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Atmospheric aerosol particles (also known as particulate matter) are central to the cause of the two greatest threats to human security: air pollution (~5 million premature deaths per year) and climate change (~0.5 million per year). Addressing these threats requires an understanding of particulate matter sources responsible for both extreme air pollution immediately affecting human health and less extreme levels affecting climate over longer timescales. Here, extraordinary levels of air pollution, with submicrometre aerosol (PM1) mass concentration surpassing 300 µg m−3, were observed in a moderately sized European city and are attributed to emissions from residential solid fuel—specifically peat and wood, often promoted as ‘slow-renewable’, ‘low-carbon’ or ‘carbon-neutral’ biomass. Using sophisticated fingerprinting techniques, we find that consumption of peat and wood in up to 12% and 1% of households, respectively, contributed up to 70% of PM1. The results from this approach can better inform emissions reduction policies and help to ensure the most appropriate air pollution sources are targeted. Given the far greater abundance of solid fuels and concomitant emissions required to match the calorific benefit of liquid fuels, even modest increases in the consumption of ‘green’-marketed solid fuels will disproportionally increase the frequency of extreme pollution events. Understanding the sources of particulate matter responsible for extreme air pollution and climate change is critical for designing adequate policies to protect the wellbeing of citizens. This study shows that extraordinary levels of particulate matter with diameter smaller than 1 µm were observed in Dublin in November 2016 and January 2017 and can be attributed to emissions from residential burning of peat and wood, often promoted as ‘slow renewables’.

8 pages, 4 figures, Organic oligomers were discovered in laboratory-generated atmospheric aerosol over a decade ago. However, evidence for the presence of oligomers in ambient aerosols is scarce and mechanisms for their formation have yet to be fully elucidated. In this work, three unique aerosol particle types internally mixed with High molecular weight organic compounds (HMW-OC) species - likely oligomers - were detected in ambient air using single particle Aerosol Time-Of-Flight Mass Spectrometry (ATOFMS) in Cork (Ireland) during winter 2009. These particle types can be described as follows: (1) HMW-OCs rich in organic nitrogen - possibly containing nitrocatechols and nitroguaiacols - originating from primary emissions of biomass burning particles during evening times; (2) HMW-OCs internally mixed with nitric acid, occurring in stagnant conditions during night time; and (3) HMW-OCs internally mixed with sea salt, likely formed via photochemical reactions during day time. The study exemplifies the power of methodologies capable of monitoring the simultaneous formation of organic and inorganic particle-phase reaction products. Primary emissions and atmospheric aging of different types of HMW-OC contributes to aerosol with a range of acidity, hygroscopic and optical properties, which can have different impacts on climate and health, This work was funded by the Ireland Higher Education Authority Programme for Research in Third Level Institutes (PRTL1) – Cycle 5, and the Irish Environmental Protection Agency. Additional founding by the Spanish Ministry of Economy through projects BIO-NUC (CGL2013-49020-R), and by the EU though the FP7-PEOPLE-2013-IOF programme (Project number 624680, MANU – Marine Aerosol NUcleations) and the Ramon y Cajal fellowship (RYC-2012-11922). The National Centre for Atmospheric Science NCAS Birmingham group is funded by the UK Natural Environment Research Council

In recent years, severe haze events often occurred in China, causing serious environmental problems. The mechanisms responsible for the haze formation, however, are still not well understood, hindering the forecast and mitigation of haze pollution. Our study of the 2012–13 winter haze events in Beijing shows that atmospheric water vapour plays a critical role in enhancing the heavy haze events. Under weak solar radiation and stagnant moist meteorological conditions in winter, air pollutants and water vapour accumulate in a shallow planetary boundary layer (PBL). A positive feedback cycle is triggered resulting in the formation of heavy haze: (1) the dispersal of water vapour is constrained by the shallow PBL, leading to an increase in relative humidity (RH); (2) the high RH induces an increase of aerosol particle size by enhanced hygroscopic growth and multiphase reactions to increase particle size and mass, which results in (3) further dimming and decrease of PBL height, and thus further depressing of aerosol and water vapour in a very shallow PBL. This positive feedback constitutes a self-amplification mechanism in which water vapour leads to a trapping and massive increase of particulate matter in the near-surface air to which people are exposed with severe health hazards.

