New particle formation is an important source of Arctic atmospheric particles and cloud condensation nuclei, yet their precursor sources and molecular-level mechanisms remain poorly understood. Here we report comprehensive ship-based observations from 19 May to 26 June 2022 from southeastern to western Greenland and into the Davis Strait's marginal ice zone to investigate sources and processes controlling atmospheric particles and cloud condensation nuclei. Our observations provide field evidence of frequent nucleation events driven by the multicomponent iodine oxoacid and sulfuric acid mechanism recently identified in laboratory studies. Newly formed particles grew rapidly beyond 20 nm on 8 out of 13 nucleation days, mainly driven by oxygenated organic molecules from aldehyde and monoterpene oxidation. We also report a previously unobserved class of iodine-containing oxygenated organic molecules that contributed to particle growth and enhanced cloud condensation nuclei formation. We show that marginal sea ice zone produces precursors that drive rapid new particle formation and enhance cloud condensation nuclei concentrations by up to 50-fold. Our findings demonstrate that Arctic iodine, sulfur and organic precursors can enhance cloud condensation nuclei abundance through new particle formation, highlighting a potential but unquantified pathway for influencing cloud cover, radiative balance and the hydrological cycle.
The Antarctic coastal zones are among the most biologically productive areas on Earth. The effect of marine microbiota on the emissions of sea spray particles, a critical factor for global climate and clouds, remains an open and actively researched question. Here, by means of in situ ship-borne bubble-bursting SSA production experiments at multiple locations around the Antarctic Peninsula, we show a 2-fold variability in the 10-500 nm size-resolved SSA number concentrations. We observed that the organic chemical composition of seawater (SW) and surface microlayers (SML) clearly impacts SSA number concentrations. SW and SML samples with saccharides, proteins, and N-osmolytes were less efficient at emitting SSA compared with waters rich in biotic material originating from lipids, such as fatty acids and polyols. We found that the dissolved organic carbon (DOC) fraction containing lipid degradation products and polyols indicates higher SSA production. Our results indicate that low concentration organic components, rather than the most abundant classes of biomolecules, influence the ability to be aerosolized, with strong chemical selectivity affecting SSA production.
The formation of cloud condensation nuclei is a critical but uncertain factor in Arctic climate dynamics. A major nuclei contributor is new particle formation, yet the geographical variations in activity and the factors driving it remain poorly understood. Here, we present a nine-year (2010–2018) analysis of atmospheric particle number size distributions from Tiksi, Russia, integrated with air mass trajectory modelling and ocean remote sensing. We show that aerosol formation rates are significantly enhanced—particle formation rates increase by 300
Black carbon (BC) is an important short-lived climate forcer that contributes to Arctic warming, yet observations of BC in the Arctic marine boundary layer remain sparse. Here, we report shipborne measurements of refractory BC (rBC) mass and particle mixing state during a cruise from southeast to west Greenland in May-June 2022. Using a single-particle soot photometer (SP2XR) and transmission electron microscopy (TEM), we characterize both rBC concentrations and individual-particle morphology, representing one of the first ship-based SP2XR data sets in the Arctic marine boundary layer. rBC concentrations were highest in the Greenland coastal region (2.4 ng m-3), compared with the open ocean (1.7 ng m-3) and the marginal ice zone (0.6 ng m-3). Mixing-state analysis shows that 54% of soot particles in coastal air masses were externally mixed, consistent with relatively fresh emissions, whereas most soot particles over the open sea and sea-ice regions were internally mixed, indicative of aged, transported aerosol. FLEXPART modeling suggests BC enhancements along the Greenland coast. Our data indicate that Greenland acts as a regional source of BC to the Arctic marine boundary layer in late spring and early summer, when midlatitude transport is weak.
