Black Carbon Radiative Effects Research Articles

Direct radiative effects of black carbon and brown carbon from Southeast Asia biomass burning with the WRF-CMAQ two-way coupled model

Black carbon (BC) and brown carbon (BrC) are significant light-absorbing components of particulate matter that impact weather and climate. Biomass burning (BB) and biofuel (BF) emissions in Southeast Asia are key global sources of BC and BrC. This study utilizes the Weather Research and Forecasting-Community Multiscale Air Quality (WRF-CMAQ) model, integrating a BrC module for the first time, alongside the Global Fire Emissions Database Version 4, to assess the direct radiative effect (DRE) of BC and BrC in March 2015 over Southeast Asia. The novel BrC module parameterizes light absorption based on the BB BC to organic aerosol (OA) ratio in each model grid and time step, aligning better with smog chamber experiments than default coefficients. Results show that BC DRE affects clear sky net radiation at the top of the atmosphere, reaching 14.6 W/m2 in Indochina and 5.1 W/m2 in southern China, while BrC DRE reaches 1.9 W/m2. Additionally, BC and BrC DRE induce a cooling effect at the Earth's surface, with the maximum reduction of the clear sky downward shortwave radiation by −36.9 W/m2 and −5.2 W/m2, respectively. BC and BrC lead to a tiny decrease (<0.1 °C) in surface temperature and an increase in upper air temperature. Surface O3 concentration tends to slightly decrease (<1.0 ppbv) due to the DRE of BC and BrC. In comparison to studies using the default coefficient, this result contributes to a more nuanced understanding of the interactions between BC, BrC, and radiation.

Weakened Aerosol‐PBL Interactions Enhance Future Air Quality Benefits Under Carbon Neutrality in China: Insights From the Advanced Variable‐Resolution Global Model

AbstractChina's pursuing the carbon neutrality goal could affect future air quality not only by reducing anthropogenic emissions but also by modulating aerosol‐planetary boundary layer (PBL) interactions. However, contributions of aerosol‐PBL interactions to future air quality benefits remain unclear. Here we conduct ensemble experiments using the variable‐resolution (VR) Community Atmosphere Model with full chemistry based on the scalable spectral element (SE) dynamical core with East Asia refined to ∼28 km (SE_VR). Additional simulations at a uniform resolution of ∼111 km (SE_UR) are conducted to help demonstrate SE_VR's advantages in projecting future air quality. Results of SE_VR show that the mean PM2.5 concentrations in China would drop to below 10 μg/m3, especially in Sichuan Basin (SCB) where the frequencies of moderate and severe air pollution events are predicted to decrease from 60.7% and 11.3% to nearly zero respectively when achieving carbon neutrality. The aerosol‐PBL interactions would be substantially weakened with anthropogenic emission reductions. At SCB and Eastern China (EC), the weakened radiative effects of black carbon (BC) would contribute 34.3% and 71.6% to the increase in PBL height (PBLH). Consequently, these weakened BC‐PBL interactions reduce the surface PM2.5 concentrations by 16.1 μg/m3 (18.9%) in SCB and 4.6 μg/m3 (16.4%) in EC. Notably, SE_VR outperforms SE_UR in projecting the frequency decrease of future air pollution events for its better reproducing current levels, particularly those caused by BC aerosols. This study highlights the importance of weakened aerosol‐PBL feedbacks on future air quality improvement and demonstrates the added values of variable‐resolution global models in air quality projections.

Impacts of elevated anthropogenic emissions on physicochemical characteristics of black-carbon-containing particles over the Tibetan Plateau

