Search

In this work, new particle formation events (NPFs) occurring at two locations in southern Italy, the urban background site of Lecce (ECO station) and the coastal site of Lamezia Terme (LMT station), are identified and analyzed. The study aims to compare the properties of NPF events at the two sites, located 225 km away from each other and characterized by marked differences in terms of emission sources and local weather dynamics. Continuous measurements of particle number size distributions, in the size range from 10 to 800 m, were performed at both sites by a mobility particle size spectrometer (MPSS). The occurrence of NPF events, observed throughout the study period that lasted 5 years, produced different results in terms of frequency of occurrence: 25 % of the days at ECO and 9 % at LMT. NPF events showed seasonal patterns: higher frequency during spring and summer at the urban background site and the autumn–winter period at the coastal site. Some of these events happened simultaneously at both sites, indicating the occurrence of the nucleation process on a large spatial scale. Cluster analysis of 72 h back trajectories showed that during the NPF events the two stations were influenced by similar air masses, most of which originated from the north-western direction. Local meteorological conditions characterized by high pressure, with a prevalence of clear skies, low levels of relative humidity (RH < 52 %), and moderate winds (3–4 m s−1) dominated the NPF events at both sites. Notable differences were observed in SO2 and PM2.5 concentrations and H2SO4 proxy levels, resulting in ∼65 %, ∼80 %, and 50 % lower levels at LMT compared to ECO, respectively. It is likely that the lower level of that which is recognized as one of the main gas precursors involved in the nucleation process could be responsible for the smaller NPF frequency of occurrence (∼60 % less than ECO) observed in LMT.

Particle hygroscopicity plays a key role in determining the particle deposition in the human respiratory tract (HRT). In this study, the effects of hygroscopicity and mixing state on regional and total deposition doses on the basis of the particle number concentration for children, adults, and the elderly were quantified using the Multiple-Path Particle Dosimetry model, based on the size-resolved particle hygroscopicity measurements at HRT-like conditions (relative humidity = 98 %) performed in the North China Plain. The measured particle population with an external mixing state was dominated by hygroscopic particles (number fraction = (91.5 ± 5.7) %, mean ± standard deviation (SD); the same below). Particle hygroscopic growth in the HRT led to a reduction by around 24 % in the total doses of submicron particles for all age groups. Such a reduction was mainly caused by the growth of hygroscopic particles and was more pronounced in the pulmonary and tracheobronchial regions. Regardless of hygroscopicity, the elderly group of people had the highest total dose among three age groups, while children received the maximum total deposition rate. With 270 nm in diameter as the boundary, the total deposition doses of particles smaller than this diameter were overestimated, and those of larger particles were underestimated, assuming no particle hygroscopic growth in the HRT. From the perspective of the daily variation, the deposition rates of hygroscopic particles with an average of (2.88 ± 0.81) × 109 particles h−1 during the daytime were larger than those at night ((2.32 ± 0.24) × 109 particles h−1). On the contrary, hydrophobic particles interpreted as freshly emitted soot and primary organic aerosols exhibited higher deposition rates at nighttime ((3.39 ± 1.34) × 108 particles h−1) than those in the day ((2.58 ± 0.76) × 108 particles h−1). The traffic emissions during the rush hours enhanced the deposition rate of hydrophobic particles. This work provides a more explicit assessment of the impact of hygroscopicity and mixing state on the deposition pattern of submicron particles in the HRT.

With the growing evidence that high particle number concentrations may impact health, modelling their emissions and understanding formation processes is necessary, especially in cities where many people are exposed. As emission inventories of particle numbers and size distribution over cities are usually not available, a methodology is defined to estimate them from PM2.5 emissions and ratios of PM1 / PM2.5 and PM0.1 / PM2.5 by activity sector. In this methodology, a fitting parameter αem is used to redistribute the number concentrations in the lowest emission diameter range. This parameter is chosen by comparing measured and simulated number concentrations during non-nucleation days. The emission size distribution is then finely discretised by conserving both mass and number in each of the size ranges where emissions are specified. The methodology is applied over Greater Paris during the MEGAPOLI campaign (July 2009). Three-dimensional simulations are performed using the chemistry transport model Polair3D/Polyphemus coupled to the aerosol module SSH-aerosol to represent the evolution of particles by condensation, evaporation, coagulation, and nucleation, with a sectional approach for the size distribution. The model is first compared to measurements during non-nucleation days, and the influence over the month of July 2009 of three different nucleation parameterisations is assessed, i.e. binary (sulfuric acid, water), ternary (sulfuric acid, ammonia, water), and heteromolecular (extremely low-volatility organic compounds (ELVOCs) from monoterpenes and sulfuric acid). The modelled number concentrations compare very well to measurements, with an average normalised mean error of 42 % for the daily number concentrations of particles larger than 10 nm and 37 % for the number concentrations of particles larger than 100 nm. The influence of the binary nucleation is low, and the ternary nucleation scheme leads to better simulated number concentrations (in terms of bias and error) at only one site out of three, but it systematically reduces the model to measurement correlation, suggesting that ternary nucleation may not be the dominant process in new particle formation. However, the relative bias and error, as well as the correlation at suburban sites, are systematically improved using the heteromolecular nucleation scheme involving sulfuric acid and ELVOCs from monoterpenes. This suggests that heteromolecular nucleation may be important in cities, especially at suburban sites in summer, and that a better characterisation of the emissions of ELVOC precursors from traffic is needed.