An aerosol chemical speciation monitor (ACSM) was deployed to study the primary nonrefractory submicron particulate matter emissions from the burning of commercially available solid fuels (peat, coal, and wood) typically used in European domestic fuel stoves. Organic mass spectra (MS) from burning wood, peat, and coal were characterized and intercompared for factor analysis against ambient data. The reference profiles characterized in this study were used to estimate the contribution of solid fuel sources, along with oil combustion, to ambient pollution in Galway, Ireland using the multilinear engine (ME-2). During periods influenced by marine air masses, local source contribution had dominant impact and nonsea-spray primary organic emissions comprised 88% of total organic aerosol mass, with peat burning found to be the greatest contributor (39%), followed by oil (21%), coal (17%), and wood (11%). In contrast, the resolved oxygenated organic aerosol (OOA) dominated the aerosol composition in continental air masses, with contributions of 50%, compared to 12% in marine air masses. The source apportionment results suggest that the use of domestic solid fuels (peat, wood, and coal) for home heating is the major source of evening and night-time particulate pollution events despite their small use.

The importance of 3D winds (in particular updraft) in atmospheric science has motivated the adaptation of airborne wind instruments developed for manned aircraft, to the small size of Remotely Piloted Aircraft Systems (RPAS). Simultaneously, enhancements in RPAS technology have increased their contribution to many fields. In atmospheric research, lightweight RPAS (

Since the 1980's, measures mitigating the impact of transboundary air pollution have been implemented successfully as evidenced in the 1980-2014 record of atmospheric sulphur pollution over the NE-Atlantic, a key region for monitoring background northern-hemisphere pollution levels. The record reveals a 72-79% reduction in annual-average airborne sulphur pollution (SO4 and SO2, respectively) over the 35-year period. The NE-Atlantic, as observed from the Mace Head research station on the Irish coast, can be considered clean for 64% of the time during which sulphate dominates PM1 levels, contributing 42% of the mass, and for the remainder of the time, under polluted conditions, a carbonaceous (organic matter and Black Carbon) aerosol prevails, contributing 60% to 90% of the PM1 mass and exhibiting a trend whereby its contribution increases with increasing pollution levels. The carbonaceous aerosol is known to be diverse in source and nature and requires sophisticated air pollution policies underpinned by sophisticated characterisation and source apportionment capabilities to inform selective emissions-reduction strategies. Inauspiciously, however, this carbonaceous concoction is not measured in regulatory Air Quality networks. The research leading to these results has received funding from the European Union’s Seventh Framework Programme (FP7/2007–2013) project BACCHUS under grant agreement n°603445, the Irish Environmental Protection Agency, the HEA PRTLI4 project. peer-reviewed

Ice nucleating particles (INP) are known to affect the amount of ice in mixed-phase clouds, thereby influencing many of their properties. The atmospheric INP concentration changes by orders of magnitude from terrestrial to marine environments, which typically contain much lower concentrations. Many modelling studies use parameterizations for heterogeneous ice nucleation and cloud ice processes that do not account for this difference because they were developed based on measurements predominantly from terrestrial environments. Errors in the assumed INP concentration will influence the simulated amount of ice in mixed-phase clouds, leading to errors in top-of-atmosphere radiative flux and ultimately the climate sensitivity of climate models. Here we develop a global model of INP concentrations relevant for mixed-phase clouds based on laboratory and field measurements of ice nucleation by K-feldspar (an ice-active component of desert dust) and marine organic aerosols (from sea spray). The simulated global distribution of INP concentrations based on these two-species agrees much better with currently available ambient measurements than when INP concentrations are assumed to depend only on temperature or particle size. Underestimation of INP concentrations in some terrestrial locations may be due to neglect of INP from other terrestrial sources. Our model indicates that, on a monthly or yearly average basis, desert dusts dominate the contribution to the INP population over much of the world, but marine organics become increasingly important in the world's remote oceans and can dominate in the Southern Ocean at some time of the year. Furthermore, we show that day-to-day variability is important and since desert dust aerosol tends to be sporadic, marine organics dominate the INP population on many days per month in much of the mid and high latitude northern hemisphere. This study advances our understanding of which aerosol species need to be included in order to adequately describe the global and regional distribution of INP in models, which will guide ice nucleation researchers on where to focus future laboratory and field work.

