Black Carbon Aerosols Research Articles

Mutual response hypothesis between surface temperature and aerosol (BC and non-BC) mass concentration observed in an urban environment

The mutual response between near surface aerosol concentration and surface temperature works in a complicated manner. A recent study has introduced a hypothesis of mutual response between surface temperature and near surface black carbon (BC) mass concentration which states that ‘more fall in morning hour surface temperature (T) contribute to the enhancement of BC fumigation peak after the sunrise which positively impacts the extra rise in mid-day temperature over a region during the day time’. Morning hour surface temperature is proportionally linked with the strength of the night time near surface temperature inversion which contributes to the enhancement of the fumigation peak of BC aerosols after the sunrise and the enhanced fumigation peak can impact the degree of the mid-day surface temperature rise by influencing the instantaneous heating. However, it didn't mention the role of non-BC aerosols. Further, the hypothesis was drawn based on the co-located ground-based observations of surface temperature and BC concentration at a rural location of peninsular India. Though, it was mentioned that the hypothesis can be tested independently of locations, but was not thoroughly validated for an urban environment where the loading of both BC and non-BC aerosols are high. In this context, the first objective of the present work is to methodically test the BC –T hypothesis over an Indian metropolitan city, Kolkata, using the suite of measurements obtained from Kolkata Camp Observatory of NARL (KCON) along with other supporting data. In addition, the validity of the hypothesis for the non-BC fraction of PM2.5 aerosols over the same location is also tested. Besides ascertaining the above-mentioned hypothesis over an urban location, it is found that the enhancement of non-BC PM2.5 aerosols peak after the sunrise can negatively influences the mid-day temperature rise over a region during the day time.

Performance evaluation of portable dual-spot micro-aethalometers for source identification of black carbon aerosols: application to wildfire smoke and traffic emissions in the Pacific Northwest

Abstract. Black carbon (BC) is a component of particulate matter, emitted from the incomplete combustion of carbonaceous fuels. The presence of BC in the atmosphere can disrupt the atmospheric radiation budget, and exposure to BC can adversely affect human health. Multi-wavelength light-absorption-based dual-spot aethalometers can be used to quantify the source and characteristics of BC from traffic or biomass-burning-based sources. However, aethalometer measurements are affected by artifacts such as aerosol loading and light scattering; hence, they often need correction to reduce measurement uncertainty. This work assesses the performance of the recently developed portable aethalometer (MA300, AethLabs). Due to their portability and ease of usage, MA300s can be suitable for mobile and personal exposure monitoring. Here, we evaluate BC concentration and source apportionment accuracy of three MA300 units relative to a widely used aethalometer, the AE33 (Magee Scientific). Synchronous field measurements were performed at a major traffic intersection during regular and wildfire-smoke-affected days in Vancouver, Canada. We find that MA300-reported BC mass concentrations were strongly correlated (Slope range between 0.73 and 1.01, with R2 = 0.9) compared to the reference instrument, yet there is visible instrumental variability in the normalized concentrations (5 %) across three units. The mean absolute error of MA300-reported BC concentrations ranged between 0.44–0.98 µg m−3, with the highest deviations observed in wildfire-smoke-affected polluted days. From the aerosol light absorption measurement perspective, MA300s tend to underestimate the absorption coefficients (babs) across the five wavelengths. UV channel light absorption results were subjected to the highest amount of noise and were found to be consistently underestimating in all the MA300 units, leading to systematic bias in source apportionment analysis. Absorption Ångström exponent values from the MA300 units were able to capture the variability of aerosol sources within a day, with a mean value of 1.15 during clean days and 1.46 during wildfire-smoke-affected days. We investigated the application of the latest non-linear aethalometer correction protocols in the MA300 and found that flow fluctuations enhanced noise across all channels, compared to onboard instrument correction. We also identify that the UV (λ = 370 nm) channel absorption measurements are most sensitive to instrumental artifacts during the wildfire-smoke-affected period. Hence, as an alternative to traditional UV and IR (λ = 880 nm)-based BC source apportionment methods, in this work, we tested the blue (λ = 470 nm) and IR wavelengths for BC source apportionment calculation. When the blue–IR-based source apportionment technique is adopted instead of the UV–IR, there is a 10 % (on average) decrease in the percentage difference of the apportioned components from the reference monitor.