Abstract. Black carbon (BC) in the Tibetan Plateau (TP) region has distinct climate effects that strongly depend on its mixing state. The aging processes of BC in the TP are subject to emissions from various regions, resulting in considerable variability of its mixing state and physicochemical properties. However, the mechanism and magnitude of this effect are not yet clear. In this study, field observations on physicochemical properties of BC-containing particles (PMBC) were conducted in the northeast (Xihai) and southeast (Lulang) regions of the TP to investigate the impacts of transported emissions from lower-altitude areas on BC characteristics in the TP. Large spatial discrepancies were found in the chemical composition of PMBC. Both sites showed higher concentrations of PMBC when they were affected by transported air masses outside the TP but with diverse chemical composition. Source apportionment for organic aerosol (OA) suggested that primary OA in the northeastern TP was attributed to hydrocarbon OA (HOA) from anthropogenic emissions, while it was dominated by biomass burning OA (BBOA) in the southeastern TP. Regarding secondary aerosol, a marked enhancement in nitrate fraction was observed on aged BC coating in Xihai when the air masses were brought by updrafts and easterly winds from lower-altitude areas. With the development of boundary layer, the enhanced turbulent mixing promoted the elevation of anthropogenic pollutants. In contrast to Xihai, the thickly coated BC in Lulang was mainly caused by elevation and transportation of biomass burning plumes from south Asia, showing a large contribution of secondary organic aerosol (SOA). The distinct transported emissions lead to substantial variations of both chemical composition and light absorption ability of BC across the TP. The thicker coating and higher mass absorption cross-section (MAC) of PMBC in air masses elevated from lower-altitude regions reveal the promoted BC aging processes and their impacts on the mixing state and light absorption of BC in the TP. These findings emphasize the vulnerability of plateau regions to influences of elevated emissions, leading to significant changes in BC concentration, mixing states and light absorption across the TP, all of which need to be considered in the evaluation of BC radiative effects for the TP region.

Modeling the Air Pollution and Aerosol‐PBL Interactions Over China Using a Variable‐Resolution Global Model

AbstractModeling air quality has always been a challenge in global models constrained by coarse grids. Here, the variable‐resolution Community Atmosphere Model with full chemistry based on the scalable spectral element (SE) dynamical core (MUSICAv0) is applied in simulating air pollution with a finer grid resolution of ∼0.25° over East Asia (SE_VR), in contrast to the same model with a uniform resolution of ∼1.0° (SE_UR). Two nudging experiments and four free‐running experiments are conducted to investigate the capabilities of SE_VR in modeling the air pollution and aerosol‐planetary boundary layer (PBL) interactions over China. Results show the regional refinement in SE_VR is essential for simulating haze events over complex terrain areas attributed to its better performance in representing the local vertical and horizontal dispersion conditions. SE_VR shows prominent advantages over SE_UR in simulating surface ozone because of better resolving spatial segregation of NOx and volatile organic compounds (VOC) chemical regimes and subsequently representing more detailed chemical processes related to ozone formation, although the model generally overestimates surface ozone over China. Further analysis of SE_VR shows the daytime radiative effect of black carbon (BC) aerosols lowers PBL height by 12.0% (17.9%), and leads to an increase of PM2.5 by 14.5% (10.8%) under the moderate (severe) air pollution conditions over Sichuan Basin. However, SE_UR has deficiencies in simulating BC‐PBL interactions due to its inability to reproduce the strong inverse temperature structure caused by BC aerosols in the lower atmosphere layer. Our results highlight the value of variable‐resolution global models for simulating air pollution and its interactions with climate.

Mixing state of black carbon at different atmospheres in north and southwest China

Abstract. Large uncertainties remain when estimating the radiative forcing by black carbon (BC) because the corresponding microphysical properties have not been well addressed. In this study, the BC size distributions were studied based on three different field campaigns at an urban site, a suburban site, and a background site in China using a single particle soot photometer (SP2) in tandem with a differential mobility diameter. Measurement results indicate that the BC particles were composed of either thinly or thickly coated aerosols. The mean number fractions of the thinly coated BC aerosols were 51 %, 67 %, and 21 % for the urban, suburban, and background sites, respectively. The corresponding thickly coated (thinly coated) core mass median diameters were 187 (154), 182 (146), and 238 (163) nm, respectively. The mean diameter of the thickly coated BC-containing aerosols was larger than that of the thinly coated BC-containing aerosols, while the mean BC core diameter of the thickly coated BC-containing aerosols was smaller than that of the thinly coated BC-containing aerosols. About 10 % of the BC-containing aerosols with the BC core are attached to the other non-BC components, which were mainly generated by coagulation between the BC and non-BC components. The measurement results in our study can be further used in modeling studies to help with constraining the uncertainties of the BC radiative effects.

