Abstract Background The implementation of emission mitigation policies in Europe over the last two decades has generally improved the air quality, which resulted in lower aerosol particle mass, particle number, and black carbon mass concentration. However, little is known whether the decreasing particle concentrations at a lower-altitude level can be observed in the free troposphere (FT), an important layer of the atmosphere, where aerosol particles have a longer lifetime and may affect climate dynamics. In this study, we used data from two high-Alpine observatories, Zugspitze-Schneefernerhaus (ZSF) and Jungfraujoch (JFJ), to assess the long-term trends on size-resolved particle number concentrations (PNCs) and equivalent black carbon (eBC) mass concentration separated for undisturbed lower FT conditions and under the influence of air from the planetary boundary layer (PBL) from 2009 to 2018.
Results The FT and PBL-influenced conditions were segregated for both sites. We found that the FT conditions in cold months were more prevalent than in warm months, while the measured aerosol parameters showed different seasonal patterns for the FT and PBL-influenced conditions. The pollutants in the PBL-influenced condition have a higher chance to be transported to high-altitudes due to the mountainous topography, leading to a higher concentration and more distinct seasonal variation, and vice versa. The long-term trends of the measured aerosol parameters were evaluated and the decreased aerosol concentrations were observed for both FT and PBL-influenced conditions. The observed decreasing trends in eBC concentration in the PBL-influenced condition are well consistent with the reported trends in total BC emission in Germany and Switzerland. The decreased concentrations in the FT condition suggest that the background aerosol concentration in the lower FT over Central Europe has correspondingly decreased. The change of back trajectories in the FT condition at ZSF and JFJ was further evaluated to investigate the other possible drivers for the decreasing trends.
Conclusions The background aerosol concentration in the lower FT over Central Europe has significantly decreased during 2009–2018. The implementation of emission mitigation policies is the most decisive factor and the decrease of the regional airmass occurrence over Central Europe also has contributed to the decreasing trends.
Anthropogenic emissions are a dominant contributor to air pollution. Consequently, mitigation policies have attempted to reduce anthropogenic pollution emissions in Europe since the 1990s. To evaluate the effectiveness of these mitigation policies, the German Ultrafine Aerosol Network (GUAN) was established in 2008, focusing on black carbon and sub-micrometer aerosol particles, especially ultrafine particles. In this investigation, trends of the size-resolved particle number concentrations (PNC) and the equivalent black carbon (eBC) mass concentration over a 10-year period (2009–2018) were evaluated for 16 observational sites for different environments among GUAN. The trend analysis was done for both, the full-length time series and on subsets of the time series in order to test the reliability of the results. The results show generally decreasing trends of both, the PNCs for all size ranges as well as eBC mass concentrations in all environments, except PNC in 10–30 nm at regional background and mountain sites. The annual slope of the eBC mass concentration varies between −7.7 % and −1.8 % per year. The slopes of the PNCs varies from −6.3 % to 2.7 %, −7.0 % to −2.0 %, and −9.5 % to −1.5 % per year (only significant trends) for 10–30 nm, 30–200 nm, and 200–800 nm particle diameter, respectively. The regional Mann-Kendall test yielded regional-scale trends of eBC mass concentration, N [30–200] and N [200–800] of −3.8 %, −2.0 % and −2.4 %, respectively, indicating an overall decreasing trend for eBC mass concentration and sub-micrometer PNC (except N [10–30] ) all over Germany. The most significant decrease was observed on working days and during daytime in urban areas, which implies a strong evidence of reduced anthropogenic emissions. For the seasonal trends, stronger reductions were observed in winter. Possible reasons for this reduction can be the increased average ambient temperatures and wind speed in winter, which resulted in less domestic heating and stronger dilution. In addition, decreased precipitation in summer also diminishes the decrease of the PNCs and eBC mass concentration. For the period of interest, there were no significant changes in long-range transport patterns. The most likely factors for the observed decreasing trends are declining anthropogenic emissions due to emission mitigation policies of the European Union.
