Black Carbon Size Distribution Research Articles

Influence of the melting temperature on the measurement of the mass concentration and size distribution of black carbon in snow

Abstract. The influence of temperature and time of snow sample melting on the measurement of mass concentration and size distribution of black carbon (BC) in snow was evaluated experimentally. In the experiments, fresh (Shirouma) and aged (Hakusan) snow samples were melted at different temperatures or at different time lengths, and the BC mass concentration and size distribution in the melted snow samples were measured using a nebulizer and a single-particle soot photometer (SP2). In the experiment where melting temperature was varied, the BC mass concentration in the liquid decreased at a melting temperature of 70 °C. This decrease was 8.0 % for the Shirouma sample and 46.4 % for the Hakusan sample and depended on BC particle size, with a significant decrease found at BC diameters less than 350 nm. A similar decrease in BC mass concentration was found when the Hakusan snow sample that had been melted at 5 °C was heated to 70 °C. The experiment in which melting time was varied indicated that BC mass concentration in the liquid did not change for the Shirouma sample but decreased significantly with a longer melting time for the Hakusan sample (38.6 %). These results indicate that melting of snow samples at high temperatures or over long time periods can significantly affect the measurement of BC mass and its size distribution, especially for aged snow samples.

Seasonal Variability of the Black Carbon Size Distribution in the Atmospheric Aerosol

Round-the-clock measurements of the black carbon size distribution in the submicron near-ground aerosol of Western Siberia performed in 2014 by the diffusion method developed by the authors are analyzed. It is revealed that the tendency for decreasing the volume median diameter and the amplitude of distribution of the black carbon is traced in the seasonal dynamics of the average monthly black carbon particle size distribution (approximated by a single-mode lognormal function) during winter-to-summer season transition. The shape of the black carbon size distributions is in agreement with measurements by other well-known methods in different geographic regions.

광학 입자 측정기 비교 측정에 의한 입경별 일평균 블랙카본 분석 - Part I

광학 입자 측정기 비교 측정에 의한 입경별 일평균 블랙카본 분석 - Part I

Improved technique for measuring the size distribution of black carbon particles in liquid water

ABSTRACTWe developed an improved technique for measuring the size distribution of black carbon (BC) particles suspended in liquid water to facilitate quantitative studies of the wet deposition of BC. The measurement system, which consists of a nebulizer and a single-particle soot photometer, incorporates two improvements into the system that we developed earlier. First, we extended the upper limit of the detectable BC size from 0.9 μm to about 4.0 μm by modifying the photo-detector for measuring the laser-induced incandescence signal. Second, we introduced a pneumatic nebulizer (Marin-5) with a high extraction efficiency (∼50.0%) that was independent of particle diameter up to 2.0 μm. For BC mass concentrations less than 70 μg L−1, we experimentally showed that the diameters of BC particles did not appreciably change during the Marin-5 extraction process, consistent with theoretical calculations. Finally, we demonstrated by laboratory experiments that the size distributions of ambient BC particles changed...

Partitioning of Black Carbon between ultrafine and fine particle modes in an urban airport vs. urban background environment

In this work, we characterize the Black Carbon (BC) aerosol in an urban airport vs. urban background environment with the objective to evaluate when and how the ultrafine BC dominates the bulk aerosol. Aerosol optical and microphysical properties were measured in a Mediterranean urban area (Rome) at sites impacted by BC sources including fossil fuels (FF), and biomass burning (BB). Experimental BC data were interpreted through measurement-constrained simulations of BC microphysics and optical properties. A “scheme” to separate the ultrafine BC was experimented on the basis of the relation found between changes in the BC partitioning between Aitken and accumulation mode particles, and relevant changes in particle size distribution and optical properties of the bulk aerosol. This separation scheme, applied to experimental data, proved useful to reveal the impact of airport and road traffic emissions. Findings may have important atmospheric implications. The experimented scheme can help separating different BC sources (FF, BB, “aged” BC) when BC size distributions may be very difficult to obtain (satellite, columnar observations, routine monitoring). Indeed, separating the ultrafine BC from the fine BC may provide significant benefits in addressing BC impact on air quality and climate.