Constraining the complex refractive index of black carbon particles using the complex forward-scattering amplitude

Black carbon is the largest contributor to global aerosol’s shortwave absorption in the current atmosphere and is an important positive climate forcer. The complex refractive index, m = mr + imi, the primary determinant of the absorbed and scattered energies of incident radiation per unit volume of particulate material, has not been accurately known for atmospheric black carbon material. An accurate value at visible wavelengths has been difficult to obtain due to the black carbon’s wavelength-scale irregularity and variability of aggregate shape, distribution in particle size, and mixing with other aerosol compounds. Here, we present a method to constrain a plausible (mr, mi) domain for black carbon from the observed distribution of the complex forward-scattering amplitude S(0°). This approach suppresses the biases due to the above-mentioned complexities. The S(0°) distribution of black carbon is acquired by performing single particle S(0°) measurements in a water medium after collecting atmospheric aerosols into water. We demonstrate the method operating at λ = 0.633 μm for constraining the refractive index of black carbon aerosols in the north-western Pacific boundary layer. From the plausible (mr, mi) domain consistent with the observed S(0°) distributions and the reported range of mass absorption cross-section, we conservatively select 1.95 + 0.96i as a recommendable value of the refractive index for uncoated black carbon at visible wavelengths. The recommendable value is 0.17 larger in mi than the widely used value 1.95 + 0.79i in current aerosol-climate models, implying a ∼16% underestimate of shortwave absorption by black carbon aerosols in current climate simulations.

Solubility Considerations for Cloud Condensation Nuclei (CCN) Activity Analysis of Pure and Mixed Black Carbon Species

Black carbon (BC) is an aerosol that is released into the atmosphere due to the incomplete burning of biomass and can affect the climate directly or indirectly. BC commonly mixes with other primary or secondary aerosols to undergo aging, thereby changing its radiative properties and cloud condensation nuclei (CCN) activity. The composition of aged BC species in the atmosphere is difficult to measure with high confidence, so their associated CCN activity can be uncertain. In this work, the CCN activity analysis of BC was performed using laboratory measurements of proxy aged BC species. Vulcan XC72R carbon black was used as the representative of BC, and three structural isomers of benzenedicarboxylic acid─phthalic acid (PTA), isophthalic acid (IPTA), and terephthalic acid (TPTA)─were mixed with BC to generate three different proxies of aged BC species. Most studies related to CCN activity analysis of BC aerosols use the traditional Köhler theory or an adsorption theory (such as the Frenkel-Halsey-Hill adsorption theory). PTA, IPTA, and TPTA fall in the sparingly water-soluble range and therefore do not fully obey either of the aforementioned theories. Consequently, a novel hybrid activity model (HAM) was used for the CCN activity analysis of the BC mixtures studied in this work. HAM combines the features of adsorption theory via the adsorption isotherm with the features of Köhler theory by incorporating solubility partitioning. The results in this work showed that HAM improves the representation of CCN activity of pure and mixed BC aerosol species with high certainty, evident from generally better goodness of fit, R2 > 0.9. This work implies that the hygroscopicity parameterization based on HAM captures the size-dependent variability in the CCN activity of the pure and aged BC species.

The density of ambient black carbon retrieved by a new method: implications for cloud condensation nuclei prediction

Abstract. The effective density of black carbon (BC) is a crucial factor that is relevant to its aging degree and adds uncertainty in evaluating its climate effect. Here, we have developed a new method to retrieve the effective density of internally mixed BC in the atmosphere, combining field observations conducted from 15 November to 14 December 2016 in urban Beijing with the Köhler theory. The uncertainty in the retrieval method was evaluated to be within ±30 %, which was primarily caused by assumptions on both the hygroscopic parameter of organics and the proportional distribution of primary organic aerosols in different hygroscopic modes. Using the method, we find that the ambient internally mixed BC, accounting for 80 % ± 20 % of total BC aerosol particles, was retrieved with a campaign mean density of 1.1 ± 0.6 g cm−3 during the observed periods. The retrieved result was comparable with that reported in the literature. By applying a lower (0.14 g cm−3) and upper (2.1 g cm−3) limit of the retrieved BC density in the cloud condensation nuclei (CCN) number concentration (NCCN) estimation, we derived that the neglect of such variations in the BC density would lead to an uncertainty of −28 %–11 % in predicting NCCN at supersaturations of 0.23 % and 0.40 %. We also find that the NCCN was more sensitive to the variations in BC density when it was <1.0 g cm−3. This illustrates the necessity of accounting for the effect of BC density on CCN activity closer to source regions where the BC particles are mostly freshly emitted. The CCN closure was achieved when introducing the retrieved real-time BC density and mixing state. This study provides a unique way of utilizing field measurements to infer ambient BC density and highlights the importance of applying variable BC density values in models when predicting CCN and assessing its relevant climate effect.

