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Aerosol particles are essential constituents of the Earth’s atmosphere, impacting the earth radiation balance directly by scattering and absorbing solar radiation, and indirectly by acting as cloud condensation nuclei. In contrast to most greenhouse gases, aerosol particles have short atmospheric residence times, resulting in a highly heterogeneous distribution in space and time. There is a clear need to document this variability at regional scale through observations involving, in particular, the in situ near-surface segment of the atmospheric observation system. This paper will provide the widest effort so far to document variability of climate-relevant in situ aerosol properties (namely wavelength dependent particle light scattering and absorption coefficients, particle number concentration and particle number size distribution) from all sites connected to the Global Atmosphere Watch network. High-quality data from almost 90 stations worldwide have been collected and controlled for quality and are reported for a reference year in 2017, providing a very extended and robust view of the variability of these variables worldwide. The range of variability observed worldwide for light scattering and absorption coefficients, single-scattering albedo, and particle number concentration are presented together with preliminary information on their long-term trends and comparison with model simulation for the different stations. The scope of the present paper is also to provide the necessary suite of information, including data provision procedures, quality control and analysis, data policy, and usage of the ground-based aerosol measurement network. It delivers to users of the World Data Centre on Aerosol, the required confidence in data products in the form of a fully characterized value chain, including uncertainty estimation and requirements for contributing to the global climate monitoring system., European Commission Joint Research Centre 654109, European ERDF funds through different Spanish R&D projects of the Spanish Ministerio de Economia, Industria y Competitividad, NorthWest University, University of Helsinki, Academy of Finland 272041, Academy of Finland project Greenhouse gas 269095 296302, Korea Meteorological Administration Research and Development Program "Development of Monitoring and Analysis Techniques for Atmospheric Composition in Korea KMA2018-00522, National Research Foundation of Korea 2017R1D1A1B06032548, Korea Meteorological Administration Research and Development Program KMI2018-01111, Taiwan Environmental Protection Administration, Ministry of Research, France, French Ministry of the Environment, United States Environmental Protection Agency, 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) LO1415, ERDF "ACTRISCZ RI" CZ.02.1.01/0.0/0.0/16_013/0001315 CGL2017-85344-R MINECO/AEI/FEDER, TIGAS-CM (Madrid Regional Government) Y2018/EMT-5177, AIRTECCM (Madrid Regional Government) P2018/EMT4329 REDMAAS2020 RED2018-102594-T CIENCIA, Spanish Ministry of Economy, Industry and Competitiveness, European Union (EU) CGL2016-78594-R, Generalitat de Catalunya AGAUR 2017 SGR41, National Institute for Aerospace Technology, Ministerio Espanol de Economia, Industria y Competitividad (MINECO) MIS 5021516, Competitiveness, Entrepreneurship and Innovation, NSRF, Ministry of Education, Universities and Research (MIUR), Norwegian Environment Agency, Swedish FORMAS; Swedish Research Council (VR), Magnus Bergvall foundation, Marta och Erik Holmberg foundation, Swedish EPA

Air pollution and particulate matter are recognised cause of increased disease incidence in exposed population. The toxicological processes underlying air pollution associated effects have been investigated by in vivo and/or in vitro experimentation. The latter is usually performed by exposing cells cultured under submerged condition to particulate matter concentration quite far from environmental exposure expected in humans. Here we report for the first time the feasibility of a direct exposure of air liquid interface cultured cells to environmental concentration of particulate matter. Inflammatory proteins release was analysed in cell medium while differential expression of selected genes was analysed in cells. Significant association of anti-oxidant genes was observed with secondary and aged aerosol, while cytochrome activation with primary and PAHs enriched ultrafine particles. The results obtained clearly show the opportunity to move from the lab bench to the field for properly understanding the toxicological effects also of ultrafine particles on selected in vitro models. © 2018 Elsevier Ltd