[1] Primary-produced sea spray aerosol, typically comprising sea-salt, but also enriched with organic matter (OM) in biologically active oceanic regions, impacts the global radiative budget through contributions to aerosol optical depth. We show that sea spray light-scattering enhancement, f(RH), as a function of relative humidity (RH) is suppressed when enriched with OM. A new hygroscopic growth factor parameterization reveals a dual hygroscopicity state, flipping from high hygroscopicity and high f(RH) to low hygroscopicity and low f(RH) as the OM mixing volume percentage exceeds ~ 55% in sea spray. Under elevated wind speeds, this affects the Top-of-atmosphere direct radiative forcing (ΔF) by reducing the cooling contribution of sea spray by ~ 5.5 times compared to pure sea-salt spray. These results suggest a positive feedback coupling between the marine biosphere, sea spray aerosol, and the direct radiative budget.

This work focuses on transport and properties of ash from the Icelandic volcano Grimsvotn that erupted in spring 2011. Atmospheric transport of volcanic ash from the eruption was simulated using the Danish Emergency Response Model of the Atmosphere (DERMA). The arrivals of volcanic particles were detected on-line at Mace Head at the West coast of Ireland during volcanic plume advection identified by high resolution time of flight aerosol mass spectrometry (HR-ToF AMS). Based on DERMA information aerosol particles were collected in Copenhagen, Denmark, before predicted arrival of the ash plume and during a period where ash was present in the air. Analysis of the meteorological conditions shows that the particles collected before arrival of the volcanic ash may serve as a good reference sample allowing identification of significant changes in ambient aerosol properties during the volcanic ash event over Copenhagen. Using single particle analysis in scanning electron microscopy (SEM), data on structure, chemical composition, size and morphology of individual volcanic ash particles from the Grimsvotn eruption after atmospheric transport to Scandinavia are provided. Particles were sliced with Focused Ion Beam (FIB). Element mappings from cross-sections through collected volcanic ash particles reveal inhomogeneous distributions of the elements K, Mg, Fe and Ti.

Sixteen years (1994 – 2009) of ozone profiling by ozonesondes at Valentia Meteorological and Geophysical Observatory, Ireland (51.94° N, 10.23° W) along with a co-located MkIV Brewer spectrophotometer for the period 1993–2009 are analyzed. Simple and multiple linear regression methods are used to infer the recent trend, if any, in stratospheric column ozone over the station. The decadal trend from 1994 to 2010 is also calculated from the monthly mean data of Brewer and column ozone data derived from satellite observations. Both of these show a 1.5 % increase per decade during this period with an uncertainty of about ±0.25 %. Monthly mean data for March show a much stronger trend of ~ 4.8 % increase per decade for both ozonesonde and Brewer data. The ozone profile is divided between three vertical slots of 0–15 km, 15–26 km, and 26 km to the top of the atmosphere and a 11-year running average is calculated. Ozone values for the month of March only are observed to increase at each level with a maximum change of +9.2 ± 3.2 % per decade (between years 1994 and 2009) being observed in the vertical region from 15 to 26 km. In the tropospheric region from 0 to 15 km, the trend is positive but with a poor statistical significance. However, for the top level of above 26 km the trend is significantly positive at about 4 % per decade. The March integrated ozonesonde column ozone during this period is found to increase at a rate of ~6.6 % per decade compared with the Brewer and satellite positive trends of ~5 % per decade.

Over forty scientists from six countries convened in Raleigh, NC on June 4-6 2012 to review the status and prospects of sea spray aerosol research. Participants were researchers from the oceanography and atmospheric science communities, including academia, private industry, and government agencies. The recommendations from the working groups are summarized in a science prioritization matrix that is meant to prioritize the research agenda and identify areas of investigation by the magnitude of their impact on proposed science questions. Str