Simplifying the calculation of light scattering properties for black carbon fractal aggregates

Abstract. Black carbon fractal aggregates have complicated shapes that make the calculation of their optical properties particularly computationally expensive. Here, a method is presented to estimate fractal aggregate light scattering properties by optimising simplified models to full light scattering calculations. It is found that there are no possible spherical models (at any size or refractive index) that well represent the light scattering in the visible or near-thermal infrared. As such, parameterisations of the light scattering as a function of the number of aggregate particles is presented as the most pragmatic choice for modelling distributions of black carbon when the large computational overheads of rigorous scattering calculations cannot be justified. This parameterisation can be analytically integrated to provide light scattering properties for lognormal distributions of black carbon fractal aggregates and return extinction cross sections with 0.1% accuracy for typical black carbon size distributions. Scattering cross sections and the asymmetry parameter can be obtained to within 3%.

Evaluation of aerosol number concentrations in NorESM with improved nucleation parameterization

Abstract. The Norwegian Earth System Model (NorESM) is evaluated against atmospheric observations of aerosol number concentrations. The model is extended to include an explicit mechanism for new particle formation and secondary organic aerosol (SOA) formation from biogenic precursors. Three nucleation mechanisms are included in NorESM: binary sulfuric acid, activation type, and organic nucleation. Ten model experiments are conducted to study the sensitivity of the simulated aerosol number concentrations to nucleation, SOA formation, black carbon size distribution and model meteorology. Simulated vertical profiles are evaluated against 12 flight campaigns. Comparison of monthly averaged aerosol number concentrations against 60 measurement sites reveals that the model with explicit nucleation and SOA scheme performs well in terms of correlation coefficient, R2 = 0.41 and a bias of −6%. NorESM generally overestimates the amplitude of the seasonal cycle, possibly due to underestimated sinks or exaggerated sensitivity to biogenic precursors.

A size-segregation method for monitoring the diurnal characteristics of atmospheric black carbon size distribution at urban traffic sites

Understanding the characteristics of the size distribution of ambient black carbon (BC) in distinct environments is critical because the influence of BC aerosols on climate, visibility, and human health depends strongly on the distribution of BC aerosols over the particle size spectrum. In this study, a novel method for determining the mass size distribution of BC in atmospheric aerosols was developed. This size-segregation method relies on measuring BC in parallel using two aethalometers, one of which is used to measure the total BC (BCT) mass concentration as a reference level and the other is used to measure the BC (BCi) mass concentration for BC sizes below specific particle sizes that are selected using a size cut-off inlet. In this study, this method was applied to measure BC in atmospheric samples at an urban traffic site. The aethalometers were operated continually from December 15, 2012 to January 31, 2013, and from February 15, 2013 to March 31, 2013. The measurement results presented in this paper are for the diurnal variation patterns, average concentrations, mass fractions, and size distributions of BC aerosols. The results indicate that BCT mass concentration is approximately 2.8 μg m−3 in the Taipei urban area. The levels of BC at this sampling site were affected markedly by traffic emission levels and local wind speed. At the sampling site, the average BC2.5/BCT, BC1.0/BCT, BC0.5/BCT, BC0.25/BCT, and BC0.1/BCT were 0.96 ± 0.04, 0.92 ± 0.07, 0.89 ± 0.04, 0.73 ± 0.10, and 0.18 ± 0.08, respectively. The results indicate that approximately 90% of the BC aerosols were smaller than 0.5 μm, that most of the BC aerosols (55%) were in the size range of 0.1–0.25 μm, and that approximately 18% of the BC aerosols were ultrafine. Moreover, the daily average mass size distribution of BC exhibited a single accumulation mode at 0.16 μm at this sampling site. The mode of the BC mass size distribution at rush hour (9 AM) was only 0.14 μm, which is smaller than the daily average. Moreover, the mode of the BC mass size distribution at an early morning hour (3 AM) was 0.18 μm, and a minor coarse mode was also observed during this period. The results further revealed that the geometric diameter (Dpg) of the BC aerosols varied between 0.14 and 0.22 μm and the geometric standard deviation (σg) of these BC aerosols ranged between 1.4 and 2.3 during the sampling period. Because BC exhibits extremely low chemical reactivity; the size distribution of BC in the atmosphere does not change substantially except through coagulation.

