Black Carbon Size Distribution Research Articles

Atmospheric concentrations of black carbon are substantially higher in spring than summer in the Arctic

A key driving factor behind rapid Arctic climate change is black carbon, the atmospheric aerosol that most efficiently absorbs sunlight. Our knowledge about black carbon in the Arctic is scarce, mainly limited to long-term measurements of a few ground stations and snap-shots by aircraft observations. Here, we combine observations from aircraft campaigns performed over nine years, and present vertically resolved average black carbon properties. A factor of four higher black carbon mass concentration (21.6 ng m−3 average, 14.3 ng m−3 median) was found in spring, compared to summer (4.7 ng m−3 average, 3.9 ng m−3 median). In spring, much higher inter-annual and geographic variability prevailed compared to the stable situation in summer. The shape of the black carbon size distributions remained constant between seasons with an average mass mean diameter of 202 nm in spring and 210 nm in summer. Comparison between observations and concentrations simulated by a global model shows notable discrepancies, highlighting the need for further model developments and intensified measurements.

The Role Played by the Bulk Hygroscopicity on the Prediction of the Cloud Condensation Nuclei Concentration Inside the Urban Aerosol Plume in Manaus, Brazil: From Measurements to Modeled Results

This work use observed and modeled data to trace a basic model that describes how the bulk chemical composition can be used to determine the aerosol size-dependency of hygroscopicity inside the urban aerosol pollution plume from Manaus, Brazil. The procedure is then used to predict the Cloud Condensation Nuclei (CCN) concentration (NCCN) from the Aerosol Size Distribution (ASD). The work briefly described hourly averaged data of ASD, Black Carbon size distribution (BCSD), Black Carbon mass concentration (BC), NCCN, and aerosol size hygroscopicity (κ) observed about 70 km downwind of the City of Manaus, inside the amazon rain forest, during 60 days of 2014, in the course of the rainy season. It uses a description of aerosol chemical composition obtained previously in the city of São Paulo, Brazil, as starting point to formulate a model that describes how particles in the pollution plume act as CCN as a function of their sizes and bulk chemical composition. A parameterization based on a polynomial fitting is proposed to determine BCSD from the BC. The measured and parameterized BCSD agree very well with more than 98% of the observed BCSDs, presenting a correlation coefficient larger than 0.9 with observation. The parameterized BC number concentration is also very well represented, with a correlation coefficient of 0.91 and a slope of 0.99 in comparison with observations. This work also studies how soot particles are incorporated in the CCN population and propose a parameterization to represent it. Simulations suggest that the larger BC particles are only partially incorporated as CCN and BC is a constraint to the fraction of aerosols that can act as CCN in all size ranges. The simulations also suggest that the incorporation of BC as CCN is probably only effective through coagulation in the presence of the wet phase. In addition, the work compares different strategies to predict observed NCCN from ASD. It is shown that the strategy presented can substantially improve the results of comparison of modeled and measured data from as bad as 2.14 ± 0.65 to as good as 1.02 ± 0.17. This study shows that the knowledge of the bulk chemical composition can be used to predict both the size-resolved chemical composition and mixing state, reducing the number of parameters needed to predict NCCN.

Size distributions, mixing state, and morphology of refractory black carbon in an urban atmosphere of northeast Asia during summer

