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- ItemAbsorption instruments inter-comparison campaign at the Arctic Pallas station(Katlenburg-Lindau : European Geosciences Union, 2021) Asmi, Eija; Backman, John; Servomaa, Henri; Virkkula, Aki; Gini, Maria I.; Eleftheriadis, Konstantinos; Müller, Thomas; Ohata, Sho; Kondo, Yutaka; Hyvärinen, AnttiAerosol 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 0.01g¯Mm-1 levels when data were averaged to 1-2g¯h. The hourly averaged atmospheric absorption measured by the reference MAAP was 0.09g¯Mm-1 (at a wavelength of 637g¯nm). When data were averaged for >1g¯h, the filter-based methods agreed to around 40g¯%. 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 (slopeCombining double low line0.95, R2Combining double low line0.78), followed by AE31 (slopeCombining double low line0.93). 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 (R2Combining double low line0.65). 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 >0.1g¯Mm-1 at 1-2g¯h averaging times. The mass absorption cross section (MAC) value measured at a range 0-0.3g¯Mm-1 was calculated using the MAAP and a single particle soot photometer (SP2), resulting in a MAC value of 16.0±5.7g¯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. © Author(s) 2021.
- ItemMultidecadal trend analysis of in situ aerosol radiative properties around the world(Katlenburg-Lindau : EGU, 2020) Collaud Coen, Martine; Andrews, Elisabeth; Alastuey, Andrés; Petkov Arsov, Todor; Backman, John; Brem, Benjamin T.; Bukowiecki, Nicolas; Couret, Cédric; Eleftheriadis, Konstantinos; Flentje, Harald; Fiebig, Markus; Gysel-Beer, Martin; Hand, Jenny L.; Hoffer, András; Hooda, Rakesh; Hueglin, Christoph; Joubert, Warren; Keywood, Melita; Eun Kim, Jeong; Kim, Sang-Woo; Labuschagne, Casper; Lin, Neng-Huei; Lin, Yong; Lund Myhre, Cathrine; Luoma, Krista; Lyamani, Hassan; Marinoni, Angela; Mayol-Bracero, Olga L.; Mihalopoulos, Nikos; Pandolfi, Marco; Prats, Natalia; Prenni, Anthony J.; Putaud, Jean-Philippe; Ries, Ludwig; Reisen, Fabienne; Sellegri, Karine; Sharma, Sangeeta; Sheridan, Patrick; Sherman, James Patrick; Sun, Junying; Titos, Gloria; Torres, Elvis; Tuch, Thomas; Weller, Rolf; Wiedensohler, Alfred; Zieger, Paul; Laj, PaoloIn 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. © 2020 Royal Society of Chemistry. All rights reserved.
- ItemA European aerosol phenomenology - 6: Scattering properties of atmospheric aerosol particles from 28 ACTRIS sites(Katlenburg-Lindau : EGU, 2018) Pandolfi, Marco; Alados-Arboledas, Lucas; Alastuey, Andrés; Andrade, Marcos; Angelov, Christo; Artiñano, Begoña; Backman, John; Baltensperger, Urs; Bonasoni, Paolo; Bukowiecki, Nicolas; Collaud Coen, Martine; Conil, Sébastien; Coz, Esther; Crenn, Vincent; Dudoitis, Vadimas; Ealo, Marina; Eleftheriadis, Kostas; Favez, Olivier; Fetfatzis, Prodromos; Fiebig, Markus; Flentje, Harald; Ginot, Patrick; Gysel, Martin; Henzing, Bas; Hoffer, Andras; Holubova Smejkalova, Adela; Kalapov, Ivo; Kalivitis, Nikos; Kouvarakis, Giorgos; Kristensson, Adam; Kulmala, Markku; Lihavainen, Heikki; Lunder, Chris; Luoma, Krista; Lyamani, Hassan; Marinoni, Angela; Mihalopoulos, Nikos; Moerman, Marcel; Nicolas, José; O'Dowd, Colin; Petäjä, Tuukka; Petit, Jean-Eudes; Pichon, Jean Marc; Prokopciuk, Nina; Putaud, Jean-Philippe; Rodríguez, Sergio; Sciare, Jean; Sellegri, Karine; Swietlicki, Erik; Titos, Gloria; Tuch, Thomas; Tunved, Peter; Ulevicius, Vidmantas; Vaishya, Aditya; Vana, Milan; Virkkula, Aki; Vratolis, Stergios; Weingartner, Ernest; Wiedensohler, Alfred; Laj, PaoloThis paper presents the light-scattering properties of atmospheric aerosol particles measured over the past decade at 28 ACTRIS observatories, which are located mainly in Europe. The data include particle light scattering (σsp) and hemispheric backscattering (σbsp) coefficients, scattering Ångström exponent (SAE), backscatter fraction (BF) and asymmetry parameter (g). An increasing gradient of σsp is observed when moving from remote environments (arctic/mountain) to regional and to urban environments. At a regional level in Europe, σsp also increases when moving from Nordic and Baltic countries and from western Europe to central/eastern Europe, whereas no clear spatial gradient is observed for other station environments. The SAE does not show a clear gradient as a function of the placement of the station. However, a west-to-east-increasing gradient is observed for both regional and mountain placements, suggesting a lower fraction of fine-mode particle in western/south-western Europe compared to central and eastern Europe, where the fine-mode particles dominate the scattering. The g does not show any clear gradient by station placement or geographical location reflecting the complex relationship of this parameter with the physical properties of the aerosol particles. Both the station placement and the geographical location are important factors affecting the intraannual variability. At mountain sites, higher σsp and SAE values are measured in the summer due to the enhanced boundary layer influence and/or new particle-formation episodes. Conversely, the lower horizontal and vertical dispersion during winter leads to higher σsp values at all low-altitude sites in central and eastern Europe compared to summer. These sites also show SAE maxima in the summer (with corresponding g minima). At all sites, both SAE and g show a strong variation with aerosol particle loading. The lowest values of g are always observed together with low σsp values, indicating a larger contribution from particles in the smaller accumulation mode. During periods of high σsp values, the variation of g is less pronounced, whereas the SAE increases or decreases, suggesting changes mostly in the coarse aerosol particle mode rather than in the fine mode. Statistically significant decreasing trends of σsp are observed at 5 out of the 13 stations included in the trend analyses. The total reductions of σsp are consistent with those reported for PM2.5 and PM10 mass concentrations over similar periods across Europe.