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Long-term measurements of the mass concentration of black carbon (BC) in the atmosphere (MBC) with well-constrained accuracy are indispensable to quantify its emission, transport, and deposition. The aerosol light absorption coefficient (babs), usually measured by a filter-based absorption photometer, including an Aethalometer (AE), is often used to estimate MBC. The measured babs is converted to MBC by assuming a value for the mass absorption cross section (MAC). Previously, we derived the MAC for AE (MAC (AE)) from measured babs and independently measured MBC values at two sites in the Arctic. MBC was measured with a filter-based absorption photometer with a heated inlet (COSMOS). The accuracy of the COSMOS-derived MBC (MBC (COSMOS)) was within about 15%. Here, we obtained additional MAC (AE) measurements to improve understanding of its variability and uncertainty. We measured babs (AE) and MBC (COSMOS) at Alert (2018–2020), Barrow (2012–2022), Ny-Ålesund (2012–2019), and Pallas (2019–2022). At Pallas, we also obtained four-wavelength photoacoustic aerosol absorption spectrometer (PAAS-4λ) measurements of babs. babs (AE) and MBC (COSMOS) were tightly correlated; the average MAC (AE) at the four sites was 11.4 ± 1.2 m2 g−1 (mean ± 1σ) at 590 nm and 7.76 ± 0.73 m2 g−1 at 880 nm. The spatial variability of MAC (AE) was about 11% (1σ), and its year-to-year variability was about 18%. We compared MAC (AE) in the Arctic with values at mid-latitudes, measured by previous studies, and with values obtained by using other types of filter-based absorption photometer, and PAAS-4λ. Copyright © 2024 American Association for Aerosol Research [ABSTRACT FROM AUTHOR]

Black carbon (BC) particles in the Arctic contribute to rapid warming of the Arctic by heating the atmosphere and snow and ice surfaces. Understanding the source contributions to Arctic BC is therefore important, but they are not well understood, especially those for atmospheric and snow radiative effects. Here we estimate simultaneously the source contributions of Arctic BC to near-surface and vertically integrated atmospheric BC mass concentrations (MBC_SRF and MBC_COL), BC deposition flux (MBC_DEP), and BC radiative effects at the top of the atmosphere and snow surface (RE BC_TOA and RE BC_SNOW) and show that the source contributions to these five variables are highly different. In our estimates, Siberia makes the largest contribution to MBC_SRF , MBC_DEP , and RE BC_SNOW in the Arctic (defined as >70 ∘ N), accounting for 70 %, 53 %, and 41 %, respectively. In contrast, Asia's contributions to MBC_COL and RE BC_TOA are largest, accounting for 37 % and 43 %, respectively. In addition, the contributions of biomass burning sources are larger (29 %–35 %) to MBC_DEP , RE BC_TOA , and RE BC_SNOW , which are highest from late spring to summer, and smaller (5.9 %–17 %) to MBC_SRF and MBC_COL , whose concentrations are highest from winter to spring. These differences in source contributions to these five variables are due to seasonal variations in BC emission, transport, and removal processes and solar radiation, as well as to differences in radiative effect efficiency (radiative effect per unit BC mass) among sources. Radiative effect efficiency varies by a factor of up to 4 among sources (1471–5326 W g -1) depending on lifetimes, mixing states, and heights of BC and seasonal variations of emissions and solar radiation. As a result, source contributions to radiative effects and mass concentrations (i.e., RE BC_TOA and MBC_COL , respectively) are substantially different. The results of this study demonstrate the importance of considering differences in the source contributions of Arctic BC among mass concentrations, deposition, and atmospheric and snow radiative effects for accurate understanding of Arctic BC and its climate impacts. [ABSTRACT FROM AUTHOR]

