Mass Absorption Cross Section Research Articles

Carbonaceous aerosol transport from the Indo-Gangetic Plain to the Himalayas: Carbon isotope evidence and light absorption characteristics

The Indo-Gangetic Plain (IGP) is a major regional and global emitter of atmospheric pollutants, which adversely affect surrounding areas such as the Himalayas. We present a comprehensive dataset on carbonaceous aerosol (CA) composition, radiocarbon (Δ14C) -based source apportionment, and light absorption of total suspended particle (TSP) samples collected over a 3-year period from high-altitude Jomsom in the central Himalayas. The 3-year mean TSP, organic carbon (OC), and elemental carbon (EC) concentrations were 92.0 ± 28.6, 9.74 ± 6.31, and 2.02 ± 1.35 μg m−3, respectively, with the highest concentrations observed during the pre-monsoon season, followed by the post-monsoon, winter, and monsoon seasons. The Δ14C analysis revealed that the contribution of fossil fuel combustion (ffossil) to EC was 47.9% ± 11.5%, which is consistent with observations in urban and remote regions in South Asia and attests that EC likely arrives in Jomsom from upwind IGP sources via long-range transport. In addition, the lowest ffossil (38.7% ± 13.3%) was observed in winter, indicating large contributions in this season from local biomass burning. The mass absorption cross-section of EC (MACEC: 8.27 ± 1.76 m2/g) and water-soluble organic carbon (MACWSOC: 0.98 ± 0.45 m2/g) were slightly higher and lower than those reported in urban regions, respectively, indicating that CA undergo an aging process. Organic aerosol coating during transport and variation of biomass burning probably led to the seasonal variation in MAC of two components. Overall, WSOC contributed considerably to the light absorption (11.1% ± 4.23%) of EC. The findings suggest that to protect glaciers of the Himalayas from pollution-related melting, it is essential to mitigate emissions from the IGP.

New method to determine black carbon mass size distribution

Abstract. Black carbon (BC) is an important atmospheric component with strong light absorption. Many attempts have been made to measure BC mass size distribution (BCMSD) for its significant impact on climate and public health. Larger-coverage BCMSD, ranging from upper submicron particles sizes to larger than 1 µm, contributes to a substantial proportion of total BC mass and absorption. However, the current time resolution of larger-coverage BCMSD measurement was limited to 1 d, which was insufficient to characterize variation of larger-coverage BCMSD. In this study, a new method to determine equivalent BCMSD (eBCMSD) was proposed from size-resolved absorption coefficient measured by an aerodynamic aerosol classifier in tandem with an aethalometer. The proposed method could measure larger-coverage eBCMSD with a time resolution as high as 1 h and was validated by comparing the measurement results with refractory BCMSD (rBCMSD) measured by a differential mobility analyzer in tandem with a single-particle soot photometer (DMA–SP2) for particle sizes larger than 300 nm during a field measurement in the Yangtze River Delta. Bulk refractory BC mass concentration (mrBC,bulk) by DMA–SP2 was underestimated by 33 % compared to bulk equivalent BC mass concentration (meBC,bulk) by this method because of the limited size range of measurement for DMA–SP2. Uncertainty analysis of this method was performed with respect to mass absorption cross-section (MAC), transfer function inversion, number fraction of BC-containing particle and instrumental noise. The results indicated that MAC was the main uncertainty source, leading to meBC,bulk values that varied from −20 % to 28 %. With the advantage of a wide size coverage up to 1.5 µm, high time resolution, easy operation and low cost, this method is expected to have wide applications in field measurement for better estimating the radiative properties and climate effects of BC.

Effect of carbonaceous components of biodiesel combustion particles on optical properties

