Single Particle Soot Photometer Research Articles

A 2-year intercomparison of three methods for measuring black carbon concentration at a high-altitude research station in Europe

Abstract. Black carbon (BC) is one of the most important climate forcers with severe health effects. Large uncertainties in radiative forcing estimation and health impact assessment arise from the fact that there is no standardized method to measure BC mass concentration. This study presents a 2-year comparison of three state-of-the-art BC measurement techniques at the high-altitude research station Pic du Midi (PDM) located in the French Pyrenees at an altitude of 2877 m above sea level. A recently upgraded Aethalometer AE33, a thermal-optical analyser Sunset and a single-particle soot photometer SP2 were deployed to measure simultaneously the mass concentration of equivalent black carbon (MeBC), elemental carbon (MEC) and refractory black carbon (MrBC), respectively. Significant deviations in the response of the instruments were observed. All techniques responded to seasonal variations in the atmospheric changes in BC levels and exhibited good correlation during the whole study period. This indicates that the different instruments quantified the same particle type despite the fact that they are based on different physical principles. However the slopes and correlation coefficients varied between instrument pairs. The largest biases were observed for the AE33 with MeBC values that were around 2 times greater than MrBC and MEC values. The principal reasons of such large discrepancy were explained by the mass absorption cross section (MAC) that was too low and C values recommended by the AE33 manufacturer and applied to the absorption coefficients measured by the AE33. In addition, the long-range transport of dust particles at PDM in spring caused significant increases in the bias between AE33 and SP2 by up to a factor 8. The Sunset MEC measurements agreed within around 17 % with the SP2 MrBC values. The largest overestimations of MEC were observed when the total carbon concentrations were below 25 µg C cm−2, which is probably linked to the incorrect determination of the organic carbon (OC)–EC split point. Another cause of the discrepancy between instruments was found to be the limited detection range of the SP2, which did not allow for the total detection of fine rBC particles. The procedure used to estimate the missing mass fraction of rBC not covered by the measurement range of the SP2 was found to be critical. We found that a time-dependent correction based on fitting the observed rBC size distribution with a multimodal lognormal distribution is needed to accurately estimate MrBC over a larger size range.

Evolution of refractory black carbon mixing state in an urban environment

The size distribution and hygroscopicity of the refractory black carbon (rBC) aerosol are critical properties for understanding its impact on human health, the extent to which the particles disperse through the atmosphere, and the effect that the particles have on clouds and the climate system. The hygroscopicity of black carbon is primarily controlled by the degree to which the black carbon cores are coated with other compounds. Here we show new measurements of rBC obtained from a single particle soot photometer at an urban location in Houston, TX, USA during the Department of Energy TRacking Aerosol Convection Interactions ExpeRiment (TRACER) campaign. We classified rBC particles into uncoated, thinly coated and thickly coated, where the latter is defined as the optical coating thickness exceeding 10 nm. To understand how aerosol aging and the prevailing winds interact to affect rBC coatings, a slice of the size distribution with rBC core diameter 143–166 nm is considered. For this slice, the average coating thickness of thickly coated particles was 29 ± 8 nm. The rBC number concentration, the fraction of thinly and thickly coated particles, and the average coating thickness strongly vary with the wind direction. We found that onshore flows are associated with lower number concentrations, more thinly coated particles, and thinner coatings when compared to offshore flows. Diurnal profiles show that the fraction of coated particles increases during daytime, likely due to photochemical aging. The estimated fraction of rBC particles that may activate into cloud droplets at 0.1% and 1% water supersaturation was generally ∼0.6% and ∼9%, respectively. This suggests that substantial further aging is needed to precondition the majority of rBC particles for incorporation into cloud droplets.