On-road black carbon instrument intercomparison and aerosol characteristics by driving environment

Large spatial variations of black carbon (BC) concentrations in the on-road and near-road environments necessitate measurements with high spatial resolution to assess exposure accurately. A series of measurements was made comparing the performance of several different BC instruments (Single Particle Soot Photometer, Photo-Acoustic Soot Spectrometer, and Aethalometer) for high time resolution mobile measurements, capable of mapping spatial gradients. All instruments were highly correlated at high time resolution (r2 = 0.80–0.89 at a 2-s resolution), however the slope ranged from 0.52 to 1.03, with the Single Particle Soot Photometer (SP2) consistently reporting the lowest BC concentrations. BC and ultrafine particle (UFP) concentrations were two-fold higher on the highway compared to surrounding roads with lower traffic counts. The BC size distribution had a mass median diameter of approximately 120 nm, which was smaller and less coated than aged urban BC. Mean UFP and BC concentrations were 2 and 1.4 times greater, respectively, during free flowing traffic on the highway compared with times when there was stop-and-go congestion, providing evidence that transit time is not a good predictor of BC or UFP exposure.

Case study of absorption aerosol optical depth closure of black carbon over the East China Sea

AbstractAbsorption aerosol optical depth (AAOD) measurements made by sun‐sky photometers are currently the only constraint available for estimates of the global radiative forcing of black carbon (BC), but their validation studies are limited. In this paper, we report the first attempt to compare AAODs derived from single‐particle soot photometer (SP2) and ground‐based sun‐sky photometer (sky radiometer, SKYNET) measurements. During the Aerosol Radiative Forcing in East Asia (A‐FORCE) experiments, BC size distribution and mixing state vertical profiles were measured using an SP2 on board a research aircraft near the Fukue Observatory (32.8°N, 128.7°E) over the East China Sea in spring 2009 and late winter 2013. The aerosol extinction coefficients (bext) and single scattering albedo (SSA) at 500 nm were calculated based on aerosol size distribution and detailed BC mixing state information. The calculated aerosol optical depth (AOD) agreed well with the sky radiometer measurements (2 ± 6%) when dust loadings were low (lidar‐derived nonspherical particle contribution to AOD less than 20%). However, under these low‐dust conditions, the AAODs obtained from sky radiometer measurements were only half of the in situ estimates. When dust loadings were high, the sky radiometer measurements showed systematically higher AAODs even when all coarse particles were assumed to be dust for in situ measurements. These results indicate that there are considerable uncertainties in AAOD measurements. Uncertainties in the BC refractive index, optical calculations from in situ data, and sky radiometer retrieval analyses are discussed.