This paper studies the influence of carbonaceous components on the optical properties of particulate matter (PM) in biodiesel combustion by conducting a bench test on an electronically controlled high-pressure common-rail diesel engine. In addition, the PM produced by the combustion of diesel oil, soybean oil methyl ester (SME), waste edible oil methyl ester (WME), and palm oil methyl ester (PME) was collected. The carbonaceous composition and optical properties of diesel and three biodiesel particulates were then analyzed. The obtained results showed that the ratio of organic carbon (OC) to total carbon (TC) in diesel PM was 0.25 and the ratio of OC/EC was 0.33. The OC to TC ratio of biodiesel PM was significantly greater than that of diesel PM, ranging between 0.59 and 0.65, with OC/EC values in the range of 1.44–1.86. The mass absorption cross-section (MAC) values of three kinds of biodiesel particles were all higher than those of diesel particles. When the incident laser wavelength increased, the difference of MAC values among four kinds of fuel particles gradually decreased. The MAC values of all the three biodiesel particles were higher than those of the diesel particles, and the difference between the MAC values of the four fuel particles gradually decreased with the increase of the incident laser wavelength. Afterwards, the “shell-core” model of particles was developed with 80 nm EC sphere as the core. At the two refractive indices, the scattering cross section, absorption cross section, and extinction cross section of the particles decrease with the increase of the incident light wavelength, and the scattering cross section, absorption cross section, and extinction cross section of the particles increase with the increase of the OC coating thickness.

Dust dominates the summer melting of glacier ablation zones on the northeastern Tibetan Plateau

Dust and black carbon (BC) can darken snow and ice surface and play pivotal roles in glacier mass loss. Thus, a quantitative assessment of their contributions to glacier summer melting is critical. During the summer of 2018, surface snow and ice were sampled, and the albedo and mass balance were continuously measured in the ablation zone of Laohugou Glacier No. 12 in the western Qilian Mountains. The physical properties of dust and BC were measured in the laboratory, and their impacts on glacier surface albedo reduction and melting were simulated. The results indicate that the ice surface in the ablation zone was enriched with substantial amounts of particles, and the average particle concentrations of these samples were hundreds of times higher than those of fresh snow. The BC mass absorption cross-sections (MACs) ranged from 3.1 m2 g−1 at 550 nm for dirty ice to 4.6 m2 g−1 for fresh snow, largely owing to meltwater percolation and particle collapse. The spectral variations in dust MACs were significantly different in the visible light bands and near-infrared bands from those in the other areas. Moreover, the two-layer surface energy and mass balance model with the new albedo parameterization formula was validated and agreed well with the experimental measurements of spectral albedo, broadband albedo, and mass balance. BC and dust combined resulted in 26.7 % and 54.4 % of the total mass loss on the cleaner and dirtier (particle enriched) surfaces in the ablation zone, respectively, compared to particle-free surfaces, and although both impurities played vital roles, dust was the more prominent factor in accelerating glacier melting on the northeastern Tibetan Plateau. This study emphasizes the importance of dust in cryosphere changes where Tibetan glaciers are strongly affected by Asian dust deposition.

The impact of atmospheric motions on source-specific black carbon and the induced direct radiative effects over a river-valley region

Abstract. Black carbon (BC) is one of the most important short-lived climate forcers, and atmospheric motions play an important role in determining its mass concentrations of pollutants. Here an intensive observation was launched in a typical river-valley city to investigate relationships between atmospheric motions and BC aerosols. Equivalent BC (eBC) source apportionment was based on an aethalometer model with the site-dependent absorption Ångström exponents (AAEs) and the mass absorption cross sections (MACs) retrieved using a positive matrix factorization (PMF) model based on observed chemical components (i.e., EC, POC, K+, Mg, Al, Si, S, Cl, Ca, V, Mn, Fe, Ni, Cu, As, Se, Br, Sr, Pb, Ga, and Zn) and primary absorption coefficients at selected wavelengths from λ=370 to 880 nm. The derived AAEs from 370 to 880 nm were 1.07 for diesel vehicular emissions, 2.13 for biomass burning, 1.74 for coal combustion, and 1.78 for mineral dust. The mean values for eBCfossil and eBCbiomass were 2.46 and 1.17 µg m−3, respectively. Wind run distances and the vector displacements of the wind in 24 h were used to construct a self-organizing map, from which four atmospheric motion categories were identified (local-scale dominant, local-scale strong and regional-scale weak, local-scale weak and regional-scale strong, and regional-scale dominant). BC pollution was found to be more likely when the influence of local-scale motions outweighed that of regional-scale motions. Cluster analysis for the back-trajectories of air mass calculated by the Hybrid Single-Particle Lagrangian Integrated Trajectory model at the study site indicated that the directions of air flow can have different impacts for different scales of motion. The direct radiative effects (DREs) of source-specific eBC were lower when the influence of regional-scale motions outweighed that of the local ones. However, due to chemical aging of the particles during transport – the DRE efficiencies under regional-scale motions were ∼ 1.5 times higher than those under more local influences. The finding that the DRE efficiency of BC increased during the regional transport suggested significant consequences in regions downwind of pollution sources and emphasizes the importance of regionally transported BC for potential climatic effects.

