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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]

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]

Aerosol light absorption was measured during a 1-month field campaign in June–July 2019 at the Pallas Global Atmospheric Watch (GAW) station in northern Finland. Very low aerosol concentrations prevailed during the campaign, which posed a challenge for the instruments' detection capabilities. The campaign provided a real-world test for different absorption measurement techniques supporting the goals of the European Metrology Programme for Innovation and Research (EMPIR) Black Carbon (BC) project in developing aerosol absorption standard and reference methods. In this study we compare the results from five filter-based absorption techniques – aethalometer models AE31 and AE33, a particle soot absorption photometer (PSAP), a multi-angle absorption photometer (MAAP), and a continuous soot monitoring system (COSMOS) – and from one indirect technique called extinction minus scattering (EMS). The ability of the filter-based techniques was shown to be adequate to measure aerosol light absorption coefficients down to around 0.01 Mm-1 levels when data were averaged to 1–2 h. The hourly averaged atmospheric absorption measured by the reference MAAP was 0.09 Mm-1 (at a wavelength of 637 nm). When data were averaged for >1 h, the filter-based methods agreed to around 40 %. COSMOS systematically measured the lowest absorption coefficient values, which was expected due to the sample pre-treatment in the COSMOS inlet. PSAP showed the best linear correlation with MAAP (slope=0.95 , R2=0.78), followed by AE31 (slope=0.93). A scattering correction applied to PSAP data improved the data accuracy despite the added noise. However, at very high scattering values the correction led to an underestimation of the absorption. The AE31 data had the highest noise and the correlation with MAAP was the lowest (R2=0.65). Statistically the best linear correlations with MAAP were obtained for AE33 and COSMOS (R2 close to 1), but the biases at around the zero values led to slopes clearly below 1. The sample pre-treatment in the COSMOS instrument resulted in the lowest fitted slope. In contrast to the filter-based techniques, the indirect EMS method was not adequate to measure the low absorption values found at the Pallas site. The lowest absorption at which the EMS signal could be distinguished from the noise was >0.1 Mm-1 at 1–2 h averaging times. The mass absorption cross section (MAC) value measured at a range 0–0.3 Mm-1 was calculated using the MAAP and a single particle soot photometer (SP2), resulting in a MAC value of 16.0±5.7 m2g-1. Overall, our results demonstrate the challenges encountered in the aerosol absorption measurements in pristine environments and provide some useful guidelines for instrument selection and measurement practices. We highlight the need for a calibrated transfer standard for better inter-comparability of the absorption results. [ABSTRACT FROM AUTHOR]

The Arctic absorbing aerosols have a high potential to accelerate global warming. Accurate and sensitive measurements of their concentrations, variability and atmospheric mixing are needed. Filter-based aerosol light absorption measurement methods are the most widely applied in the Arctic. Those will be the focus of this study. Aerosol light absorption was measured during one month field campaign in June–July 2019 at the Pallas Global AtmosphericWatch (GAW) station in northern Finland. The campaign provided a real-world test for different absorption measurement techniques supporting the goals of the EMPIR BC metrology project in developing aerosol absorption standard and reference methods. Very low aerosol concentrations prevailed during the campaign which imposed a challenge for the instruments detection. In this study we compare the results from five filter-based absorption techniques: Aethalometer models AE31 and AE33, Particle Soot Absorption Photometer (PSAP), Multi Angle Absorption Photometer (MAAP) and Continuous Soot Monitoring System (COSMOS), and from one indirect method called Extinction Minus Scattering (EMS). The sensitivity of the filter-based techniques was adequate to measure aerosol light absorption coefficients down to around 0.05 Mm-1 levels. The average value measured during the campaign using MAAP was 0.09 Mm-1 (at wavelength of 637 nm). When data were averaged for >1h, an agreement of around 20% was obtained between instruments. COSMOS measured systematically the lowest absorption coefficient values, which was expected due to the sample pre-treatment in COSMOS inlet. PSAP showed the best linear correlation with MAAP (R2 = 0.85), followed by AE33 and COSMOS (R2 = 0.84). The noisy data from AE31 resulted in a slightly lower, yet a significant, correlation with MAAP (R2 = 0.46). In contrast to the filter-based techniques, the sensitivity of the indirect EMS method to measure aerosol absorption was not adequate at such low concentrations levels. An absorption coefficient on the order of >1 Mm-1 was estimated as the lowest limit, to reliably distinguish the signal from the noise. Throughout the campaign the aerosol was highly scattering with an average single-scattering albedo of 0.97. Two different air-mass origins could be identified: the north-east and from the north-west. The north-eastern air masses contained higher fraction of thickly coated light absorbing particles than the westerly air masses. Aerosol scattering, absorption and the particle coating thickness increased on the last ten days of the campaign during the north-eastern air flow. The simultaneous changes in aerosol source region, mixing state, concentration and particle optical size were reflected in the instruments' response in a complex way. The observed decrease in aerosol size suggested additional activation of secondary particle formation mechanisms. The results demonstrate the challenges encountered in the Arctic absorbing aerosol measurements. The applicability and uncertainties of different techniques are discussed and new knowledge on the absorbing aerosol characteristics in summer Arctic air masses reference to the source region is provided. [ABSTRACT FROM AUTHOR]

In order to assess the evolution of aerosol parameters affecting climate change, a long-term trend analysis of aerosol optical properties was performed on time series from 52 stations situated across five continents. The time series of measured scattering, backscattering and absorption coefficients as well as the derived single scattering albedo, backscattering fraction, scattering and absorption Ångström exponents covered at least 10 years and up to 40 years for some stations. The non-parametric seasonal Mann–Kendall (MK) statistical test associated with several pre-whitening methods and with Sen's slope was used as the main trend analysis method. Comparisons with general least mean square associated with autoregressive bootstrap (GLS/ARB) and with standard least mean square analysis (LMS) enabled confirmation of the detected MK statistically significant trends and the assessment of advantages and limitations of each method. Currently, scattering and backscattering coefficient trends are mostly decreasing in Europe and North America and are not statistically significant in Asia, while polar stations exhibit a mix of increasing and decreasing trends. A few increasing trends are also found at some stations in North America and Australia. Absorption coefficient time series also exhibit primarily decreasing trends. For single scattering albedo, 52 % of the sites exhibit statistically significant positive trends, mostly in Asia, eastern/northern Europe and the Arctic, 22 % of sites exhibit statistically significant negative trends, mostly in central Europe and central North America, while the remaining 26 % of sites have trends which are not statistically significant. In addition to evaluating trends for the overall time series, the evolution of the trends in sequential 10-year segments was also analyzed. For scattering and backscattering, statistically significant increasing 10-year trends are primarily found for earlier periods (10-year trends ending in 2010–2015) for polar stations and Mauna Loa. For most of the stations, the present-day statistically significant decreasing 10-year trends of the single scattering albedo were preceded by not statistically significant and statistically significant increasing 10-year trends. The effect of air pollution abatement policies in continental North America is very obvious in the 10-year trends of the scattering coefficient – there is a shift to statistically significant negative trends in 2009–2012 for all stations in the eastern and central USA. This long-term trend analysis of aerosol radiative properties with a broad spatial coverage provides insight into potential aerosol effects on climate changes. [ABSTRACT FROM AUTHOR]