Potential Impacts on Ozone and Climate From a Proposed Fleet of Supersonic Aircraft

AbstractThere has been renewed interest in developing commercial supersonic transport aircraft due to the increased overall demands by the public for air travel, the aspiration for more intercontinental travel, and the desire for shorter flight times. Various companies and academic institutions have been actively considering the designs of such supersonic aircraft. As these new designs are developed, the environmental impact on ozone and climate of these fleets need to be explored. This study examines one such proposed commercial supersonic fleet of 55‐seater that is projected to fly at Mach 2.2, corresponding to cruise altitudes of 17–20 km, and which would burn 122.32 Tg of fuel and emit 1.78 Tg of NOx each year. Our analyses indicate this proposed fleet would cause a 0.74% reduction in global column ozone (∼2 Dobson Units), which is mainly attributed to the large amounts of nitrogen oxides released in the atmosphere from the supersonic aircraft. The maximum ozone loss occurs at the tropics in the fall season, with a reduction of −1.4% in the total column ozone regionally. The stratospheric‐adjusted radiative forcing on climate from this fleet was derived based on changes in atmospheric concentrations of ozone (59.5 mW/m2), water vapor (10.1 mW/m2), black carbon (−3.9 mW/m2) and sulfate aerosols (−20.3 mW/m2), resulting in a net non‐CO2, non‐contrail forcing of 45.4 mW/m2, indicating an overall warming effect.

Black carbon in contrasting environments in India: Temporal variability, source apportionment and radiative forcing

Analyses of black carbon (BC) data from three different environments in India - Delhi megacity, Srinagar metropolitan and Gulmarg hill station, showed that Delhi had the highest annual average BC concentration (12.3 ± 10.2 μg m−3), followed by Srinagar (4.3 ± 5 μg m−3) and Gulmarg (2.4 ± 2 μg m−3). The inflow of aerosols from the neighboring agricultural regions, notably during Winter, causes Delhi to have the highest seasonal average BC (16.8 μg m−3). Srinagar had the highest average seasonal BC during autumn (6.3 μg m−3) due to the burning of horticulture residue and hardwood for charcoal making and residential heating. At Gulmarg, on the other hand, the winter season's high BC (2.2 μg m−3) is due to the increased emissions from the tourist traffic, snowmobile/ATVs and wood burning for residential heating. BC concentrations in Delhi and Srinagar were roughly in line with their population size. However, compared to sites with the similar population, BC at Gulmarg was roughly twice higher than the other sites. There was a higher contribution to BC from fossil fuels than biomass burning at all three sites, which indicates that cars are the primary source of BC. Overall, values of BC aerosol optical properties in Delhi are much higher than those in Srinagar and Gulmarg. During the cold season, continental air masses transport BC from the neighboring areas to Delhi and westerlies enhance the local BC loading at Srinagar and Gulmarg. The predominant presence of absorbing aerosols, particularly BC, during late autumn and winter at all three sites leads to an increase in aerosol optical depth (AOD), a reduction in single scattering albedo (SSA) and an increase in asymmetry parameter (AP). As a result, there is a significant increase in the radiative forcing of the atmosphere (RFATM), with the highest values observed in January in Delhi (+71.5 W m−2) and Srinagar (+56.05 W m−2), and in November at Gulmarg (+18.5 W m−2). These findings suggest that small rural towns that are affected by seasonal emissions, low planetary boundary layers, and frequent temperature inversions, can contribute to a substantial amount of radiative forcing. This study provides a larger perspective on increasing BC in Delhi, and urban-rural fringe areas in the Indian Himalayas, which is crucial for identifying what actions must be taken to control BC emissions to reduce impacts on cryosphere, human health and other sectors.