Black carbon (BC) exerts profound impacts on air quality, human health, and climate. Here, we investigated concentrations and size distributions of refractory BC (rBC) and mixing state and morphology of rBC-containing particles in urban Seoul for 2019 summer. Mass concentrations of rBC ranged from 0.02 μgm−3 to 2.89 μgm−3, and daily maximums of rBC mass, daily minimums of rBC mass median diameter (MMD) (110–130 nm), and shell-to-core ratio (Rshell/core) occurred with NO2 maximums during morning rush hour. As the first report of ground observations on rBC mixing state, these results indicate that vehicle emission is a major local source of rBC in Seoul. MMDs of 127–146 nm and the greatest mass loadings of ≥1 μg m−3 were accompanied by high O3 and PM2.5 concentrations, in contrast to the largest MMDs (135–165 nm) associated with transport from upstream regions.The average Rshell/core was 1.25 for the rBC mass-equivalent diameter (DrBC) of 140–220 nm. Rshell/core increased gradually through the day and was positively correlated with Ox concentration, indicating photochemical aging of rBC particles. Co-emissions of rBC and volatile organic compounds from vehicles facilitated internal mixing during the daytime. However, Rshell/core tended to be low at temperature >∼30 °C, while 58 % of rBC particles with Rshell/core exceeding 1.25 were found at nighttime under relative humidity >75 %. These results demonstrate that the mixing state of freshly-emitted rBC particles was altered through coating by photochemically oxidized vapors during the day and hygroscopic growth at night. Additionally, the delay-time approach revealed rBC morphological characteristics, the most common being the bare type (74 %), and the attached type (6 %) was relatively large in numbers during morning rush hour. Therefore, it is suggested that during summer, rBC particles from traffic emissions should be considered in parallel to winter pollution mitigation strategies in urban atmosphere of northeast Asia.

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.

Estimation of real-time brown carbon absorption: An observationally constrained Mie theory-based optimization method

Methods to estimate absorption of brown carbon (BrC), a significant fraction of atmospheric absorption, rely on estimating the difference between total measured absorption at near-UV, and that of black carbon (BC). Extrapolation of absorption measured at near-IR wavelengths (assumed exerted by BC alone) use different assumptions of the wavelength dependence of absorption Ångström exponent (AAEBC). Here, we develop an improved method exploiting real-time multi-wavelength absorption and particle count measurements in a Mie based optimization framework, incorporating spectral observational constraints (measured absorption at 880 nm and AAE880-660). An optimization approach, using a Mie model with core-shell and core-gray shell mixing schemes, is used to derive BC size distribution parameters (absorbing core diameter and scattering shell thickness). Goodness of fit (Mie optimization model vs. measurement) was R = 0.77–0.94 (near-IR absorption) and within 4%–30% for BrC estimation. A sensitivity analysis of input parameters (BC geometric standard deviation and refractive index) bounded estimated BrC of 32%. Application to a polluted urban site (Delhi) and a regional background site (Darjeeling) estimated BrC absorption (% contribution) at 370 nm as 18–117 Mm−1 (15%–29%) and 2–12 Mm−1 (5%–21%), respectively. Estimated BrC absorption was larger at the regional background site (Darjeeling) but smaller at the polluted site (Delhi) when compared to constant AAE and two-component approaches. Method efficacy is reinforced through larger estimated BrC absorption at Delhi coinciding with agricultural stubble burning periods in North India. The developed method uses multi-wavelength absorption observational constraints to improve the robustness of BrC estimation.

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

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

Mass concentration and origin of black carbon in spring snow on glaciers in the Alaska Range

Black carbon (BC) is one of the light-absorbing particles that reduce the albedo of snow surfaces. Snow samples were taken from the surface of three glaciers in the Alaska Range in mid-April 2017. The BC size distribution and concentration were analyzed with a laser-induced incandescence (LII) method. The BC concentration of the snow samples was 1–6 μg L−1 and 0.5–3.1 μg L−1 at a depth of 0–2 cm (surface) and 2–10 cm (subsurface), respectively. These values are comparable to other Arctic areas and are considered to be the Alaskan background level. The BC concentrations are 0.5% of those of insoluble solid particles (ISPs) measured using an electrical sensing zone method. The surface albedo change due to BC and other ISPs concentrations was estimated to be 0.004–0.007 for the snow surface in April. The ablation at the observation sites on Gulkana Glacier would be 1.2% larger in the ablation season due to black carbon deposition. The chemical transport model revealed that 17%–34% of BC originates from biomass burning in Asia and Siberia, and 60% of BC originates from China in this study.