Measurements of throughfall (TF) and wet deposition (WD) are a common method to assess nitrogen (N) and base cation (BC) deposition to forests. Using TF and WD, dry deposition (DD) is usually calculated with a canopy budget model (CBM) assuming similar BC to Na+ ratios in WD and DD. This assumption is especially uncertain for K+, since K+ is often bound to smaller particles compared to Na+. Here we asses this assumption by comparing the DD of K+ estimated with the CBM (DDKCBM) to the DD of K+ simulated with a process oriented DD model (“inferential model”, DDKINF). Simulation experiments were performed at two indicator forest stands (“virtual” broadleaved (BL) and coniferous (CF) forest) based on six years of daily PM2.5 and PM10 concentrations and weekly WD observations measured at the rural background research station Melpitz, Germany. On average, the K+:Na+ ratio in WD was 0.24 while the K+:Na+ ratio in DDINF was 0.43 (CF) and 0.40 (BL), respectively. Accordingly, DDKCBM would need to be multiplied by a correction factor of 1.77 (CF) and 1.66 (BL) to match DDKINF, with substantial variation between years (lowest correction factor: 0.98, highest correction factor: 3.89). However, applying the correction factors in CBM calculations at nearby ICP Forests monitoring sites had only little effect on total (WD+DD) deposition rates of N and BC. The results were robust against changes in the meteorological data used for the inferential model. Uncertainty arises from periods affected by presence of particles larger than 10 µm diameter, not covered by local measurements. A corresponding lower boundary estimate for the average underestimation of DDKCBM is a correction factor of 1.37 (CF) and 1.29 (BL). More work is required to assess to what extend the observed underestimation of DDKCBM is confirmed by other methods and at sites with different atmospheric conditions.

Anthropogenic and natural emissions contribute to enhanced concentrations of aerosols in the Arctic winter and early spring, with most attention being paid to anthropogenic aerosols that contribute to so-called Arctic haze. Less-well-studied wintertime sea-spray aerosols (SSAs) under Arctic haze conditions are the focus of this study, since they can make an important contribution to wintertime Arctic aerosol abundances. Analysis of field campaign data shows evidence for enhanced local sources of SSAs, including marine organics at Utqiaġvik (formerly known as Barrow) in northern Alaska, United States, during winter 2014. Models tend to underestimate sub-micron SSAs and overestimate super-micron SSAs in the Arctic during winter, including the base version of the Weather Research Forecast coupled with Chemistry (WRF-Chem) model used here, which includes a widely used SSA source function based on Gong et al. (1997). Quasi-hemispheric simulations for winter 2014 including updated wind speed and sea-surface temperature (SST) SSA emission dependencies and sources of marine sea-salt organics and sea-salt sulfate lead to significantly improved model performance compared to observations at remote Arctic sites, notably for coarse-mode sodium and chloride, which are reduced. The improved model also simulates more realistic contributions of SSAs to inorganic aerosols at different sites, ranging from 20 %–93 % in the observations. Two-thirds of the improved model performance is from the inclusion of the dependence on SSTs. The simulation of nitrate aerosols is also improved due to less heterogeneous uptake of nitric acid on SSAs in the coarse mode and related increases in fine-mode nitrate. This highlights the importance of interactions between natural SSAs and inorganic anthropogenic aerosols that contribute to Arctic haze. Simulation of organic aerosols and the fraction of sea-salt sulfate are also improved compared to observations. However, the model underestimates episodes with elevated observed concentrations of SSA components and sub-micron non-sea-salt sulfate at some Arctic sites, notably at Utqiaġvik. Possible reasons are explored in higher-resolution runs over northern Alaska for periods corresponding to the Utqiaġvik field campaign in January and February 2014. The addition of a local source of sea-salt marine organics, based on the campaign data, increases modelled organic aerosols over northern Alaska. However, comparison with previous available data suggests that local natural sources from open leads, as well as local anthropogenic sources, are underestimated in the model. Missing local anthropogenic sources may also explain the low modelled (sub-micron) non-sea-salt sulfate at Utqiaġvik. The introduction of a higher wind speed dependence for sub-micron SSA emissions, also based on Arctic data, reduces biases in modelled sub-micron SSAs, while sea-ice fractions, including open leads, are shown to be an important factor controlling modelled super-micron, rather than sub-micron, SSAs over the north coast of Alaska. The regional results presented here show that modelled SSAs are more sensitive to wind speed dependence but that realistic modelling of sea-ice distributions is needed for the simulation of local SSAs, including marine organics. This study supports findings from the Utqiaġvik field campaign that open leads are the primary source of fresh and aged SSAs, including marine organic aerosols, during wintertime at Utqiaġvik; these findings do not suggest an influence from blowing snow and frost flowers. To improve model simulations of Arctic wintertime aerosols, new field data on processes that influence wintertime SSA production, in particular for fine-mode aerosols, are needed as is improved understanding about possible local anthropogenic sources.

Early growth of atmospheric particles is essential for their survival and ability to participate in cloud formation. Many different atmospheric vapors contribute to the growth, but even the main contributors still remain poorly identified in many environments, such as high-altitude sites. Based on measured organic vapor and sulfuric acid concentrations under ambient conditions, particle growth during new particle formation events was simulated and compared with the measured particle size distribution at Chacaltaya Global Atmosphere Watch station in Bolivia (5240 m a.s.l.) during April and May 2018, as a part of the SALTENA (Southern Hemisphere high-ALTitude Experiment on particle Nucleation and growth) campaign . The simulations showed that the detected vapors were sufficient to explain the observed particle growth, although some discrepancies were found between modelled and measured particle growth rates. This study gives an insight on the key factors affecting the particle growth on the site. Low volatile organic compounds were found to be the main contributor to the particle growth, covering on average 65 % of simulated particle mass in particle with diameter of 40 nm In addition, sulfuric acid had a major contribution to the particle growth, covering at maximum 39 % of simulated particle mass in 40 nm particle during periods when volcanic activity was detected on the area, suggesting that volcanic emissions can greatly enhance the particle growth.