Based on the results of a pilot study in 2007, which found high mixing ratios of molecular iodine (I2) above the intertidal macroalgae (seaweed) beds at Mweenish Bay (Ireland), we extended the study to nine different locations in the vicinity of Mace Head Atmospheric Research Station on the west coast of Ireland during a field campaign in 2009. The mean values of I2 mixing ratio found above the macroalgae beds at nine different locations ranged from 104 to 393 ppt, implying a high source strength of I2. Such mixing ratios are sufficient to result in photochemically driven coastal new-particle formation events. Mixing ratios above the Ascophyllum nodosum and Fucus vesiculosus beds increased with exposure time: after 6 h exposure to ambient air the mixing ratios were one order of magnitude higher than those initially present. This contrasts with the emission characteristics of Laminaria digitata, where most I2 was emitted within the first half hour of exposure. Discrete in situ measurements (offline) of I2 emission from ambient air-exposed chamber experiments of L. digitata, A. nodosum and F. vesiculosus substantially supported the field observations. Further online and time-resolved measurements of the I2 emission from O3-exposed macroalgal experiments in a chamber confirmed the distinct I2 emission characteristics of A. nodosum and F. vesiculosus compared to those of L. digitata. The emission rates of A. nodosum and F. vesiculosus were comparable to or even higher than L. digitata after the initial exposure period of ~20–30 min. We suggest that A. nodosum and F. vesiculosus may provide an important source of photolabile iodine in the coastal boundary layer and that their impact on photochemistry and coastal new-particle formation should be reevaluated in light of their longer exposure at low tide and their widespread distribution.

[1] Initial efforts toward developing a combined organic-inorganic sea spray source function parameterization for large-scale models made use of chlorophyll-a (Chl-a) and wind speed as input parameters to combine oceanic biology and atmospheric dynamics. These studies reported a modest correlation coefficient (0.55) between chlorophyll-a and organic matter (OM) enrichment in sea spray, suggesting that chlorophyll-a is only partially suitable for predicting organic enrichment. A reconstructed chlorophyll-a field of the North Atlantic Ocean from GlobColour reveals an improved correlation of 0.72 between the fractional mass contribution of organics in sea spray and chlorophyll-a concentration. A similar analysis, using colored dissolved and detrital organic material absorption and particulate organic carbon concentration, revealed slightly lower correlation coefficients (0.65 and 0.68). These results indicate that to date, chlorophyll-a is the best biological surrogate for predicting sea spray organic enrichment. In fact, considering the minimal difference between the correlation coefficients obtained with the three ocean color products, there is no reason to substitute chlorophyll-a, which is the most accurate parameter obtained from ocean color data, with other biological surrogates being generally affected by larger and less known errors. The observed time lag between chlorophyll-a concentration and organic matter enrichment in aerosol suggests that biological processes in oceanic surface waters and their timescales should be considered when modeling the production of primary marine organic aerosol.

The Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) instrument on the polar orbiter Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) is an elastic backscatter lidar that produces a global uniformly-calibrated aerosol data set. Several Calibration/Validation (Cal/Val) studies for CALIOP conducted with ground-based lidars and CALIOP data showed large aerosol profile disagreements, both random and systematic. In an attempt to better understand these problems, we undertook a series of ground-based lidar measurements in Atlanta, Georgia, which did not provide better agreement with CALIOP data than the earlier efforts, but rather prompted us to investigate the statistical limitations of such comparisons. Meaningful Cal/Val requires intercomparison data sets with small enough uncertainties to provide a check on the maximum expected calibration error. For CALIOP total attenuated backscatter, reducing the noise to the required level requires averaging profiles along the ground track for distances of at least 1,500 km. Representative comparison profiles often cannot be acquired with ground-based lidars because spatial aerosol inhomogeneities introduce systematic error into the averages. These conclusions have implications for future satellite lidar Cal/Val efforts, because planned satellite lidars measuring aerosol backscatter, wind vector, and CO2 concentration profiles may all produce data requiring considerable along-track averaging for meaningful Cal/Val.

Highly time-resolved measurements of nitrous acid (HONO) were carried out with a highly sensitive long path absorption photometer (LOPAP) at an urban site of Xi'an in Western China from 24 July to 6 August 2015 to investigate the atmospheric variations, sources, and formation pathways of HONO. The concentrations of HONO vary from 0.02 to 4.3ppbv with an average of 1.12ppbv for the entire measurement period. The variation trends of HONO and NO2 are very similar and positively correlated which, together with the similar diurnal profiles of HONO/NO2 ratio and HONO, suggest the importance of heterogeneous conversion of HONO from NO2. The nocturnal HONO level is governed by heterogeneous formation from NO2, followed by homogeneous formation of NO with OH and then by direct emissions. Further, it is found that the heterogeneous formation of HONO is largely affected by relative humidity and aerosol surface. Daytime HONO budget analysis indicates that an additional unknown source with HONO production rate of 0.75ppbvh-1 is required to explain the observed HONO concentration, which contributes 60.8% of the observed daytime HONO.