Measured black carbon deposition over the central Himalayan glaciers: Concentrations in surface snow and impact on snow albedo reduction

Deposition of ambient black carbon (BC) aerosols over snow-covered areas reduces surface albedo and accelerates snowmelt. Based on in-situ atmospheric BC data and the WRF-Chem model, we estimated the dry and wet deposition of BC over the Yala glacier of the central Himalayan region in Nepal during 2016–2018. The maximum and minimum BC dry deposition was reported in pre- and post-monsoon respectively. Approximately 50% of annual dry deposition occurred in the pre-monsoon season (March to May) and 27% of the annual dry deposition occurred in April. The total dry BC deposition rate was estimated as ∼4.6 μg m−2 day−1 providing a total deposition of 531 μg m−2 during the pre-monsoon season. The contribution of biomass burning and fossil fuel sources to BC deposition on an annual basis was 28% and 72% respectively. The annual accumulated wet deposition of BC was 196 times higher than the annual dry deposition. The ten months of observed dry deposition of BC (October 1, 2016 to August 31, 2017 – except December 2016) was ∼39% lower than that of WRF-Chem's estimated annual dry deposition from September 1, 2016 to August 31, 2017 partially due to model bias. The deposited content of BC over the snow surface has an important role in albedo reduction, therefore snow samples were collected from the surface of the Yala Glacier and the surrounding region in April 2016, 2017, and 2018. Samples were analyzed for BC mass concentration through the thermal optical analysis and single particle soot photometer method. The BC calculated via the thermal optical method was in the range of 352–854 ng g−1, higher than the BC calculated through the particle soot photometer method and estimated BC in 2 cm surface snow (imperial equation). The maximum surface snow albedo reduction due to BC was 8.8%, estimated by a widely used snow radiative transfer model and a linear regression equation.

Relating the single particle soot photometer (SP2) signal response to soot maturity

Relating the single particle soot photometer (SP2) signal response to soot maturity

Higher absorption enhancement of black carbon in summer shown by 2-year measurements at the high-altitude mountain site of Pic du Midi Observatory in the French Pyrenees

Abstract. Black-carbon-containing particles strongly absorb light, causing substantial radiative heating of the atmosphere. The climate-relevant properties of black carbon (BC) are poorly constrained in high-altitude mountain regions, where many complex interactions between BC, radiation, clouds and snow have important climate implications. This study presents 2-year measurements of BC microphysical and optical properties at the Pic du Midi (PDM) research station, a high-altitude observatory located at 2877 m above sea level in the French Pyrenees. Among the long-term monitoring sites in the world, PDM is subject to limited influence from the planetary boundary layer (PBL), making it a suitable site for characterizing the BC in the free troposphere (FT). The classification of the dominant aerosol type using aerosol spectral optical properties indicates that BC is the predominant aerosol absorption component at PDM and controls the variation in single-scattering albedo (SSA) throughout the 2 years. Single-particle soot photometer (SP2) measurements of refractory BC (rBC) show a mean mass concentration (MrBC) of 35 ng m−3 and a relatively constant rBC core mass-equivalent diameter of about 180 nm, which are typical values for remote mountain sites. Combining the MrBC with in situ absorption measurements, a rBC mass absorption cross-section (MACrBC) of 9.2 ± 3.7 m2 g−1 at λ=880 nm has been obtained, which corresponds to an absorption enhancement (Eabs) of ∼2.2 compared to that of bare rBC particles with equal rBC core size distribution. A significant reduction in the ΔMrBC/ΔCO ratio when precipitation occurred along the air mass transport suggests wet removal of rBC. However we found that the wet removal process did not affect the rBC size, resulting in unchanged Eabs. We observed a large seasonal contrast in rBC properties with higher MrBC and Eabs in summer than in winter. In winter a high diurnal variability in MrBC (Eabs) with higher (lower) values in the middle of the day was linked to the injection of rBC originating from the PBL. On the contrary, in summer, MrBC showed no diurnal variation despite more frequent PBL conditions, implying that MrBC fluctuations are rather dominated by regional and long-range transport in the FT. Combining the ΔMrBC/ΔCO ratio with air mass transport analysis, we observed additional sources from biomass burning in summer leading to an increase in MrBC and Eabs. The diurnal pattern of Eabs in summer was opposite to that observed in winter with maximum values of ∼2.9 observed at midday. We suggest that this daily variation may result from a photochemical process driving the rBC mixing state rather than a change in BC emission sources. Such direct 2-year observations of BC properties provide quantitative constraints for both regional and global climate models and have the potential to close the gap between model-predicted and observed effects of BC on the regional radiation budget and climate. The results demonstrate the complex influence of BC emission sources, transport pathways, atmospheric dynamics and chemical reactivity in driving the light absorption of BC.