Seasonal contrast in size distributions and mixing state of black carbon and its association with PM<sub>1.0</sub> chemical composition from the eastern coast of India

Abstract. Over the Indian region, aerosol absorption is considered to have a potential impact on the regional climate, monsoon and hydrological cycle. Black carbon (BC) is the dominant absorbing aerosol, whose absorption potential is determined mainly by its microphysical properties, including its concentration, size and mixing state with other aerosol components. The Indo-Gangetic Plain (IGP) is one of the regional aerosol hot spots with diverse sources, both natural and anthropogenic, but still the information on the mixing state of the IGP aerosols, especially BC, is limited and a significant source of uncertainty in understanding their climatic implications. In this context, we present the results from intensive measurements of refractory BC (rBC) carried out over Bhubaneswar, an urban site in the eastern coast of India, which experiences contrasting air masses (the IGP outflow or coastal/marine air masses) in different seasons. This study helps to elucidate the microphysical characteristics of BC over this region and delineates the IGP outflow from the other air masses. The observations were carried out as part of South West Asian Aerosol Monsoon Interactions (SWAAMI) collaborative field experiment during July 2016–May 2017, using a single-particle soot photometer (SP2) that uses a laser-induced incandescence technique to measure the mass and mixing state of individual BC particles and an aerosol chemical speciation monitor (ACSM) to infer the possible coating material. Results highlighted the distinctiveness in aerosol microphysical properties in the IGP air masses. BC mass concentration was highest during winter (December–February) (∼1.94±1.58 µg m−3), when the prevailing air masses were mostly of IGP origin, followed by post-monsoon (October–November) (mean ∼1.34±1.40 µg m−3). The mass median diameter (MMD) of the BC mass size distributions was in the range 0.190–0.195 µm, suggesting mixed sources of BC, and, further, higher values (∼ 1.3–1.8) of bulk relative coating thickness (RCT) (ratio of optical and core diameters) were seen, indicating a significant fraction of highly coated BC aerosols in the IGP outflow. During the pre-monsoon (March–May), when marine/coastal air masses prevailed, BC mass concentration was lowest (∼0.82±0.84 µg m−3), and larger BC cores (MMD > 0.210 µm) were seen, suggesting distinct source processes, while RCT was ∼ 1.2–1.3, which may translate into higher extent of absolute coating on BC cores, which may have crucial regional climate implications. During the summer monsoon (July–September), BC size distributions were dominated by smaller cores (MMD ≤ 0.185 µm), with the lowest coating indicating fresher BC, likely from fossil fuel sources. A clear diurnal variation pattern of BC and RCT was noticed in all the seasons, and daytime peak in RCT suggested enhanced coating on BC due to the condensable coating material originating from photochemistry. Examination of submicrometre aerosol chemical composition highlighted that the IGP outflow was dominated by organics (47 %–49 %), and marine/coastal air masses contained higher amounts of sulfate (41 %–47 %), while ammonium and nitrate were seen in minor amounts, with significant concentrations only during the IGP air mass periods. The diurnal pattern of sulfate resembled that of the RCT of rBC particles, whereas organic mass showed a pattern similar to that of the rBC mass concentration. Seasonally, the coating on BC showed a negative association with the mass concentration of sulfate during the pre-monsoon season and with organics during the post-monsoon season. These are the first experimental data on the mixing state of BC from a long time series over the Indian region and include new information on black carbon in the IGP outflow region. These data help in improving the understanding of regional BC microphysical characteristics and their climate implications.

Changes in black carbon and PM2.5 in Tokyo in 2003-2017.

Black carbon (BC) particles cause adverse health effects and contribute to the heating of the atmosphere by absorbing visible solar radiation. Efforts have been made to reduce BC emissions, especially in urban areas; however, long-term measurements of BC mass concentration (MBC) are very limited in Japan. We report MBC measurements conducted in Tokyo from 2003 to 2017, showing that MBC decreased by a factor of 3 from 2003 to 2010 and was stable from 2010 to 2017. Fine particulate concentrations (PM2.5) decreased by a much smaller factor during 2003–2010. The diurnal variations of BC size distributions suggest that the BC in Tokyo originates mainly from local sources, even after 2010. Our three-dimensional model calculations show that BC from the Asian continent contributes a small portion (about 20%) of the annual average MBC in the Kanto region of Japan, which includes Tokyo. This indicates that continued reduction of BC emissions inside Japan should be effective in further decreasing MBC.