Aerosol-cloud interactions (ACI) constitute the single largest uncertainty in anthropogenic radiative forcing. To reduce the uncertainties and gain more confidence in the simulation of ACI, models need to be evaluated against observations, in particular against measurements of cloud condensation nuclei (CCN). Numerous observations of CCN number concentration exist, and many closure studies have been performed to predict CCN number concentrations based on particle number size distributions, chemical composition, and the κ-Köhler theory. Most of these studies provide details for short time periods or focus on special environmental conditions. These observations, however, cannot address questions of large-scale temporal and spatial CCN variability. Here we analyze long-term observations of CCN number concentrations, particle number size distributions and chemical composition from twelve sites on three continents. Eight of these stations are part of the European Aerosols, Clouds, and Trace gases Research InfraStructure (ACTRIS). We group the observatories into categories according to their official classification: coastal background (Barrow, Alaska; Mace Head, Ireland; Finokalia, Crete; Noto Peninsula, Japan), rural background (Melpitz, Germany; Cabauw, the Netherlands; Vavihill, Sweden), alpine sites (Puy de Dôme, France; Jungfraujoch, Switzerland), remote forest sites (ATTO, Brazil; SMEAR, Finland) and the urban environment (Seoul, South Korea). Expectedly, CCN characteristics are highly variable across regions. However, they also vary within categories, most strongly in the coastal background group, where CCN number concentrations can vary by up to a factor of 30 within one season. In terms of particle activation behavior, most continental stations exhibit very similar relative activation ratios across the range of 0.1 to 1.0 % supersaturation. At the coastal sites the activation ratios spread more widely across the SS spectrum. Several stations show strong seasonal cycles of CCN number concentrations and particle number size distributions, e.g., at Barrow (Arctic Haze in spring), at the alpine stations (stronger influence of polluted boundary layer air masses in summer), the rain forest (wet and dry season), or Finokalia (forest fire influence in fall). The rural background and urban sites exhibit relatively little variability throughout the year while short-term variability can be high especially at the urban site. The average hygroscopicity parameter, κ, calculated from the chemical composition of submicron particles, was highest at the coastal site of Mace Head (0.6) and the lowest at the rain forest station ATTO (0.2–0.3). We performed closure studies to predict CCN number concentrations from the particle number size distribution and chemical composition measurements. The prediction accuracy for the average concentrations is high. The ratio between predicted and measured CCN concentrations is between 0.87 and 1.4. The temporal variability is also well represented, as reflected by Pearson correlation coefficients > 0.87. We also conducted a series of sensitivity studies for the ratio of predicted versus measured CCN concentration, where we varied the hygroscopicity parameter κ, and made simple assumptions for aerosol particle number concentrations and size distributions. Uncertain particle number concentrations and their size distributions significantly impair the accuracy in predicting temporal variability and hence of absolute concentrations, while the effect of uncertain κ values is limited to the predicted CCN number concentration. Information on CCN number concentrations at many locations is important to better characterize ACI and their radiative forcing. Long-term comprehensive aerosol particle characterizations are labor intensive and costly. For observatories where such efforts are out of scope to obtain nevertheless long-term information of CCN number concentrations, we recommend conducting collocated CCN number concentration and particle number size distribution measurements at individual locations throughout one year at least to derive a seasonally resolved hygroscopicity parameter. This way, CCN number concentrations can be calculated based on continued particle number size distribution information only. This approach is a good alternative to deriving kappa from time-resolved chemical composition measurements which are costly and may still not cover the appropriate size range. Additionally, given the variability in observations at sites of the same category, a certain density in spatial coverage of observations is needed, especially along coastlines. We recommend operating "migrating-CCNCs" at priority locations, identified by model evaluation, around the globe where long-term particle number size distribution data are already available.