Local and remote climate impacts of future African aerosol emissions

Abstract. The potential future trend in African aerosol emissions is uncertain, with a large range found in future scenarios used to drive climate projections. The future climate impact of these emissions is therefore uncertain. Using the Shared Socioeconomic Pathway (SSP) scenarios, transient future experiments were performed with the UK Earth System Model (UKESM1) to investigate the effect of African emissions following the high emission SSP370 scenario as the rest of the world follows the more sustainable SSP119, relative to a global SSP119 control. This isolates the effect of Africa following a relatively more polluted future emissions pathway. Compared to SSP119, SSP370 projects higher non-biomass-burning (non-BB) aerosol emissions, but lower biomass burning emissions, over Africa. Increased shortwave (SW) absorption by black carbon aerosol leads to a global warming, but the reduction in the local incident surface radiation close to the emissions is larger, causing a local cooling effect. The local cooling persists even when including the higher African CO2 emissions under SSP370 than SSP119. The global warming is significantly higher by 0.07 K when including the non-BB aerosol increases and higher still (0.22 K) when including all aerosols and CO2. Precipitation also exhibits complex changes. Northward shifts in the Inter-tropical Convergence Zone (ITCZ) occur under relatively warm Northern Hemisphere land, and local rainfall is enhanced due to mid-tropospheric instability from black carbon absorption. These results highlight the importance of future African aerosol emissions for regional and global climate and the spatial complexity of this climate influence.

Informed Multi‐Scale Approach Applied to the British Columbia Fires of Late Summer 2017

AbstractPyrocumulonimbus (PyroCb) clouds have a complex origin dependent on fire dynamics and meteorological conditions. When a pyrocumulonimbus cloud develops and is maintained over a period of time, it can inject significant aerosol into the troposphere and lower stratosphere, resulting in a longer‐term (months to years) occurrence of aerosol in the stratosphere. In this work, we investigate the British Columbia wildfires on 12–13 August 2017 using a multi‐scale simulation framework. We use the output of a physics‐based wildfire model (FIRETEC) with parameterized energy, particle, and gas emissions to drive the upper atmospheric aerosol mass injection within a regional cloud resolving model (HIGRAD). We demonstrate that vertical motions produced by latent heat release of the condensation of ice and cloud particles within the PyroCbs induce another 5 km of lifting of the simulated aerosol plume. Primary black carbon and organic aerosols (OAs) alone may not be enough to explain the observed aerosol burden, thus we show that secondary OA produced via condensation of gases by the fires, ash, and possibly dust can enhance lofted aerosol mass. A simulation with all emission mechanisms active, driven by the observed fuel load and environmental conditions, reasonably reproduces an aerosol profile inferred from observational data.

Source apportionment of black carbon aerosols by isotopes (14C and 13C) and Bayesian modeling from two remote islands in east Asian outflow region

We report the results of source apportionment of combustion-derived black carbon (BC), in PM2.5 aerosols collected from the East Asian continental outflow region at two islands; Okinawa and Fukue during the period from October 2009 to May 2010. The 14C contents of BC from Okinawa (Cape Hedo) and Fukue islands (Fukue) varied from 24.4 to 34.2 pMC and from 18.1 to 43.0 pMC, respectively. Source apportionment of BC was conducted by using a simple 14C mass balance model and a dual-isotope Bayesian Markov chain Monte Carlo model. Biomass combustion contributions (e.g., wood fuel and crop residues) were 23–31 % (mean 27 ± 3 %) at Cape Hedo and 15–38 % (mean 27 ± 12 %) at Fukue. Both sites were equally affected by biomass combustion, whose levels are similar to those observed in the hotspot regions (megacities) in China. Fossil fuel contributions (e.g., oil, gasoline, and diesel) were 69–77 % (mean 74 ± 3 %) with 2–69 % from coal and 3–76 % from liquid fossil at Cape Hedo, and 55–85 % (mean 73 ± 12 %) at Fukue with 3 % from coal and 53–56 % from liquid fuel for the early winter. Those variations for both sites showed significantly different source region-specific trends and this trend was also consistent with the results of the air mass trajectory analysis with a higher contribution of coal-BC from North China including Beijing, and East China including Shanghai. In spring, we found a higher contribution of liquid fossil fuel combustion (e.g., traffic) over the East China Sea, including Pacific air masses, suggesting that the possible contribution of ship emissions was relatively high. Although our results for isotopes-based source apportionment of BC are preliminary, these findings suggest that long-term monitoring of BC aerosols, even in remote sites of Asian outflows, and source-specific descriptions of BC are important to improve climate models. We also recommend further measurements for implementing regionally tailored mitigation.