Comparison of light absorption properties for various absorbing particles

We experimentally determined optical properties of various absorbing particles such as nigrosins, black-dyed polystyrene latex, and diesel black carbon (BC). The absorption coefficient (Q abs) was measured to determine the absorption cross section (σ abs) for given particle sizes. Our experimental system consists of a differential mobility analyzer (DMA), a condensation particle counter (CPC), a multi-angle absorption photometer (MAAP), an elemental carbon/organic carbon (EC/OC) analyzer, an aerosol sampler, a dilution device, and a diesel engine. We diluted the exhaust from the diesel engine in order to provide similarity to aerosol particles of accumulation mode in the atmosphere. We measured the size distribution of diesel BC using the DMA and the CPC. The mode diameter was changed as the diesel BC was grown. We measured the number concentration (N) and the absorption coefficient for black carbon using the CPC and the MAAP, respectively. Then, we obtained absorption cross sections for various particle sizes. Preliminary result showed that the absorption cross section for diesel BC having a 200-nm diameter was measured to be 1.06 × 10−14 m2/particle. For diesel BC, mass concentrations measured by the MAAP were in good agreement with those measured by the OC/EC analyzer.

Evaluation of a Method to Measure Black Carbon Particles Suspended in Rainwater and Snow Samples

We conducted a detailed evaluation of a method for measuring the mass concentrations and size distributions of black carbon (BC) particles in rainwater and snow. The method uses an ultrasonic nebulizer (USN) and a single particle soot photometer (SP2). The USN disperses sample water into micron-size droplets at a constant rate and then dries them to release BC particles into the air. The masses of individual BC particles are measured by the SP2, using the laser-induced incandescence technique. The loss of BC particles during the extraction from liquid water to air depends on their sizes. We determined the size-dependent extraction efficiency using polystyrene latex (PSL) spheres with 12 different diameters between 107 and 1025 nm. The PSL concentrations in water were measured by the light extinction at 532 nm. The extraction efficiency of the USN showed a broad maximum of about 10% in the diameter range 200–500 nm and decreased substantially at larger sizes. The accuracy and reproducibility of the measure...

Black carbon mass size distributions of diesel exhaust and urban aerosols measured using differential mobility analyzer in tandem with Aethalometer

Black carbon (BC) is the dominant component of the light absorbing aerosols in the atmosphere, changing earth's radiative balance and affecting the climate. The mixing state and size distribution of atmospheric BC are largely unknown and cause uncertainties in climate models. BC is also a major component of diesel PM emissions, recently classified by World Health Organization as Category I Carcinogen, and has been associated with various adverse health effects. This study presents a novel approach of direct and continuous measurement of BC mass size distribution by tandem operation of a differential mobility spectrometry and a refined Aethalometer. A condensation particle counter was deployed in parallel with the Aethalometer to determine particle number size distribution. A wide range of particle sizes (20–600 nm) was investigated to determine the BC modal characteristics in fresh diesel engine tailpipe emissions and in different urban environments including a typical urban ambient site and a busy roadside. The study provided a demonstration of a new analytic approach and showed the evolution of BC mass size distribution from fresh engine emissions to the aged aerosols in the roadside and ambient environments. The results potentially can be used to refine the input for climate modeling to determine the effect of particle-bound atmospheric BC on the global climate.

The mass and number size distributions of black carbon aerosol over Europe

Abstract. Black carbon-containing aerosol particles play an important role in the direct and indirect radiative forcing of climate. However, the magnitude and sign of the net radiative effect is strongly dependent on the physical properties of the black carbon (BC) component of the particles, such as mass concentration, number size distribution and mixing state. Here we use a global aerosol model combined with aircraft measurements of BC particle number and size from the Single Particle Soot Photometer (SP2) to assess the realism with which these physical properties are predicted by global models. The comparison reveals a substantial mismatch between the measured and modelled BC size distribution over the size range of the SP2 instrument (90–400 nm BC diameter). The model predicts BC particle number concentrations a factor ~3.5–5.7 higher than measured and a mode diameter that is ~40–65 nm smaller than observed. More than ~90% of the model particles with dry diameters ≳260 nm contain BC, while the observations suggest only 14% on average. These model–observation biases in the BC properties are considerably greater than for the overall particle distribution, suggesting that the discrepancy is associated with model assumptions about the size and mixing state of the emitted carbonaceous particles. We expect the discrepancy in BC size distribution to be common among most global aerosol models, with implications for model estimates of absorption optical depth and direct radiative forcing.