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

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

Concentrations and Size Distributions of Black Carbon in the Surface Snow of Eastern Antarctica in 2011

AbstractKnowledge of black carbon (BC) concentrations and size distributions within surface snow in Antarctica is limited. However, these measurements are important to understanding global aerosol transport from combustion sources, and BC contributes to positive radiative forcing. This study analyzed the concentrations and size distributions of BC and inorganic ions in snow samples collected at the Syowa station in Antarctica from April to December 2011 and along a traverse route to an inland (Mizuho) station. The BC size distributions in snow were bimodal with mass median diameters of ~140 and ~690 nm. We also estimated the mass median diameter from unimodal distributions and found smaller diameters than were reported by other studies. The mass concentrations of BC in snow were higher in inland samples than in Syowa samples. Among Syowa samples, the BC concentrations in December (2117.3 ng L−1 on average) were higher than in other periods (288.2 ng L−1 on average). The December samples experienced ambient temperatures above 0 °C, and the atmospheric BC concentrations did not increase simultaneously. Inorganic ions originated from the ocean and decreased with increasing distance from the coastal area. We conclude that the BC concentrations in surface snow increased mainly by postdeposition processes through the loss of water mass due to melting, evaporation, and sublimation. Our study is the first to report detailed BC concentrations and size distributions in eastern Antarctica, and the results will help to evaluate BC global transport, the snow albedo estimations in this region, and the climate impacts of BC.

Estimating Source Region Influences on Black Carbon Abundance, Microphysics, and Radiative Effect Observed Over South Korea

AbstractEast Asia is the strongest global source region for anthropogenic black carbon (BC), the most important light‐absorbing aerosol contributing to direct radiative climate forcing. To provide extended observational constraints on regional BC distributions and impacts, in situ measurements of BC were obtained with a single particle soot photometer during the May/June 2016 Korean‐United States Air Quality aircraft campaign (KORUS‐AQ) in South Korea. Unique chemical tracer relationships were associated with BC sourced from different regions. The extent and variability in vertical BC mass burden for 48 profiles over a single site near Seoul were investigated using back trajectory and chemical tracer analysis. Meteorologically driven changes in transport influenced the relative importance of different source regions, impacting observed BC loadings at all altitudes. Internal mixing and size distributions of BC further demonstrated dependence on source region: BC attributed to China had a larger mass median diameter (180 ± 13 nm) than BC attributed to South Korea (152 ± 25 nm), and BC associated with long‐range transport was less thickly coated (60 ± 4 nm) than that sourced from South Korea (75 ± 16 nm). The column BC direct radiative effect at the top of the atmosphere was estimated to be W/m2, with average values for different meteorological periods varying by a factor of 2 due to changes in the BC vertical profile. During the campaign, BC sourced from South Korea (≤ 31%), China (22%), and Russia (14%) were the most significant single‐region contributors to the column direct radiative effect.

Measurement and modeling of the multiwavelength optical properties of uncoated flame-generated soot

Abstract. Optical properties of flame-generated black carbon (BC) containing soot particles were quantified at multiple wavelengths for particles produced using two different flames: a methane diffusion flame and an ethylene premixed flame. Measurements were made for (i) nascent soot particles, (ii) thermally denuded nascent particles, and (iii) particles that were coated and then thermally denuded, leading to the collapse of the initially lacy, fractal-like morphology. The measured mass absorption coefficients (MACs) depended on soot maturity and generation but were similar between flames for similar conditions. For mature soot, here corresponding to particles with volume-equivalent diameters >∼160 nm, the MAC and absorption Ångström exponent (AAE) values were independent of particle collapse while the single-scatter albedo increased. The MAC values for these larger particles were also size-independent. The mean MAC value at 532 nm for larger particles was 9.1±1.1 m2 g−1, about 17 % higher than that recommended by Bond and Bergstrom (2006), and the AAE was close to unity. Effective, theory-specific complex refractive index (RI) values are derived from the observations with two widely used methods: Lorenz–Mie theory and the Rayleigh–Debye–Gans (RDG) approximation. Mie theory systematically underpredicts the observed absorption cross sections at all wavelengths for larger particles (with x>0.9) independent of the complex RI used, while RDG provides good agreement. (The dimensionless size parameter x=πdp/λ, where dp is particle diameter and λ is wavelength.) Importantly, this implies that the use of Mie theory within air quality and climate models, as is common, likely leads to underpredictions in the absorption by BC, with the extent of underprediction depending on the assumed BC size distribution and complex RI used. We suggest that it is more appropriate to assume a constant, size-independent (but wavelength-specific) MAC to represent absorption by uncoated BC particles within models.

