scholarly journals Estimates of mass absorption cross sections of black carbon for filter-based absorption photometers in the Arctic

2021 ◽  
Author(s):  
Sho Ohata ◽  
Tatsuhiro Mori ◽  
Yutaka Kondo ◽  
Sangeeta Sharma ◽  
Antti Hyvärinen ◽  
...  

Abstract. Long-term measurements of atmospheric mass concentrations of black carbon (BC) are needed to investigate changes in its emission, transport, and deposition. However, depending on instrumentation, parameters related to BC such as aerosol absorption coefficient (babs) have been measured instead. Most ground-based measurements of babs in the Arctic have been made by filter-based absorption photometers, including particle soot absorption photometers (PSAP), continuous light absorption photometer (CLAP), Aethalometers, and multi-angle absorption photometers (MAAP). The measured babs can be converted to mass concentrations of BC (MBC) by assuming the value of the mass absorption cross section (MAC; MBC = babs/MAC). However, the accuracy of conversion of babs to MBC has not been adequately assessed. Here, we introduce a systematic method for deriving MAC values from babs measured by these instruments and independently measured MBC. In this method, MBC was measured with a filter-based absorption photometer with a heated inlet (COSMOS). COSMOS-derived MBC (MBC (COSMOS)) is traceable to a rigorously calibrated single particle soot photometer (SP2) and the absolute accuracy of MBC (COSMOS) has been demonstrated previously to be about 15 % in Asia and the Arctic. The necessary conditions for application of this method are a high correlation of the measured babs with independently measured MBC, and long-term stability of the regression slope, which is denoted as MACcor (MAC derived from the correlation). In general, babs–MBC (COSMOS) correlations were high (r2 = 0.76–0.95 for hourly data) at Alert in Canada, Ny-Ålesund in Svalbard, Barrow in Alaska, Pallastunturi in Finland, and Fukue in Japan, and stable for up to 10 years. We successfully estimated MACcor values (10.6–15.2 m2 g−1 at a wavelength of 550 nm) for these instruments and these MACcor values can be used to obtain error-constrained estimates of MBC from babs measured at these sites even in the past, when COSMOS measurements were not made. Because the absolute values of MBC in these Arctic sites estimated by this method are consistent with each other, they are applicable to the study of spatial and temporal variation of MBC in the Arctic and to evaluation of the performance of numerical model calculations.

2020 ◽  
Author(s):  
Sho Ohata ◽  
Tatsuhiro Mori ◽  
Yutaka Kondo ◽  
Sangeeta Sharma ◽  
Antti Hyvärinen ◽  
...  

Abstract. Long-term measurements of black carbon (BC) are warranted for investigating changes in its emission, transport, and deposition. However, depending on instrumentation, parameters related to BC such as aerosol absorption coefficient (babs) have been measured instead. Most ground-based measurements of babs in the Arctic have been made by filter-based absorption photometers, including multi-angle absorption photometers (MAAP), particle soot absorption photometers (PSAP), continuous light absorption photometer (CLAP), and Aethalometers. The measured babs can be converted to atmospheric mass concentrations of BC (MBC) by assuming the value of the mass absorption cross section (MAC = babs/MBC). However, the accuracy of conversion of babs to MBC has not been adequately assessed. Here, we introduce a systematic method for deriving MAC values from babs measured by these instruments and independently measured MBC. In this method, MBC was measured with a filter-based absorption photometer with a heated inlet (COSMOS). COSMOS-derived MBC (MBC (COSMOS)) is traceable to a rigorously calibrated single particle soot photometer (SP2) and the absolute accuracy of MBC (COSMOS) has been demonstrated previously to be about 15 % in Asia and the Arctic. The necessary conditions for application of this method are a high correlation of the measured babs with independently measured MBC, and long-term stability of the correlation slope, which represents the MAC. In general, babs – MBC (COSMOS) correlations were high (r2 = 0.84–0.96 for hourly data) at Fukue in Japan, Barrow in Alaska, Ny-Ålesund in Svalbard, Pallastunturi in Finland, and Alert in Canada, and stable up to for 10 years. We successfully estimated MAC values (11.0–15.2 m2 g−1 at a wavelength of 550 nm) for these instruments and these MAC values can be used to obtain error-constrained estimates of MBC from babs measured at these sites even in the past, when COSMOS measurements were not made. Because the absolute values of MBC in these Arctic sites estimated by this method are consistent with each other, they are applicable to study spatial and temporal variation of MBC and to evaluate performance of numerical model calculations.


2010 ◽  
Vol 10 (1) ◽  
pp. 219-237 ◽  
Author(s):  
R. Subramanian ◽  
G. L. Kok ◽  
D. Baumgardner ◽  
A. Clarke ◽  
Y. Shinozuka ◽  
...  

Abstract. A single particle soot photometer (SP2) was operated on the NCAR C-130 during the MIRAGE campaign (part of MILAGRO), sampling black carbon (BC) over Mexico. The highest BC concentrations were measured over Mexico City (sometimes as much as 2 μg/m3) and over hill-fires to the south of the city. The age of plumes outside of Mexico City was determined using a combination of HYSPLIT trajectories, WRF-FLEXPART modeling and CMET balloon tracks. As expected, older, diluted air masses had lower BC concentrations. A comparison of carbon monoxide (CO) and BC suggests a CO background of around 65 ppbv, and a background-corrected BC/COnet ratio of 2.89±0.89 (ng/m3-STP)/ppbv (average ± standard deviation). This ratio is similar for fresh emissions over Mexico City, as well as for aged airmasses. Comparison of light absorption measured with a particle soot absorption photometer (PSAP) and the SP2 BC suggests a BC mass-normalized absorption cross-section (MAC) of 10.9±2.1 m2/g at 660 nm (or 13.1 m2/g @ 550 nm, assuming MAC is inversely dependent on wavelength). This appears independent of aging and similar to the expected absorption cross-section for aged BC, but values, particularly in fresh emissions, could be biased high due to instrument artifacts. SP2-derived BC coating indicators show a prominent thinly-coated BC mode over the Mexico City Metropolitan Area (MCMA), while older air masses show both thinly-coated and thickly-coated BC. Some 2-day-old plumes do not show a prominent thickly-coated BC mode, possibly due to preferential wet scavenging of the likely-hydrophilic thickly-coated BC.