Contrasting source contributions of Arctic black carbon to atmospheric concentrations, deposition flux, and atmospheric and snow radiative effects

Abstract. Black carbon (BC) particles in the Arctic contribute to rapid warming of the Arctic by heating the atmosphere and snow and ice surfaces. Understanding the source contributions to Arctic BC is therefore important, but they are not well understood, especially those for atmospheric and snow radiative effects. Here we estimate simultaneously the source contributions of Arctic BC to near-surface and vertically integrated atmospheric BC mass concentrations (MBC_SRF and MBC_COL), BC deposition flux (MBC_DEP), and BC radiative effects at the top of the atmosphere and snow surface (REBC_TOA and REBC_SNOW) and show that the source contributions to these five variables are highly different. In our estimates, Siberia makes the largest contribution to MBC_SRF, MBC_DEP, and REBC_SNOW in the Arctic (defined as &gt;70∘ N), accounting for 70 %, 53 %, and 41 %, respectively. In contrast, Asia's contributions to MBC_COL and REBC_TOA are largest, accounting for 37 % and 43 %, respectively. In addition, the contributions of biomass burning sources are larger (29 %–35 %) to MBC_DEP, REBC_TOA, and REBC_SNOW, which are highest from late spring to summer, and smaller (5.9 %–17 %) to MBC_SRF and MBC_COL, whose concentrations are highest from winter to spring. These differences in source contributions to these five variables are due to seasonal variations in BC emission, transport, and removal processes and solar radiation, as well as to differences in radiative effect efficiency (radiative effect per unit BC mass) among sources. Radiative effect efficiency varies by a factor of up to 4 among sources (1471–5326 W g−1) depending on lifetimes, mixing states, and heights of BC and seasonal variations of emissions and solar radiation. As a result, source contributions to radiative effects and mass concentrations (i.e., REBC_TOA and MBC_COL, respectively) are substantially different. The results of this study demonstrate the importance of considering differences in the source contributions of Arctic BC among mass concentrations, deposition, and atmospheric and snow radiative effects for accurate understanding of Arctic BC and its climate impacts.

Brown carbon from biomass burning imposes strong circum-Arctic warming

Brown carbon from biomass burning imposes strong circum-Arctic warming

Assessment of the combined radiative effects of black carbon in the atmosphere and snowpack in the Northern Hemisphere constrained by surface observations

In this study, the total radiative effect of black carbon (BC) in both the atmosphere and seasonal snowpack across the snow-covered area has been investigated over the Northern Hemisphere.

Wintertime vertical distribution of black carbon and single scattering albedo in a semi-arid region derived from tethered balloon observations

The vertical distribution of atmospheric aerosols plays an essential role in aerosol–radiation and aerosol–cloud interactions. Because of strong light absorption, the radiative effects of black carbon (BC) are highly sensitive to its vertical distribution; the lack of high-resolution observations is the reason for their poor quantification. We used a tethered balloon platform to acquire high-resolution vertical profiles of BC, particle number concentration, and meteorological parameters in the semi-arid region of Northwest China in December 2018. A total of 112 BC profiles were classified into four vertical distribution categories, which were determined by local emissions, regional transport, vertical mixing due to the ABL evolution, and topography. BC profiles with peaks near or above the atmospheric boundary layer (ABL) accounted for 57% of the profiles. Vertical single scattering albedo (SSA) profiles were subsequently calculated using the profiles of BC and particle size distribution. The vertical SSA distribution is generally modulated by BC profiles. The diurnal variations of the BC and SSA profiles were summarized using a boundary-layer normalization method. In the ABL, BC decreased and SSA increased with increasing height at 02:00, 08:00, and 20:00, while both BC and SSA exhibited a uniform distribution at 14:00. The SSA decreased above the ABL at 14:00, which might have had a profound impact on ABL development. These results provide a better understanding of the vertical BC and SSA distributions, which can also be used to reduce uncertainties in estimating the BC radiative effects.