Development of a parameterization of black carbon aging for use in general circulation models

Abstract. A parameterization of black carbon (BC) aging in the atmosphere is developed for use in general circulation models (GCMs) that separately treat hydrophobic BC and hydrophilic BC modes but do not explicitly calculate the aging processes of BC. The rate of BC aging is expressed as the conversion rate from hydrophobic BC to hydrophilic BC modes (i.e., inverse of the e-folding time of the conversion, 1/τBC). In this study, the conversion rates are estimated using results of detailed calculations by a size and mixing state resolved aerosol box model with numerous initial conditions. We introduce a new concept, the hydrophobic-BC-mass-normalized coating rate (VBC), defined as the rate of increase of the mass concentration of condensed materials on hydrophobic BC normalized by the hydrophobic BC mass concentration. Although the conversion rate largely varies depending on the atmospheric conditions and the concentrations of chemical species, we find that the variations of the conversion rate are generally expressed well by a unique function of VBC for given lognormal size distributions of hydrophobic BC. The parameterized conversion rate is expressed as a function of VBC, which enables the representation of diurnal and seasonal variations of the BC aging rate and its spatial differences in polluted and clean air, while other widely used constant conversion rates cannot. Application of our newly developed parameterization to GCMs will provide more reliable estimates of the spatial distribution of BC and its radiative effects at regional and global scales.

Assessing Single Particle Soot Photometer and Integrating Sphere/Integrating Sandwich Spectrophotometer measurement techniques for quantifying black carbon concentration in snow

Abstract. We evaluate the performance of the Single Particle Soot Photometer (SP2) and the Integrating Sphere/Integrating Sandwich Spectrophotometer (ISSW) in quantifying the concentration of refractory black carbon (BC) in snow samples. We find that the SP2 can be used to measure BC mass concentration in snow with substantially larger uncertainty (60%) than for atmospheric sampling (<30%). Achieving this level of accuracy requires careful assessment of nebulizer performance and SP2 calibration with consideration of the fact that BC in snow can exist in larger sizes than typically observed in the atmosphere. Once these issues are addressed, the SP2 is able to measure the size distribution and mass concentration of BC in the snow. Laboratory comparison of the SP2 and the ISSW revealed significant biases in the estimate of BC concentration from the ISSW when test samples contained dust or non-absorbing particulates. These results suggest that current estimates of BC mass concentration in snow or ice formed from fallen snow using either the SP2 or the ISSW may be associated with significant underestimates of uncertainty.

Emission characteristics of black carbon in anthropogenic and biomass burning plumes over California during ARCTAS‐CARB 2008

The impact of aerosols on regional air quality and climate necessitates improved understanding of their emission and microphysical properties. The size distributions of black carbon (BC) and light scattering particles (LSP) were measured with a single particle soot photometer on board the NASA DC‐8 aircraft during the ARCTAS mission 2008. Air sampling was made in the air plumes of both urban and forest fire emissions over California during the CARB (California Air Resources Board) phase of the mission. A total of eleven plumes were identified using SO2and CH3CN tracers for fossil fuel (FF) combustion and biomass burning (BB), respectively. The enhancements of BC and LSP in BB plumes were significantly higher compared to those in FF plumes. The average mass concentration of BC in BB plumes was more than twice that in FF plumes. Except for the BC/CO ratio, distinct emission ratios of BC/CO2, BC/CH3CN, CH3CN/CO, and CO/CO2were observed in the plumes from the two sources. Similarly, the microphysical properties of BC and LSP also showed distinct behaviors. The BC count median diameter (CMD) of 115 ± 5 nm in FF plumes was smaller compared to 141 ± 9 nm in the BB plumes. BC aerosols were thickly coated in BB plumes, the average shell/core ratios were 1.47 and 1.24 in BB and FF plumes, respectively. In the total mass of submicron aerosols, organic aerosols constituted about 67% in the FF plumes and 84% in BB plumes. The contribution of sulfate was also significant in the FF plumes.