The interaction between water vapor and aerosol nanoparticles is important in atmospheric processes. Hygroscopicity of sub-10 nm organic nanoparticles and their concentration-dependent thermodynamic properties (e.g., water activity) in the highly supersaturated concentration range are, however, scarcely available. Here we investigate the size dependence of hygroscopicity of organics (i.e., levoglucosan, D-glucose) in dry particle diameter down to 6 nm using a nano-hygroscopicity tandem differential mobility analyzer (nano-HTDMA). Our results show that there is only weak size-dependent hygroscopic growth of both levoglucosan and D-glucose nanoparticles with diameters down to 20 nm. In the diameter range smaller than 20 nm (down to 6 nm), we observed strong size-dependent hygroscopic growth for D-glucose nanoparticles. The hygroscopic growth factors cannot be determined for levoglucosan below 20 nm due to its evaporation. In addition, we compare hygroscopicity measurements for levoglucosan and D-glucose nanoparticles with E-AIM (standard UNIFAC – functional group activity coefficients), the ideal solution theory, and differential Köhler analysis (DKA) predictions. The ideal solution theory describes the measured hygroscopic growth factors of levoglucosan with diameters down to 20 nm and D-glucose nanoparticles with diameters larger than 60 nm, while E-AIM (standard UNIFAC) can successfully predict the growth factors of D-glucose nanoparticles with diameters from 100 down to 6 nm at RH above 88 %–40 % (e.g., at RH above 88 % for 100 nm D-glucose, at RH above 40 % for 6 nm D-glucose). The use of the DKA method leads to good agreement with measured hygroscopic growth factors of D-glucose aerosol nanoparticles with diameters from 100 down to 6 nm. Predicted water activity for these aqueous organic solutions (i.e., levoglucosan, D-glucose) from different parameterization methods agrees well with observations in the low solute concentration range (< 20 mol kg−1) and starts to deviate from observations in the high solute concentration (> 20 mol kg−1).

To fight against the first wave of Coronavirus disease 2019 (COVID-19) in 2020, lockdown measures were implemented in most European countries. These lockdowns had well-documented effects on human mobility. We assessed the impact of the lockdown implementation and relaxation on air pollution by comparing daily particulate matter (PM), nitrogen dioxide (NO2), and ozone (O3) concentrations, as well as particle number size distributions (PNSD) and particle light absorption coefficients in-situ measurement data with values expected if no COVID-19 epidemic had occurred at 28 sites across Europe for the period 17 February – 31 May 2020. Expected PM, NO2 and O3 concentrations were calculated from the 2020 Copernicus Atmospheric Monitoring Service (CAMS) Ensemble forecasts, combined with 2019 CAMS Ensemble forecasts and measurement data. On average, lockdown implementations did not lead to a decrease in PM2.5 mass concentrations at urban sites, while relaxations resulted in a +26 ± 21% rebound. The impacts of lockdown implementation and relaxation on NO2 concentrations were more consistent (−29 ± 17 %, and +31 ± 30 %, respectively). The implementation of the lockdown measures also induced statistically significant increases in O3 concentrations at half of all sites (+13 % on average). An enhanced oxidizing capacity of the atmosphere could have boosted the production of secondary aerosol at those places. Changes in the wavelength dependence of the particle light absorption coefficients and PNSD were also examined at 14 and 13 sites, respectively. Since these variables are not calculated by the CAMS model, expected values were estimated from 2017–2019 measurement data. A significant change in the relative contributions of wood and fossil fuel burning to the concentration of black carbon during the lockdown was detected at 7 sites. The contribution of particles smaller than 70 nm to the total number of particles significantly changed at most of the urban sites, with a mean decrease of −7 ± 5 % coinciding with the lockdown implementation. Our study shows that the response of PM2.5 and PM10 mass concentrations to lockdown measures was not systematic at various sites across Europe for multiple reasons, the relationship between road traffic intensity and particulate air pollution being more complex than expected.

Residential wood combustion is a widespread practice in Europe with a serious impact on air quality, especially in mountainous areas. While there is a significant number of studies conducted in deep urbanized valleys and basins, little is known about the air pollution processes in rural shallow hollows, where around 30 % of the people in mountainous areas across Europe live. We aim to determine the influence of ground temperature inversions on wood combustion aerosol pollution in hilly, rural areas. The study uses Retje karst hollow (Loški Potok, Slovenia) as a representative site for mountainous and hilly rural areas in central and south-eastern Europe with residential wood combustion. Sampling with a mobile monitoring platform along the hollow was performed in December 2017 and January 2018. The backpack mobile monitoring platform was used for the determination of equivalent black carbon (eBC) and particulate matter (PM) mass concentrations along the hollow. To ensure high quality of mobile measurement data, intercomparisons of mobile instruments with reference instruments were performed at two air quality stations during every run. Our study showed that aerosol pollution events in the relief depression were associated with high local emission intensities originating almost entirely from residential wood burning and shallow temperature inversions (58 m on average). The eBC and PM mass concentrations showed stronger associations with the potential temperature gradient (R2=0.8) than with any other meteorological parameters taken into account (ambient temperature, relative humidity, wind speed, wind direction, and precipitation). The strong association between the potential temperature gradient and pollutant concentrations suggests that even a small number of emission sources (total 243 households in the studied hollow) in similar hilly and mountainous rural areas with frequent temperature inversions can significantly increase the levels of eBC and PM and deteriorate local air quality. During temperature inversions the measured mean eBC and PM2.5 mass concentrations in the whole hollow were as high as 4.5±2.6 and 48.0 ± 27.7 µg m−3, respectively, which is comparable to larger European urban centres.

Black carbon (BC) aerosols play an important role in climate systems. Estimating BC’s radiative effect requires knowledge of its mixing state and light absorption enhancement resulting from coatings by other materials. Observational studies have reported much lower light absorption enhancement factors (Eabs) than expected from laboratory studies and model estimates. This has led to an intensive debate on the true magnitude of BC’s climate impact. We find that the observed, apparently small Eabs cannot reflect the overall effect of BC coatings, as it does not include the persisting absorption enhancement by extremely low-volatility (eLV) organics that remain on the BC particles after passing through thermodenuders. Our observations show that eLV organics are extensively present in BC coatings, with a mass fraction of ∼5%–100%. Accounting for these eLV coatings, the observation estimates of Eabs increase substantially to up to 1.8–2.0. Our results highlight a strong radiative warming effect from atmospheric BC.