Aerosol particles are a complex component of the atmospheric system which influence climate directly by interacting with solar radiation, and indirectly by contributing to cloud formation. The variety of their sources, as well as the multiple transformations they may undergo during their transport (including wet and dry deposition), result in significant spatial and temporal variability of their properties. Documenting this variability is essential to provide a proper representation of aerosols and cloud condensation nuclei (CCN) in climate models. Using measurements conducted in 2016 or 2017 at 62 ground-based stations around the world, this study provides the most up-to-date picture of the spatial distribution of particle number concentration (Ntot) and number size distribution (PNSD, from 39 sites). A sensitivity study was first performed to assess the impact of data availability on Ntot's annual and seasonal statistics, as well as on the analysis of its diel cycle. Thresholds of 50g% and 60g% were set at the seasonal and annual scale, respectively, for the study of the corresponding statistics, and a slightly higher coverage (75g%) was required to document the diel cycle. Although some observations are common to a majority of sites, the variety of environments characterizing these stations made it possible to highlight contrasting findings, which, among other factors, seem to be significantly related to the level of anthropogenic influence. The concentrations measured at polar sites are the lowest (g1/4g102gcm-3) and show a clear seasonality, which is also visible in the shape of the PNSD, while diel cycles are in general less evident, due notably to the absence of a regular day-night cycle in some seasons. In contrast, the concentrations characteristic of urban environments are the highest (g1/4g103-104gcm-3) and do not show pronounced seasonal variations, whereas diel cycles tend to be very regular over the year at these stations. The remaining sites, including mountain and non-urban continental and coastal stations, do not exhibit as obvious common behaviour as polar and urban sites and display, on average, intermediate Ntot (g1/4g102-103gcm-3). Particle concentrations measured at mountain sites, however, are generally lower compared to nearby lowland sites, and tend to exhibit somewhat more pronounced seasonal variations as a likely result of the strong impact of the atmospheric boundary layer (ABL) influence in connection with the topography of the sites. ABL dynamics also likely contribute to the diel cycle of Ntot observed at these stations. Based on available PNSD measurements, CCN-sized particles (considered here as either >50gnm or >100gnm) can represent from a few percent to almost all of Ntot, corresponding to seasonal medians on the order of g1/4g10 to 1000gcm-3, with seasonal patterns and a hierarchy of the site types broadly similar to those observed for Ntot. Overall, this work illustrates the importance of in situ measurements, in particular for the study of aerosol physical properties, and thus strongly supports the development of a broad global network of near surface observatories to increase and homogenize the spatial coverage of the measurements, and guarantee as well data availability and quality. The results of this study also provide a valuable, freely available and easy to use support for model comparison and validation, with the ultimate goal of contributing to improvement of the representation of aerosol-cloud interactions in models, and, therefore, of the evaluation of the impact of aerosol particles on climate. ; NOAA base funding supports the observatories BRW, BND, MLO, SMO, SPO and THD, where efforts of the dedicated observatory staff and of programmer Derek Hageman are appreciated. BRW observations are also supported in part by the Atmospheric Radiation Measurement (ARM) user facility, a US Department of Energy (DOE) Office of Science user facility managed by the Biological and Environmental Research programme. Measurements at Welgegund are supported by North-West University, the University of Helsinki and the Finnish Meteorological Institute. This publication also forms part of the output of the Biogeochemistry Research Infrastructure Platform (BIOGRIP) of the Department of Science and Innovation of South Africa. Pallas and SMEAR II are grateful for the support of the Academy of Finland Centre of Excellence programme (project no. 272041), the Academy of Finland project Greenhouse gas, aerosol and albedo variations in the changing Arctic (project no. 269095), and the Novel Assessment