Influence of Emissions and Aqueous Processing on Particles Containing Black Carbon in a Polluted Urban Environment: Insights From a Soot Particle‐Aerosol Mass Spectrometer

AbstractInorganic and organic coatings on black carbon (BC) particles can enhance light absorption and affect atmospheric lifetimes of BC‐containing particles and thus have significant implications for climate. To study the physical and chemical characteristics of atmospheric BC and BC‐associated coatings, a soot particle‐aerosol mass spectrometer was deployed during the winter of 2014–2015 in Fresno, a city located in the San Joaquin Valley of California, to selectively analyze BC‐containing particles. Comparing soot particle‐aerosol mass spectrometer measurements to those from the collocated single‐particle soot photometer (SP2) and high‐resolution aerosol mass spectrometer, we found that 17% of total submicrometer aerosol mass was associated with BC‐containing particles, suggesting that a majority of the fine particles in Fresno contained no BC. Most BC‐containing particles appeared to be associated with residential wood burning and vehicular traffic. These particles typically had a bulk‐average mass ratio of coating to BC (Rcoat/rBC) less than 2. However, during periods of persistent fog larger Rcoat/rBC values were observed, with the coatings primarily composed of secondary inorganic and organic components that likely resulted from aqueous‐phase processing. Specifically, compared to periods with less fog, the BC coating increased in concentration and contained a larger fraction of nitrate and oxidized organic matter. The size distributions of BC and associated organic coating were generally centered around 300 nm in vacuum aerodynamic diameter. However, during foggy periods BC had an additional peak at ~400 nm and organics and nitrate displayed a prominent mode in the accumulation size range.

Scavenging ratio of black carbon in the Arctic and the Antarctic

Long-term monitoring of atmospheric aerosols and their interaction with radiation, cloud, and cryosphere over the Arctic and the Antarctic are very important for the global climate change related issues. In this regard, for conducting aerosol measurements, India has extended the concerted efforts to the Svalbard region of the Norwegian Arctic (Himadri, 78°55′N 11°56′E, 8 m a.s.l.) in the northern hemisphere and the Larsemann Hills of coastal Antarctic (Bharati, 69°24.4′S 76°11.7′E, 40 m a.s.l.) in the southern hemisphere. In the present study, we have examined the role of black carbon (BC) deposition in darkening the polar snow in different sunlit seasons and estimated the scavenging ratio of BC over both the poles from simultaneous measurements of atmospheric and snow deposited BC concentrations. The study reveals distinct spatio-temporal variability of BC in polar snow, even though the concentrations are, in general, low (<12 ppbw, parts per billion by weight). During local summer seasons, the BC in snow at the Arctic (median ∼ 7.98 ppbw) was higher than that at the Antarctica (median ∼ 1.70 ppbw). Concurrent with this, the scavenging ratio (SR) also showed large variability over both the poles. Relatively higher values of SR over the Antarctica (mean ∼ 119.54 ± 23.04; during southern hemispheric summer) in comparison to that over the Arctic (mean ∼ 69.48 ± 4.79; during northern hemispheric spring) clearly indicate the difference in removal mechanisms (aerosol mixing, aging and size distribution) of BC from the atmosphere over distinct polar environments. Measurement of spectral incoming and reflected radiances over the Arctic snow during the early spring season of 2017 indicated the values of surface broadband albedo varying between 0.64 and 0.79. The Snow, Ice and Aerosol Radiative (SNICAR) model simulated values of spectral albedo correlated well with the measured ones and indicated the role of dust absorption, in addition to that of BC, in changing the snow albedo. This information needs to be accurately incorporated in the radiative transfer models for the accurate estimation of snow albedo forcing over the Polar Regions.

