Although black carbon (BC) is one of the key atmospheric particulate components driving climate change and air quality, there is no agreement on the terminology that considers all aspects of specific ...properties, definitions, measurement methods, and related uncertainties. As a result, there is much ambiguity in the scientific literature of measurements and numerical models that refer to BC with different names and based on different properties of the particles, with no clear definition of the terms. The authors present here a recommended terminology to clarify the terms used for BC in atmospheric research, with the goal of establishing unambiguous links between terms, targeted material properties and associated measurement techniques.
Scattering of solar radiation by aerosol particles is highly dependent on relative humidity (RH) as hygroscopic particles take up water with increasing RH. To achieve a better understanding of the ...effect of aerosol hygroscopic growth on light scattering properties and radiative forcing, the aerosol scattering coefficients at RH in the range of 40 to ~ 90 % were measured using a humidified nephelometer system in the Yangtze River Delta of China in March 2013. In addition, the aerosol size distribution and chemical composition were measured. During the observation period, the mean and standard deviation (SD) of enhancement factors at RH = 85 % for the scattering coefficient (f(85 %)), backscattering coefficient (fb(85 %)), and hemispheric backscatter fraction (f beta (85 %)) were 1.58 plus or minus 0.12, 1.25 plus or minus 0.07, and 0.79 plus or minus 0.04, respectively, i.e., aerosol scattering coefficient and backscattering coefficient increased by 58 and 25 % as the RH increased from 40 to 85 %. Concurrently, the aerosol hemispheric backscatter fraction decreased by 21 %. The relative amount of organic matter (OM) or inorganics in PM1 was found to be a main factor determining the magnitude of f(RH). The highest values of f(RH) corresponded to the aerosols with a small fraction of OM, and vice versa. The relative amount of NO3- in fine particles was strongly correlated with f(85 %), which suggests that NO3- played a vital role in aerosol hygroscopic growth during this study. The mass fraction of nitrate also had a close relationship to the curvature of the humidograms; higher mass fractions of nitrate were associated with humidograms that had the least curvature. Aerosol hygroscopic growth caused a 47 % increase in the calculated aerosol direct radiative forcing at 85 % RH, compared to the forcing at 40 % RH.
Long‐term measurements of the light absorption coefficient (babs) obtained with a particle soot absorption photometer (PSAP), babs (PSAP), have been previously reported for Barrow, Alaska, and ...Ny‐Ålesund, Spitsbergen, in the Arctic. However, the effects on babs of other aerosol chemical species coexisting with black carbon (BC) have not been critically evaluated. Furthermore, different mass absorption cross section (MAC) values have been used to convert babs to BC mass concentration (MBC = babs/MAC). We used a continuous soot monitoring system (COSMOS), which uses a heated inlet to remove volatile aerosol compounds, to measure babs (babs (COSMOS)) at these sites during 2012–2015. Field measurements and laboratory experiments have suggested that babs (COSMOS) is affected by about 9% on average by sea‐salt aerosols. MBC values derived by COSMOS (MBC (COSMOS)) using a MAC value obtained by our previous studies agreed to within 9% with elemental carbon concentrations at Barrow measured over 11 months. babs (PSAP) was higher than babs (COSMOS), by 22% at Barrow (PM1) and by 43% at Ny‐Ålesund (PM10), presumably due to the contribution of volatile aerosol species to babs (PSAP). Using babs (COSMOS) as a reference, we derived MBC (PSAP) from babs (PSAP) measured since 1998. We also established the seasonal variations of MBC at these sites. Seasonally averaged MBC (PSAP) decreased at a rate of about 0.55 ± 0.30 ng m−3 yr−1. We also compared MBC (COSMOS) and scaled MBC (PSAP) values with previously reported data and evaluated the degree of inconsistency in the previous data.