of Black Carbon in the Eurasian Arctic: From Historical Concentrations and Sources to Future Climate Impacts (NABCEA, project no. 296302). Aerosol measurements at Anmyeon-do were supported by the Korea Meteorological Administration Research and Development Program "Development of Monitoring and Analysis Techniques for Atmospheric Composition in Korea" under grant KMA2018-00522. Measurements at Gosan were supported by the National Research Foundation of Korea (2017R1D1A1B06032548) and the Korea Meteorological Administration Research and Development Program under grant KMI2018-01111. The Lulin station is operated under the grants funded by the Taiwan Environmental Protection Administration. WLG is supported by the China Meteorological Administration, where efforts of the dedicated observatory staff are appreciated. Sites PDM, PUY, GIF, CHC and RUN are partially operated with the support of CNRS-INSU under the long-term observation programme and the French Ministry for Research under the ACTRIS-FR national research infrastructure. PDM and GIF received specific support from the French Ministry of the Environment. ATMO Occitanie is mentioned for sampling operations at PDM. Measurements at SIRTA are hosted by CNRS and by the alternative energies and atomic energy commission (CEA) with additional contributions from the French Ministry of the Environment through its funding to the reference laboratory for air quality monitoring (LCSQA). PUY is grateful for support from ATMO Auvergne Rhône Alpes for sampling operations and the support from the personnel of the Observatoire de Physique du Globe de Clermont-Ferrand (OPGC). The specific support of the Institut de Recherche et Développement (IRD) in France and the Universidad Mayor de San Andrés in Bolivia support operations at CHC operations. The Steamboat Ski Resort provided logistical support and in-kind donations for SPL. The Desert Research Institute is a permittee of the Medicine Bow–Routt National Forests and an equal opportunity service provider and employer. SPL appreciates the extensive assistance of the NOAA/ESRL Federated Aerosol Network, of Ian McCubbin, site manager of SPL, and of Ty Atkins, Joe Messina, Dan Gilchrist and Maria Garcia, who provided technical assistance with the maintenance and data quality control for the aerosol instruments. SGP measurements/mentorship were supported by DOE-7F-30118 and staff on site. The Cape Grim Baseline Air Pollution Monitoring Station is grateful to the Australian Bureau of Meteorology for their long-term and continued support and all the staff from the Bureau of Meteorology and CSIRO, who have contributed to the generation of records reported here. The aerosol measurements at the Jungfraujoch were conducted with financial support from MeteoSwiss (GAW-CH aerosol monitoring programme) and from the European Union as well as the Swiss State Secretariat for Education, Research and Innovation (SERI) for the European Research Infrastructure for the observation of Aerosol, Clouds and Trace Gases (ACTRIS). The International Foundation High Altitude Research Station Jungfraujoch and Gornergrat (HFSJG) is mentioned for providing the research platform at the Jungfraujoch. The aerosol measurements at Kosetice received funding from the European Union's Horizon 2020 research and innovation programme under grant agreement no. 654109 and from the project for support of the national research infrastructure ACTRIS – participation of the Czech Republic (ACTRIS-CZ – LM2015037) supported by the Ministry of Education, Youth and Sports of CR within National Sustainability Program I (NPU I), grant agreement no. LO1415. The measurements were also supported by ERDF "ACTRIS-CZ RI" (no. CZ.02.1.01/0.0/0.0/16_013/0001315). Measurements at the Madrid site were funded by the following projects: CRISOL (CGL2017–85344-R MINECO/AEI/FEDER, UE), TIGAS-CM (Madrid Regional Government Y2018/EMT5177), AIRTEC-CM (Madrid Regional Government P2018/EMT4329), REDMAAS2020 (RED2018-102594-T CIENCIA) and Red de Excelencia ACTRIS-ESPAÑA (CGL2017-90884-REDT). Measurements at Montsec and Montseny were supported by the Spanish Ministry of Economy, Industry and Competitiveness and FEDER funds under project HOUSE (CGL2016-78594-R) and by the Generalitat de Catalunya (AGAUR 2017 SGR41 and the DGQA). Aerosol measurements at El Arenosillo Observatory are supported by the National Institute for Aerospace Technology and by different R&D projects of the Ministerio Español de Economía, Industria y Competitividad (MINECO). Aerosol measurements at UGR are supported by the Spanish Ministry