Significant influence of nitrate on light absorption enhancement of refractory black carbon in the winter of 2022 in Beijing

The mixing state of refractory black carbon (rBC) aerosols is regarded as a major uncertainty in climate-forcing assessments. This study measured the size distribution and mixing state of rBC using a single-particle soot photometer in the winter of 2022 at an urban site in Beijing. During the campaign, the mean mass concentration of rBC was 0.79 ± 0.63 μg m−3, much lower than that observed in Beijing in the winter of 2013. The number and mass median diameter of the rBC cores were 97 and 200 nm, respectively. The average relative coating thicknesses (RCT) of rBC-containing particles was 1.45 ± 0.27 and average light absorption enhancement (Eabs) was 1.43 ± 0.22. Similar to Eabs, RCT and secondary inorganic aerosols (SIA), especially nitrate, increased with increasing relative humidity. This suggests that higher SIA mass fraction in aerosol with a higher relative humidity in the environment results in a thicker coating and black carbon ageing, thus enhancing light absorption. RCT and Eabs increased rapidly with the increase of PM1 loading but increased slowly when the PM1 mass concentration exceeded 60 μg m−3. This indicates that a further increase in the NR-PM1 species at high PM loading does not increase the thickness of the coatings; therefore, there is no further increase in Eabs. The effects of the chemical composition of the Eabs obtained using the Lindeman, Merenda, and Gold method showed that nitrate plays a prominent role in the enhancement of light absorption, followed by SOA. The rBC mass concentration exhibited clear day-low and night-high patterns which were influenced by the synergetic effects of the boundary layer and emissions. RCT and Eabs presented similar diurnal variations, peaking in the afternoon, which was consistent with the pattern of SIA. This suggests that the SIA produced via photochemical reactions supports the ageing of black carbon-containing particles, leading to light-absorption enhancement. The back-trajectory analysis showed the highest values of rBC mass concentration, RCT, and Eabs appeared in the S cluster suggested that the rBC-containing particles transported from south Beijing were more aged with a thicker coating. While the rBC-containing particles from northern and northwestern Beijing had lower RCT and Eabs values.

Black carbon: a general review of its sources, analytical methods, and environmental effects in snow and ice in the Tibetan Plateau.

Tibetan Plateau (TP) is known as the water tower of Asia, and glaciers are solid reservoirs that can regulate the amount of water. Black carbon (BC), as one of the important factors accelerating glacier melting, is causing evident environmental effects in snow and ice. However, a systematical summary of the potential sources, analytical methods, distributions, and environmental effects of BC in snow and ice on the TP's glaciers is scarce. Therefore, this study drew upon existing research on snow and ice BC on glaciers of the TP to describe the detection methods and uncertainties associated with them to clarify the concentrations of BC in snow and ice and their climatic effects. The primary detection methods are the optical method, the thermal-optical method, the thermochemical method, and the single-particle soot photometer method. However, few studies have systematically compared the results of BC and this study found that concentrations of BC in different types of snow and ice varied by 1-3 orders of magnitude, which drastically affected the regional hydrologic process by potentially accelerating the ablation of glaciers by approximately 15% and reducing the duration of snow accumulation by 3-4 days. In general, results obtained from the various testing methods differ drastically, which limited the systematical discussion. Accordingly, a universal standard for the sampling and measurement should be considered in the future work, which will be beneficial to facilitate the comparison of the spatiotemporal features and to provide scientific data for the model-simulated climatic effects of BC.

Numerical investigation on retrieval errors of mixing states of fractal black carbon aerosols using single-particle soot photometer based on Mie scattering and the effects on radiative forcing estimation