The loss of Arctic Sea ice enlarges the ocean water surface exposed to wind speed, increasing the emissions of sea spray aerosols (SSAs). Given the unique evolution of upper ocean salinity waters and ice-associated ecosystems, it is crucial to improve Arctic-specific SSA parametrizations to represent the currently poorly understood feedback processes. Here, by using Arctic ship-borne in situ aerosol tank laboratory experiments, we study SSA produced from open ocean, open leads, and melt ponds. We find a complex nonlinear, yet unresolved variation in SSA production associated with salinity and organic composition. Specifically, we find that melt ponds drastically reduce SSA production, whereas ice algal microgels may enhance it. During the summer 2017 cruise (research vessel Araon), we also carried out aerosol ambient measurements across the Chukchi and East Siberian Seas. Size resolved ambient particle number concentrations reveal at least 17% and 42% of ambient number aerosol concentrations (N10-300 nm and N100-300 nm, respectively) are possibly attributable to SSA. Our results may help modeling experiments using SSA parametrization currently suffering from large uncertainty for constraining the sea spray emission fluxes from leads, melt ponds, and salinity gradients encountered in the Arctic Ocean.
BTEX (benzene, toluene, ethylbenzene, and m-xylene,p-xylene, and o-xylene) are significant urban air pollutants. This study examines BTEX variability across 7 European countries using data from 22 monitoring sites in different urban settings (urban background, traffic, industry, and suburban background). Results indicate that the relative abundance of BTEX in urban areas follows the order toluene > benzene > m,p-xylene > o-xylene > ethylbenzene, with median mixing ratios of 266 ± 152, 163 ± 74, 129 ± 88, 53 ± 35, and 45 ± 27 ppt during the years 2017–2022, respectively. Seasonal trends show benzene had similar median concentrations across urban background, traffic, and industrial sites, indicating mixed sources. Toluene levels were highest in traffic and industrial areas, highlighting road traffic and industrial emissions. Ethylbenzene and xylenes showed equivalent levels in traffic and industrial areas but were lower in urban backgrounds. Peak BTEX levels occurred during morning and evening rush hours, linked to traffic, heating, and atmospheric stagnation. B/T ratios ranged from 0.29 ± 0.11 to 1.35 ± 0.95, and X/E ratios ranged from 1.75 ± 0.91 to 3.68 ± 0.30, indicating primary pollution from local traffic, followed by solvents, coatings, and biomass burning. Lifetime cancer risk from BTEX exposure was below the definite risk threshold (10−4) but above the permissible risk level (10−6), suggesting moderate risk from benzene and ethylbenzene, particularly in traffic and industrial areas. Additionally, the health index of BTEX at monitoring sites was generally lower than the threshold limit value, suggesting a low non-carcinogenic risk overall. This study offers essential insights into BTEX pollution in urban European environments.
In order to reduce the uncertainty of aerosol radiative forcing in global climate models, we need to better understand natural aerosol sources which are important to constrain the current and pre-industrial climate. Here, we analyse particle number size distributions (PNSDs) collected during a year (2015) across four coastal and inland Antarctic research bases (Halley, Marambio, Dome C and King Sejong). We utilise k-means cluster analysis to separate the PNSD data into six main categories. “Nucleation” and “bursting” PNSDs occur 28 %–48 % of the time between sites, most commonly at the coastal sites of Marambio and King Sejong where air masses mostly come from the west and travel over extensive regions of sea ice, marginal ice and open ocean and likely arise from new particle formation. “Aitken high”, “Aitken low” and “bimodal” PNSDs occur 37 %–68 % of the time, most commonly at Dome C on the Antarctic Plateau, and likely arise from atmospheric transport and ageing from aerosol originating likely in both the coastal boundary layer and free troposphere. “Pristine” PNSDs with low aerosol concentrations occur 12 %–45 % of the time, most commonly at Halley, located at low altitudes and far from the coastal melting ice and influenced by air masses from the west. Not only the sea spray primary aerosols and gas to particle secondary aerosol sources, but also the different air masses impacting the research stations should be kept in mind when deliberating upon different aerosol precursor sources across research stations. We infer that both primary and secondary components from pelagic and sympagic regions strongly contribute to the annual seasonal cycle of Antarctic aerosols. Our simultaneous aerosol measurements stress the importance of the variation in atmospheric biogeochemistry across the Antarctic region.