Analysis of the Effect of Optical Properties of Black Carbon on Ozone in an Urban Environment at the Yangtze River Delta, China

Black carbon (BC) reduces the photolysis coefficient by absorbing solar radiation, thereby affecting the concentration of ozone (O3) near the ground. The influence of BC on O3 has thus received much attention. In this study, Mie scattering and the tropospheric Ultraviolet and Visible radiation model are used to analyze the effect of BC optical properties on radiation. Combined with data of O3 precursors in Nanjing in 2014, an EKMA curve is drawn, and the variations in O3 concentration are further investigated using a zero-dimensional box mechanism model (NCAR MM). When O3 precursors are unchanged, radiation and O3 show a highly similar tendency in response to changing BC optical properties (R=0.997). With the increase of modal radius, the attenuation of fresh BC to radiation and O3 first trends upward before decreasing. In the mixing process, the attenuation of BC to radiation and O3 presents an upward tendency with the increase of relative humidity but decreases rapidly before increasing slowly with increasing thickness of coating. In addition, mass concentration is another major factor. When the BC to PM2.5 ratio increases to 5% in Nanjing, the radiation decreases by approximately 0.13%–3.71% while O3 decreases by approximately 8.13%–13.11%. The radiative effect of BC not only reduces O3 concentration but also changes the EKMA curve. Compared with the NOx control area, radiation has a significant influence on the VOCs control area. When aerosol optical depth (AOD) increases by 17.15%, the NOx to VOCs ratio decreases by 8.27%, and part of the original NOx control area is transferred to the VOCs control area.

Real-Time Black Carbon Emissions from Light-Duty Passenger Vehicles Using a Portable Emissions Measurement System

Black carbon (BC) is considered the second largest anthropogenic climate forcer, but the radiative effects of BC are highly correlated with its combustion sources. On-road vehicles are an important source of anthropogenic BC. However, there are major uncertainties in the estimates of the BC emissions from on-road light-duty passenger vehicles (LDPVs), and results obtained with the portable emissions measurement system (PEMS) method are particularly lacking. We developed a PEMS platform and evaluated the on-road BC emissions from ten in-use LDPVs. We demonstrated that the BC emission factors (EFs) of gasoline direction injection (GDI) engine vehicles range from 1.10 to 1.56 mg·km−1, which are higher than the EFs of port fuel injection (PFI) engine vehicles (0.10–0.17 mg·km−1) by a factor of 11. The BC emissions during the cold-start phase contributed 2%–33% to the total emissions. A strong correlation (R2 = 0.70) was observed between the relative BC EFs and average vehicle speed, indicating that traffic congestion alleviation could effectively mitigate BC emissions. Moreover, BC and particle number (PN) emissions were linearly correlated (R2 = 0.90), and compared to PFI engine vehicles, the instantaneous PN-to-BC emission rates of GDI engine vehicles were less sensitive to vehicle specific power-to-velocity (VSPV) increase in all speed ranges.

Measurement report: Source and mixing state of black carbon aerosol in the North China Plain: implications for radiative effect

Abstract. Establishment of the sources and mixing state of black carbon (BC) aerosol is essential for assessing its impact on air quality and climatic effects. A winter campaign (December 2017–January 2018) was performed in the North China Plain (NCP) to evaluate the sources, coating composition, and radiative effects of BC under the background of emission reduction. Results showed that the sources of liquid fossil fuels (i.e., traffic emissions) and solid fuels (i.e., biomass and coal burning) contributed 69 % and 31 % to the total equivalent BC (eBC) mass, respectively. These values were arrived at by using a combination of multi-wavelength optical approach with the source-based aerosol absorption Ångström exponent values. The air quality model indicated that local emissions were the dominant contributors to BC at the measurement site. However, regional emissions from NCP were a critical factor for high BC pollution. A single-particle aerosol mass spectrometer identified six classes of elemental carbon (EC)-containing particles. They included EC coated by organic carbon and sulfate (52 % of total EC-containing particles); EC coated by Na and K (24 %); EC coated by K, sulfate, and nitrate (17 %); EC associated with biomass burning (6 %); pure-EC (1 %); and others (1 %). Different BC sources exhibited distinct impacts on the EC-containing particles. A radiative transfer model showed that the amount of detected eBC can produce an atmospheric direct radiative effect of +18.0 W m−2 and a heating rate of 0.5 K d−1. This study shows that reductions of solid fuel combustion-related BC may be an effective way of mitigating regional warming in the NCP.