Abstract. The mixing state of black carbon (BC) aerosols, which is the diameter ratio of coated particle to BC core (Dp/Dc), can be retrieved by the single-particle soot photometer (SP2). However, the retrieved Dp/Dc contains errors, because the core–shell model and Mie scattering calculation are normally employed in the retrieval principle of SP2 and the spherical core–shell structure seriously deviated from the real morphology of coated BC. In this study, fractal models are constructed to represent thinly and thickly coated BC particles for optical simulations, the differential scattering cross-sections are selected as references to conduct optical retrieval of particle diameter (Dp) based on Mie theory, just like the retrieval principle of SP2, and the volume equivalent diameter of BC core (Dc) is the same for fractal and spherical models. Then, the retrieval errors of the mixing state (Dp/Dc) of BC are investigated from numerical aspects, and the estimation accuracy of BC radiative forcing is analyzed through the simple forcing efficiency (SFE) equation with SP2 retrieval results taken into consideration. Results show that SP2 retrieved Dp/Dc based on Mie theory underestimates the realistic Dp/Dc of coated BC at most particle sizes. The retrieval errors of Dp/Dc of thinly coated BC for both single particles and particle groups are larger than those of thickly coated BC. In addition, evaluation errors of radiative forcing of coated BC caused by retrieval errors of SP2 are up to about 55 % and 95 % at 1064 and 532 nm, respectively. This study provides meaningful referential understandings of the retrieved Dp/Dc of SP2 based on Mie scattering.

Black carbon concentrations and modeled smoke deposition fluxes to the bare-ice dark zone of the Greenland Ice Sheet

Abstract. Ice–albedo feedbacks in the ablation region of the Greenland Ice Sheet (GrIS) are difficult to constrain and model due, in part, to our limited understanding of the seasonal evolution of the bare-ice region. To help fill observational gaps, 13 surface samples were collected on the GrIS across the 2014 summer melt season from patches of snow and ice that were visibly light, medium, and dark colored. These samples were analyzed for their refractory black carbon (rBC) concentrations and size distributions with a single-particle soot photometer coupled to a characterized nebulizer. We present a size distribution of rBC in fresh snow on the GrIS and from the weathering crust in the bare-ice dark zone of the GrIS. The size distributions from the weathering crust samples appear unimodal and were overall smaller than the fresh snow sample, with a peak around 0.3 µm. The fresh snow sample contained very large rBC particles that had a pronounced bimodality in the peak size distributions, with peaks around 0.2 and 2 µm. rBC concentrations ranged from a minimum of 3 µg-rBC/L-H2O in light-colored patches at the beginning and end of the melt season to a maximum of 32 µg-rBC/L-H2O in a dark patch in early August. On average, the rBC concentrations were higher (20 ± 10 µg-rBC/L-H2O) in patches that were visibly dark, compared to medium patches (7 ± 2 µg-rBC/L-H2O) and light patches (4 ± 1 µg-rBC/L-H2O), suggesting that BC aggregation contributed to snow aging on the GrIS, and vice versa. Additionally, concentrations peaked in light and dark patches in early August, which is likely due to smoke transport from wildfires in northern Canada and Alaska, as supported by the Navy Aerosol Analysis and Prediction System (NAAPS) reanalysis model. According to the model output, 26 mg m−3 of biomass-burning-derived smoke was deposited between 1 April and 30 August, of which 85 % came from wet deposition, and 67 % was deposited during our sample collection time frame. The increase in the rBC concentration and size distributions immediately after the modeled smoke deposition fluxes suggest that biomass burning smoke is a source of BC to the dark zone of the GrIS. Thus, the role of BC in the seasonal evolution of the ice–albedo feedbacks should continue to be investigated in the weathering crust of the bare-ice zone of the GrIS.

Airborne investigation of black carbon interaction with low-level, persistent, mixed-phase clouds in the Arctic summer

Abstract. Aerosol–cloud interaction is considered one of the largest sources of uncertainty in radiative forcing estimations. To better understand the role of black carbon (BC) aerosol as a cloud nucleus and the impact of clouds on its vertical distribution in the Arctic, we report airborne in situ measurements of BC particles in the European Arctic near Svalbard during the “Arctic CLoud Observations Using airborne measurements during polar Day” (ACLOUD) campaign held in the summer of 2017. BC was measured with a single-particle soot photometer aboard the Polar 6 research aircraft from the lowest atmospheric layer up to approximately 3500 m a.s.l (metres above sea level). During in-cloud flight transects, BC particles contained in liquid droplets (BC residuals) were sampled through a counterflow virtual impactor (CVI) inlet. Four flights, conducted in the presence of low-level, surface-coupled, inside-inversion, and mixed-phase clouds over sea ice, were selected to address the variability in BC above, below, and within the cloud layer. First, the increase in size and coating thickness of BC particles from the free troposphere to the cloud-dominated boundary layer confirmed that ground observations were not representative of upper atmospheric layers. Second, although only 1 % of liquid droplets contained a BC particle, the higher number concentration of BC residuals than BC particles sampled below cloud indicated that the totality of below-cloud BC was activated by nucleation scavenging but also that alternative scavenging processes such as the activation of free-tropospheric BC at the cloud top might occur. Third, the efficient exchange of aerosol particles at cloud bottom was confirmed by the similarity of the size distribution of BC residuals and BC particles sampled below cloud. Last, the increase in the BC residual number concentration (+31 %) and geometric mean diameter (+38 %) from the cloud top to the cloud bottom and the absolute enrichment in larger BC residuals compared with outside of the cloud supported the hypothesis of concomitant scavenging mechanisms but also suggested the formation of BC agglomerates caused by cloud processing. The vertical evolution of BC properties from inside the cloud and below the cloud indicated an efficient aerosol exchange at cloud bottom, which might include activation, cloud processing, and sub-cloud release of processed BC agglomerates. In the case of persistent low-level Arctic clouds, this cycle may reiterate multiple times, adding an additional degree of complexity to the understanding of cloud processing of BC particles in the Arctic.