International audience; We evaluated a modified VBS (volatility basis set) scheme to treat biomass-burning-like organic aerosol (BBOA) implemented in CAMx (Comprehensive Air Quality Model with extensions). The updated scheme was param-eterized with novel wood combustion smog chamber experiments using a hybrid VBS framework which accounts for a mixture of wood burning organic aerosol precursors and their further functionalization and fragmentation in the atmosphere. The new scheme was evaluated for one of the winter EMEP intensive campaigns (February-March 2009) against aerosol mass spectrometer (AMS) measurements performed at 11 sites in Europe. We found a considerable improvement for the modelled organic aerosol (OA) mass compared to our previous model application with the mean fractional bias (MFB) reduced from −61 to −29 %. We performed model-based source apportionment studies and compared results against positive matrix factorization (PMF) analysis performed on OA AMS data. Both model and observations suggest that OA was mainly of secondary origin at almost all sites. Modelled secondary organic aerosol (SOA) contributions to total OA varied from 32 to 88 % (with an average contribution of 62 %) and absolute concentrations were generally under-predicted. Modelled primary hydrocarbon-like organic aerosol (HOA) and primary biomass-burning-like aerosol (BBPOA) fractions contributed to a lesser extent (HOA from 3 to 30 %, and BBPOA from 1 to 39 %) with average contributions of 13 and 25 %, respectively. Modelled BBPOA fractions were found to represent 12 to 64 % of the total residential-heating-related OA, with increasing contributions at stations located in the northern part of the domain. Source apportionment studies were performed to assess the contribution of residential and non-residential combustion precursors to the total SOA. Non-residential combustion and road transportation sector contributed about 30-40 % to SOA formation (with increasing contributions at urban and near industrialized sites), whereas residential combustion (mainly related to wood burning) contributed to a larger extent, around 60-70 %. Contributions to OA from residential combustion precursors in different volatility ranges were Published by Copernicus Publications on behalf of the European Geosciences Union. 7654 G. Ciarelli et al.: Modelling winter organic aerosol at the European scale with CAMx also assessed: our results indicate that residential combustion gas-phase precursors in the semivolatile range (SVOC) contributed from 6 to 30 %, with higher contributions predicted at stations located in the southern part of the domain. On the other hand, the oxidation products of higher-volatility precursors (the sum of intermediate-volatility compounds (IVOCs) and volatile organic compounds (VOCs)) contribute from 15 to 38 % with no specific gradient among the stations. Although the new parameterization leads to a better agreement between model results and observations, it still under-predicts the SOA fraction, suggesting that uncertainties in the new scheme and other sources and/or formation mechanisms remain to be elucidated. Moreover, a more detailed characterization of the semivolatile components of the emissions is needed.

Cloud condensation nuclei (CCN) number concentrations alongside with submicrometer particle number size distributions and particle chemical composition have been measured at atmospheric observatories of the Aerosols, Clouds, and Trace gases Research InfraStructure (ACTRIS) as well as other international sites over multiple years. Here, harmonized data records from 11 observatories are summarized, spanning 98,677 instrument hours for CCN data, 157,880 for particle number size distributions, and 70,817 for chemical composition data. The observatories represent nine different environments, e.g., Arctic, Atlantic, Pacific and Mediterranean maritime, boreal forest, or high alpine atmospheric conditions. This is a unique collection of aerosol particle properties most relevant for studying aerosol-cloud interactions which constitute the largest uncertainty in anthropogenic radiative forcing of the climate. The dataset is appropriate for comprehensive aerosol characterization (e.g., closure studies of CCN), model-measurement intercomparison and satellite retrieval method evaluation, among others. Data have been acquired and processed following international recommendations for quality assurance and have undergone multiple stages of quality assessment.