Key Points
We evaluated the accuracy of black carbon (BC) measurements at Barrow, Alaska, and Ny‐Ålesund, Spitsbergen, in the Arctic
At Barrow, seasonally averaged BC mass concentrations decreased in winter and summer at a rate of 0.55 ± 0.30 ng m−3 yr−1 during 1998–2015
We established seasonal variations of BC at the two sites and evaluated the causes of the inconsistency of the previously reported data
During summer of 2004, about 2.7 million hectare of boreal forest burned in Alaska, the largest annual area burned on record, and another 3.1 million hectare burned in Canada. This study explores the ...impact of emissions from these fires on light absorbing aerosol concentration levels, aerosol optical depths (AOD), and albedo at the Arctic stations Barrow (Alaska), Alert (Canada), Summit (Greenland), and Zeppelin/Ny Ålesund on Spitsbergen (Norway). The Lagrangian particle dispersion model FLEXPART was run backward from these sites to identify periods that were influenced by forest fire pollution plumes. It is shown that the fires led to enhanced values of particle light absorption coefficients (σap) at all of these sites. Barrow, about 1000 km away from the fires, was affected by several fire pollution plumes, one leading to spectacularly high 3‐hour mean σap values of up to 32 Mm−1, more than the highest values measured in Arctic Haze. AOD measurements for a wavelength of 500 nm saturated but were estimated at above 4–5 units, unprecedented in the station records. Fire plumes were transported through the atmospheric column over Summit continuously for 2 months, during which all measured AOD values were enhanced, with maxima up to 0.4–0.5 units. Equivalent black carbon concentrations at the surface at Summit were up to 600 ng m−3 during two major episodes, and Alert saw at least one event with enhanced σap values. FLEXPART results show that Zeppelin was located in a relatively unaffected part of the Arctic. Nevertheless, there was a 4‐day period with daily mean σap > 0.3 Mm−1, the strongest episode of the summer half year, and enhanced AOD values. Elevated concentrations of the highly source‐specific compound levoglucosan positively confirmed that biomass burning was the source of the aerosols at Zeppelin. In summary, this paper shows that boreal forest fires can lead to elevated concentrations of light absorbing aerosols throughout the entire Arctic. Enhanced AOD values suggest a substantial impact of these plumes on radiation transmission in the Arctic atmosphere. During the passage of the largest fire plume, a pronounced drop of the albedo of the snow was observed at Summit. We suggest that this is due to the deposition of light absorbing particles on the snow, with further potentially important consequences for the Arctic radiation budget.
We synthesised observations of total particle number (CN) concentration from 36 sites around the world. We found that annual mean CN concentrations are typically 300–2000 cm−3 in the marine boundary ...layer and free troposphere (FT) and 1000–10 000 cm−3 in the continental boundary layer (BL). Many sites exhibit pronounced seasonality with summer time concentrations a factor of 2–10 greater than wintertime concentrations. We used these CN observations to evaluate primary and secondary sources of particle number in a global aerosol microphysics model. We found that emissions of primary particles can reasonably reproduce the spatial pattern of observed CN concentration (R2=0.46) but fail to explain the observed seasonal cycle (R2=0.1). The modeled CN concentration in the FT was biased low (normalised mean bias, NMB=−88%) unless a secondary source of particles was included, for example from binary homogeneous nucleation of sulfuric acid and water (NMB=−25%). Simulated CN concentrations in the continental BL were also biased low (NMB=−74%) unless the number emission of anthropogenic primary particles was increased or a mechanism that results in particle formation in the BL was included. We ran a number of simulations where we included an empirical BL nucleation mechanism either using the activation-type mechanism (nucleation rate, J, proportional to gas-phase sulfuric acid concentration to the power one) or kinetic-type mechanism (J proportional to sulfuric acid to the power two) with a range of nucleation coefficients. We found that the seasonal CN cycle observed at continental BL sites was better simulated by BL particle formation (R2=0.3) than by increasing the number emission from primary anthropogenic sources (R2=0.18). The nucleation constants that resulted in best overall match between model and observed CN concentrations were consistent with values derived in previous studies from detailed case studies at individual sites. In our model, kinetic and activation-type nucleation parameterizations gave similar agreement with observed monthly mean CN concentrations.