New particle formation (NPF) is a major source of atmospheric aerosol particles, including cloud condensation nuclei (CCN), by number globally. Previous research has highlighted that NPF is less frequent but more intense at roadsides compared to urban background. Here, we closely examine NPF at both background and roadside sites in urban Central Europe. We show that the concentration of oxygenated organic molecules (OOMs) is greater at the roadside, and the condensation of OOMs along with sulfuric acid onto new particles is sufficient to explain the growth at both sites. We identify a hitherto unreported traffic-related OOM source contributing 29% and 16% to total OOMs at the roadside and background, respectively. Critically, this hitherto undiscovered OOM source is an essential component of urban NPF. Without their contribution to growth rates and the subsequent enhancements to particle survival, the number of >50 nm particles produced by NPF would be reduced by a factor of 21 at the roadside site. Reductions to hydrocarbon emissions from road traffic may thereby reduce particle numbers and CCN counts.
Atmospheric new particle formation (NPF) is a naturally occurring phenomenon, during which high concentrations of sub-10 nm particles are created through gas to particle conversion. The NPF is observed in multiple environments around the world. Although it has observable influence onto annual total and ultrafine particle number concentrations (PNC and UFP, respectively), only limited epidemiological studies have investigated whether these particles are associated with adverse health effects. One plausible reason for this limitation may be related to the absence of NPF identifiers available in UFP and PNC data sets. Until recently, the regional NPF events were usually identified manually from particle number size distribution contour plots. Identification of NPF across multi-annual and multiple station data sets remained a tedious task. In this work, we introduce a regional NPF identifier, created using an automated, machine learning based algorithm. The regional NPF event tag was created for 65 measurement sites globally, covering the period from 1996 to 2023. The discussed data set can be used in future studies related to regional NPF.
Studies revealed airports as a prominent source of ultrafine particles (UFP), which can disperse downwind to residential areas, raising health concerns. To expand our understanding of how air traffic-related emissions influence total particle number concentration (PNC) in the airport's surrounding areas, we conduct long-term assessment of airborne particulate exposure before and after relocation of air traffic from "Otto Lilienthal" Airport (TXL) to Berlin Brandenburg Airport "Willy Brandt" (BER) in Berlin, Germany. Here, we provide insights into the spatial-temporal variability of PNC measured in 16 schools recruited for Berlin-Brandenburg Air Study (BEAR). The results show that the average PNC in Berlin was 7900 ± 7000 cm-3, consistent with other European cities. The highest median PNC was recorded in spring (6700 cm-3) and the lowest in winter (5100 cm-3). PNC showed a bi-modal increase during morning and evening hours at most measurement sites due to road-traffic emissions. A comparison between measurements at the schools and fixed monitoring sites revealed good agreement at distances up to 5 km. A noticeable decline in this agreement occurred as the distance between measurement sites increased. After TXL was closed, PNC in surrounding areas decreased by 30 %. The opposite trend was not seen after BER was re-opened after the COVID-lock-down, as the air traffic has not reached the full capacity yet. The analysis of particle number size distribution data showed that UFP number fraction exhibit seasonal variations, with higher values in spring and autumn. This can be explained by nucleation events, which notably affected PNC. The presented findings will play a pivotal role in forthcoming source attribution and epidemiological investigations, offering a holistic understanding of airports' impact on airborne pollutant levels and their health implications. The study calls for further investigations of air-traffic-related physical-chemical pollutant properties in areas found further away (> 10 km) from airports.
Air ions are electrically charged particles in air. They are ubiquitous in the natural environment and affect the Earth's radiation budget by accelerating the formation and growth of new aerosol particles. Despite this, few datasets exist exploring these effects in the urban environment. A neutral cluster and air ion spectrometer was deployed in Leipzig, Germany, to measure the number size distribution of charged particles from 0.8 to 42 nm, between 27 July and 25 August 2022. Following previous analyses, charged particles were classified into small (0.8-1.6 nm), intermediate (1.6-7.5 nm), and large (7.5-22 nm) fractions by mass diameter, and their mean concentrations (sum of positive and negative polarities) during the campaign were 405, 71.6, and 415 cm-3, respectively. The largest peaks in intermediate and large ions were explained by new particle formation (NPF), with intermediate ions correlating well with sulfuric acid dimer. Smaller morning and evening peaks were coincident with black carbon concentrations and attributed to primary emissions. NPF events, observed on 30 % of days, coincided with intense solar radiation and elevated sulfuric acid dimer. Small charged particles were primarily associated with radioactive decay and highest during the early hours, and they are unrelated to primary emissions or NPF. The apparent contributions of charged particles to 3 and 7.5 nm particle formation rates were 5.7 % and 12.7 %, respectively, with mean growth rates of 4.0 nm h(-1) between 3-7.5 nm and 5.2 nm h(-1) between 7.5 and 22 nm. The ratio of charged to total particle formation rates at 3 nm suggests a minor role for charged particles in NPF. We conclude that NPF is a primary source of > 3 nm ions in our data, with primary emissions being the major source in the absence of NPF.