Evaluation of a method to quantify the number concentrations of submicron water-insoluble aerosol particles based on filter sampling and complex forward-scattering amplitude measurements

Water-insoluble aerosol particles (WIAPs), such as black carbon (BC), mineral dust, and primary biological aerosol particles (PBAPs), affect climate through their interaction with radiation and clouds. However, with the exception of BC, methods to identify WIAP types and quantify their number concentrations are limited. Here, we evaluated a method that has been recently developed to measure the number concentrations of submicron WIAPs based on atmospheric aerosol measurements at an urban site in Nagoya, Japan. In this method, atmospheric aerosol particles are collected on a filter and dispersed in water. Then, the complex forward-scattering amplitudes of individual particles are measured. This complex parameter reflects the complex refractive index, volume, and shape of each measured particle, enabling the characterization of these physical properties from the signals. The WIAPs were classified as BC-like, dust-like, and PBAP-like particles based on their complex amplitude data. The number concentrations of BC-like particles were strongly correlated with those of refractory BC particles measured by a Single Particle Soot Photometer. BC-like and dust-like particles dominated the population of the submicron WIAPs, which was also confirmed using electron microscopy and Wideband Integrated Bioaerosol Sensor observations. Under the observed atmospheric conditions, the number concentrations of WIAPs were measured with their dispersion efficiency from a filter to water of approximately 50%. These results indicate that our method based on filter sampling and complex forward-scattering amplitude measurements has the potential to become a new technique for quantifying the spatio-temporal distributions of WIAPs.

Black carbon content of traffic emissions significantly impacts black carbon mass size distributions and mixing states

Abstract. Both the size and mixing state of black carbon (BC)-containing aerosols are crucial in estimating the environmental, health and climate impacts of BC. Traffic emissions are a major global source of BC; however, parameterization of BC mass size distributions and mixing states associated with traffic remains lacking due to its dependence on vehicle types and driving conditions. To investigate BC mass size distributions and mixing states associated with traffic emissions, a field campaign was conducted in the Guangzhou urban area during winter, which used a system coupling a differential mobility analyzer (DMA) and a single-particle soot photometer (SP2) to measure BC mass size distributions in the range of 100 to 700 nm. The resolved primary organic aerosols were hydrocarbon-like organic aerosols (HOA) and cooking-like organic aerosols (COA), as well as refractory BC (rBC), which was detected by the DMA–SP2 and correlated highly with HOA (R2=0.88), confirming that traffic emissions are the dominant source of atmospheric BC during the observations. The BC mass size distribution was found to be best fitted by a lognormal distribution, with a geometric mean (Dg,BC) of 258±16 nm, varying between 200 and 300 nm. During daytime, active formation of secondary nitrate and organic aerosols was observed, but it had little effect on the variations of BC mass size distributions. Further analyses revealed that Dg,BC was moderately correlated with rBC / HOA (R2=0.41) in a linear form of Dg,BC=34×rBC/HOA+177, demonstrating that the BC content of traffic emissions significantly impacts the BC mass size distributions. In addition, the size-dependent fractions of BC-containing aerosols in all types of aerosols (fBCc) and the fraction of identified externally mixed (bare/thinly coated) BC particles in all BC-containing aerosols (fext) were also characterized. It was found that the daytime secondary aerosol formation reduced both fBCc and fext, with the decrease in fext being more pronounced for larger particles, possibly due to the higher relative coating thickness. Variations in fext during nighttime were mainly controlled by the emission conditions. For example, fext for 600 nm particles decreased from 0.82 to 0.46 as rBC / HOA increased from 1 to 3.5, while the mass ratios of secondary aerosols to rBC varied little, demonstrating that the BC content also significantly affects the mixing states of freshly emitted BC from traffic emissions. This study suggests that BC content can be used as the key factor to parameterize both the BC mass size distribution and mixing states from traffic emissions, which warrants future comprehensive investigation. In addition, other sources such as biomass burning and coal combustion also contribute substantially to BC emissions, and it was important to investigate whether BC content of other major BC sources than traffic is also important in determining BC mass size distributions and mixing states. Overall, results of this study have significant implications for accurate representation of BC from different sources when modeling the impacts of BC.