Size–resolved mixing state of ambient refractory black carbon aerosols in Beijing during the XXIV Olympic winter games

Atmospheric loading of black carbon aerosols influences air quality and visibility, and their mixing state and aerosol chemistry were sensitive to both emission scenarios and regional transport. In this study, the aerodynamic size-resolved mixing state of refractory black carbon aerosols (rBC) was investigated using a novel tandem system consisting of an aerodynamic aerosol classifier (AAC), a single particle soot photometer (SP2), and single-particle-aerosol mass spectrometry (SPA-MS) during the XXIV Olympic Winter Games (OWG) at an urban site in Beijing. Particles with aerodynamic diameter (Dae) of 200 nm and 300 nm were selected by AAC to focus on the effect of relative differences in morphology on the coating thickness, coating compositions, and optical properties of rBC particles. We found that rBC-containing particles with Dae of 300 nm were characterized by a rBC core with a count median diameter (CMD) of 108 ± 4 nm that typically have regular morphology (χ:mean∼1), higher relative coating thickness (RCT: mean ∼1.9), and strong light absorption enhancement (Eabs: mean ∼1.5). The rBC-containing particles with Dae = 200 nm normally had irregular shapes (χ:mean∼1.4) and weak Eabs (Eabs: mean ∼1.37). Classification based on air mass clustering and air pollution level revealed that the coating thickness of rBC particles only exhibited unimodal patterns under clean air conditions and distinct bimodal distributions under heavy pollution conditions, implying multiple origins of rBC particles, even during OWG periods. The coating thickness and Eabs of rBC particles were greater when influenced by the higher RH air from east. Furthermore, the chemical compositions of the rBC coating quantitatively determined by SPA-MS were used to estimate the possible origins of the Dae = 300 nm, featured by a thicker coating thickness and stronger light absorption enhancement. Our results showed that rBC particles were primarily mixed with organics, nitrate, and sulfate during the XXIV OWG period. The organic components have a limited role in increasing rBC coatings under polluted conditions, while the alkali metal ions (K and Na) associated with traffic emissions and the secondary inorganic species favor the formation of thick coatings. Higher RH makes limited contributions to rBC mixed with sulfate and organics only (BCOC*_S) and pure BC. The relatively fresh BC could directly mix with organics and sulfate at low RH levels while evolving to mix with nitrate at high RH conditions. In addition to high concentrations of locally emitted precursors and high RH that tend to form thick coatings of nitrate-related rBC aerosols, secondary transport from the west and southwest also contributes to rBC aerosols mixed with nitrate with relatively thick coatings.

Effects of transport on a biomass burning plume from Indochina during EMeRGe-Asia identified by WRF-Chem