High Sensitivity of Arctic Black Carbon Radiative Effects to Subgrid Vertical Velocity in Aerosol Activation

AbstractThe representation of aerosol activation into cloud droplets in climate models is important for accurate understanding of aerosol radiative impacts on the Arctic climate, but it remains highly uncertain. Here we show that the uncertainty range of subgrid vertical velocity (SVV) and maximum supersaturation (SSmax) in aerosol activation produces fourfold to fivefold differences in the direct radiative effect of black carbon (BC) in the Arctic (0.091–0.40 W m−2) because SVV and SSmax determine the activated fraction and wet removal efficiency of aerosols. Aerosols are particularly sensitive to SVV in remote regions but not near their sources because many aerosols near sources are not yet influenced by wet removal processes. Our results demonstrate that SVV treatment is a major source of uncertainty in Arctic aerosol simulations and may be key for reducing the large discrepancies among global models in estimates of BC and its radiative effects in the Arctic.

Combining atmospheric and snow radiative transfer models to assess the solar radiative effects of black carbon in the Arctic

Abstract. The magnitude of solar radiative effects (cooling or warming) of black carbon (BC) particles embedded in the Arctic atmosphere and surface snow layer was explored on the basis of case studies. For this purpose, combined atmospheric and snow radiative transfer simulations were performed for cloudless and cloudy conditions on the basis of BC mass concentrations measured in pristine early summer and more polluted early spring conditions. The area of interest is the remote sea-ice-covered Arctic Ocean in the vicinity of Spitsbergen, northern Greenland, and northern Alaska typically not affected by local pollution. To account for the radiative interactions between the black-carbon-containing snow surface layer and the atmosphere, an atmospheric and snow radiative transfer model were coupled iteratively. For pristine summer conditions (no atmospheric BC, minimum solar zenith angles of 55∘) and a representative BC particle mass concentration of 5 ng g−1 in the surface snow layer, a positive daily mean solar radiative forcing of +0.2 W m−2 was calculated for the surface radiative budget. A higher load of atmospheric BC representing early springtime conditions results in a slightly negative mean radiative forcing at the surface of about −0.05 W m−2, even when the low BC mass concentration measured in the pristine early summer conditions was embedded in the surface snow layer. The total net surface radiative forcing combining the effects of BC embedded in the atmosphere and in the snow layer strongly depends on the snow optical properties (snow specific surface area and snow density). For the conditions over the Arctic Ocean analyzed in the simulations, it was found that the atmospheric heating rate by water vapor or clouds is 1 to 2 orders of magnitude larger than that by atmospheric BC. Similarly, the daily mean total heating rate (6 K d−1) within a snowpack due to absorption by the ice was more than 1 order of magnitude larger than that of atmospheric BC (0.2 K d−1). Also, it was shown that the cooling by atmospheric BC of the near-surface air and the warming effect by BC embedded in snow are reduced in the presence of clouds.

Particle Size and Mixing State of Freshly Emitted Black Carbon from Different Combustion Sources in China.

Modeling studies have highlighted that accurate simulations of radiative effect of black carbon (BC) require knowledge about the particle size and mixing state of freshly emitted BC from combustion sources. However, the information is absent in China due to lack of available measurements. In this study, we present the particle size and mixing state of fresh BC emitted from diesel vehicles (DV), brick kilns (BK), residential crop residue burnings (CR), and residential firewood burnings (FW) in September-October 2014 at North China Plain by field measurement. The mass median diameters of BC cores (whole particles including cores and coatings) above the limit of measurement (i.e., > 70 nm) from these sources are ∼155 (∼194), ∼230 (∼306), ∼250 (∼438) and ∼273 (∼426) nm, respectively, and corresponding size ratios (i.e., mixing state) are ∼1.25, ∼1.33, ∼1.75, and ∼1.56, respectively. Compared with the values commonly used in model based on the laboratory experiments and the field measurements in developed countries, larger particle sizes and higher mixing sate of freshly emitted BC in China may enhance their light absorption and cloud condensation nuclei activities during atmospheric transport. The available data could be used to improve future model development on radiative effect of BC in China.