Atmospheric aerosol particles are a complex combination of primary emitted sources (biogenic and anthropogenic) and secondary aerosol resulting from the aging processes such as condensation, coagulation, and cloud processing. To better understand their sources, investigations have been focused on source identification in urban areas in the past, while rural background stations are normally less impacted by surrounding anthropogenic sources. Therefore, they are predisposed for studying the impact of long-range transport of anthropogenic aerosols. Moreover, long-term measurements can help to study the potential temporal changes in the sources. Here, the chemical composition and organic aerosol sources of submicron aerosol particles were investigated at the Central European rural-background research station, Melpitz, using a one yearlong dataset determined by an aerosol chemical speciation monitor (ACSM) and a multi-angle absorption photometer (MAAP) from September 2016 to August 2017. Melpitz represents due to its location the Central European aerosol. It is an ideal location to investigate the impact of long-range transport, since the location is influenced by less polluted air masses from westerly directions and more polluted continental air masses from Eastern Europe. The organic aerosol (OA) dominated the submicron particle mass concentration and showed strong seasonal variability ranging from 39 % (in winter) to 58 % (in summer). It was followed by sulphate (15 % and 20 %) and nitrate (24 % and 11 %). The OA source identification was performed using rolling positive matrix factorisation (PMF) approach to account for the potential temporal changes in the source profile (SoFi Pro). It was possible to split OA into five-factors with a distinct temporal variability and mass spectral signature. Three were associated to anthropogenic primary OA (POA) sources: hydrocarbon-like OA (HOA, 5.2 % of OA mass in winter and 6.8 % in summer), biomass burning OA (BBOA, 10.6 % and 6.1 %) and coal combustion OA (CCOA, 23 % and 8.7 %). Another two are secondary/processed oxygenated OA (OOA) sources: less-oxidized OOA (LO-OOA, 28.4 % and 36.7 %) and more-oxidized OOA (MO-OOA, 32.8 % and 41.8 %). Since equivalent black carbon (eBC) was clearly associated with the identified POA factors (sum of HOA, BBOA and CCOA, R2= 0. 87), eBC’s contribution to each of the POA factors was achieved using a multi-linear regression model. Consequently, CCOA represented the main anthropogenic sources of carbonaceous aerosol (sum of OA and eBC) not only during winter (56 % of POA in winter) but also in summer (13 % of POA in summer), followed by BBOA (29 % and 69 % of POA in winter and summer, respectively) and HOA (15 % and 18 % of POA in winter and summer, respectively). A seasonal air mass cluster analysis was used to understand the geographical origins of the different aerosol types and show that during both winter and summer time, PM1 (PM with aerodynamic diameter smaller than 1 µm) air masses with eastern influence was always associated with the highest mass concentration and the highest coal combustion fraction. Since during winter time, CCOA is a combination of domestic heating and power plants emissions, the summer contribution of CCOA emphasises the critical importance of coal power plants emissions to rural background aerosols and its impact on air quality, through long-range transportation.

Dimethyl sulfide (DMS) is the primary natural contributor to the atmospheric sulfur burden. Observations concerning the fate of DMS oxidation products after long-range transport in the remote free troposphere are, however, sparse. Here we present quantitative chemical ionization mass spectrometric measurements of DMS and its oxidation products sulfuric acid (H2SO4), methanesulfonic acid (MSA), dimethylsulfoxide (DMSO), dimethylsulfone (DMSO2), methanesulfinic acid (MSIA), methyl thioformate (MTF), methanesulfenic acid (MSEA, CH3SOH), and a compound of the likely structure CH3S(O)2OOH in the gas phase, as well as measurements of the sulfate and methanesulfonate aerosol mass fractions. The measurements were performed at the Global Atmosphere Watch (GAW) station Chacaltaya in the Bolivian Andes located at 5240 m above sea level (a.s.l.). DMS and DMS oxidation products are brought to the Andean high-altitude station by Pacific air masses during the dry season after convective lifting over the remote Pacific ocean to 6000–8000 m a.s.l. and subsequent long-range transport in the free troposphere (FT). Most of the DMS reaching the station is already converted to the rather unreactive sulfur reservoirs DMSO2 in the gas phase and methanesulfonate (MS−) in the particle phase, which carried nearly equal amounts of sulfur to the station. The particulate sulfate at Chacaltaya is however dominated by regional volcanic emissions during the time of the measurement and not significantly affected by the marine air masses. In one of the FT events, even some DMS was observed next to reactive intermediates such as methyl thioformate, dimethylsulfoxide, and methanesulfinic acid. Also for this event, back trajectory calculations show that the air masses came from above the ocean (distance >330 km) with no local surface contacts. This study demonstrates the potential impact of marine DMS emissions on the availability of sulfur-containing vapors in the remote free troposphere far away from the ocean.

In the Arctic, new particle formation (NPF) and subsequent growth processes are the keys to produce Aitken-mode particles, which under certain conditions can act as cloud condensation nuclei (CCNs). The activation of Aitken-mode particles increases the CCN budget of Arctic low-level clouds and, accordingly, affects Arctic climate forcing. However, the growth mechanism of Aitken-mode particles from NPF into CCN range in the summertime Arctic boundary layer remains a subject of current research. In this combined Arctic cruise field and modeling study, we investigated Aitken-mode particle growth to sizes above 80 nm. A mechanism is suggested that explains how Aitken-mode particles can become CCN without requiring high water vapor supersaturation. Model simulations suggest the formation of semivolatile compounds, such as methanesulfonic acid (MSA) in fog droplets. When the fog droplets evaporate, these compounds repartition from CCNs into the gas phase and into the condensed phase of nonactivated Aitken-mode particles. For MSA, a mass increase factor of 18 is modeled. The postfog redistribution mechanism of semivolatile acidic and basic compounds could explain the observed growth of >20 nm h−1 for 60-nm particles to sizes above 100 nm. Overall, this study implies that the increasing frequency of NPF and fog-related particle processing can affect Arctic cloud properties in the summertime boundary layer.