Although many studies have discussed the impact of Europe's air quality, very limited research focused on the detailed phenomenology of ambient trace elements (TEs) in PM10 in urban atmosphere. This study compiled long-term (2013-2022) measurements of speciation of ambient urban PM10 from 55 sites of 7 countries (Switzerland, Spain, France, Greece, Italy, Portugal, UK), aiming to elucidate the phenomenology of 20 TEs in PM10 in urban Europe. The monitoring sites comprised urban background (UB, n = 26), traffic (TR, n = 10), industrial (IN, n = 5), suburban background (SUB, n = 7), and rural background (RB, n = 7) types. The sampling campaigns were conducted using standardized protocols to ensure data comparability. In each country, PM10 samples were collected over a fixed period using high-volume air samplers. The analysis encompassed the spatio-temporal distribution of TEs, and relationships between TEs at each site. Results indicated an annual average for the sum of 20 TEs of 90 +/- 65 ng/m(3), with TR and IN sites exhibiting the highest concentrations (130 +/- 66 and 131 +/- 80 ng/m(3), respectively). Seasonal variability in TEs concentrations, influenced by emission sources and meteorology, revealed significant differences (p < 0.05) across all monitoring sites. Estimation of TE concentrations highlighted distinct ratios between non-carcinogenic and carcinogenic metals, with Zn (40 +/- 49 ng/m(3)), Ti (21 +/- 29 ng/m(3)), and Cu (23 +/- 35 ng/m(3)) dominating non-carcinogenic TEs, while Cr (5 +/- 7 ng/m(3)), and Ni (2 +/- 6 ng/m(3)) were prominent among carcinogenic ones. Correlations between TEs across diverse locations and seasons varied, in agreement with differences in emission sources and meteorological conditions. This study provides valuable insights into TEs in pan-European urban atmosphere, contributing to a comprehensive dataset for future environmental protection policies.
Manganese (Mn) is a key cofactor in enzymes responsible for lignin decay (mainly Mn peroxidase), regulating the rate of litter degradation and carbon (C) turnover in temperate and boreal forest biomes.While soil Mn is mainly derived from bedrock, atmospheric Mn could also contribute to soil Mn cycling, especially within the surficial horizon, with implications for soil C cycling. However, quantification of the atmospheric Mn cycle, which comprises emissions from natural (desert dust, sea salts, volcanoes, primary biogenic particles, and wildfires) and anthropogenic sources (e.g. industrialization and land-use change due to agriculture) transport, and deposition into the terrestrial and marine ecosystem, remains uncertain. Here, we use compiled emission datasets for each identified source to model and quantify the atmospheric Mn cycle with observational constraints. We estimated global emissions of atmospheric Mn in aerosols (<10 µm in aerodynamic diameter) to be 1500 Gg Mn yr-1. Approximately 32% of the emissions come from anthropogenic sources. Deposition of the anthropogenic Mn shortened soil Mn “pseudo” turnover times in surficial soils about 1-m depth (ranging from 1,000 to over 10,000,000 years) by 1-2 orders of magnitude in industrialized regions. Such anthropogenic Mn inputs boosted the Mn-to-N ratio of the atmospheric deposition in non-desert dominated regions (between 5×10-5 and 0.02) across industrialized areas, but still lower than soil Mn-to-N ratio by 1-3 orders of magnitude. Correlation analysis revealed a negative relationship between Mn deposition and topsoil C density across temperate and (sub)tropical forests, illuminating the role of Mn deposition in these ecosystems.