Emissions of black carbon (BC) particles from anthropogenic and natural sources contribute to climate change and human health impacts. Therefore, they need to be accurately quantified to develop an effective mitigation strategy. Although the spread of the emission flux estimates for China have recently narrowed under the constraints of atmospheric observations, consensus has not been reached regarding the dominant emission sector. Here, we quantified the contribution of the residential sector, as 64% (44–82%) in 2019, using the response of the observed atmospheric concentration in the outflowing air during Feb–Mar 2020, with the prevalence of the COVID-19 pandemic and restricted human activities over China. In detail, the BC emission fluxes, estimated after removing effects from meteorological variability, dropped only slightly (− 18%) during Feb–Mar 2020 from the levels in the previous year for selected air masses of Chinese origin, suggesting the contributions from the transport and industry sectors (36%) were smaller than the rest from the residential sector (64%). Carbon monoxide (CO) behaved differently, with larger emission reductions (− 35%) in the period Feb–Mar 2020, suggesting dominance of non-residential (i.e., transport and industry) sectors, which contributed 70% (48–100%) emission during 2019. The estimated BC/CO emission ratio for these sectors will help to further constrain bottom-up emission inventories. We comprehensively provide a clear scientific evidence supporting mitigation policies targeting reduction in residential BC emissions from China by demonstrating the economic feasibility using marginal abatement cost curves. [ABSTRACT FROM AUTHOR]

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 (PSAPs), continuous light absorption photometers (CLAPs), Aethalometers, and multi-angle absorption photometers (MAAPs). 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 MAC cor (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 (NOAA Barrow Observatory) in Alaska, Pallastunturi in Finland, and Fukue in Japan and stable for up to 10 years. We successfully estimated MAC cor values (10.8–15.1 m 2 g -1 at a wavelength of 550 nm for hourly data) for these instruments, and these MAC cor 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 at these Arctic sites estimated by this method are consistent with each other, they are applicable to the study of spatial and temporal variation in MBC in the Arctic and to evaluation of the performance of numerical model calculations. [ABSTRACT FROM AUTHOR]

A long-term, robust observational record of atmospheric black carbon (BC) concentrations at Fukue Island for 2009–2019 was produced by unifying the data from a continuous soot monitoring system (COSMOS) and a Multi-Angle Absorption Photometer (MAAP). This record was then used to analyze emission trends from China. We identified a rapid reduction in BC concentrations of (-5.8±1.5) % yr -1 or - 48 % from 2010 to 2018. We concluded that an emission change of (-5.3±0.7) % yr -1 , related to changes in China of as much as -4.6 % yr -1 , was the main underlying driver. This evaluation was made after correcting for the interannual meteorological variability (IAV) by using the regional atmospheric chemistry model simulations from the Weather Research and Forecasting (WRF) and Community Multiscale Air Quality (CMAQ) models (collectively WRF/CMAQ) with the constant emissions. This resolves the current fundamental disagreements about the sign of the BC emissions trend from China over the past decade as assessed from bottom-up emission inventories. Our analysis supports inventories reflecting the governmental clean air actions after 2010 (e.g., MEIC1.3, ECLIPSE versions 5a and 6b, and the Regional Emission inventory in ASia (REAS) version 3.1) and recommends revisions to those that do not (e.g., Community Emissions Data System – CEDS). Our estimated emission trends were fairly uniform across seasons but diverse among air mass origins. Stronger BC reductions, accompanied by a reduction in carbon monoxide (CO) emissions, occurred in regions of south-central East China, while weaker BC reductions occurred in north-central East China and northeastern China. Prior to 2017, the BC and CO emissions trends were both unexpectedly positive in northeastern China during winter months, which possibly influenced the climate at higher latitudes. The pace of the estimated emissions reduction over China surpasses the Shared Socioeconomic Pathways (SSPs with reference to SSP1, specifically) scenarios for 2015–2030, which suggests highly successful emission control policies. At Fukue Island, the BC fraction of fine particulate matter (PM 2.5) also steadily decreased over the last decade. This suggests that reductions in BC emissions started without significant delay when compared to other pollutants such as NOx and SO2 , which are among the key precursors of scattering PM 2.5. [ABSTRACT FROM AUTHOR]