The occurence of new particle formation (NPF) events was investigated at four sites in the boreal forest environment (Hyytiälä SMEAR II and Värriö SMEAR I in Finland; Tomsk-Fonovaya and ZOTTO in Siberia, Russia), by analyzing measured particle number size-distributions (PNSD) and theoretical calculations of particle survival probabilities. NPF events were less frequent at the Siberian sites than at the Finnish sites. This is likely linked to lower survival probabilities of the freshly-formed particles at the Siberian sites, due to higher coagulational losses and lower particle growth rates. Another factor affecting the frequency of observed NPF events is the minimum detectable particle size. When the NPF event classification was made for Hyytiälä, Värriö and Tomsk-Fonovaya sites based on PNSD starting from 15 nm instead of 3 nm, the observed NPF frequencies decreased. This result highlights the importance of measuring PNSD starting from sub-10 nm particles, in order to obtain reliable estimates of the NPF characteristics.

Atmospheric particles are important reaction vessels for multiphase chemistry. We conducted a meta-analysis of previous field observations in various environments (includes ocean, urban and rural regions), showing that particle hygroscopicity inhomogeneity (PHI) is ubiquitous for the continental atmospheric particles, in which a considerable part of the particulate matters is hydrophobic (10%–33% on average). However, the effects of PHI in quantifying the uptake process of reactive gases are still unclear. Here, taking N2O5 uptake as an example, we showed that using a laboratory-based parameterization scheme without considering the PHI might result in a misestimation of uptake rate coefficient, especially under low ambient relative humidity (RH). Such misestimation may be caused by the differences of the uptake coefficients, as well as the proportion of surface area concentration (SA) between hydrophilic and hydrophobic particles. We suggested that the PHI should be well-considered in establishing the reactive traces gases heterogeneous uptake parameterizations.

To improve ambient air quality during the 2008 Summer Olympic and Paralympic Games, the Chinese Government and Beijing’s municipal government implemented comprehensive emission control policies in Beijing and its neighboring regions before and during this period. The goal of this study was to investigate the association between particulate air pollution and cause-specific respiratory mortality before, during and after the period of the Olympic Games. Further, we wanted to assess whether changes in pollutant concentrations were linked to changes in respiratory mortality. We obtained daily data on mortality due to respiratory diseases (coded as J00-J99 according to the International Classification of Diseases and Related Health Problems 10th revision [ICD10]) and pneumonia (ICD10: J12–18), meteorology, particulate matter less than 10 µm or 2.5 μm in diameter (PM10, PM2.5) and particle number size distribution from official monitoring networks and sites located on the Peking University campus between May 20 and December 1, 2008. We assessed the effects of particulate air pollution on daily respiratory mortality using confounder-adjusted Quasi-Poisson regression models. Furthermore, we estimated air pollution effects for three periods—before (May 20 to July 20, 2008), during (August 1 to September 20, 2008) and after (October 1 to December 1, 2008)—by including interaction terms in the models. We found associations between different particle metrics and respiratory and pneumonia mortality, with more pronounced effects in smaller particle size ranges. For example, an interquartile range increase of 7,958 particles/cm3 in ultrafine particles (particles

In a warming Arctic the increased occurrence of new particle formation (NPF) is believed to originate from the declining ice coverage during summertime. Understanding the physico-chemical properties of newly formed particles, as well as mechanisms that control both particle formation and growth in this pristine environment, is important for interpreting aerosol–cloud interactions, to which the Arctic climate can be highly sensitive. In this investigation, we present the analysis of NPF and growth in the high summer Arctic. The measurements were made on-board research vessel Polarstern during the PS106 Arctic expedition. Four distinctive NPF and subsequent particle growth events were observed, during which particle (diameter in a range 10–50 nm) number concentrations increased from background values of approx. 40 up to 4000 cm−3. Based on particle formation and growth rates, as well as hygroscopicity of nucleation and the Aitken mode particles, we distinguished two different types of NPF events. First, some NPF events were favored by negative ions, resulting in more-hygroscopic nucleation mode particles and suggesting sulfuric acid as a precursor gas. Second, other NPF events resulted in less-hygroscopic particles, indicating the influence of organic vapors on particle formation and growth. To test the climatic relevance of NPF and its influence on the cloud condensation nuclei (CCN) budget in the Arctic, we applied a zero-dimensional, adiabatic cloud parcel model. At an updraft velocity of 0.1 m s−1, the particle number size distribution (PNSD) generated during nucleation processes resulted in an increase in the CCN number concentration by a factor of 2 to 5 compared to the background CCN concentrations. This result was confirmed by the directly measured CCN number concentrations. Although particles did not grow beyond 50 nm in diameter and the activated fraction of 15–50 nm particles was on average below 10 %, it could be shown that the sheer number of particles produced by the nucleation process is enough to significantly influence the background CCN number concentration. This implies that NPF can be an important source of CCN in the Arctic. However, more studies should be conducted in the future to understand mechanisms of NPF, sources of precursor gases and condensable vapors, as well as the role of the aged nucleation mode particles in Arctic cloud formation.