27 pages, 12 figures, supplement https://doi.org/10.5194/acp-23-389-2023.-- Data availability: All data sets used in this work that were obtained during the MOSAiC campaign will be made publicly available by 1 January 2023 via PANGAEA (https://www.pangaea.de/, last access: June 2022) or are already publicly available in the Department of Energy Atmospheric Radiation Measurement program (ARM) user facility data discovery tool (https://adc.arm.gov/discovery/#/, last access: March 2022). Data from the PANGAEA archive include the following. Meteorological observations from Polarstern: Schmithüsen, H.: Continuous meteorological surface measurement during POLARSTERN cruise PS122/1. Alfred Wegener Institute, Helmholtz Centre for Polar and Marine Research, Bremerhaven, PANGAEA [data set], https://doi.org/10.1594/PANGAEA.935221, 2021a. Schmithüsen, H.: Continuous meteorological surface measurement during POLARSTERN cruise PS122/2. Alfred Wegener Institute, Helmholtz Centre for Polar and Marine Research, Bremerhaven, PANGAEA [data set], https://doi.org/10.1594/PANGAEA.935222, 2021b. Schmithüsen, H.: Continuous meteorological surface measurement during POLARSTERN cruise PS122/3. Alfred Wegener Institute, Helmholtz Centre for Polar and Marine Research, Bremerhaven, PANGAEA [data set], https://doi.org/10.1594/PANGAEA.935223, 2021c. Schmithüsen, H.: Continuous meteorological surface measurement during POLARSTERN cruise PS122/4. Alfred Wegener Institute, Helmholtz Centre for Polar and Marine Research, Bremerhaven, PANGAEA [data set], https://doi.org/10.1594/PANGAEA.935224, 2021d. Schmithüsen, H.: Continuous meteorological surface measurement during POLARSTERN cruise PS122/5. Alfred Wegener Institute, Helmholtz Centre for Polar and Marine Research, Bremerhaven, PANGAEA [data set], https://doi.org/10.1594/PANGAEA.935225, 2021e. Black carbon (BC): Heutte, B., Beck, I., Quéléver, L., Jokinen, T., Laurila, T., Dada, L., Schmale, J.: Equivalent black carbon concentration in 10 minutes time resolution, measured in the Swiss container during MOSAiC 2019/2020, PANGAEA [data set], https://doi.org/10.1594/PANGAEA.952251, 2022. Particle number concentration (CPC3025): Beck, I., Quéléver, L., Laurila, T., Jokinen, T., and Schmale, J.: Continuous corrected particle number concentration data in 10 sec resolution, measured in the Swiss aerosol container during MOSAiC 2019/2020, PANGAEA [data set], https://doi.org/10.1594/PANGAEA.941886, 2022b. The ARM data include the following: Kuang, C., Singh, A., and Howie, J.: Scanning mobility particle sizer (AOSSMPS), ARM [data set], https://doi.org/10.5439/1476898, 2022. Kuang, C., Salwen, C., Boyer, M., and Singh, A.: Condensation Particle Counter (AOSCPCF), ARM [data set], https://doi.org/10.5439/1046184, 2022. The land-based PNSD data: Alert: Personal communication from Tak Chan and Sangeeta Sharma, 2022 (for details, see Croft et al., 2016). Villum: Personal communication from Jakob Boyd Pernov, 2022 (for details, see Nguyen et al., 2016). Zeppelin: Personal communication from Peter Tunved, 2022 (for details, see Tunved et al., 2013). Tiksi: Personal communication from Eija Asmi, 2022 (for details, see Asmi et al., 2016). Utqiaġvik: Freud, E., Krejci, R., Tunved, P., Leaitch, W. R., Nguyen, Q. T., Massling, A., Skov, H., and Barrie, L.: Hourly mean homogenised (dry diameter range 20 to 500 nm) observations of aerosol number size distributions from station Barrow, 2007-09-20 to 2015-07-09, PANGAEA [data set], https://doi.org/10.1594/PANGAEA.877329, 2017b. The land-based BC data: Villum: Personal communications from Daniel Thomas, Jakob Klenø Nøjgaard, and Andreas Massling, 2022 (for details, see Thomas et al., 2022). NOAA Barrow Atmospheric Baseline Observatory (Utqiaġvik) during 2020: personal communication from Elisabeth Andrews, 2022 (for processing details, see Schmale et al., 2022). Gruvebadet. The PSAP data are accessible at the Italian Arctic Data Center operated by the National Research Council of Italy: https://data.iadc.cnr.it/erddap/tabledap/ebc_2010_2020.html (last access: December 2021, refer to Schmale et al., 2022, for additional details). All other BC data sets used in this work will be made publicly available on EBAS (http://ebas-data.nilu.no/, last access: December 2021, refer to Schmale et al., 2022, for additional details). The Arctic Oscillation (AO) data are publicly available from the NOAA and the National Weather Service: https://www.cpc.ncep.noaa.gov/products/precip/CWlink/daily_ao_index/ao.shtml (last access: June 2022). An archive of the FLEXPART model output and quick looks for the whole campaign can be found at https://img.univie.ac.at/webdata/mosaic (last access: March 2022), The Arctic environment is rapidly changing due to accelerated warming in the region. The warming trend is driving a decline in sea ice extent, which thereby enhances feedback loops in the surface energy budget in the Arctic. Arctic aerosols play an important role in the radiative balance and hence the climate response in the region, yet direct observations of aerosols over the Arctic Ocean are limited. In this study, we investigate the annual cycle in the aerosol particle number size distribution (PNSD), particle number concentration (PNC), and black carbon (BC) mass concentration in the central Arctic during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition. This is the first continuous, year-long data set of aerosol PNSD ever collected over the sea ice in the central Arctic Ocean. We use a k-means cluster analysis, FLEXPART simulations, and inverse modeling to evaluate seasonal patterns and the influence of different source regions on the Arctic aerosol population. Furthermore, we compare the aerosol observations to land-based sites across the Arctic, using both long-term measurements and observations during the year of the MOSAiC expedition (2019–2020), to investigate interannual variability and to give context to the aerosol characteristics from within the central Arctic. Our analysis identifies that, overall, the central Arctic exhibits typical seasonal patterns of aerosols, including anthropogenic influence from Arctic haze in winter and secondary aerosol processes in summer. The seasonal pattern corresponds to the global radiation, surface air temperature, and timing of sea ice melting/freezing, which drive changes in transport patterns and secondary aerosol processes. In winter, the Norilsk region in Russia/Siberia was the dominant source of Arctic haze signals in the PNSD and BC observations, which contributed to higher accumulation-mode PNC and BC mass concentrations in the central Arctic than at land-based observatories. We also show that the wintertime Arctic Oscillation (AO) phenomenon, which was reported to achieve a record-breaking positive phase during January–March 2020, explains the unusual timing and magnitude of Arctic haze across the Arctic region compared to longer-term observations. In summer, the aerosol PNCs of the nucleation and Aitken modes are enhanced; however, concentrations were notably lower in the central Arctic over the ice pack than at land-based sites further south. The analysis presented herein provides a current snapshot of Arctic aerosol processes in an environment that is characterized by rapid changes, which will be crucial for improving climate model predictions, understanding link, This research has been supported by the Academy of Finland (grant no. 337552), Horizon 2020 (EMME-CARE, grant no. 856612), the US Department of Energy (grant no. DE-SC0022046), and the Swiss Polar Institute (grant no. 188478), With the institutional support of the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000928-S)

