions

Abstract. Aerosol emissions from biofuel combustion impact both health and climate; however, while reducing emissions through improvements to combustion technologies will improve health, the net effect on climate is largely unconstrained. In this study, we examine sensitivities in global aerosol concentration, direct radiative climate effect, and cloud-albedo aerosol indirect climate effect to uncertainties in biofuel emission factors, optical mixing state, and model nucleation and background secondary organic aerosol (SOA). We use the Goddard Earth Observing System global chemical-transport model (GEOS-Chem) with TwO Moment Aerosol Sectional (TOMAS) microphysics. The emission factors include amount, composition, size, and hygroscopicity, as well as optical mixing-state properties. We also evaluate emissions from domestic coal use, which is not biofuel but is also frequently emitted from homes. We estimate the direct radiative effect assuming different mixing states (homogeneous, core-shell, and external) with and without absorptive organic aerosol (brown carbon). We find the global-mean direct radiative effect of biofuel emissions ranges from −0.02 to +0.06 W m−2 across all simulation/mixing-state combinations with regional effects in source regions ranging from −0.2 to +0.8 W m−2. The global-mean cloud-albedo aerosol indirect effect (AIE) ranges from +0.01 to −0.02 W m−2 with regional effects in source regions ranging from −1.0 to −0.05 W m−2. The direct radiative effect is strongly dependent on uncertainties in emissions mass, composition, emissions aerosol size distributions, and assumed optical mixing state, while the indirect effect is dependent on the emissions mass, emissions aerosol size distribution, and the choice of model nucleation and secondary organic aerosol schemes. The sign and magnitude of these effects have a strong regional dependence. We conclude that the climate effects of biofuel aerosols are largely unconstrained, and the overall sign of the aerosol effects is unclear due to uncertainties in model inputs. This uncertainty limits our ability to introduce mitigation strategies aimed at reducing biofuel black carbon emissions in order to counter warming effects from greenhouse gases. To better understand the climate impact of particle emissions from biofuel combustion, we recommend field/laboratory measurements to narrow constraints on (1) emissions mass, (2) emission size distribution, (3) mixing state, and (4) ratio of black carbon to organic aerosol.

Brown carbon aerosol in the North American continental troposphere: sources, abundance, and radiative forcing

Abstract. Chemical components of organic aerosol (OA) selectively absorb light at short wavelengths. In this study, the prevalence, sources, and optical importance of this so-called brown carbon (BrC) aerosol component are investigated throughout the North American continental tropospheric column during a summer of extensive biomass burning. Spectrophotometric absorption measurements on extracts of bulk aerosol samples collected from an aircraft over the central USA were analyzed to directly quantify BrC abundance. BrC was found to be prevalent throughout the 1 to 12 km altitude measurement range, with dramatic enhancements in biomass-burning plumes. BrC to black carbon (BC) ratios, under background tropospheric conditions, increased with altitude, consistent with a corresponding increase in the absorption Ångström exponent (AAE) determined from a three-wavelength particle soot absorption photometer (PSAP). The sum of inferred BC absorption and measured BrC absorption at 365 nm was within 3 % of the measured PSAP absorption for background conditions and 22 % for biomass burning. A radiative transfer model showed that BrC absorption reduced top-of-atmosphere (TOA) aerosol forcing by ~ 20 % in the background troposphere. Extensive radiative model simulations applying this study background tropospheric conditions provided a look-up chart for determining radiative forcing efficiencies of BrC as a function of a surface-measured BrC : BC ratio and single scattering albedo (SSA). The chart is a first attempt to provide a tool for better assessment of brown carbon's forcing effect when one is limited to only surface data. These results indicate that BrC is an important contributor to direct aerosol radiative forcing.