Heterogeneous characteristics and absorption enhancement of refractory black carbon in an urban city of China

In this study, field measurement was conducted using an integrated online monitoring system to characterize heterogeneous properties and light absorption of refractory black carbon (rBC). rBC particles are mainly from the incomplete combustion of carbonaceous fuels. With the data collected from a single particle soot photometer, thickly coated (BCkc) and thinly coated (BCnc) particles are characterized with their lag times. With different responses to the precipitation, a dramatical decline of 83 % in the number concentration of BCkc is shown after rainfall, while that of BCnc decreases by 39 %. There is a contrast in core size distribution that BCkc is always with larger particle sizes but has smaller core mass median diameters (MMD) than BCnc. The mean rBC-containing particle mass absorption cross-section (MAC) is 6.70 ± 1.52 m2 g−1, while the corresponding rBC core is 4.90 ± 1.02 m2 g−1. Interestingly, there are wide variations in the core MAC values which range by 57 % from 3.79 to 5.95 m2 g−1, which are also closely related to those of the whole rBC-containing particles with a Pearson correlation of 0.58 (p < 0.01). Errors would be made if we eliminate the discrepancies and set the core MAC as a constant when calculating absorption enhancement (Eabs). In this study, the mean Eabs is 1.37 ± 0.11 while the source apportionment shows that there are five contributors of Eabs including secondary aging (37 %), coal combustion (26 %), fugitive dust (15 %), biomass burning (13 %) and traffic-related emissions (9 %). Secondary aging is found to be the highest contributor due to the liquid phase reactions in formations of secondary inorganic aerosol. Our study characterizes property diversities and provides insights into the sources impacting the light absorption of rBC and will be helpful for controlling it in the future.

Measurement report: Black carbon properties and concentrations in southern Sweden urban and rural air – the importance of long-range transport

Abstract. Soot, or black carbon (BC), aerosol is a major climate forcer with severe health effects. The impacts depend strongly on particle number concentration, size and mixing state. This work reports on two field campaigns at nearby urban and rural sites, 65 km apart, in southern Sweden during late summer 2018. BC was measured using a single-particle soot photometer (SP2) and Aethalometers (AE33). Differences in BC concentrations between the sites are driven primarily by local traffic emissions. Equivalent and refractory BC mass concentrations at the urban site were on average a factor 2.2 and 2.5, with peaks during rush hour up to a factor ∼4, higher than the rural background levels. The number fraction of particles containing a soot core was significantly higher in the city. BC particles at the urban site were on average smaller by mass and had less coating owing to fresh traffic emissions. The organic components of the fresh traffic plumes were similar in mass spectral signature to hydrocarbon-like organic aerosol (HOA), commonly associated with traffic. Despite the intense local traffic (∼ 30 000 vehicles passing per day), PM1, including organic aerosol, was dominated by aged continental air masses even at the curbside site. The fraction of thickly coated particles at the urban site was highly correlated with the mass concentrations of all measured chemical species of PM1, consistent with aged, internally mixed aerosol. Trajectory analysis for the whole year showed that air masses arriving at the rural site from eastern Europe contained approximately double the amount of BC compared to air masses from western Europe. Furthermore, the largest regional emissions of BC transported to the rural site, from the Malmö–Copenhagen urban area, are discernible above background levels only when precipitation events are excluded. We show that continental Europe and not the Malmö–Copenhagen region is the major contributor to the background BC mass concentrations in southern Sweden.