Atmospheric heating rate due to black carbon aerosols: Uncertainties and impact factors

This study investigates the impacts of black carbon (BC) properties (vertical concentration, shape, size, and mixing state) and atmospheric variables (cloud and aerosol loading, surface albedo, and solar zenith angle) on BC radiative effects. Observations from aircraft measurements, lidar, and the Aerosol Robotic Network (AERONET) are used to constrain BC and aerosol properties. The library for radiative transfer (Libradtran) model is used to calculate BC radiative forcing (RF). BC optical properties are obtained from numerical modeling with aggregate or spherical structures and different size distributions. By modifying the optical properties, different BC geometries and size distributions result in uncertainties in RF and heating rate less than 30%, while the uncertainty in heating rate due to different BC mixing states is as large as ~80%. The vertical distribution of BC concentrations explains less than 10% of the relative differences in RF and heating rate in the atmosphere, but can induce different heating rate vertical profiles, thus different planetary boundary layer (PBL) stabilities. Due to the significant influence of cloudy and aerosol conditions on incident solar radiation, atmospheric conditions play an important role in determining the BC heating rate. Meanwhile, the effects of surface albedo and solar zenith angle on the BC heating rate are most significantly near the surface. Taking the above factors into account, we introduce an empirical approximation of the BC heating rate to estimate its influence on the atmosphere. With the simple formula, the BC heating rate for a particular atmospheric layer can be approximated when the vertical condition is known, and this can be further applied to determine whether BC promotes or suppresses PBL development. Considering the importance of the BC vertical concentration in its heating rate, we suggest that light-absorbing aerosols and their vertical distributions must be better measured and modeled to improve the understanding of their radiative effects and interaction with PBL.

Quantifying snow darkening and atmospheric radiative effects of black carbon and dust on the South Asian monsoon and hydrological cycle: experiments using variable-resolution CESM

Abstract. Black carbon (BC) and dust impart significant effects on the South Asian monsoon (SAM), which is responsible for ∼80 % of the region's annual precipitation. This study implements a variable-resolution (VR) version of the Community Earth System Model (CESM) to quantify two radiative effects of absorbing BC and dust on the SAM. Specifically, this study focuses on the snow darkening effect (SDE), as well as how these aerosols interact with incoming and outgoing radiation to facilitate an atmospheric response (i.e., aerosol–radiation interactions, ARIs). By running sensitivity experiments, the individual effects of SDE and ARI are quantified, and a theoretical framework is applied to assess these aerosols' impacts on the SAM. It is found that ARIs of absorbing aerosols warm the atmospheric column in a belt coincident with the May–June averaged location of the subtropical jet, bringing forth anomalous upper-tropospheric (lower-tropospheric) anticyclogenesis (cyclogenesis) and divergence (convergence). This anomalous arrangement in the mass fields brings forth enhanced rising vertical motion across South Asia and a stronger westerly low-level jet, the latter of which furnishes the Indian subcontinent with enhanced Arabian Gulf moisture. Precipitation increases of 2 mm d−1 or more (a 60 % increase in June) result across much of northern India from May through August, with larger anomalies (+5 to +10 mm d−1) in the western Indian mountains and southern Tibetan Plateau (TP) mountain ranges due to orographic and anabatic enhancement. Across the Tibetan Plateau foothills, SDE by BC aerosols drives large precipitation anomalies of &gt; 6 mm d−1 (a 21 %–26 % increase in May and June), comparable to ARI of absorbing aerosols from April through August. Runoff changes accompany BC SDE-induced snow changes across Tibet, while runoff changes across India result predominantly from dust ARI. Finally, there are large differences in the simulated SDE between the VR and traditional 1∘ simulations, the latter of which simulates a much stronger SDE and more effectively modifies the regional circulation.

The importance of the representation of air pollution emissions for the modeled distribution and radiative effects of black carbon in the Arctic