Downwind evolution of the volatility and mixing state of near-road aerosols near a US interstate highway

Abstract. We present spatial measurements of particle volatility and mixing state at a site near a North Carolina interstate highway (I-40) applying several heating (thermodenuder; TD) experimental approaches. Measurements were conducted in summer 2015 and winter 2016 in a roadside trailer (10 m from road edge) and during downwind transects at different distances from the highway under favorable wind conditions using a mobile platform. Results show that the relative abundance of semi-volatile species (SVOCs) in ultrafine particles decreases with downwind distance, which is consistent with the dilution and mixing of traffic-sourced particles with background air and evaporation of semi-volatile species during downwind transport. An evaporation kinetics model was used to derive particle volatility distributions by fitting TD data. While the TD-derived distribution apportions about 20–30 % of particle mass as semi-volatile (SVOCs; effective saturation concentration, C∗ ≥ 1µm−3) at 10 m from the road edge, approximately 10 % of particle mass is attributed to SVOCs at 220 m, showing that the particle-phase semi-volatile fraction decreases with downwind distance. The relative abundance of semi-volatile material in the particle phase increased during winter. Downwind spatial gradients of the less volatile particle fraction (that remaining after heating at 180 °C) were strongly correlated with black carbon (BC). BC size distribution and mixing state measured using a single-particle soot photometer (SP2) at the roadside trailer showed that a large fraction (70–80 %) of BC particles were externally mixed. Heating experiments with a volatility tandem differential mobility analyzer (V-TDMA) also showed that the nonvolatile fraction in roadside aerosols is mostly externally mixed. V-TDMA measurements at different distances downwind from the highway indicate that the mixing state of roadside aerosols does not change significantly (e.g., BC mostly remains externally mixed) within a few hundred meters from the highway. Our analysis indicates that a superposition of volatility distributions measured in laboratory vehicle tests and of background aerosol can be used to represent the observed partitioning of near-road particles. The results from this study show that exposures and impacts of BC and semi-volatile organics-containing particles in a roadside microenvironment may differ across seasons and under changing ambient conditions.

Seasonal Progression of the Deposition of Black Carbon by Snowfall at Ny‐Ålesund, Spitsbergen

AbstractDeposition of black carbon (BC) aerosol in the Arctic lowers snow albedo, thus contributing to warming in the region. However, the processes and impacts associated with BC deposition are poorly understood because of the scarcity and uncertainties of measurements of BC in snow with adequate spatiotemporal resolution. We sampled snowpack at two sites (11 m and 300 m above sea level) at Ny‐Ålesund, Spitsbergen, in April 2013. We also collected falling snow near the surface with a windsock from September 2012 to April 2013. The size distribution of BC in snowpack and falling snow was measured using a single‐particle soot photometer combined with a characterized nebulizer. The BC size distributions did not show significant variations with depth in the snowpack, suggesting stable size distributions in falling snow. The BC number and mass concentrations (CNBC and CMBC) at the two sites agreed to within 19% and 10%, respectively, despite the sites' different snow water equivalent (SWE) loadings. This indicates the small influence of the amount of SWE (or precipitation) on these quantities. Average CNBC and CMBC in snowpack and falling snow at nearly the same locations agreed to within 5% and 16%, after small corrections for artifacts associated with the sampling of the falling snow. This comparison shows that the dry deposition was a small contributor to the total BC deposition. CMBC were highest (2.4 ± 3.0 μg L−1) in December–February and lowest (1.2 ± 1.2 μg L−1) in September–November.

Emissions from prescribed burning of agricultural fields in the Pacific Northwest