Long-term measurements of black carbon (BC) aerosols by filter-based absorption photometers with a heated inlet (COSMOS) in different regions have been useful in elucidating spatial variations and radiative impacts of BC. Evaluations of mass concentrations of BC (MBC) measured by the COSMOS have been made by our previous studies through comparisons with other measurement techniques. However, how variations in the microphysical properties of BC and the co-existing light scattering aerosols affect the COSMOS measurements should be evaluated in more detail. In this study, we assessed these potential effects under various field environments in the Arctic and in the East Asia. From the slopes of the correlation plots between the MBC values measured by the COSMOS and a single-particle soot photometer, the average accuracy of the COSMOS was estimated as ∼10% in the MBC range 1–3000 ng m−3. On an hourly basis, the estimated sensitivity of the COSMOS MBC values to the changes in the BC size distributions was less than 10%, within the typical variabilities of BC size at individual observation sites. The COSMOS measurements depended little on the mixing states of BC and the concentrations of co-existing light scattering aerosols, except in the maritime air masses of East Asia, where the relative abundance of sea salt to BC was very high. The MBC measured by COSMOS also well agreed with elemental carbon measurements. Our results demonstrate the high reliability of COSMOS measurements under various environments. Copyright © 2019 American Association for Aerosol Research [ABSTRACT FROM AUTHOR]

Aerosol particles can contribute to the Arctic amplification (AA) by direct and indirect radiative effects. Specifically, black carbon (BC) in the atmosphere, and when deposited on snow and sea ice, has a positive warming effect on the top-of-atmosphere (TOA) radiation balance during the polar day. Current climate models, however, are still struggling to reproduce Arctic aerosol conditions. We present an evaluation study with the global aerosol-climate model ECHAM6.3-HAM2.3 to examine emission-related uncertainties in the BC distribution and the direct radiative effect of BC. The model results are comprehensively compared against the latest ground and airborne aerosol observations for the period 2005–2017, with a focus on BC. Four different setups of air pollution emissions are tested. The simulations in general match well with the observed amount and temporal variability in near-surface BC in the Arctic. Using actual daily instead of fixed biomass burning emissions is crucial for reproducing individual pollution events but has only a small influence on the seasonal cycle of BC. Compared with commonly used fixed anthropogenic emissions for the year 2000, an up-to-date inventory with transient air pollution emissions results in up to a 30 % higher annual BC burden locally. This causes a higher annual mean all-sky net direct radiative effect of BC of over 0.1 W m -2 at the top of the atmosphere over the Arctic region (60–90 ∘ N), being locally more than 0.2 W m -2 over the eastern Arctic Ocean. We estimate BC in the Arctic as leading to an annual net gain of 0.5 W m -2 averaged over the Arctic region but to a local gain of up to 0.8 W m -2 by the direct radiative effect of atmospheric BC plus the effect by the BC-in-snow albedo reduction. Long-range transport is identified as one of the main sources of uncertainties for ECHAM6.3-HAM2.3, leading to an overestimation of BC in atmospheric layers above 500 hPa, especially in summer. This is related to a misrepresentation in wet removal in one identified case at least, which was observed during the ARCTAS (Arctic Research of the Composition of the Troposphere from Aircraft and Satellites) summer aircraft campaign. Overall, the current model version has significantly improved since previous intercomparison studies and now performs better than the multi-model average in the Aerosol Comparisons between Observation and Models (AEROCOM) initiative in terms of the spatial and temporal distribution of Arctic BC. [ABSTRACT FROM AUTHOR]

We 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 little during their growth into cloud droplets under supersaturation of water vapor. Using our improved system, we measured the size distributions of BC particles simultaneously in air and rainwater in Tokyo during summer 2014. We observed that the size distributions of BC particles in rainwater shifted to larger sizes compared with those observed in ambient air, indicating that larger BC particles in air were removed more efficiently by precipitation. Copyright © 2016 American Association for Aerosol Research [ABSTRACT FROM AUTHOR]