Application of machine learning approaches in the analysis of mass absorption cross-section of black carbon aerosols: Aerosol composition dependencies and sensitivity analyses

Application of machine learning approaches in the analysis of mass absorption cross-section of black carbon aerosols: Aerosol composition dependencies and sensitivity analyses

Estimating mass-absorption cross-section of ambient black carbon aerosols: Theoretical, empirical, and machine learning models

Estimating mass-absorption cross-section of ambient black carbon aerosols: Theoretical, empirical, and machine learning models

Concentrations and light absorption properties of PM2.5 organic and black carbon based on online measurements in Lanzhou, China

To elucidate the variations in mass concentrations of organic carbon (OC) and black carbon (BC) in PM2.5 and their light absorption characteristics in Lanzhou, we conducted one-year online measurements by using a newly developed total carbon analyzer (TCA08) coupled with an aethalometer (AE33) from July 2018 to July 2019. The mean OC and BC concentrations were 6.4 ± 4.4 and 2.0 ± 1.3 µg/m3, respectively. Clear seasonal variations were observed for both components, with winter having the highest concentrations, followed by autumn, spring, and summer. The diurnal variations of OC and BC concentrations were similar throughout the year, with daily two peaks occurring in the morning and evening, respectively. A relatively low OC/BC ratio (3.3 ± 1.2, n = 345) were observed, indicating that fossil fuel combustion was the primary source of the carbonaceous components. This is further substantiated by relatively low biomass burning contribution (fbiomass: 27.1% ± 11.3%) to BC using aethalometer based measurement though fbiomass value which increased significantly in winter (41.6% ± 5.7%). We estimated a considerable brown carbon (BrC) contribution to the total absorption coefficient (babs) at 370 nm (yearly average of 30.8% ± 11.1%), with a winter maximum of 44.2% ± 4.1% and a summer minimum of 19.2% ± 4.2%. Calculation of the wavelength dependence of total babs revealed an annual mean AAE370-520 value of 4.2 ± 0.5, with slightly higher values in spring and winter. The mass absorption cross-section of BrC also exhibited higher values in winter, with an annual mean of 5.4 ± 1.9 m2/g, reflecting the impact of emissions from increased biomass burning on BrC concentrations.

Vehicle exhausts contribute high near-UV absorption through carbonaceous aerosol during winter in a fast-growing city of Sichuan Basin, China

Carbonaceous aerosols pose significant climatic impact, however, their sources and respective contribution to light absorption vary and remain poorly understood. In this work, filter-based PM2.5 samples were collected in winter of 2021 at three urban sites in Yibin, a fast-growing city in the south of Sichuan Basin, China. The composition characteristics of PM2.5, light absorption and source of carbonaceous aerosol were analyzed. The city-wide average concentration of PM2.5 was 87.4 ± 31.0 μg/m3 in winter. Carbonaceous aerosol was the most abundant species, accounting for 42.5% of the total PM2.5. Source apportionment results showed that vehicular emission was the main source of PM2.5 during winter, contributing 34.6% to PM2.5. The light absorption of black carbon (BC) and brown carbon (BrC) were derived from a simplified two-component model. We apportioned the light absorption of carbonaceous aerosols to BC and BrC using the Least Squares Linear Regression with optimal angstrom absorption exponent of BC (AAEBC). The average absorption of BC and BrC at 405 nm were 51.6 ± 21.5 Mm−1 and 17.7 ± 8.0 Mm−1, respectively, with mean AAEBC = 0.82 ± 0.02. The contribution of BrC to the absorption of carbonaceous reached 26.1% at 405 nm. Based on the PM2.5 source apportionment and the mass absorption cross-section (MAC) value of BrC at 405 nm, vehicle emission was found to be the dominant source of BrC in winter, contributing up to 56.4%. Therefore, vehicle emissions mitigation should be the primary and an effective way to improve atmospheric visibility in this fast-developing city.