Abstract. Aerosol particles can contribute to the Arctic amplification (AA) by direct and indirect radiative effects. Specifically, black carbon (BC) in the atmosphere, and when deposited on snow and sea ice, has a positive warming effect on the top-of-atmosphere (TOA) radiation balance during the polar day. Current climate models, however, are still struggling to reproduce Arctic aerosol conditions. We present an evaluation study with the global aerosol-climate model ECHAM6.3-HAM2.3 to examine emission-related uncertainties in the BC distribution and the direct radiative effect of BC. The model results are comprehensively compared against the latest ground and airborne aerosol observations for the period 2005–2017, with a focus on BC. Four different setups of air pollution emissions are tested. The simulations in general match well with the observed amount and temporal variability in near-surface BC in the Arctic. Using actual daily instead of fixed biomass burning emissions is crucial for reproducing individual pollution events but has only a small influence on the seasonal cycle of BC. Compared with commonly used fixed anthropogenic emissions for the year 2000, an up-to-date inventory with transient air pollution emissions results in up to a 30 % higher annual BC burden locally. This causes a higher annual mean all-sky net direct radiative effect of BC of over 0.1 W m−2 at the top of the atmosphere over the Arctic region (60–90∘ N), being locally more than 0.2 W m−2 over the eastern Arctic Ocean. We estimate BC in the Arctic as leading to an annual net gain of 0.5 W m−2 averaged over the Arctic region but to a local gain of up to 0.8 W m−2 by the direct radiative effect of atmospheric BC plus the effect by the BC-in-snow albedo reduction. Long-range transport is identified as one of the main sources of uncertainties for ECHAM6.3-HAM2.3, leading to an overestimation of BC in atmospheric layers above 500 hPa, especially in summer. This is related to a misrepresentation in wet removal in one identified case at least, which was observed during the ARCTAS (Arctic Research of the Composition of the Troposphere from Aircraft and Satellites) summer aircraft campaign. Overall, the current model version has significantly improved since previous intercomparison studies and now performs better than the multi-model average in the Aerosol Comparisons between Observation and Models (AEROCOM) initiative in terms of the spatial and temporal distribution of Arctic BC.

Open fires in Greenland in summer 2017: transport, deposition and radiative effects of BC, OC and BrC emissions

Abstract. Highly unusual open fires burned in western Greenland between 31 July and 21 August 2017, after a period of warm, dry and sunny weather. The fires burned on peatlands that became vulnerable to fires by permafrost thawing. We used several satellite data sets to estimate that the total area burned was about 2345 ha. Based on assumptions of typical burn depths and emission factors for peat fires, we estimate that the fires consumed a fuel amount of about 117 kt C and emitted about 23.5 t of black carbon (BC) and 731 t of organic carbon (OC), including 141 t of brown carbon (BrC). We used a Lagrangian particle dispersion model to simulate the atmospheric transport and deposition of these species. We find that the smoke plumes were often pushed towards the Greenland ice sheet by westerly winds, and thus a large fraction of the emissions (30 %) was deposited on snow- or ice-covered surfaces. The calculated deposition was small compared to the deposition from global sources, but not entirely negligible. Analysis of aerosol optical depth data from three sites in western Greenland in August 2017 showed strong influence of forest fire plumes from Canada, but little impact of the Greenland fires. Nevertheless, CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) lidar data showed that our model captured the presence and structure of the plume from the Greenland fires. The albedo changes and instantaneous surface radiative forcing in Greenland due to the fire emissions were estimated with the SNICAR model and the uvspec model from the libRadtran radiative transfer software package. We estimate that the maximum albedo change due to the BC and BrC deposition was about 0.007, too small to be measured. The average instantaneous surface radiative forcing over Greenland at noon on 31 August was 0.03–0.04 W m−2, with locally occurring maxima of 0.63–0.77 W m−2 (depending on the studied scenario). The average value is up to an order of magnitude smaller than the radiative forcing from other sources. Overall, the fires burning in Greenland in the summer of 2017 had little impact on the Greenland ice sheet, causing a small extra radiative forcing. This was due to the – in a global context – still rather small size of the fires. However, the very large fraction of the emissions deposited on the Greenland ice sheet from these fires could contribute to accelerated melting of the Greenland ice sheet if these fires become several orders of magnitude larger under future climate.

Black carbon radiative effects highly sensitive to emitted particle size when resolving mixing-state diversity

Post-industrial increases in atmospheric black carbon (BC) have a large but uncertain warming contribution to Earth’s climate. Particle size and mixing state determine the solar absorption efficiency of BC and also strongly influence how effectively BC is removed, but they have large uncertainties. Here we use a multiple-mixing-state global aerosol microphysics model and show that the sensitivity (range) of present-day BC direct radiative effect, due to current uncertainties in emission size distributions, is amplified 5–7 times (0.18–0.42 W m−2) when the diversity in BC mixing state is sufficiently resolved. This amplification is caused by the lifetime, core absorption, and absorption enhancement effects of BC, whose variability is underestimated by 45–70% in a single-mixing-state model representation. We demonstrate that reducing uncertainties in emission size distributions and how they change in the future, while also resolving modeled BC mixing state diversity, is now essential when evaluating BC radiative effects and the effectiveness of BC mitigation on future temperature changes.