Abstract. The Indochina biomass burning (BB) season in springtime has a substantial environmental impact on the surrounding areas in Asia. In this study, we evaluated the environmental impact of a major long-range BB transport event on 19 March 2018 (a flight of the High Altitude and Long Range Research Aircraft (HALO; https://www.halo-spp.de, last access: 14 February 2023) research aircraft, flight F0319) preceded by a minor event on 17 March 2018 (flight F0317). Aircraft data obtained during the campaign in Asia of the Effect of Megacities on the transport and transformation of pollutants on the Regional to Global scales (EMeRGe) were available between 12 March and 7 April 2018. In F0319, results of 1 min mean carbon monoxide (CO), ozone (O3), acetone (ACE), acetonitrile (ACN), organic aerosol (OA), and black carbon aerosol (BC) concentrations were up to 312.0, 79.0, 3.0, and 0.6 ppb and 6.4 and 2.5 µg m−3, respectively, during the flight, which passed through the BB plume transport layer (BPTL) between the elevation of 2000–4000 m over the East China Sea (ECS). During F0319, the CO, O3, ACE, ACN, OA, and BC maximum of the 1 min average concentrations were higher in the BPTL by 109.0, 8.0, 1.0, and 0.3 ppb and 3.0 and 1.3 µg m−3 compared to flight F0317, respectively. Sulfate aerosol, rather than OA, showed the highest concentration at low altitudes (<1000 m) in both flights F0317 and F0319 resulting from the continental outflow in the ECS. The transport of BB aerosols from Indochina and its impacts on the downstream area were evaluated using a Weather Research Forecasting with Chemistry (WRF-Chem) model. The modeling results tended to overestimate the concentration of the species, with examples being CO (64 ppb), OA (0.3 µg m−3), BC (0.2 µg m−3), and O3 (12.5 ppb) in the BPTL. Over the ECS, the simulated BB contribution demonstrated an increasing trend from the lowest values on 17 March 2018 to the highest values on 18 and 19 March 2018 for CO, fine particulate matter (PM2.5), OA, BC, hydroxyl radicals (OH), nitrogen oxides (NOx), total reactive nitrogen (NOy), and O3; by contrast, the variation of J(O1D) decreased as the BB plume's contribution increased over the ECS. In the lower boundary layer (<1000 m), the BB plume's contribution to most species in the remote downstream areas was <20 %. However, at the BPTL, the contribution of the long-range transported BB plume was as high as 30 %–80 % for most of the species (NOy, NOx, PM2.5, BC, OH, O3, and CO) over southern China (SC), Taiwan, and the ECS. BB aerosols were identified as a potential source of cloud condensation nuclei, and the simulation results indicated that the transported BB plume had an effect on cloud water formation over SC and the ECS on 19 March 2018. The combination of BB aerosol enhancement with cloud water resulted in a reduction of incoming shortwave radiation at the surface in SC and the ECS by 5 %–7 % and 2 %–4 %, respectively, which potentially has significant regional climate implications.

Pyrocumulonimbus affect average stratospheric aerosol composition.

Pyrocumulonimbus (pyroCb) are wildfire-generated convective clouds that can inject smoke directly into the stratosphere. PyroCb have been tracked for years, yet their apparent rarity and episodic nature lead to highly uncertain climate impacts. In situ measurements of pyroCb smoke reveal its distinctive and exceptionally stable aerosol properties and define the long-term influence of pyroCb activity on the stratospheric aerosol budget. Analysis of 13 years of airborne observations shows that pyroCb are responsible for 10 to 25% of the black carbon and organic aerosols in the "present-day" lower stratosphere, with similar impacts in both the North and South Hemispheres. These results suggest that, should pyroCb increase in frequency and/or magnitude in future climates, they could generate dominant trends in stratospheric aerosol.

Black carbon aerosols over Indian Ocean have unique source fingerprint and optical characteristics during monsoon season

Effects of aerosols such as black carbon (BC) on climate and buildup of the monsoon over the Indian Ocean are insufficiently quantified. Uncertain contributions from various natural and anthropogenic sources impede our understanding. Here, we use observations over 5 y of BC and its isotopes at a remote island observatory in northern Indian Ocean to constrain loadings and sources during little-studied monsoon season. Carbon-14 data show a highly variable yet largely fossil (65 ± 15%) source mixture. Combining carbon-14 with carbon-13 reveals the impact of African savanna burning, which occasionally approach 50% (48 ± 9%) of the total BC loadings. The BC mass-absorption cross-section for this regime is 7.6 ± 2.6 m2/g, with higher values during savanna fire input. Taken together, the combustion sources, longevity, and optical properties of BC aerosols over summertime Indian Ocean are different than the more-studied winter aerosol, with implications for chemical transport and climate model simulations of the Indian monsoon.