Prescribed burns of winter wheat stubble and Kentucky bluegrass fields in northern Idaho and eastern Washington states (U.S.A.) were sampled using ground-, aerostat-, airplane-, and laboratory-based measurement platforms to determine emission factors, compare methods, and provide a current and comprehensive set of emissions data for air quality models, climate models, and emission inventories. Batch measurements of PM2.5, volatile organic compounds (VOCs), polycyclic aromatic hydrocarbons (PAHs), and polychlorinated dibenzodioxins/dibenzofurans (PCDDs/PCDFs), and continuous measurements of black carbon (BC), particle mass by size, CO, CO2, CH4, and aerosol characteristics were taken at ground level, on an aerostat-lofted instrument package, and from an airplane. Biomass samples gathered from the field were burned in a laboratory combustion facility for comparison with these ground and aerial field measurements. Emission factors for PM2.5, organic carbon (OC), CH4, and CO measured in the field study platforms were typically higher than those measured in the laboratory combustion facility. Field data for Kentucky bluegrass suggest that biomass residue loading is directly proportional to the PM2.5 emission factor; no such relationship was found with the limited wheat data. CO2 and BC emissions were higher in laboratory burn tests than in the field, reflecting greater carbon oxidation and flaming combustion conditions. These distinctions between field and laboratory results can be explained by measurements of the modified combustion efficiency (MCE). Higher MCEs were recorded in the laboratory burns than from the airplane platform. These MCE/emission factor trends are supported by 1–2 min grab samples from the ground and aerostat platforms. Emission factors measured here are similar to other studies measuring comparable fuels, pollutants, and combustion conditions. The size distribution of refractory BC (rBC) was single modal with a log-normal shape, which was consistent among fuel types when normalized by total rBC mass. The field and laboratory measurements of the Angstrom exponent (α) and single scattering albedo (ω) exhibit a strong decreasing trend with increasing MCEs in the range of 0.9–0.99. Field measurements of α and ω were consistently higher than laboratory burns, which is likely due to less complete combustion. When VOC emissions are compared with MCE, the results are consistent for both fuel types: emission factors increase as MCE decreases.

Sensitivity of climate effects of black carbon in China to its size distributions

The climate effects of black carbon (BC) aerosols are sensitive to BC size distributions and this sensitivity over China is studied using a regional climate model, namely RIEMS2.0. A new size-resolved scheme is developed based on observational data. The simulated BC concentrations with the new scheme are better compared with the observation than the previous uniform scheme, which is likely to overestimate BC concentrations, radiative forcings, and warming effects in many regions of China due to its simple assumption on BC size. The simulation with the size-resolved scheme suggests a reduction of the all-sky radiative forcing of BC at the top of atmosphere (TOA) by 0–0.25Wm−2 over the most study domain. Correspondingly, the warming effect of BC is weakened by −0.04 to −0.16K over most parts of South China and North China. The difference in BC-induced precipitation between the two schemes varies irregularly from region to region, ranging from −2.8 to 2.8mmd−1. With the size-resolved scheme, the BC radiative properties and the climate effects are reassessed and the means (ranges) over the study domain are summarized as follows. The annual mean surface concentration of BC is 0.88μg/m3, ranging from 1 to 8μg/m3 over North China and Central China. The all-sky and clear-sky radiative forcings of BC at the TOA are 0.43 and 0.39W/m2, respectively. Over most parts of Southwest China, Central China, and North China, the BC warming effect prevails, with enhanced temperature of 0.04–0.28K. BC aerosols usually enhance precipitation in South China and North China, ranging from 0.40 to 2.8mmd−1.

Effects of wet deposition on the abundance and size distribution of black carbon in East Asia

AbstractAn improved understanding of the variations in the mass concentration and size distribution of black carbon (BC) in the free troposphere (FT) over East Asia, where BC emissions are very high, is needed to reliably estimate the radiative forcing of BC in climate models. We measured these parameters and the carbon monoxide (CO) concentration by conducting the Aerosol Radiative Forcing in East Asia (A‐FORCE) 2013W aircraft campaign in East Asia in winter 2013 and compared these data with measurements made in the same region in spring 2009. The median BC concentrations in the FT originating from North China (NC) and South China (SC) showed different seasonal variations, which were primarily caused by variations in meteorological conditions. CO concentrations above the background were much higher in SC than in NC in both seasons, suggesting a more active upward transport of CO. In SC, precipitation greatly increased from winter to spring, leading to an increased wet deposition of BC. As a result, the median BC concentration in the FT was highest in SC air in winter. This season and region were optimal for the effective transport of BC from the planetary boundary layer to the FT. The count median diameters of the BC size distributions generally decreased with altitude via wet removal during upward transport. The altitude dependence of the BC size distributions was similar in winter and spring, in accord with the similarity in the BC mixing state. The observed BC concentrations and microphysical properties will be useful for evaluating the performance of climate models.