Understanding aerosol particle activation is essential for evaluating aerosol indirect effects (AIEs) on climate. Long-term measurements of aerosol particle activation help to understand the AIEs and narrow down the uncertainties of AIEs simulation. However, they are still scarce. In this study, more than 4 years of comprehensive aerosol measurements were utilized at the central European research station of Melpitz, Germany, to gain insight into the aerosol particle activation and provide recommendations on improving the prediction of number concentration of cloud condensation nuclei (CCN, NCCN). (1) The overall CCN activation characteristics at Melpitz are provided. As supersaturation (SS) increases from 0.1 % to 0.7 %, the median NCCN increases from 399 to 2144 cm−3, which represents 10 % to 48 % of the total particle number concentration with a diameter range of 10–800 nm, while the median hygroscopicity factor (κ) and critical diameter (Dc) decrease from 0.27 to 0.19 and from 176 to 54 nm, respectively. (2) Aerosol particle activation is highly variable across seasons, especially at low-SS conditions. At SS=0.1 %, the median NCCN and activation ratio (AR) in winter are 1.6 and 2.3 times higher than the summer values, respectively. (3) Both κ and the mixing state are size-dependent. As the particle diameter (Dp) increases, κ increases at Dp of ∼40 to 100 nm and almost stays constant at Dp of 100 to 200 nm, whereas the degree of the external mixture keeps decreasing at Dp of ∼40 to 200 nm. The relationships of κ vs. Dp and degree of mixing vs. Dp were both fitted well by a power-law function. (4) Size-resolved κ improves the NCCN prediction. We recommend applying the κ–Dp power-law fit for NCCN prediction at Melpitz, which performs better than using the constant κ of 0.3 and the κ derived from particle chemical compositions and much better than using the NCCN (AR) vs. SS relationships. The κ–Dp power-law fit measured at Melpitz could be applied to predict NCCN for other rural regions. For the purpose of improving the prediction of NCCN, long-term monodisperse CCN measurements are still needed to obtain the κ–Dp relationships for different regions and their seasonal variations.

Black carbon (BC) from incomplete combustion of biomass or fossil fuels is the strongest absorbing aerosol component in the atmosphere. Optical properties of BC are essential in climate models for quantification of their impact on radiative forcing. The global climate models, however, consider BC to be spherical particles, which causes uncertainties in their optical properties. Based on this, an increasing number of model-based studies provide databases and parameterization schemes for the optical properties of BC, using more realistic fractal aggregate morphologies. In this study, the reliability of the different modelling techniques of BC was investigated by comparing them to laboratory measurements. The modelling techniques were examined for bare BC particles in the first step and for BC particles with organic material in the second step. A total of six morphological representations of BC particles were compared, three each for spherical and fractal aggregate morphologies. In general, the aggregate representation performed well for modelling the particle light absorption coefficient σabs, single-scattering albedo SSA, and mass absorption cross-section MACBC for laboratory-generated BC particles with volume mean mobility diameters dp,V larger than 100 nm. However, for modelling Ångström absorption exponent AAE, it was difficult to suggest a method due to size dependence, although the spherical assumption was in better agreement in some cases. The BC fractal aggregates are usually modelled using monodispersed particles, since their optical simulations are computationally expensive. In such studies, the modelled optical properties showed a 25 % uncertainty in using the monodisperse size method. It is shown that using the polydisperse size distribution in combination with fractal aggregate morphology reduces the uncertainty in measured σabs to 10 % for particles with dp,V between 60–160 nm. Furthermore, the sensitivities of the BC optical properties to the various model input parameters such as the real and imaginary parts of the refractive index (mre and mim), the fractal dimension (Df), and the primary particle radius (app) of an aggregate were investigated. When the BC particle is small and rather fresh, the change in the Df had relatively little effect on the optical properties. There was, however, a significant relationship between app and the particle light scattering, which increased by a factor of up to 6 with increasing total particle size. The modelled optical properties of BC are well aligned with laboratory-measured values when the following assumptions are used in the fractal aggregate representation: mre between 1.6 and 2, mim between 0.50 and 1, Df from 1.7 to 1.9, and app between 10 and 14 nm. Overall, this study provides experimental support for emphasizing the importance of an appropriate size representation (polydisperse size method) and an appropriate morphological representation for optical modelling and parameterization scheme development of BC.