Between June 2006 and September 2009, an instrumented light aircraft measured over 400 vertical profiles of aerosol and trace gas properties over eastern and central Illinois. The primary objectives ...of this program were to (1) measure the in situ aerosol properties and determine their vertical and temporal variability and (2) relate these aircraft measurements to concurrent surface and satellite measurements. The primary profile location was within 15 km of the NOAA/ESRL surface aerosol monitoring station near Bondville, Illinois. Identical instruments at the surface and on the aircraft ensured that the data from both platforms would be directly comparable and permitted a determination of how representative surface aerosol properties were of the lower column. Aircraft profiles were also conducted occasionally at two other nearby locations to increase the frequency of A-Train satellite underflights for the purpose of comparing in situ and satellite-retrieved aerosol data. Measurements of aerosol properties conducted at low relative humidity over the Bondville site compare well with the analogous surface aerosol data and do not indicate any major sampling issues or that the aerosol is radically different at the surface compared with the lowest flyby altitude of ~ 240 m above ground level. Statistical analyses of the in situ vertical profile data indicate that aerosol light scattering and absorption (related to aerosol amount) decreases substantially with increasing altitude. Parameters related to the nature of the aerosol (e.g., single-scattering albedo, Ångström exponent, etc.), however, are relatively constant throughout the mixed layer, and do not vary as much as the aerosol amount throughout the profile. While individual profiles often showed more variability, the median in situ single-scattering albedo was 0.93–0.95 for all sampled altitudes. Several parameters (e.g., submicrometer scattering fraction, hemispheric backscattering fraction, and scattering Ångström exponent) suggest that the fraction of smaller particles in the aerosol is larger near the surface than at high altitudes. The observed dependence of scattering on size, wavelength, angular integration range, and relative humidity, together with the spectral dependence of absorption, show that the aerosol at higher altitudes is larger, less hygroscopic, and more strongly absorbing at shorter wavelengths, suggesting an increased contribution from dust or organic aerosols. The aerosol profiles show significant differences among seasons. The largest amounts of aerosol (as determined by median light extinction profile measurements) throughout most of the sampled column were observed during summer, with the lowest amounts in the winter and intermediate values in the spring and fall. The highest three profile levels (3.1, 3.7, 4.6 km), however, showed larger median extinction values in the spring, which could reflect long-range transport of dust or smoke aerosols. The aerosols in the mixed layer were darkest (i.e., lowest single-scattering albedo) in the fall, in agreement with surface measurements at Bondville and other continental sites in the US. In situ profiles of aerosol radiative forcing efficiency showed little seasonal or vertical variability. Underflights of the CALIPSO satellite show reasonable agreement in a majority of retrieved profiles between aircraft-measured extinction at 532 nm (adjusted to ambient relative humidity) and CALIPSO-retrieved extinction, and suggest that routine aircraft profiling programs can be used to better understand and validate satellite retrieval algorithms. CALIPSO tended to overestimate the aerosol extinction at this location in some boundary layer flight segments when scattered or broken clouds were present, which could be related to problems with CALIPSO cloud screening methods. The in situ aircraft-collected aerosol data suggest extinction thresholds for the likelihood of aerosol layers being detected by the CALIOP lidar. In this study, aerosol layers with light extinction (532 nm) values > 50 Mm−1 were detected by CALIPSO ~ 95% of the time, while aerosol layers with extinction values lower than 10 Mm−1 had a detection efficiency of < 2%. For all collocated comparison cases, a 50% probability of detection falls at an in situ extinction level of 20–25 Mm−1. These statistical data offer guidance as to the likelihood of CALIPSO's ability to retrieve aerosol extinction at various locations around the globe.
The distribution of black carbon (BC) in the atmosphere and the deposition of BC on snow surfaces since pre-industrial time until present are modelled with the Oslo CTM2 model. The model results are ...compared with observations including recent measurements of BC in snow in the Arctic. The global mean burden of BC from fossil fuel and biofuel sources increased during two periods. The first period, until 1920, is related to increases in emissions in North America and Europe, and the last period after 1970 are related mainly to increasing emissions in East Asia. Although the global burden of BC from fossil fuel and biofuel increases, in the Arctic the maximum atmospheric BC burden as well as in the snow was reached in 1960s, with a slight reduction thereafter. The global mean burden of BC from open biomass burning sources has not changed significantly since 1900. With current inventories of emissions from open biomass sources, the modelled burden of BC in snow and in the atmosphere north of 65° N is small compared to the BC burden of fossil fuel and biofuel origin. From the concentration changes radiative forcing time series due to the direct aerosol effect as well as the snow-albedo effect is calculated for BC from fossil fuel and biofuel. The calculated radiative forcing in 2000 for the direct aerosol effect is 0.35 W m−2 and for the snow-albedo effect 0.016 W m−2 in this study. Due to a southward shift in the emissions there is an increase in the lifetime of BC as well as an increase in normalized radiative forcing, giving a change in forcing per unit of emissions of 26 % since 1950.