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.

Measurement of number and mass size distributions of light-absorbing iron oxide aerosols in liquid water with a modified single-particle soot photometer

Measurement of number and mass size distributions of light-absorbing iron oxide aerosols in liquid water with a modified single-particle soot photometer

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.

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.

Refractory black carbon aerosols in rainwater in the summer of 2019 in Beijing: Mass concentration, size distribution and wet scavenging ratio

Black carbon (BC) aerosols in the atmosphere play a significant role in climate systems due to their strong ability to absorb solar radiation. The lifetime of BC depends on atmospheric transport, aging and consequently on wet scavenging processes (in-cloud and below-cloud scavenging). In this study, sequential rainwater samples in eight rainfall events collected in 2 mm interval were measured by a tandem system including a single particle soot photometer (SP2) and a nebulizer. The results showed that the volume-weighted average (VWA) mass concentrations of refractory black carbon (rBC) in each rainfall event varied, ranging from 10.8 to 78.9 µg/L. The highest rBC concentrations in the rainwater samples typically occurred in the first fraction from individual rainfall events. The geometric mean median mass-equivalent diameter (MMD) decreased under precipitation, indicating that rBC with larger sizes was relatively aged and preferentially removed by wet scavenging. A positive correlation (R2 = 0.73) between the VWA mass concentrations of rBC in rainwater and that in ambient air suggested the important contribution of scavenging process. Additionally, the contributions of in-cloud and below-cloud scavenging were distinguished and accounted for 74% and 26% to wet scavenging, respectively. The scavenging ratio of rBC particles was estimated to be 0.06 on average. This study provides helpful information for better understanding the mechanism of rBC wet scavenging and reducing the uncertainty of numerical simulations of the climate effects of rBC.

Simulating wildfire emissions and plume rise using geostationary satellite fire radiative power measurements: a case study of the 2019 Williams Flats fire

Abstract. We use the Weather Research and Forecasting with Chemistry (WRF-Chem) model with new implementations of GOES-16 wildfire emissions and plume rise based on fire radiative power (FRP) to interpret aerosol observations during the 2019 NASA-NOAA FIREX-AQ field campaign and perform model evaluations. We compare simulated aerosol concentrations and optical properties against observations of black carbon aerosol from the NOAA Single Particle Soot Photometer (NOAA-SP2), organic aerosol from the CU High-Resolution Aerosol Mass Spectrometer (HR-AMS), and aerosol backscatter coefficients from the high-spectral-resolution lidar (HSRL) system. This study focuses on the Williams Flats fire in Washington, which was repeatedly sampled during four science flights by the NASA DC-8 (3–8 August 2019). The emissions and plume-rise methodologies are implemented following NOAA's operational High-Resolution Rapid Refresh coupled with Smoke (HRRR-Smoke) forecasting model. In addition, new GOES-16 FRP-based diurnal cycle functions are developed and incorporated into WRF-Chem. The FIREX-AQ observations represented a diverse set of sampled environments ranging from fresh/aged smoke from the Williams Flats fire to remnants of plumes transported over long distances. The Williams Flats fire resulted in significant aerosol enhancements during 3–8 August 2019, which were substantially underestimated by the standard version of WRF-Chem. The simulated black carbon (BC) and organic carbon (OC) concentrations increased between a factor of 92–125 (BC) and a factor of 28–78 (OC) with the new implementation compared to the standard WRF-Chem version. These increases resulted in better agreement with the FIREX-AQ airborne observations for BC and OC concentrations (particularly for fresh smoke sampling phases) and aerosol backscatter coefficients. The model still showed a low bias in simulating the aerosol loadings observed in aged plumes from Williams Flats. WRF-Chem with the FRP-based plume rise simulated similar plume heights to the standard plume-rise model in WRF-Chem. The simulated plume heights (for both versions) compared well with estimated plume heights using the HSRL measurements. Therefore, the better agreement with observations was mainly driven by the higher emissions in the FRP-based version. The model evaluations also highlighted the importance of accurately accounting for the wildfire diurnal cycle and including adequate representation of the underlying chemical mechanisms, both of which could significantly impact model forecasting performance.