of Economy and Competitiveness through projects no. CGL2016-81092-R, CGL2017-90884-REDT, RTI2018-097864-B-I00 and PGC2018-098770-B-I00 and by the Andalusia Regional Government through project no. P18-RT-3820. FKL, HAC and DEM are grateful for funding by project PANhellenic infrastructure for Atmospheric Composition and climate change (MIS 5021516), which is implemented under action Reinforcement of the Research and Innovation Infrastructure, funded by operational programme Competitiveness, Entrepreneurship and Innovation (NSRF 2014-2020) and co-financed by Greece and the European Union (European Regional Development Fund). CPC measurements at Sonnblick are supported by the Climate and Air Quality Commission of the Austrian Academy of Sciences and the office of the provincial government Salzburg, Unit 5/02. At CMN, aerosol measurements were partially supported by the Italian Ministry of Research and Education. Measurements at Birkenes II are financed by the Norwegian Environment Agency. VAV is grateful for various Swedish FORMAS, Swedish Research Council (VR) grants and the Magnus Bergvall and Märta och Erik Holmberg foundations and the Swedish EPA for making the research possible at the VAV site. NMY wishes to thank the many technicians and scientists of the Neumayer overwintering crews, whose outstanding commitment enabled continuous, high-quality aerosol records over many years. Gunter Löschau is acknowledged for his contribution to the data acquisition at ANB, DTC and DRN. Financial support This research was supported by the European Commission's Horizon 2020 Framework Programme (ACTRIS2 (grant agreement no. 654109)), the University of Helsinki, the Finnish Meteorological Institute, the Department of Science and Innovation of South Africa, the Academy of Finland Centre of Excellence programme (project no. 272041), the Academy of Finland project Greenhouse gas, aerosol and albedo variations in the changing Arctic (project no. 269095), the Novel Assessment of Black Carbon in the Eurasian Arctic: From Historical Concentrations and Sources to Future Climate Impacts (NABCEA, project no. 296302), the Korea Meteorological Administration Research and Development Program "Development of Monitoring and Analysis Techniques for Atmospheric Composition in Korea" (grant no. KMA2018-00522), the National Research Foundation of Korea (grant no. 2017R1D1A1B06032548), the Korea Meteorological Administration Research and Development Program (grant no. KMI2018-01111), the Taiwan Environmental Protection Administration, the China Meteorological Administration, the National Scientific Foundation of China (41675129, 41875147), the National Key R&D Program of the Ministry of Science and Technology of the People's Republic of China (grant no. 2016YFC0203305 and 2018YFC0213204), the Chinese Academy of Meteorological Sciences (2020KJ001), the Innovation Team for Haze-fog Observation and Forecasts of MOST and CMA, CNRS-INSU, the French Ministry for Research under the ACTRIS-FR national research infrastructure, the French Ministry of the Environment, MeteoSwiss (GAW-CH aerosol monitoring programme), the Swiss State Secretariat for Education, Research and Innovation (SERI), the Ministry of Education, Youth and Sports of CR within National Sustainability Program I (NPU I, grant no. LO1415), ERDF "ACTRISCZ RI" (grant no. CZ.02.1.01/0.0/0.0/16_013/0001315), CRISOL (CGL2017-85344-R MINECO/AEI/FEDER, UE), TIGAS-CM (Madrid Regional Government Y2018/EMT-5177), AIRTEC-CM (Madrid Regional Government P2018/EMT4329), REDMAAS2020 (RED2018-102594-T CIENCIA), Red de Excelencia ACTRIS-ESPAÑA (CGL2017-90884-REDT), the Spanish Ministry of Economy, Industry and Competitiveness, FEDER funds (project HOUSE, grant no. CGL2016-78594-R), the Generalitat de Catalunya (AGAUR 2017 SGR41 and the DGQA), the National Institute for Aerospace Technology, the Ministerio Español de Economía, Industria y Competitividad (MINECO), the Spanish Ministry of Economy and Competitiveness (projects no. CGL2016-81092-R, CGL2017-90884-REDT, RTI2018-097864-B-I00 and PGC2018-098770-B-I00), the Andalusia Regional Government (project no. P18-RT-3820), the PANhellenic infrastructure for Atmospheric Composition and climate change (MIS 5021516), Research and Innovation Infrastructure, Competitiveness, Entrepreneurship and Innovation (grant no. NSRF 2014-2020), the Italian Ministry of Research and Education, the Norwegian Environment Agency, Swedish FORMAS, the Swedish Research Council (VR), the Magnus Bergvall foundation, the Märta och Erik Holmberg foundation, and the Swedish EPA. ; Peer reviewed