Currently many ground-based atmospheric stations include in-situ measurements of aerosol physical and optical properties, resulting in more than 20 long-term (> 10 yr) aerosol measurement sites in the Northern Hemisphere and Antarctica. Most of these sites are located at remote locations and monitor the aerosol particle number concentration, wavelength-dependent light scattering, backscattering, and absorption coefficients. The existence of these multi-year datasets enables the analysis of long-term trends of these aerosol parameters, and of the derived light scattering Ångström exponent and backscatter fraction. Since the aerosol variables are not normally distributed, three different methods (the seasonal Mann-Kendall test associated with the Sen's slope, the generalized least squares fit associated with an autoregressive bootstrap algorithm for confidence intervals, and the least-mean square fit applied to logarithms of the data) were applied to detect the long-term trends and their magnitudes. To allow a comparison among measurement sites, trends on the most recent 10 and 15 yr periods were calculated. No significant trends were found for the three continental European sites. Statistically significant trends were found for the two European marine sites but the signs of the trends varied with aerosol property and location. Statistically significant decreasing trends for both scattering and absorption coefficients (mean slope of −2.0% yr−1) were found for most North American stations, although positive trends were found for a few desert and high-altitude sites. The difference in the timing of emission reduction policy for the Europe and US continents is a likely explanation for the decreasing trends in aerosol optical parameters found for most American sites compared to the lack of trends observed in Europe. No significant trends in scattering coefficient were found for the Arctic or Antarctic stations, whereas the Arctic station had a negative trend in absorption coefficient. The high altitude Pacific island station of Mauna Loa presents positive trends for both scattering and absorption coefficients.

A regional climate model is used to assess changes in atmospheric ozone for the years 2030, 2050 and 2100 relative to 2006 brought about by changes in meteorology and emissions. The simulations are evaluated against ozone measurements for 2006, exhibiting good agreement between the model-predicted measurements and the measured annual cycles. Under the RCP6 emission scenario used in these simulations, average ozone mixing ratios are set to reduce by 2.0 ppb over domains encompassing Europe and the North East Atlantic between 2006 and 2100 with the most significant decrease occurring after 2050 due to the pattern in changing emissions. Peak reductions of more than 8 ppb are observed during summer time over mainland Europe by 2100. Model output was studied for three relevant sub-domains, namely the North East Atlantic, Ireland and Europe. The relative contribution of changes in both emissions and meteorology is assessed. Over the whole domain, changing emissions are predominantly responsible for changes in surface ozone; although over the North East Atlantic domain, the changing emissions do not perturb surface ozone trends and the decrease in 2100 levels is entirely attributable to changing meteorology.

Many of the next generation of global climate models will include aerosol schemes which explicitly simulate the microphysical processes that determine the particle size distribution. These models enable aerosol optical properties and cloud condensation nuclei (CCN) concentrations to be determined by fundamental aerosol processes, which should lead to a more physically based simulation of aerosol direct and indirect radiative forcings. This study examines the global variation in particle size distribution simulated by twelve global aerosol microphysics models to quantify model diversity and to identify any common biases against observations. Evaluation against size distribution measurements from a new European network of aerosol supersites shows that the mean model agrees quite well with the observations at many sites on the annual mean, but there are some seasonal biases common to many sites. In particular, at many of these European sites, the accumulation mode number concentration is biased low during winter and Aitken mode concentrations tend to be overestimated in winter and underestimated in summer. At high northern latitudes, the models strongly underpredict Aitken and accumulation particle concentrations compared to the measurements, consistent with previous studies that have highlighted the poor performance of global aerosol models in the Arctic. In the marine boundary layer, the models capture the observed meridional variation in the size distribution, which is dominated by the Aitken mode at high latitudes, with an increasing concentration of accumulation particles with decreasing latitude. Considering vertical profiles, the models reproduce the observed peak in total particle concentrations in the upper troposphere due to new particle formation, although modelled peak concentrations tend to be biased high over Europe. Overall, the multi-model-mean dataset simulates the global variation of the particle size distribution with a good degree of skill, suggesting that most of the individual global aerosol microphysics models are performing well, although the large model diversity indicates that some models are in poor agreement with the observations. Further work is required to better constrain size-resolved primary and secondary particle number sources, and an improved understanding of nucleation and growth (e.g. the role of nitrate and secondary organics) will improve the fidelity of simulated particle size distributions.