Air quality is one of the most important factors in public health. While outdoor air quality is widely studied, the indoor environment has been less scrutinised, even though time spent indoors is typically much greater than outdoors. The emergence of low-cost sensors can help assess indoor air quality. This study provides a new methodology, utilizing low-cost sensors and source apportionment techniques, to understand the relative importance of indoor and outdoor air pollution sources upon indoor air quality. The methodology is tested with three sensors placed in different rooms inside an exemplar house (bedroom, kitchen and office) and one outdoors. When the family was present, the bedroom had the highest average concentrations for PM2.5 and PM10 (3.9 ± 6.8 ug/m3 and 9.6 ± 12.7 μg/m3 respectively), due to the activities undertaken there and the presence of softer furniture and carpeting. The kitchen, while presenting the lowest PM concentrations for both size ranges (2.8 ± 5.9 ug/m3 and 4.2 ± 6.9 μg/m3 respectively), presented the highest PM spikes, especially during cooking times. Increased ventilation in the office resulted in the highest PM1 concentration (1.6 ± 1.9 μg/m3), highlighting the strong effect of infiltration of outdoor air for the smallest particles. Source apportionment, via positive matrix factorisation (PMF), showed that up to 95 % of the PM1 was found to be of outdoor sources in all the rooms. This effect was reduced as particle size increased, with outdoor sources contributing >65 % of the PM2.5, and up to 50 % of the PM10, depending on the room studied. The new approach to elucidate the contributions of different sources to total indoor air pollution exposure, described in this paper, is easily scalable and translatable to different indoor locations.
This study aims to picture the phenomenology of urban ambient total lung deposited surface area (LDSA) (including head/throat (HA), tracheobronchial (TB), and alveolar (ALV) regions) based on multiple path particle dosimetry (MPPD) model during 2017-2019 period collected from urban background (UB, n = 15), traffic (TR, n = 6), suburban background (SUB, n = 4), and regional background (RB, n = 1) monitoring sites in Europe (25) and USA (1). Briefly, the spatial-temporal distribution characteristics of the deposition of LDSA, including diel, weekly, and seasonal patterns, were analyzed. Then, the relationship between LDSA and other air quality metrics at each monitoring site was investigated. The result showed that the peak concentrations of LDSA at UB and TR sites are commonly observed in the morning (06:00-8:00 UTC) and late evening (19:00-22:00 UTC), coinciding with traffic rush hours, biomass burning, and atmospheric stagnation periods. The only LDSA night-time peaks are observed on weekends. Due to the variability of emission sources and meteorology, the seasonal variability of the LDSA concentration revealed significant differences (p = 0.01) between the four seasons at all monitoring sites. Meanwhile, the correlations of LDSA with other pollutant metrics suggested that Aitken and accumulation mode particles play a significant role in the total LDSA concentration. The results also indicated that the main proportion of total LDSA is attributed to the ALV fraction (50 %), followed by the TB (34 %) and HA (16 %). Overall, this study provides valuable information of LDSA as a predictor in epidemiological studies and for the first time presenting total LDSA in a variety of European urban environments.
Estimates of tyre and brake wear emission factors are presented, derived from data collected from roadside and urban background sites on the premises of the University of Birmingham, located in the UK's second largest city. Size-fractionated particulate matter samples were collected at both sites concurrently in the spring/summer of 2019 and analysed for elemental concentrations and magnetic properties. Using Positive Matrix Factorisation (PMF), three sources were identified in the roadside mass increment of the 1.0-9.9 & mu;m stages of MOUDI impactors located at both sites, namely: brake dust (7.1%); tyre dust (9.6%); and crustal (83%). The large fraction of the mass apportioned to crustal material was suspected to be mainly from a nearby construction site rather than resuspension of road dust. By using Ba and Zn as elemental tracers, brake and tyre wear emission factors were estimated as 7.4 mg/veh.km and 9.9 mg/veh.km, respectively, compared with the PMF-derived equivalent values of 4.4 mg/veh.km and 11 mg/veh.km. Based on the magnetic measurements, an emission factor can be estimated independently for brake dust of 4.7 mg/veh.km. A further analysis was carried out on the concurrently measured roadside increment in the particle number size distribution (10 nm-10 & mu;m). Four factors were identified in the hourly measurements: traffic exhaust nucleation; traffic exhaust solid particles; windblown dust; and an unknown source. The high increment of the windblown dust factor, 3.2 & mu;g/m3, was comparable in magnitude to the crustal factor measured using the MOUDI samples (3.5 & mu;g/m3). The latter's polar plot indicated that this factor was dominated by a large neighbouring construction site. The number emission factors of the exhaust solid particle and exhaust nucleation factors were estimated as 2.8 and 1.9 x 1012/veh.km, respectively.