Observations on the decadal variability of aerosol in eastern Himalayan foothills: Evidence of an anthropologically induced positive shift

The decadal variability of direct radiative effects of aerosols is investigated at Dibrugarh, a site in northeast India (NEI) at the eastern Himalayan foothills, primarily using multi-wavelength solar radiometer measurements spanning from October 2001 to February 2020. The ground-based aerosol observations are combined with satellite remote sensing, reanalysis data, and model simulations to study the change in atmospheric particle loading over the region. Observations indicate a statistically significant increase (∼0.015 yr−1) in Aerosol Optical Depth (AOD) during the last two decades in line with an increase in human activity. As compared to 2001–2007 (we call it as Stage I), the aerosol burden has grown rapidly during 2008 until 2020 (Stage II). AOD at 500 nm is found to increase by ∼40% from Stage I to Stage II, resulting in an increase in the aerosol direct radiative forcing (DRF) at the top of the atmosphere (TOA) by ∼43% during stage II (∼−16.0 W m-2), from the base value of −11.2 W m−2 in Stage I. Decreasing biomass burning activities, black carbon aerosol mass concentration, and high sulfate and organic aerosols are the primary factors responsible for the trend in TOA cooling by −0.46 W m−2 yr−1. This is further aided by the decrease in rainfall over NEI. MERRA-2 data analysis shows a similar enhancements in aerosol load over the entire NEI and the adjacent highly polluted Indo-Gangetic Plains (IGP). A similar feature is seen over the IGP, primarily driven by anthropogenic emissions, but precedes that in NEI by about a year. A simulation of the regional climate model (RegCM) over the south Asian domain quantifies the contribution of aerosol loading over NEI due to the aerosols carried from the IGP. In the highest aerosol loading period, about 12–30% of the aerosols, equivalent to 15–30% of atmospheric warming, are transported from the IGP to the NEI.

Size and light absorption of miniature-inverted-soot-generator particles during operation with various fuel mixtures

The Argonaut miniature inverted soot generator (MISG) serves as a convenient and stable source of soot black-carbon aerosol particles. The MISG performance has been previously characterized for ethylene and propane, in a simple two-flow setup of fuel and air. These fuels produce soot size distributions with geometric median diameters (GMDs) of 150–200 nm. These sizes are substantially larger than the soot particles emitted from typical internal-combustion and aviation gas turbine engines. Here, we sought to produce substantially smaller soot particles, representative of aviation gas turbine engine emissions, by using five different fuels (acetylene, methane, ethylene, propane, and dimethyl ether) and by enriching the combustion air with oxygen. We developed a rapid screening protocol for each fuel, to allow the full range of stable flame conditions to be explored. We monitored the size distribution, mass concentration, and mass absorption cross section (MAC) of denuded MISG soot in real time. We considered only operating conditions where stable soot mass concentrations above 3 μg/m3 were emitted, corresponding to a non-flickering and open-tipped flame. For virtually all operating conditions, the measured MAC was consistent with literature values for mature soot. The only exception was a propane-acetylene mixture, for which the measured MAC was much lower than literature values. The observed GMDs fell into two groups, and we did not identify any trends leading to the mixtures falling into either group. The two groups were at approximately 100 nm and 160 nm. Therefore, while this study identified conditions that reduced the soot particles to 100 nm, it did not identify conditions where even smaller soot particles could be produced. This study has demonstrated that the soot properties produced by the MISG are highly repeatable and relatively insensitive to fuel composition.

Source apportionment of black carbon aerosols in winter across China

Black carbon (BC) aerosols emitted from incomplete combustion of fossil fuels, biofuels, and biomass have significant effects on the environment and human health. Combustion-derived BC aerosols are an important component in haze pollution. High concentrations of BC aerosols were found in fine particulate matter (PM2.5) in China, and source apportionment was the strategy underpinning targeted mitigation actions. Here, we present a Bayesian statistical model, a three-dimensional array of a stable carbon isotope (δ13C) and the ratios of non-sea-salt K+ to BC (nss-K+/BC) and ΔBC/ΔCO that is a reasonably inexpensive and rapid way to constrain BC source apportionments. This study analyzed 551 daily PM2.5 samples collected in January 2018 in 18 large cities and at 1 remote site scattered across China. The results show that BC concentrations were generally higher in cities in northern China than they were in cities in southern China. Source apportionments indicate that BC in 44% of cities was mainly from liquid fuel combustion. In other sites, including 39% of cities, one suburban site, and one remote site, BC was mainly from biomass burning. These findings suggest that to improve air quality, the Chinese government should further strengthen controls on liquid fuel combustion and consider controlling biomass burning.