2010 ◽  
Vol 10 (5) ◽  
pp. 12133-12184 ◽  
Author(s):  
D. Hirdman ◽  
J. F. Burkhart ◽  
H. Sodemann ◽  
S. Eckhardt ◽  
A. Jefferson ◽  
...  

Abstract. As a part of the IPY project POLARCAT (Polar Study using Aircraft, Remote Sensing, Surface Measurements and Models, of Climate, Chemistry, Aerosols and Transport) and building on previous work (Hirdman et al., 2010), this paper studies the long-term trends of both atmospheric transport as well as equivalent black carbon (EBC) and sulphate for the three Arctic stations Alert, Barrow and Zeppelin. We find a general downward trend in the measured EBC concentrations at all three stations, with a decrease of −2.1±0.4 ng m−3 yr−1 (for the years 1989–2008) and −1.4±0.8 ng m−3 yr−1 (2002–2009) at Alert and Zeppelin respectively. The decrease at Barrow is, however, not statistically significant. The measured sulphate concentrations show a decreasing trend at Alert and Zeppelin of −15±3 ng m−3 yr−1 (1985–2006) and −1.3±1.2 ng m−3 yr−1 (1990–2008) respectively, while the trend at Barrow is unclear. To reveal the influence of different source regions on these trends, we used a cluster analysis of the output of the Lagrangian particle dispersion model FLEXPART run backward in time from the measurement stations. We have investigated to what extent variations in the atmospheric circulation, expressed as variations in the frequencies of the transport from four source regions with different emission rates, can explain the long-term trends in EBC and sulphate measured at these stations. We find that the long-term trend in the atmospheric circulation can only explain a minor fraction of the overall downward trend seen in the measurements of EBC (0.3–7.2%) and sulphate (0.3–5.3%) at the Arctic stations. The changes in emissions are dominant in explaining the trends. We find that the highest EBC and sulphate concentrations are associated with transport from Northern Eurasia and decreasing emissions in this region drive the downward trends. Northern Eurasia (cluster: NE, WNE and ENE) is the dominant emission source at all Arctic stations for both EBC and sulphate during most seasons. In wintertime, there are indications that the EBC emissions from the eastern parts of Northern Eurasia (ENE cluster) have increased over the last decade.


2021 ◽  
Author(s):  
Sho Ohata ◽  
Makoto Koike ◽  
Atsushi Yoshida ◽  
Nobuhiro Moteki ◽  
Kouji Adachi ◽  
...  

Abstract. Vertical profiles of the mass concentration of black carbon (BC) were measured at altitudes up to 5 km during the PAMARCMiP aircraft-based field experiment conducted around the Northern Greenland Sea (Fram Strait) during March and April 2018, with operation base Station Nord (81.6° N, 16.7° W). Median BC mass concentrations in individual altitude ranges were 7–18 ng m–3 at standard temperature and pressure at altitudes below 4.5 km. These concentrations were systematically lower than previous observations in the Arctic in spring conducted by ARCTAS-A in 2008 and NETCARE in 2015 and similar to those observed during HIPPO3 in 2010. Column amounts of BC for altitudes below 5 km in the Arctic (> 66.5° N, COLBC), observed during the ARCTAS-A and NETCARE experiments were higher by factors of 4.2 and 2.7, respectively, than those of the PAMARCMiP experiment. These differences could not be explained solely by the different locations of the experiments. The year-to-year variation of COLBC values generally corresponded to that of biomass burning activities in northern high latitudes over western and eastern Eurasia. Furthermore, numerical model simulations estimated the year-to-year variation of contributions from anthropogenic sources to be smaller than 30–40 %. These results suggest that the year-to-year variation of biomass burning activities likely affected BC amounts in the Arctic troposphere in spring, at least in the years examined in this study. The year-to-year variations in BC mass concentrations were also observed at the surface at high Arctic sites Ny-Ålesund and Barrow, although their magnitudes were slightly lower than those in COLBC. Numerical model simulations in general successfully reproduced the observed COLBC values for PAMARCMiP and HIPPO3 (within a factor of 2), whereas they markedly underestimated the values for ARCTAS-A and NETCARE by factors of 3.7–5.8 and 3.3–5.0, respectively. Because anthropogenic contributions account for nearly all of the COLBC (82–98 %) in PAMARCMiP and HIPPO3, the good agreements between the observations and calculations for these two experiments suggest that anthropogenic contributions were generally well reproduced. However, the significant underestimations of COLBC for ARCTAS-A and NETCARE suggest that biomass burning contributions were underestimated. In this study, we also investigated plumes with enhanced BC mass concentrations, which were affected by biomass burning emissions, observed at 5 km altitude. Interestingly, the mass-averaged diameter of BC (core) and the shell-to-core diameter ratio of BC-containing particles in the plumes were generally not very different from those in other air sampled, which were considered to be mostly aged anthropogenic BC. These observations provide useful bases to evaluate numerical model simulations of the BC radiative effect in the Arctic region in spring.


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