Vertical variation in aerosol optical properties [e.g. Single Scattering Albedo (SSA) and aerosol extinction coefficient] over a polluted environment is extremely important for better understanding of columnar radiative characteristics. The present case study over a typical polluted environment (New Delhi) discusses the vertical profile (ground to 700 m) of modelled optical properties of atmospheric particles at different altitudes. Here, we used the aerosol physico-chemical data generated in the tethered balloon-based observation conducted at CSIR-NPL, New Delhi (28° 38′ 10″ N, 77° 10′ 17″ E) from 21st −27th February 2014. Based on the microscopic observations of individual particles, we developed the aerosol model shapes (coated spheres) for simulating their optical properties. Total three cases were considered for simulating the aerosol optics at varying altitude; Case A: External mixture of coated dust and coated sulfate particles; Case B: External mixture of coated dust, coated sulfate, coated OC (Organic Carbon) and coated EC (Elemental Carbon) (with assumption that 6% EC at ground level); Case C: External mixture of coated dust, coated sulfate, coated OC and coated EC (with assumption that 10% EC at ground level). At 550 nm wavelength, the value of SSA has been found to be highest (i.e. 0.985) at 200 m altitude for Case A while Case B (i.e. 0.9523) and Case C (i.e. 0.9291) show highest values at 500 m altitude. SSA was found to be maximum at 500 m altitude for both Case B and Case C due to the presence of lowest graphitic counts at that particular altitude. Case B and Case C exhibit similar pattern but differ in magnitude, this is due to two EC extremities at ground level i.e. minima (6%) and maxima (10%). The percentage deviation in SSA from ground level to 700 m was found to be highest for Case C (i.e. 5.95%) followed by Case B (i.e. 4.19%) and Case A (i.e. 1.4%). Modelled aerosol optical properties within boundary layer may improve our understanding about the thermodynamics of lower atmosphere.

A consortium of polar scientists combined observational forces in a field campaign of unprecedented complexity to uncover the secrets of clouds and their role in Arctic amplification. Two research aircraft, an icebreaker research vessel, an ice-floe camp including an instrumented tethered balloon, and a permanent ground-based measurement station were employed in this endeavour. Clouds play an important role in Arctic amplification. This term represents the recently observed enhanced warming of the Arctic relative to the global increase of near-surface air temperature. However, there are still important knowledge gaps regarding the interplay between Arctic clouds and aerosol particles, surface properties, as well as turbulent and radiative fluxes that inhibit accurate model simulations of clouds in the Arctic climate system. In an attempt to resolve this so-called Arctic cloud puzzle, two comprehensive and closely coordinated field studies were conducted: the ”Arctic CLoud Observations Using airborne measurements during polar Day (ACLOUD)” aircraft campaign, and the ”Physical feedbacks of Arctic boundary layer, Sea ice, Cloud and AerosoL (PASCAL)” ice breaker expedition. Both observational studies were performed in the framework of the German ”ArctiC Amplification:Climate Relevant Atmospheric and SurfaCe Processes, and Feedback Mechanisms (AC)3” project. They took place in the vicinity of Svalbard (Norway) in May and June 2017. ACLOUD and PASCAL explored four pieces of the Arctic cloud puzzle: Cloud properties, aerosol impact on clouds, atmospheric radiation, and turbulent-dynamical processes. The two instrumented Polar 5 and Polar 6 aircraft, the icebreaker research vessel (RV) Polarstern, an ice-floe camp including an instrumented tethered balloon, and the permanent, ground-based measurement station at Ny-Ålesund (Svalbard) were employed to observe Arctic low and mid-level, mixed-phase clouds, and to investigate related atmospheric and surface processes. The Polar 5 aircraft served as a remote sensing observatory examining the clouds from above by downward-looking sensors; the Polar 6 aircraft operated as a flying in-situ measurement laboratory sampling inside and below the clouds. Most of the collocated Polar 5/6 flights were conducted either above RV Polarstern or over the Ny-Ålesund station, both of which monitored the clouds from below using similar but upward-looking remote sensing techniques as the Polar 5 aircraft. Several of the flights were carried out underneath collocated satellite tracks. The paper motivates the scientific objectives of the ACLOUD/PASCAL observations and describes the measured quantities, retrieved parameters, and the applied complementary instrumentation. Furthermore, it discusses selected measurement results, and poses critical research questions to be answered in future papers analyzing the data from the two field campaigns.