Carbonaceous aerosols remote sensing from geostationary satellite observation, Part I: Algorithm development using critical reflectance

Current aerosol remote sensing without using multi-view satellite sensors still fail to retrieve its components directly, such as black carbon (BC) and organic carbon (OC) simultaneously due to the limitations on available observations. In this study, A new general carbonaceous aerosol retrieval strategy for geostationary single-view satellite observations is implemented based on a method of critical reflectance, to retrieve the parameters of BC and extra OC concentration from measured radiance without prior quantification of Aerosol Optical Thickness (AOT). The method is based on measuring the change in upward reflectance between clear and hazy days over a varying surface reflectance, with the aim of finding a balance between brightening due to scattering and darkening due to absorption. Since aerosols in the proposed algorithm are considered as a mixture of BC, OC and clustered shell aerosols, this balance can be used to retrieve concentration parameters of these components via radiative transfer models. Sensitivity tests indicate that different scenarios of BC and OC volume fractions can introduce certain sensitivity pattern on critical reflectance. The retrieval is achieved by minimizing the differences between measured critical reflectance and a set of look-up tables (LUTs). Random sampling consensus (RANSAC) is also used in the strategy to reduce the influence of clouds and anomalous pixels on the retrievals. Since critical reflectance should be calculated by comparing geometrically consistent clear and hazy images, the algorithm is more suitable for geostationary satellites with constant viewing geometries. An initial validation and application applied to Himawari images over the North China Plain (NCP) shows that the carbonaceous aerosol retrievals are highly consistent with the expectations in terms of spatial and temporal patterns. The retrievals of BC and OC concentration follow the daily fluctuations of the Aethalometers observations and feature small differences in mean values throughout the month. Additionally, the AOTs at 0.55 μm can be also satisfactorily reproduced based on the carbonaceous aerosol retrievals, resulting in a mean absolute error of 0.089 and a correlation coefficient of 0.870. The main errors in the method arise from shell model assumptions, RANSAC fitting bias, inconsistent clear reference AOT in LUT, and geometric inconsistency between the clear reference and hazy images. This work indicates that the BC and OC concentration in high resolution can be acquired through the geostationary single-view remote sensing for the further air quality and climate studies.

The pollution characterization of black carbon aerosols in the southwest suburb of beijing from 2013 to 2019

Multi-year monitoring of black carbon (BC) concentrations has been conducted for the period December 2012 to January 2020 in Beijing. Equivalent BC1 (EBC1) and equivalent BC2 (EBC2) were measured using an EEL43D black carbon meter (throughout the sampling period) and a multi-wavelength absorption black carbon instrument (MABI, July 2021 to January 2020), respectively. A series of harsh measures resulted in a gradual decreasing in EBC1 mass concentration, with an annual average value of 5.38 ± 3.22 μg m−3. EBC1 mass concentration reached the peak in winter during these seven years. EBC1 mass concentration exhibited statistically negative correlations with planetary boundary layer height (R = −0.4) and ventilation coefficient (R = −0.3). The local atmospheric parameters such as temperature, wind speed, relative humidity and visibility also showed inverse relationship with EBC1. EBC1 mass concentration is in a trough during the year with high cumulative rainfall, indicating the removal effect of rainfall on BC. The accuracy of the new MABI instrument was verified and the mass absorption coefficient was re-estimated. The results revealed the relative contribution of biomass burning to EBC2 was 45% (0.08–3.93 μg m−3) during study period. The fossil fuels and traffic emission were the dominating source of EBC2 in most of the months, but biomass burning contributes more to EBC2 during the winter heating period.

Distribution and variability of Black Carbon Aerosol and its response to specific Meteorological Occurrences: A case study on the Indian city of Ranchi

Distribution and variability of Black Carbon Aerosol and its response to specific Meteorological Occurrences: A case study on the Indian city of Ranchi