Diesel engines are a major contributor to emissions of both Black Carbon (BC) and ultrafine particles. Analysis of data from the only roadside monitoring site in Europe with a continuous dataset for size-segregated particle number count (Marylebone Road, London) from 2010 to 2021 reveals that the growing number of vehicles fitted with a Diesel Oxidation Catalyst (DOC) and Diesel Particle Filter (DPF) has been very effective in controlling the emissions of solid particles and hence BC, but that there has been little change in the liquid mode (<30 nm) particles, and that concentrations of ultrafine particles (<100 nm) still well exceed the threshold for "high" concentrations (>104 cm-3 /24-hour mean) defined by WHO. BC declined by 81% between 2014 and 2021, but the ultrafine particle (<100 nm) count declined by only 26%. Consequently, in locations worldwide with heavy diesel traffic, concentrations of ultrafine particles are likely to remain "high" for the foreseeable future unless more effective abatement technologies are implemented.
The Arctic is a rapidly changing ecosystem, with complex ice–ocean–atmosphere feedbacks. An important process is new particle formation (NPF), from gas-phase precursors, which provides a climate forcing effect. NPF has been studied comprehensively at different sites in the Arctic, ranging from those in the High Arctic and those at Svalbard to those in the continental Arctic, but no harmonised analysis has been performed on all sites simultaneously, with no calculations of key NPF parameters available for some sites. Here, we analyse the formation and growth of new particles from six long-term ground-based stations in the Arctic (Alert, Villum, Tiksi, Zeppelin Mountain, Gruvebadet, and Utqiaġvik). Our analysis of particle formation and growth rates in addition to back-trajectory analysis shows a summertime maxima in the frequency of NPF and particle formation rate at all sites, although the mean frequency and particle formation rates themselves vary greatly between sites, with the highest at Svalbard and lowest in the High Arctic. The summertime growth rate, condensational sinks, and vapour source rates show a slight bias towards the southernmost sites, with vapour source rates varying by around an order of magnitude between the northernmost and southernmost sites. Air masses back-trajectories during NPF at these northernmost sites are associated with large areas of sea ice and snow, whereas events at Svalbard are associated with more sea ice and ocean regions. Events at the southernmost sites are associated with large areas of land and sea ice. These results emphasise how understanding the geographical variation in surface type across the Arctic is key to understanding secondary aerosol sources and providing a harmonised analysis of NPF across the Arctic.
Successful air quality management and control not only requires measurements of air pollution levels. It also requires information on the sources of air pollution, and their relative magnitudes and importance, to plan and enact cost-effective control measures. This paper provides an important breakthrough towards the wider and more comprehensive use of source apportionment via low-cost techniques. Low-cost sensor measurements, along with the statistical methods of Positive Matrix Factorization (PMF) and k-means clustering, were able to successfully pinpoint and quantify the main sources of pollution in three regulatory important sites (a construction site, a quarry and a roadside). The anticipated levels of pollution, which were dependent on meteorological conditions and temporal variations, were assessed. The analysis provides information crucial for successful air quality management and control at a significantly lower cost than previously achieved. The strengths and weaknesses of the methodologies used are illustrated and discussed.
Atmospheric aerosols are important drivers of Arctic climate change through aerosol-cloud-climate interactions. However, large uncertainties remain on the sources and processes controlling particle numbers in both fine and coarse modes. Here, we applied a receptor model and an explainable machine learning technique to understand the sources and drivers of particle numbers from 10 nm to 20 μm in Svalbard. Nucleation, biogenic, secondary, anthropogenic, mineral dust, sea salt and blowing snow aerosols and their major environmental drivers were identified. Our results show that the monthly variations in particles are highly size/source dependent and regulated by meteorology. Secondary and nucleation aerosols are the largest contributors to potential cloud condensation nuclei (CCN, particle number with a diameter larger than 40 nm as a proxy) in the Arctic. Nonlinear responses to temperature were found for biogenic, local dust particles and potential CCN, highlighting the importance of melting sea ice and snow. These results indicate that the aerosol factors will respond to rapid Arctic warming differently and in a nonlinear fashion.