Characterization of Propane Fueled Flames: A Significant Source of Brown Carbon

In this study, we developed a framework for interpreting the in situ morphological properties of black carbon (BC, also referred to as “soot” due to combustion relevance) mixed with primary organic aerosol. Integration of the experiment considering primary organic aerosol (POA) evaporation from the soot particles was examined using a Differential mass–mobility analyzer (DMA) and showed the untold story of the mixing of BC and POA. We also hypothesize that morphological transformation of soots and determined such as (i) the evaporation of externally and internally mixed POA led to a decline in the particle number and size of monodisperse aerosol; (ii) presence of externally mixed BC was interpreted from the occurrence of two peaks of soot upon heating; (iii) heat-induced collapse of the BC core possibly resulted from the evaporation of material from the voids and effect of heat; (iv) volume equivalent to changes in the mobility diameter represented evaporation of POA from the surface and collapse upon heating. POA constituted a high fraction (20–40% by mass) of aerosol mass from these flames and was predominantly (i.e., 92–97% by mass) internally mixed with BC. POA was found to be highly light absorptive, i.e., an Ångström absorption exponent (AAE) value of (in general) >1.5 was estimated for BC + POA at 405/781 nm wavelengths. Interestingly, a much more highly absorptive POA [mass absorption cross-section (MAC)-5 m2 g−1] at 405 nm was discovered under a specific flame setting, which was comparable to MACs of BC particles (8–9 m2 g−1).

A quadcopter unmanned aerial system (UAS)-based methodology for measuring biomass burning emission factors

Abstract. Biomass burning (BB) emits large quantities of greenhouse gases (GHG) and aerosols that impact the climate and adversely affect human health. Although much research has focused on quantifying BB emissions on regional to global scales, field measurements of BB emission factors (EFs) are sparse, clustered and indicate high spatio-temporal variability. EFs are generally calculated from ground or aeroplane measurements with respective potential biases towards smouldering or flaming combustion products. Unmanned aerial systems (UAS) have the potential to measure BB EFs in fresh smoke, targeting different parts of the plume at relatively low cost. We propose a light-weight UAS-based method to measure EFs for carbon monoxide (CO), carbon dioxide (CO2), methane (CH4), and nitrous oxide (N2O) as well as PM2.5 (TSI Sidepak AM520) and equivalent black carbon (eBC, microAeth AE51) using a combination of a sampling system with Tedlar bags which can be analysed on the ground and with airborne aerosol sensors. In this study, we address the main challenges associated with this approach: (1) the degree to which a limited number of samples is representative for the integral smoke plume and (2) the performance of the lightweight aerosol sensors. While aerosol measurements can be made continuously in a UAS set-up thanks to the lightweight analysers, the representativeness of our Tedlar bag filling approach was tested during prescribed burning experiments in the Kruger National Park, South Africa. We compared fire-averaged EFs from UAS-sampled bags for savanna fires with integrated EFs from co-located mast measurements. Both measurements matched reasonably well with linear R2 ranging from 0.81 to 0.94. Both aerosol sensors are not factory calibrated for BB particles and therefore require additional calibration. In a series of smoke chamber experiments, we compared the lightweight sensors with high-fidelity equipment to empirically determine specific calibration factors (CF) for measuring BB particles. For the PM mass concentration from a TSI Sidepak AM520, we found an optimal CF of 0.27, using a scanning mobility particle sizer and gravimetric reference methods, although the CF varied for different vegetation fuel types. Measurements of eBC from the Aethlabs AE51 aethalometer agreed well with the multi-wavelength aethalometer (AE33) (linear R2 of 0.95 at λ=880 nm) and the wavelength corrected multi-angle absorption photometer (MAAP, R2 of 0.83 measuring at λ=637 nm). However, the high variability in observed BB mass absorption cross-section (MAC) values (5.2±5.1 m2 g−1) suggested re-calibration may be required for individual fires. Overall, our results indicate that the proposed UAS set-up can obtain representative BB EFs for individual savanna fires if proper correction factors are applied and operating limitations are well understood.