Urban traffic is a significant contributor of particulate matter to the environment (Kessinger et al. in https://www.umweltbundesamt.de/sites/default/files/medien/5750/publikationen/hgp_luftqualitaet_2020_bf.pdf, 2021). Hence, there is a high interest in the measured data of roadside immission measurement station. In the federal state Saxony (Germany), the State Office for Environment, Agriculture and Geology (LfULG) is responsible for supervision of the air pollution. In a joint project, the LfULG, the Leibniz Institute for Tropospheric Research (TROPOS) and the Chair of Combustion Engines and Powertrain Systems of the Technical University of Dresden (Lehrstuhl für Verbrennungsmotoren und Antriebssysteme, LVAS) measured the particulate immission* from a selection of passenger cars in an “environment simulation” Weinhold et al. (https://publikationen.sachsen.de/bdb/artikel/36768q, 2020). Especially direct injection spark ignition engines, DISI, without particle filter have a high particulate matter emission, depending on the operating condition. However, an increase of the particulate matter immission due to the rising market penetration of DISI engines was not measurable at the immission measurement stations of LfULG. To investigate the effect of vehicle exhaust emission and immission, an experiment was developed to measure particulate matter immission similar to road conditions on a chassis dynamometer. Five used cars with different engines, exhaust after treatment systems and mileage were evaluated regarding their emissions and particulate immissions. Unexpectedly, a high amount of ultrafine particulate matter smaller 100 nm was found during the emission measurements, although the exhaust emissions were completely extracted to the CVS measurement system. It was concluded that these particles were assignable to break and tire wear. This paper summarizes the most important findings, the complete report is available in Weinhold et al. (https://publikationen.sachsen.de/bdb/artikel/36768q, 2020).

A unique data set derived from remote sensing, airborne, and ground-based in situ measurements is presented. This measurement report highlights the known complexity of comparing multiple aerosol optical parameters examined with different approaches considering different states of humidification and atmospheric aerosol concentrations. Mie-theory-based modeled aerosol optical properties are compared with the respective results of airborne and ground-based in situ measurements and remote sensing (lidar and photometer) performed at the rural central European observatory at Melpitz, Germany. Calculated extinction-to-backscatter ratios (lidar ratios) were in the range of previously reported values. However, the lidar ratio is a function of the aerosol type and the relative humidity. The particle lidar ratio (LR) dependence on relative humidity was quantified and followed the trend found in previous studies. We present a fit function for the lidar wavelengths of 355, 532, and 1064 nm with an underlying equation of fLR(RH, γ(λ))=fLR(RH=0,λ)×(1-RH)-γ(λ), with the derived estimates of γ(355 nm) = 0.29 (±0.01), γ(532 nm) = 0.48 (±0.01), and γ(1064 nm) = 0.31 (±0.01) for central European aerosol. This parameterization might be used in the data analysis of elastic-backscatter lidar observations or lidar-ratio-based aerosol typing efforts. Our study shows that the used aerosol model could reproduce the in situ measurements of the aerosol particle light extinction coefficients (measured at dry conditions) within 13 %. Although the model reproduced the in situ measured aerosol particle light absorption coefficients within a reasonable range, we identified many sources for significant uncertainties in the simulations, such as the unknown aerosol mixing state, brown carbon (organic material) fraction, and the unknown aerosol mixing state wavelength-dependent refractive index. The modeled ambient-state aerosol particle light extinction and backscatter coefficients were smaller than the measured ones. However, depending on the prevailing aerosol conditions, an overlap of the uncertainty ranges of both approaches was achieved.

The formation of black carbon fractal aggregates (BCFAs) from combustion and subsequent ageing involves several stages resulting in modifications of particle size, morphology, and composition over time. To understand and quantify how each of these modifications influences the BC radiative forcing, the optical properties of BCFAs are modelled. Owing to the high computational time involved in numerical modelling, there are some gaps in terms of data coverage and knowledge regarding how optical properties of coated BCFAs vary over the range of different factors (size, shape, and composition). This investigation bridged those gaps by following a state-of-the-art description scheme of BCFAs based on morphology, composition, and wavelength. The BCFA optical properties were investigated as a function of the radius of the primary particle (ao), fractal dimension (Df), fraction of organics (forganics), wavelength (λ), and mobility diameter (Dmob). The optical properties are calculated using the multiple-sphere T-matrix (MSTM) method. For the first time, the modelled optical properties of BC are expressed in terms of mobility diameter (Dmob), making the results more relevant and relatable for ambient and laboratory BC studies. Amongst size, morphology, and composition, all the optical properties showed the highest variability with changing size. The cross sections varied from 0.0001 to 0.1 µm2 for BCFA Dmob ranging from 24 to 810 nm. It has been shown that MACBC and single-scattering albedo (SSA) are sensitive to morphology, especially for larger particles with Dmob > 100 nm. Therefore, while using the simplified core–shell representation of BC in global models, the influence of morphology on radiative forcing estimations might not be adequately considered. The Ångström absorption exponent (AAE) varied from 1.06 up to 3.6 and increased with the fraction of organics (forganics). Measurement results of AAE ≫ 1 are often misinterpreted as biomass burning aerosol, it was observed that the AAE of purely black carbon particles can be ≫ 1 in the case of larger BC particles. The values of the absorption enhancement factor (Eλ) via coating were found to be between 1.01 and 3.28 in the visible spectrum. The Eλ was derived from Mie calculations for coated volume equivalent spheres and from MSTM for coated BCFAs. Mie-calculated enhancement factors were found to be larger by a factor of 1.1 to 1.5 than their corresponding values calculated from the MSTM method. It is shown that radiative forcings are highly sensitive to modifications in morphology and composition. The black carbon radiative forcing ΔFTOA (W m−2) decreases up to 61 % as the BCFA becomes more compact, indicating that global model calculations should account for changes in morphology. A decrease of more than 50 % in ΔFTOA was observed as the organic content of the particle increased up to 90 %. The changes in the ageing factors (composition and morphology) in tandem result in an overall decrease in the ΔFTOA. A parameterization scheme for optical properties of BC fractal aggregates was developed, which is applicable for modelling, ambient, and laboratory-based BC studies. The parameterization scheme for the cross sections (extinction, absorption, and scattering), single-scattering albedo (SSA), and asymmetry parameter (g) of pure and coated BCFAs as a function of Dmob were derived from tabulated results of the MSTM method. Spanning an extensive parameter space, the developed parameterization scheme showed promisingly high accuracy up to 98 % for the cross sections, 97 % for single-scattering albedos (SSAs), and 82 % for the asymmetry parameter (g).

