Seasonality of the particle number concentration and size distribution: a global analysis retrieved from the network of Global Atmosphere Watch (GAW) near-surface observatories

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 Sci-ences (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), AIRTECCM (Madrid Regional Government P2018/EMT4329), REDMAAS2020 (RED2018-102594-T CIENCIA), Red de Excelencia ACTRIS-ESPANA (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 Espanol de Economia, Industria y Competitividad (MINECO), the Spanish Ministry of Economy and Competitiveness (projects no. CGL2016-81092-R, CGL2017-90884-REDT, RTI2018-097864-BI00 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 20142020), the Italian Ministry of Research and Education, the Norwegian Environment Agency, Swedish FORMAS, the Swedish Research Council (VR), the Magnus Bergvall foundation, the Marta och Erik Holmberg foundation, and the Swedish EPA.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 (N-tot) and number size distribution (PNSD, from 39 sites). A sensitivity study was first performed to assess the impact of data availability on N-tot's annual and seasonal statistics, as well as on the analysis of its diel cycle. Thresholds of 50% and 60% were set at the seasonal and annual scale, respectively, for the study of the corresponding statistics, and a slightly higher coverage (75 %) 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 (similar to 10(2) cm(-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 (similar to 10(3)-10(4) cm(-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 N-tot (similar to 10(2)-10(3) cm(-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 N-tot observed at these stations. Based on available PNSD measurements, CCN-sized particles (considered here as either >50 nm or >100 nm) can represent from a few percent to almost all of N-tot, corresponding to seasonal medians on the order of similar to 10 to 1000 cm(-3), with seasonal patterns and a hierarchy of the site types broadly similar to those observed for N-tot. 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.European Commission's Horizon 2020 Framework Programme (ACTRIS2) 654109University of HelsinkiFinnish Meteorological InstituteDepartment of Science and Innovation of South AfricaAcademy of Finland 272041Academy of Finland project Greenhouse gas, aerosol and albedo variations in the changing Arctic 269095Novel Assessment of Black Carbon in the Eurasian Arctic: From Historical Concentrations and Sources to Future Climate Impacts (NABCEA) 296302Korea Meteorological Administration Research and Development Program "Development of Monitoring and Analysis Techniques for Atmospheric Composition in Korea" KMA2018-00522National Research Foundation of Korea 2017R1D1A1B06032548Korea Meteorological Administration Research and Development Program KMI2018-01111Taiwan Environmental Protection AdministrationChina Meteorological AdministrationNational Natural Science Foundation of China (NSFC) 41675129 41875147National Key R&D Program of the Ministry of Science and Technology of the People's Republic of China 2016YFC0203305 2018YFC0213204Chinese Academy of Meteorological Sciences 2020KJ001Innovation Team for Haze-fog Observation and Forecast of MOST Innovation Team for Haze-fog Observation and Forecast of CMA Innovation Team for Haze-fog Observation and Forecast of CNRS-INSUFrench Ministry for Research under the ACTRIS-FR national research infrastructureFrench Ministry of the Environment, MeteoSwiss (GAW-CH aerosol monitoring programme)Swiss State Secretariat for Education, Research and Innovation (SERI)Ministry of Education, Youth and Sports of CR within National Sustainability Program I (NPU I) LO1415ERDF "ACTRISCZ RI" CZ.02.1.01/0.0/0.0/16_013/0001315CRISOL CGL2017-85344TIGAS-CM (Madrid Regional Government) Y2018/EMT-5177AIRTECCM (Madrid Regional Government) P2018/EMT4329REDMAAS2020 RED2018-102594-TRed de Excelencia ACTRIS-ESPANA CGL2017-90884-REDTSpanish Ministry of Economy, Industry and Competitiveness, FEDER funds CGL2016-78594-RGeneralitat de CatalunyaGeneral Electric AGAUR 2017 SGR41National Institute for Aerospace TechnologyMinisterio Espanol de Economia, Industria y Competitividad (MINECO) Spanish Government CGL2017-90884-REDT CGL2016-81092-R RTI2018-097864-BI00 PGC2018-098770-B-I00Andalusia Regional Government P18-RT-3820PANhellenic infrastructure for Atmospheric Composition and climate change MIS 5021516Research and Innovation Infrastructure, Competitiveness, Entrepreneurship and Innovation NSRF 20142020Ministry of Education, Universities and Research (MIUR)Norwegian Environment Agency, Swedish FORMASSwedish Research CouncilMagnus Bergvall foundationMarta och Erik Holmberg foundationSwedish EP