Secondary Organic Aerosol (SOA) from Photo-Oxidation of Toluene: 1 Influence of Reactive Nitrogen, Acidity and Water Vapours on Optical Properties

Many climate models treat the light-absorbing SOA component called “brown carbon” (BrC) as non-light absorbing because its formation and transformations are poorly understood. We therefore investigated the influence of reactive nitrogen (NOx, NH3)-, acidity (H2SO4)-, and water-mediated chemistry on SOA formed by the photo-oxidation of toluene, the subsequent formation and transformation of BrC, and its optical properties. We discovered that nitrogen-poor (NP) SOA is formed when the molar ratio of NOx to reacted toluene (henceforth, [NOx/ΔHC]) is 0.15 or less, whereas nitrogen-rich (NR) SOA is formed when [NOx/ΔHC] > 0.15. NR and NP SOA have markedly different characteristics. The light absorption coefficient (Babs) and mass absorption cross-section (MAC) of the SOA increased with [NOx/ΔHC] under both the NP and NR regimes. For NP SOA, the MAC increased with [NOx/ΔHC] independently of the relative humidity (RH). However, the MAC of NR SOA was RH-dependent. Under both NP and NR regimes, acidity promoted SOA browning while NH3 increased Babs and MAC at 80% RH. The highest MAC was observed at the lowest RH (20%) for acidic NR SOA, and it was postulated that the MAC of SOA depends mainly on the pH and the [H+]free/[SOA mass] ratio of the aqueous SOA phase.

Seasonal variations in fire conditions are important drivers in the trend of aerosol optical properties over the south-eastern Atlantic

Abstract. From June to October, southern Africa produces one-third of the global biomass burning (BB) emissions by widespread fires. BB aerosols are transported westward over the south-eastern Atlantic with the mid-tropospheric winds, resulting in significant radiative effects. Ascension Island (ASI) is located midway between Africa and South America. From June 2016 to October 2017, a 17-month in situ observation campaign on ASI found a low single-scattering albedo (SSA) as well as a high mass absorption cross-section of black carbon (MACBC), demonstrating the strong absorbing marine boundary layer in the south-eastern Atlantic. Here we investigate the monthly variations of critical optical properties of BB aerosols, i.e. SSA and MACBC, during the BB seasons and the driving factors behind these variations. Both SSA and MACBC increase from June to August and decrease in September and October. The average SSA during the BB seasons is 0.81 at 529 nm wavelength, with the highest mean ∼ 0.85 in October and the lowest ∼ 0.78 in August. The absorption enhancement (Eabs) derived from the MACBC shows similar trends with SSA, with the average during the whole of the BB seasons at ∼ 1.96 and ∼ 2.07 in 2016 and 2017, respectively. As the Eabs is higher than the ∼ 1.5 commonly adopted value by climate models, this result suggests the marine boundary layer in the south-eastern Atlantic is more absorbing than model simulations. We find the enhanced ratio of BC to CO (ΔBC/ΔCO, equal to BC/ΔCO as the BC background concentration is considered to be 0) is well correlated with SSA and MACBC, providing a simple way to estimate the aerosol optical characteristics in the south-eastern Atlantic. The exponential function we proposed can approximate SSA and MACBC with BC/ΔCO, and when BC/ΔCO is small it can capture the rapid growth of SSA as BC/ΔCO decreases. BC/ΔCO is influenced by combustion conditions and aerosol scavenging. From the analysis of the location of BB, the primary source fuel, the water content in the fuel, combined with the mean cloud cover and precipitation in the transport areas of the BB plume, we conclude that the increase in BC/ΔCO from June to August is likely to be caused by burning becoming more flaming. The reduction in the water content of fuels may be responsible for the change in the burning conditions from June to August. The decrease in BC/ΔCO in September and October may be caused by two factors, one being a lower proportion of flaming conditions, possibly associated with a decrease in mean surface wind speed in the burning area, and the other being an increase in precipitation in the BB transport pathway, leading to enhanced aerosol scavenging, which ultimately results in an increase in SSA and MACBC.