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 measured mass concentration of BC in sample water after long-term storage were about ±25% and ±35%, respectively. We tested the method by analyzing rainwater and surface snow samples collected in Okinawa and Sapporo, respectively. The measured number size distributions of BC in these samples showed negligible contributions of BC particles larger than 300 nm to the total number of BC particles. A dominant fraction of BC mass in these samples was observed in the diameter range 100–500 nm. Copyright 2013 American Association for Aerosol Research [ABSTRACT FROM AUTHOR]

Reducing uncertainties associated with measurements of black carbon (BC) particles is critical for improved quantification of their impacts on climate and health. We compared BC measurements using a continuous soot-monitoring system (COSMOS) and a multi-angle absorption photometer (MAAP) to assess their uncertainties. We found that measurements by COSMOS and MAAP instruments correlate strongly to each other, and their hourly ratio showed minimal temporal variations, but the MAAP values were systematically higher by a factor of 1.56 ± 0.19 (1σ), based on simultaneous observations on Fukue, a remote island in Japan, for about a year. This factor was almost independent of the air mass origins and seasons. Measurements in central Tokyo for about 2 months also yielded a similar relationship, with a systematic difference factor of ∼1.8. It is likely that the systematic differences are caused by differences in the conditions/protocols in the thermal/optical BC determinations used for calibration of each optical instrument. Based on results from the COSMOS instrument calibrated using an elemental carbon and organic carbon analyzer with thermal/optical transmittance correction, the MAAP absorption cross section (6.6 m2 g−1) needs to be systematically increased to 10.3 m2 g−1 at 639 nm for Fukue when b abs values derived from the built-in software are used. Small temporal fluctuations in the ratios of MAAP-derived BC to COSMOS-derived BC were possibly caused by humidity effects and temporal variations in the optical properties of the measured particles. For MAAP, we also found that low filter-transmittance (0.2–0.5) could either increase or decrease the BC reading. The current best recommendations with the MAAP instrument are to use an increased cross section, to use data with high filter-transmittance (>0.5) only, and to control humidity. Copyright 2012 American Association for Aerosol Research [ABSTRACT FROM AUTHOR]

We used a single-particle soot photometer (SP2) to measure the mass of individual black carbon (BC) particles down to ∼ 0.5 fg by means of laser-induced incandescence with an intra-cavity, continuous-wave laser. The incandescence of nine different types of BC samples was investigated to provide a physical basis for choosing appropriate BC materials for SP2 calibration. We estimated the vaporization temperatures of these BC samples from the spectral dependence of incandescence at the limit of the small size parameter x, for which spectral dependence of emissivity is known a priori. The vaporization temperatures differed by less than 2.2% among the samples. For the x < 1 regime of particle size, the peak amplitude of the incandescence signal measured by the SP2 was linearly proportional to the particle mass. The slopes of such linear proportionality were positively correlated with | (m2-1)/(m2+2)|, where the m is the complex refractive index of the BC particle. For particles in which x > 1, the rate of increase in the peak amplitude of the incandescence signal with increasing particle mass was negatively correlated with the compactness of particle shape, consistent with the theoretical prediction of emissivity, which accounts for particle shape. The incandescence-BC mass relationships were similar between fullerene soot and ambient soot sampled in Tokyo, thus suggesting that fullerene soot is a suitable calibration standard for SP2 measurements of ambient soot. [ABSTRACT FROM AUTHOR]