In this study, we present the development of a mobile system to measure real-world total respiratory tract deposition of inhaled ambient black carbon (BC). Such information can be used to supplement the existing knowledge on air pollution-related health effects, especially in the regions where the use of standard methods and intricate instrumentation is limited. The study is divided in two parts. Firstly, we present the design of portable system and methodology to evaluate the exhaled air BC content. We demonstrate that under real-world conditions, the proposed system exhibit negligible particle losses, and can additionally be used to determine the minute ventilation. Secondly, exemplary experimental data from the system is presented. A feasibility study was conducted in the city of La Paz, Bolivia. In a pilot experiment, we found that the cumulative total respiratory tract deposition dose over 1-h commuting trip would result in approximately 2.6 μg of BC. This is up to 5 times lower than the values obtained from conjectural approach (e.g. using physical parameters from previously reported worksheets). Measured total respiratory tract deposited BC fraction varied from 39% to 48% during walking and commuting inside a micro-bus, respectively. To the best of our knowledge, no studies focusing on experimental determination of real-world deposition dose of BC have been performed in developing regions. This can be especially important because the BC mass concentration is significant and determines a large fraction of particle mass concentration. In this work, we propose a potential method, recommendations, as well as the limitations in establishing an easy and relatively cheap way to estimate the respiratory tract deposition of BC. In this study we present a novel method to measure real-world respiratory tract deposition dose of Black Carbon. Results from a pilot study in La Paz, Bolivia, are presented. (Less)

As nitrous acid (HONO) photolysis is an important source of hydroxyl radical (OH), apportionment of the ambient HONO sources is necessary to better understand atmospheric oxidation. Based on the data HONO-related species and various parameters measured during the one-month campaign at Wangdu (a rural site in North China plain) in summer 2014, a box model was adopted with input of current literature parametrizations for various HONO sources (nitrogen dioxide heterogeneous conversion, photoenhanced conversion, photolysis of adsorbed nitric acid and particulate nitrate, acid displacement, and soil emission) to reveal the relative importance of each source at the rural site. The simulation results reproduced the observed HONO production rates during noontime in general but with large uncertainty from both the production and destruction terms. NO2 photoenhanced conversion and photolysis of particulate nitrate were found to be the two major mechanisms with large potential of HONO formation but the associated uncertainty may reduce their importance to be nearly negligible. Soil nitrite was found to be an important HONO source during fertilization periods, accounted for (80 ± 6)% of simulation HONO during noontime. For some episodes of the biomass burning, only the NO2 heterogeneous conversion to HONO was promoted significantly. In summary, the study of the HONO budget is still far from closed, which would require a significant effort on both the accurate measurement of HONO and the determination of related kinetic parameters for its production pathways.