La Paz and El Alto are two fast-growing high-altitude Bolivian cities forming the second largest metropolitan area in the country, located between 3200 and 4050 m a.s.l. Together they host a growing population of around 1.8 million people. The air quality in this conurbation is strongly influenced by urbanization. However, there are no comprehensive studies that have assessed the sources of air pollution and their impacts on health. Despite being neighboring cities, the drastic change in altitude and topography between La Paz and El Alto together with different socio-economic activities lead to different sources, dynamics and transport of particulate matter (PM). In this investigation, PM10 samples were collected at two urban background stations located in La Paz and El Alto between April 2016 and June 2017. The samples were later analyzed for a wide range of chemical species including numerous source tracers (OC, EC, water-soluble ions, sugar anhydrides, sugar alcohols, trace metals, and molecular organic species). The US-EPA Positive Matrix Factorization (PMF v.5.0) receptor model was then applied for source apportionment of PM10. This is the first source apportionment study in South America that incorporates a large set of organic markers (such as levoglucosan, polycyclic aromatic hydrocarbons – PAH, hopanes and alkanes) together with inorganic species. The multisite PMF resolved 11 main sources of PM. The largest annual contribution to PM10 came from two major sources: the ensemble of the four vehicular emissions sources (exhaust and non-exhaust), together responsible for 35 % and 25 % of the measured PM in La Paz and El Alto, respectively, and dust contributing 20 % and 32 % to the total. Secondary aerosols contributed 22 % (24 %) in La Paz (El Alto). Agriculture-related smoke from biomass burning originated in the Bolivian lowlands and neighboring countries contributed to 8 % (7 %) of the total PM10 mass annually. This contribution increased to 17 % (13 %) between August–October. Primary biogenic emissions were responsible for 13 % (7 %) of the measured PM10 mass. Finally, it was possible to identify a profile related to open waste burning occurring between the months of May and August. Despite the fact that this source contributed only to 2 % (5 %) of the total PM10 mass, it constitutes the second largest source of PAHs, compounds potentially hazardous to health. Our analysis resulted in the identification of two specific traffic-related sources. In addition, we also identified a lubricant source (not frequently identified) and a non-exhaust emissions source. This study shows that PM10 concentrations in La Paz and El Alto region are mostly impacted by a limited number of local sources. In conclusion, dust, traffic emissions, open waste burning and biomass burning are the main sources to target in order to improve air quality in both cities.

Background Data from extensive mobile measurements (MM) of air pollutants provide spatially resolved information on pedestrians’ exposure to particulate matter (black carbon (BC) and PM2.5 mass concentrations). Objective We present a distributional regression model in a Bayesian framework that estimates the effects of spatiotemporal factors on the pollutant concentrations influencing pedestrian exposure. Methods We modeled the mean and variance of the pollutant concentrations obtained from MM in two cities and extended commonly used lognormal models with a lognormal-normal convolution (logNNC) extension for BC to account for instrument measurement error. Results The logNNC extension significantly improved the BC model. From these model results, we found local sources and, hence, local mitigation efforts to improve air quality, have more impact on the ambient levels of BC mass concentrations than on the regulated PM2.5. Significance Firstly, this model (logNNC in bamlss package available in R) could be used for the statistical analysis of MM data from various study areas and pollutants with the potential for predicting pollutant concentrations in urban areas. Secondly, with respect to pedestrian exposure, it is crucial for BC mass concentration to be monitored and regulated in areas dominated by traffic-related air pollution.

Ice-nucleating particles (INPs) initiate the primary ice formation in clouds at temperatures above ca. −38 ∘C and have an impact on precipitation formation, cloud optical properties, and cloud persistence. Despite their roles in both weather and climate, INPs are not well characterized, especially in remote regions such as the Arctic. We present results from a ship-based campaign to the European Arctic during May to July 2017. We deployed a filter sampler and a continuous-flow diffusion chamber for offline and online INP analyses, respectively. We also investigated the ice nucleation properties of samples from different environmental compartments, i.e., the sea surface microlayer (SML), the bulk seawater (BSW), and fog water. Concentrations of INPs (NINP) in the air vary between 2 to 3 orders of magnitudes at any particular temperature and are, except for the temperatures above −10 ∘C and below −32 ∘C, lower than in midlatitudes. In these temperature ranges, INP concentrations are the same or even higher than in the midlatitudes. By heating of the filter samples to 95 ∘C for 1 h, we found a significant reduction in ice nucleation activity, i.e., indications that the INPs active at warmer temperatures are biogenic. At colder temperatures the INP population was likely dominated by mineral dust. The SML was found to be enriched in INPs compared to the BSW in almost all samples. The enrichment factor (EF) varied mostly between 1 and 10, but EFs as high as 94.97 were also observed. Filtration of the seawater samples with 0.2 µm syringe filters led to a significant reduction in ice activity, indicating the INPs are larger and/or are associated with particles larger than 0.2 µm. A closure study showed that aerosolization of SML and/or seawater alone cannot explain the observed airborne NINP unless significant enrichment of INP by a factor of 105 takes place during the transfer from the ocean surface to the atmosphere. In the fog water samples with −3.47 ∘C, we observed the highest freezing onset of any sample. A closure study connecting NINP in fog water and the ambient NINP derived from the filter samples shows good agreement of the concentrations in both compartments, which indicates that INPs in the air are likely all activated into fog droplets during fog events. In a case study, we considered a situation during which the ship was located in the marginal sea ice zone and NINP levels in air and the SML were highest in the temperature range above −10 ∘C. Chlorophyll a measurements by satellite remote sensing point towards the waters in the investigated region being biologically active. Similar slopes in the temperature spectra suggested a connection between the INP populations in the SML and the air. Air mass history had no influence on the observed airborne INP population. Therefore, we conclude that during the case study collected airborne INPs originated from a local biogenic probably marine source.