Absorption enhancement of black carbon particles in a Mediterranean city and countryside: effect of particulate matter chemistry, ageing and trend analysis

Abstract. Black carbon (BC) is recognized as the most important warming agent among atmospheric aerosol particles. The absorption efficiency of pure BC is rather well-known, nevertheless the mixing of BC with other aerosol particles can enhance the BC light absorption efficiency, thus directly affecting Earth's radiative balance. The effects on climate of the BC absorption enhancement due to the mixing with these aerosols are not yet well constrained because these effects depend on the availability of material for mixing with BC, thus creating regional variations. Here we present the mass absorption cross-section (MAC) and absorption enhancement of BC particles (Eabs), at different wavelengths (from 370 to 880 nm for online measurements and at 637 nm for offline measurements) measured at two sites in the western Mediterranean, namely Barcelona (BCN; urban background) and Montseny (MSY; regional background). The Eabs values ranged between 1.24 and 1.51 at the urban station, depending on the season and wavelength used as well as on the pure BC MAC used as a reference. The largest contribution to Eabs was due to the internal mixing of BC particles with other aerosol compounds, on average between a 91 % and a 100 % at 370 and 880 nm, respectively. Additionally, 14.5 % and 4.6 % of the total enhancement at the short ultraviolet (UV) wavelength (370 nm) was due to externally mixed brown carbon (BrC) particles during the cold and the warm period, respectively. On average, at the MSY station, a higher Eabs value was observed (1.83 at 637 nm) compared to BCN (1.37 at 637 nm), which was associated with the higher fraction of organic aerosols (OA) available for BC coating at the regional station, as denoted by the higher organic carbon to elemental carbon (OC:EC) ratio observed at MSY compared to BCN. At both BCN and MSY, Eabs showed an exponential increase with the amount of non-refractory (NR) material available for coating (RNR-PM). The Eabs at 637 nm at the MSY regional station reached values up to 3 during episodes with high RNR-PM, whereas in BCN, Eabs kept values lower than 2 due to the lower relative amount of coating materials measured at BCN compared to MSY. The main sources of OA influencing Eabs throughout the year were hydrocarbon OA (HOA) and cooking-related OA (COA), i.e. primary OA (POA) from traffic and cooking emissions, respectively, at both 370 and 880 nm. At the short UV wavelength (370 nm), a strong contribution to Eabs from biomass burning OA (BBOA) and less oxidized oxygenated OA (LO-OOA) sources was observed in the colder period. Moreover, we found an increase of Eabs with the ageing state of the particles, especially during the colder period. This increase of Eabs with particle ageing was associated with a larger relative amount of secondary OA (SOA) compared to POA. The availability of a long dataset at both stations from offline measurements enabled a decade-long trend analysis of Eabs at 637 nm, that showed statistically significant (s.s.) positive trends of Eabs during the warmer months at the MSY station. This s.s. positive trend in MSY mirrored the observed increase of the OC:EC ratio over time. Moreover, in BCN during the COVID-19 lockdown period in spring 2020 we observed a sharp increase of Eabs due to the observed sharp increase of the OC:EC ratio. Our results show similar values of Eabs to those found in the literature for similar background stations.

The Light Absorption Heating Method for Measurement of Light Absorption by Particles Collected on Filters

A new instrument for the quantification of light absorption by particles collected on filters has been developed to address long standing environmental questions about light-absorbing particles in air, water, and on snow and ice. The Light Absorption Heating Method (LAHM) uses temperature changes when filters are exposed to light to quantify absorption. Through the use of calibration standards, the observed temperature response of unknown materials can be related to the absorption cross section of the substance collected on the filter. Here, we present a detailed description of the instrument and calibration. The results of the calibration tests using a common surrogate for black carbon, Fullerene soot, show that the instrument provides stable results even when exposed to adverse laboratory conditions, and that there is little drift in the instrument over longer periods of time. Calibration studies using Fullerene soot suspended in water, airborne propane soot, as well as atmospheric particulates show consistent results for absorption cross section when using accepted values for the mass absorption cross section of the soot and when compared to results from a 3-wavelength photoacoustic instrument. While filter sampling cannot provide the time resolution of other instrumentation, the LAHM instrument fills a niche where time averaging is reasonable and high-cost instrumentation is not available. The optimal range of absorption cross sections for LAHM is from 0.1 to 5.0 cm2 (~1.0–50.0 µg soot) for 25 mm filters and 0.4 to 20 cm2 (4.0–200.0 µg soot) for 47 mm filters, with reduced sensitivity to higher values.