An accurate but simple quantification of the fraction of aerosol particles that can act as cloud condensation nuclei (CCN) is needed for implementation in large-scale models. Data on aerosol size ...distribution, chemical composition, and CCN concentration from six different locations have been analyzed to explore the extent to which simple assumptions of composition and mixing state of the organic fraction can reproduce measured CCN number concentrations. Fresher pollution aerosol as encountered in Riverside, CA, and the ship channel in Houston, TX, cannot be represented without knowledge of more complex (size-resolved) composition. For aerosol that has experienced processing (Mexico City, Holme Moss (UK), Point Reyes (CA), and Chebogue Point (Canada)), CCN can be predicted within a factor of two assuming either externally or internally mixed soluble organics although these simplified compositions/mixing states might not represent the actual properties of ambient aerosol populations, in agreement with many previous CCN studies in the literature. Under typical conditions, a factor of two uncertainty in CCN concentration due to composition assumptions translates to an uncertainty of ~15% in cloud drop concentration, which might be adequate for large-scale models given the much larger uncertainty in cloudiness.
Mobility particle size spectrometers often referred to as DMPS (Differential Mobility Particle Sizers) or SMPS (Scanning Mobility Particle Sizers) have found a wide range of applications in ...atmospheric aerosol research. However, comparability of measurements conducted world-wide is hampered by lack of generally accepted technical standards and guidelines with respect to the instrumental set-up, measurement mode, data evaluation as well as quality control. Technical standards were developed for a minimum requirement of mobility size spectrometry to perform long-term atmospheric aerosol measurements. Technical recommendations include continuous monitoring of flow rates, temperature, pressure, and relative humidity for the sheath and sample air in the differential mobility analyzer. We compared commercial and custom-made inversion routines to calculate the particle number size distributions from the measured electrical mobility distribution. All inversion routines are comparable within few per cent uncertainty for a given set of raw data. Furthermore, this work summarizes the results from several instrument intercomparison workshops conducted within the European infrastructure project EUSAAR (European Supersites for Atmospheric Aerosol Research) and ACTRIS (Aerosols, Clouds, and Trace gases Research InfraStructure Network) to determine present uncertainties especially of custom-built mobility particle size spectrometers. Under controlled laboratory conditions, the particle number size distributions from 20 to 200 nm determined by mobility particle size spectrometers of different design are within an uncertainty range of around ±10% after correcting internal particle losses, while below and above this size range the discrepancies increased. For particles larger than 200 nm, the uncertainty range increased to 30%, which could not be explained. The network reference mobility spectrometers with identical design agreed within ±4% in the peak particle number concentration when all settings were done carefully. The consistency of these reference instruments to the total particle number concentration was demonstrated to be less than 5%. Additionally, a new data structure for particle number size distributions was introduced to store and disseminate the data at EMEP (European Monitoring and Evaluation Program). This structure contains three levels: raw data, processed data, and final particle size distributions. Importantly, we recommend reporting raw measurements including all relevant instrument parameters as well as a complete documentation on all data transformation and correction steps. These technical and data structure standards aim to enhance the quality of long-term size distribution measurements, their comparability between different networks and sites, and their transparency and traceability back to raw data.
Values for Mie‐equivalent aerosol asymmetry parameter (g) were derived using a variety of methods from the large suite of measurements (in situ and remote from surface and aircraft) made in Oklahoma ...during the 2003 aerosol Intensive Operations Period (IOP). Median values derived for dry asymmetry parameter at 550 nm ranged between 0.55 and 0.63 over all instruments and for all derivation methods, with the exception of one instrument which did not measure over the full size range of optically important aerosol. Median values for the “wet” asymmetry parameter (i.e., asymmetry parameter at humidity conditions closer to ambient) were between 0.59 and 0.72. Values for g derived for surface and airborne in situ measurements were highly correlated, but in situ and remote sensing measurements both at the surface and aloft did not agree as well because of vertical inhomogeneity of the aerosol. Radiative forcing calculations suggest that a 10% decrease in g would result in a 19% reduction in top of atmosphere radiative forcing for the conditions observed during the IOP. Comparison of the different methods for deriving g suggests that in computing the asymmetry parameter, aerosol size is the most important parameter to measure; composition is less important except for how it influences the hygroscopic growth (i.e., size) of particles.
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