Size dependence of wet removal of black carbon aerosols during transport from the boundary layer to the free troposphere

Size distributions of black carbon (BC) measured by aircraft over East Asia in spring 2009 were highly correlated with BC transport efficiency in air parcels uplifted from the planetary boundary layer to the free troposphere. The average single‐particle BC mass decreased with decreasing transport efficiency, which suggests that aerosols containing larger BC mass were removed more efficiently. This is the first successful observation of the size‐dependent wet removal of aerosols, qualitatively consistent with the Köhler theory. The size distribution of BC uplifted to the free troposphere with high efficiency was similar to the size distribution of BC in the planetary boundary layer. Conversely, the size distribution of BC uplifted with low efficiency was similar to that of background air in the free troposphere. We conclude that wet removal during upward transport is important in controlling the size distribution of BC in the free troposphere.

Black carbon aerosol characterization in a coastal city in South China using a single particle soot photometer

Abstract Black carbon (BC) is the dominant light-absorbing aerosol component in the atmosphere and plays an important role in atmospheric pollution and climate change. The light-absorbing properties of BC rely on particle size, shape, composition, as well as the BC mixing state with other aerosol components, thus more thorough exploration of BC aerosol characteristics is critical in understanding its atmospheric sources and effects. In this study, a newly-developed Single Particle Soot Photometer (SP2) was deployed in Shenzhen, China, for continuous BC measurements to obtain the important information about size distribution and mixing state of BC under severe air pollution conditions of China. The mean BC mass concentrations were found to be 6.0 and 4.1 μg m−3 at an urban site (UT) in the fall and winter, respectively, while it is much lower (2.6 μg m−3) at a rural site (BG) in the fall. The mass size distributions of BC in volume equivalent diameter (VED) at the three sites showed a similar lognormal pattern, with the peak diameter at BG (222 nm) slightly larger than at the UT (210 nm) site. As to mixing state, the average percentage of internally mixed BC at the UT site was detected to be 40% and 46% in the fall and winter, respectively, while that at the BG site in the fall was only a slightly higher (47%), which implies that fresh local fossil fuel combustions were still significant at this rural site. The analysis of extremely high BC concentrations (>20 μg m−3) at UT indicates that they were a complex of comparable contributions from both local fresh emissions and regional transport under unfavorable meteorology. Other characteristics of BC aerosol and their influencing factors in Shenzhen were also discussed.

Evaluation of a Method for Measurement of the Concentration and Size Distribution of Black Carbon Particles Suspended in Rainwater

We make detailed evaluations of a method of measuring the mass concentration and size distribution of black carbon (BC) particles suspended in water for the purpose of application to rainwater samples. Water samples were aerosolized with an ultrasonic nebulizer. Generated water droplets were dried in order to extract airborne BC particles. The mass of each BC particle was then measured by a Single Particle Soot Photometer (SP2), based on the laser-induced incandescence technique. Under the optimized operating conditions of our measurement system, the overall efficiency of the extraction of BC particles from rainwater was determined to be 11.4% ± 0.83% by mass, resulting in a total uncertainty of about ±20% for the measurement of the BC concentration in rainwater. The change in efficiency due to water-soluble species was found to be negligibly small for rainwater samples analyzed in this study. The determination of the efficiency by using standard BC solutions was necessary at an appropriate frequency because changes in the overall conditions of the system lead to changes in the efficiency in the long term. The size of BC particles in rainwater can be overestimated because of the coagulation of BC particles in the process of extraction by the nebulizer. This effect increased with the increase in BC concentration in rainwater. The effect can be minimized by dilution of rainwater samples by pure water. The volume of a rainwater sample required for BC measurement was less than 5 mL, enabling measurement for weak rain or highly time-resolved measurements during each rain event.