Seasonal variation of optical properties and source apportionment of black and brown carbon in Xi'an, China

To acquire the seasonal variation of black carbon (BC) and brown carbon (BrC) light absorption (Abs), PM2.5 samples were obtained over an entire year of 2018 and analyzed for chemical composition and wavelength-dependent light absorption. Contributions of AbsBC and AbsBrC, the absorption Ångström exponent (AAE) and mass absorption cross section (MAC) are examined. The results show that while BC was the dominant light absorbing carbonaceous component at 780 nm–980 nm, BrC made a significant contribution to light absorption at shorter wavelengths (405 nm and 445 nm), especially during spring. At 405 nm, BrC experienced the dominant light absorption contribution in spring, autumn and winter, whereas BC had a greater contribution in summer. The annual average of BrC contributions to total absorption at 405 nm (56.3%) is higher than that of BC (43.7%), with lower BrC contributions at longer wavelengths. Average MACs for BC and BrC at 405 nm were 5.67 ± 10.4 and 1.74 ± 3.78 m2g-1, respectively. The MACBC versus MACBrC were well correlated in autumn and winter implying that BC and BrC had similar primary sources (biomass burning and fossil fuel combustion). Source factors and source-specific seasonal contribution to light absorption were identified using positive matrix factorization (PMF) modeling. Traffic-related emissions had the largest contribution to light absorption in all seasons at all wavelengths. Biomass burning had a greater impact in spring and winter, and coal combustion contributed the highest levels in winter. Mineral dust had minor contributions to light absorption in all seasons.

Characterization of soot produced by the mini inverted soot generator with an atmospheric simulation chamber

Abstract. The performance of a mini inverted soot generator (MISG) has been investigated at ChAMBRe (Chamber for Aerosol Modelling and Bio-aerosol Research) by studying the properties of soot particles generated by ethylene and propane combustion. This work deepens and expands the existing characterization of the MISG, which also exploits an atmospheric simulation chamber (ASC). Different from previous works, MISG performance has been also tested at different fuel flows and higher global equivalence ratios. MISG exhausts were investigated after their injection inside the atmospheric simulation chamber, which is another novelty of this work. Starting from an extensive classification of combustion conditions and resulting flame shapes, the MISG exhaust was characterized in terms of concentration of emitted particles and gases, particle size distribution, and optical properties. Soot particles were also collected on quartz fibre filters and then analysed by optical and thermal–optical techniques to measure the spectral dependence of the absorption coefficient babs​​​​​​​ and their composition in terms of elemental carbon and organic carbon (EC and OC). Significant differences could be observed when the MISG was fuelled with ethylene and propane in terms of particle size. In particular, the production of super-micrometric aggregates was observed for ethylene combustion. With equal combustion conditions, ethylene produced a higher number concentration of particles and smaller mode diameters. Soot particles produced by propane combustion resulted in higher EC : TC (total carbon) ratios and they were more light absorbing than particles generated by ethylene combustion. Values of the mass absorption cross section (MAC) and of the Ångström absorption exponent (AAE) turned out to be compatible with the literature, even if there were some specific differences. The comprehensive characterization of the MISG soot particles is an important piece of information to design and perform experiments in atmospheric simulation chambers. Particles with well-known properties can be used, for example, to investigate the possible interactions between soot and other atmospheric pollutants, the effects of meteorological variables on soot properties, and the oxidative and toxicological potential of soot particles.

Size-dependent mass absorption cross-section of soot particles from various sources

The mass absorption cross-section (MAC) of combustion-generated soot is used in pollution and emissions measurements to quantify the mass concentration of soot and in atmospheric modelling to predict the radiative effects of soot on climate. Previous work has suggested that the MAC of soot particles may change with their size, due to (1) internal scattering among monomers in the soot aggregate, (2) the correlation of soot primary-particle diameter with aggregate size, (3) quantum confinement effects, or (4) a size-dependent degree of soot graphitization. Here, we report a size-dependent MAC for ex-situ soot sampled from two commercially available diffusion-flame soot generators, one aviation turbine engine, and one diesel generator. We also incorporate literature data. We show that the MAC increases with aggregate size until a plateau is reached at single particle masses between 4 and 30 fg (approximately 300–650 nm soot mobility diameter). The smallest particles may have MACs 50%–80% smaller than the largest, depending on the source, while the largest particles have MACs within the range reported by previous measurements on polydisperse samples. Moreover, we show that models of hypotheses (1), (2), and (3) do not describe our measurement results, leaving hypothesis (4) as the only remaining candidate.