Abstract: We demonstrate a new method to measure refractive indices m of small nonspherical particles by simultaneous measurement of particle volume and light-scattering cross section. In contrast to traditional methods, this method can suppress uncertainties due to unknown particle shape. As demonstration of the method, laboratory experiments using an aerosol particle mass analyzer (APM) and single-particle soot photometer (SP2) have been conducted to determine the refractive indices of seven types of commercial black carbon particles and ambient soot at 1064nm wavelength. Difference in measured |(m 2−1)/(m 2+2)| values among the seven commercial black carbon samples is consistent with the difference in their crystalline structures identified by a transmission electron microscope. The complex refractive index m=(n, k) of ambient soot particles in Tokyo urban area was determined to be m=(2.26±0.13, 1.26±0.13). [Copyright &y& Elsevier]

Because of the increased temporal and spatial resolutions of the sensors onboard recently launched satellites, satellite-based surface aerosol concentration, which is usually estimated from the aerosol optical depth (AOD), is expected to become a strategic tool for air quality studies in the future. By further exploring the relationships of aerosol concentrations and their optical properties using ground observations, the accuracies of these products can be improved. Here, we analyzed collocated observations of surface mass concentrations of fine particulate matter (PM2.5) and black carbon (BC), as well as columnar aerosol optical properties from a sky radiometer and aerosol extinction profiles obtained by multi-axis differential optical absorption spectroscopy (MAX-DOAS), during the 2019–2020 period. We focused the analyses on a daily scale, emphasizing the role of the ultraviolet (UV) spectral region. Generally, the correlation between the AOD of the fine fraction (i.e., fAOD) and the PM2.5 surface concentration was moderately strong, regardless of considerations of boundary layer humidity and altitude. In contrast, the fAOD of the partial column below 1 km, which was obtained by combining sky radiometer and MAX-DOAS retrievals, better reproduced the variability of the PM2.5 and resulted in a linear relationship. In the same manner, we demonstrated that the absorption AOD of the fine fraction (fAAOD) of the partial column was related to the variability of the BC concentration. Analogous analyses based on aerosol products from the Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2) confirmed these findings and highlighted the importance of the shape of the aerosol profile. Overall, our results indicated a remarkable consistency among the retrieved datasets, and between the datasets and MERRA-2 products. These results confirmed the well-known sensitivity to aerosol absorption in the UV spectral region; they also highlighted the efficacy of combined MAX-DOAS and sky radiometer observations. [ABSTRACT FROM AUTHOR]

Abstract: The sectoral and regional contributions from northern hemisphere anthropogenic and biomass burning emission sectors to black carbon (BC) distributions over the continental United States (CONUS) in summer 2008 are studied using the Sulfur Transport and dEposition Model (STEM). North American (NA) emissions heavily (>70% of total emissions) affect the BC levels from the surface to ∼5 km, while non-NA plumes compose more than half of the BC above ∼5 km. Among all sectors, NA and non-NA biomass burning, NA transportation and non-NA residential emissions are the major contributors. The sectoral contributions vary among ten regions defined by the US Environmental Protection Agency (EPA): NA anthropogenic emissions enhance northeastern US BC levels; biomass burning strongly impacts northern California and southeastern US; and the influence of extra-regional plumes is largest in the northwestern US but extends to eastern US. The mean contribution from non-NA sources to US surface BC is ∼0.05 μg m−3, with a maximum value of ∼0.11 μg m−3 in the northwestern US. The non-NA contributions to column BC are higher than to surface BC, ranging from 30% to 80%, depending on region. EPA region 8 is most sensitive to extra-regional BC, partially explaining the observed increasing BC trend there during the past decades associated with the increasing Asian BC emissions. Measurements from the June 24 DC-8 flight during the ARCTAS-CARB field campaign show that BC/(organic matter + nitrate + sulfate) mass ratios fairly well represent BC''s warming potential over southern California, which can be approximated by BC/(organic matter + sulfate) and BC/sulfate for plumes affected and unaffected by fires, respectively. The responses of BC/(organic matter + sulfate) and BC/sulfate to removing each emission sector are further discussed, indicating that mitigating NA transportation emissions has the highest potential for regional air quality and climate co-benefits. [Copyright &y& Elsevier]