Mobile measurements of PM2.5 and black carbon (BC) mass concentrations were performed near regular monitoring stations in order to gain deeper understanding of the drivers of pedestrian exposure to traffic-related air pollution. The following investigations have been done: A) Yearlong measurements in an area around a street canyon approximately 3 km airline distance from the city center of Leipzig showed that the spatial distributions of both pollutants are elevated during wintertime. The patterns of the BC mass concentration, however, consistently showed a strong influence from traffic emissions in the street, while the PM2.5 mass concentration was more dependent on the regional background and less on urban sources. B) Measurements in the city of Dresden near two regular monitoring stations, one at a roadside and one in urban background areas revealed differences between the two in terms of the BC mass concentrations, with slightly higher concentrations at the traffic area. However, no significant differences between the spatial distributions of PM2.5 mass concentrations were observed. The background measurements of the PM2.5 mass concentrations seem to be generally representative for the residential area. C) Measurements near a regular monitoring station located at a junction of the inner-city ring road of Leipzig showed that it is representative of its immediate vicinity in terms of BC mass concentrations. However, the PM2.5 mass concentration varied by a factor 2, reaching the highest levels near in the central tram station about 200 m away. The central tram station seems to significantly influence the PM2.5 mass concentration. These results of the three studies provide a better understanding of the variability of these two parameters in urban areas in Leipzig and Dresden, helping local policy makers to interpret better the measured air pollution.

Aerosolized black carbon is monitored worldwide to quantify its impact on air quality and climate. Given its importance, measurements of black carbon mass concentrations must be conducted with instruments operating in quality-checked and ensured conditions to generate data which are reliable and comparable temporally and geographically. In this study, we report the results from the largest characterization and intercomparison of filter-based absorption photometers, the Aethalometer model AE33, belonging to several European monitoring networks. Under controlled laboratory conditions, a total of 23 instruments measured mass concentrations of black carbon from three well-characterized aerosol sources: synthetic soot, nigrosin particles, and ambient air from the urban background of Leipzig, Germany. The objective was to investigate the individual performance of the instruments and their comparability; we analyzed the response of the instruments to the different aerosol sources and the impact caused by the use of obsolete filter materials and the application of maintenance activities. Differences in the instrument-to-instrument variabilities from equivalent black carbon (eBC) concentrations reported at 880 nm were determined before maintenance activities (for soot measurements, average deviation from total least square regression was −2.0 % and the range −16 % to 7 %; for nigrosin measurements, average deviation was 0.4 % and the range −15 % to 17 %), and after they were carried out (for soot measurements, average deviation was −1.0 % and the range −14 % to 8 %; for nigrosin measurements, the average deviation was 0.5 % and the range −12 % to 15 %). The deviations are in most of the cases explained by the type of filter material employed by the instruments, the total particle load on the filter, and the flow calibration. The results of this intercomparison activity show that relatively small unit-to-unit variability of AE33-based particle light absorbing measurements is possible with well-maintained instruments. It is crucial to follow the guidelines for maintenance activities and the use of the proper filter tape in the AE33 to ensure high quality and comparable black carbon (BC) measurements among international observational networks., ACTRIS and COLOSSAL provided financial support for the execution of the experiments. Instrument S04-00387 is operated and maintained thanks to the Spanish Ministry of Science and Innovation (project nos. CGL2016-81092-R, CGL2017-42 90884REDT, and RTI2018.101154.A.I00). Gloria Titos is funded by the Juan de la Cierva-Incorporación postdoctoral program (grant no. IJCI-2016-29838). IMT Lille Douai (Joel Ferreira De Brito, Veronique Riffault) received financial support from the Labex CaPPA project, which is funded by the French National Research Agency (ANR) through the PIA (Programme d'Investissement d'Avenir) (contract no. ANR-11-LABX-0005-01), and the CLIMIBIO project; both projects are financed by the Regional Council “Hauts-de-France” and the European Regional Development Fund (ERDF). The operation of instruments S00-00055 and S02-00156 is funded by the projects CRISOL (MINECO/AEI/FEDER, UE; grant no. CGL2017-85344-R) and TIGAS-CM (grant no. Y2018/EMT-5177).

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.