Black carbon and organic carbon dataset over the Third Pole

Abstract. The Tibetan Plateau and its surroundings, also known as the Third Pole, play an important role in the global and regional climate and hydrological cycle. Carbonaceous aerosols (CAs), including black carbon (BC) and organic carbon (OC), can directly or indirectly absorb and scatter solar radiation and change the energy balance on the Earth. CAs, along with the other atmospheric pollutants (e.g., mercury), can be frequently transported over long distances into the inland Tibetan Plateau. During the last decades, a coordinated monitoring network and research program named “Atmospheric Pollution and Cryospheric Changes” (APCC) has been gradually set up and continuously operated within the Third Pole regions to investigate the linkage between atmospheric pollutants and cryospheric changes. This paper presents a systematic dataset of BC, OC, water-soluble organic carbon (WSOC), and water-insoluble organic carbon (WIOC) from aerosols (20 stations), glaciers (17 glaciers, including samples from surface snow and ice, snow pits, and 2 ice cores), snow cover (2 stations continuously observed and 138 locations surveyed once), precipitation (6 stations), and lake sediment cores (7 lakes) collected across the Third Pole, based on the APCC program. These data were created based on online (in situ) and laboratory measurements. High-resolution (daily scale) atmospheric-equivalent BC concentrations were obtained by using an Aethalometer (AE-33) in the Mt. Everest (Qomolangma) region, which can provide new insight into the mechanism of BC transportation over the Himalayas. Spatial distributions of BC, OC, WSOC, and WIOC from aerosols, glaciers, snow cover, and precipitation indicated different features among the different regions of the Third Pole, which were mostly influenced by emission sources, transport pathways, and deposition processes. Historical records of BC from ice cores and lake sediment cores revealed the strength of the impacts of human activity since the Industrial Revolution. BC isotopes from glaciers and aerosols identified the relative contributions of biomass and fossil fuel combustion to BC deposition on the Third Pole. Mass absorption cross sections of BC and WSOC from aerosol, glaciers, snow cover, and precipitation samples were also provided. This updated dataset is released to the scientific communities focusing on atmospheric science, cryospheric science, hydrology, climatology, and environmental science. The related datasets are presented in the form of excel files. BC and OC datasets over the Third Pole are available to download from the National Cryosphere Desert Data Center (https://doi.org/10.12072/ncdc.NIEER.db0114.2021; Kang and Zhang, 2021).

Optical properties of morphologically complex black carbon aerosols: Effects of coatings

Optical properties are computed for fractal-like aggregate black carbon (BC) aerosols coated with different substances. Two models are used for these aerosols: (i) the coated aggregate model (model I), where coating is added to the voids and surroundings of BC fractal-like aggregates; and (ii) the closed-cell aggregate model (model II), where coating is added concentrically to each monomer of BC fractal-like aggregates. Our results favor choosing the coated aggregate model (model I) to simulate scattering and absorption by coated BC aerosols because this model is morphologically more realistic, and because this model yields mass absorption cross section (MAC) and backscattering linear depolarization ratio (LDR) values that are consistent with field measurements. Moreover the corresponding computed degree of linear polarization (DoLP) and LDR values are very sensitive to changes in the coating volume fraction (fvol) and the coating refractive index (m). With the same absorbing BC core, the MAC value increases steadily with increasing fvol and m values. For example, using a density of 1.8 g/cm3 and BC refractive index 1.95 + i0.79, the calculated MAC values for uncoated BC aggregates range from 6.2 to 6.8 m2/g at 0.55 µm. When coating material is applied to the BC aggregates, the calculated MAC values for model I particles increase to between 9.8 and 13.2 m2/g (depending on m) when fvol = 87.5%. The backscattering LDR values also tend to increase with the increasing m values for the shapes and sizes considered in our study. For model I particles, the backscattering LDR values span a wide range of 4.2–27.8% at a wavelength of 0.35 µm at fvol = 87.5% when m increases from 1.33 to 1.55. Our results are relevant to analyses of polarimetric and lidar observations of smoke particles, especially when these particles undergo hygroscopic growth.