Stable carbon isotope ratios in marine aerosol collected over the Southern Indian Ocean revealed δ13C values ranging from −20.0‰ to −28.2‰. The isotope ratios exhibited a strong correlation with the fractional organic matter (OM) enrichment in sea spray aerosol. The base-level isotope ratio of −20.0‰ is characteristic of an aged Dissolved Organic Matter (DOM) pool contributing a relatively homogeneous background level of DOM to oceanic waters. The range of isotope ratios, extending down to −28.2‰, is characteristic of more variable, stronger, and fresher Particulate Organic Matter (POM) pool driven by trophic level interactions. We present a conceptual dual-pool POM-DOM model which comprises a ‘young’ and variable POM pool which dominates enrichment in sea-spray and an ‘aged’ but invariant DOM pool which is, ultimately, an aged end-product of processed ‘fresh’ POM. This model is harmonious with the preferential enrichment of fresh colloidal and nano-gel lipid-like particulate matter in sea spray particles and the observed depleted δ13C ratio resulting from isotope equilibrium fractionation coupled with enhanced plankton photosynthesis in cold water (−2 °C to +8 °C). These results re-assert the hypothesis that OM enrichment in sea-spray is directly linked to primary production and, consequently, can have implications for climate-aerosol-cloud feedback systems.

Homogeneous nucleation and subsequent cluster growth leads to the formation of new aerosol particles in the atmosphere(1). The nucleation of sulfuric acid and organic vapours is thought to be responsible for the formation of new particles over continents(1,2), whereas iodine oxide vapours have been implicated in particle formation over coastal regions(3-7). The molecular clustering pathways that are involved in atmospheric particle formation have been elucidated in controlled laboratory studies of chemically simple systems(2,8-10), but direct molecular-level observations of nucleation in atmospheric field conditions that involve sulfuric acid, organic or iodine oxide vapours have yet to be reported(11). Here we present field data from Mace Head, Ireland, and supporting data from northern Greenland and Queen Maud Land, Antarctica, that enable us to identify the molecular steps involved in new particle formation in an iodine-rich, coastal atmospheric environment. We find that the formation and initial growth process is almost exclusively driven by iodine oxoacids and iodine oxide vapours, with average oxygen-to-iodine ratios of 2.4 found in the clusters. On the basis of this high ratio, together with the high concentrations of iodic acid (HIO3) observed, we suggest that cluster formation primarily proceeds by sequential addition of HIO3, followed by intracluster restructuring to I2O5 and recycling of water either in the atmosphere or on dehydration. Our study provides ambient atmospheric molecular-level observations of nucleation, supporting the previously suggested role of iodine-containing species in the formation of new aerosol particles(3-7,12-18), and identifies the key nucleating compound.

International audience; In the atmosphere nighttime removal of volatile organic compounds is initiated to a large extent by reaction with the nitrate radical (NO3) forming organic nitrates which partition between gas and particulate phase. Here we show based on particle phase measurements performed at a suburban site in the Netherlands that organic nitrates contribute substantially to particulate nitrate and organic mass. Comparisons with a chemistry transport model indicate that most of the measured particulate organic nitrates are formed by NO3 oxidation. Using aerosol composition data from three intensive observation periods at numerous measurement sites across Europe, we conclude that organic nitrates are a considerable fraction of fine particulate matter (PM1) at the continental scale. Organic nitrates represent 34% to 44% of measured submicron aerosol nitrate and are found at all urban and rural sites, implying a substantial potential of PM reduction by NOx emission control.

The third intensive measurement period (IMP) organised by the European Monitoring and Evaluation Programme (EMEP) under the UNECE CLTRAP took place in summer 2012 and winter 2013, with PM10 filter samples concurrently collected at 20 (16 EMEP) regional background sites across Europe for subsequent analysis of their mineral dust content. All samples were analysed by the same or a comparable methodology. Higher PM10 mineral dust loadings were observed at most sites in summer (0.5–10 µg m−3) compared to winter (0.2–2 µg m−3), with the most elevated concentrations in the southern- and easternmost countries, accounting for 20–40 % of PM10. Saharan dust outbreaks were responsible for the high summer dust loadings at western and central European sites, whereas regional or local sources explained the elevated concentrations observed at eastern sites. The eastern Mediterranean sites experienced elevated levels due to African dust outbreaks during both summer and winter. The mineral dust composition varied more in winter than in summer, with a higher relative contribution of anthropogenic dust during the former period. A relatively high contribution of K from non-mineral and non-sea-salt sources, such as biomass burning, was evident in winter at some of the central and eastern European sites. The spatial distribution of some components and metals reveals the influence of specific anthropogenic sources on a regional scale: shipping emissions (V, Ni, and SO42−) in the Mediterranean region, metallurgy (Cr, Ni, and Mn) in central and eastern Europe, high temperature processes (As, Pb, and SO42−) in eastern countries, and traffic (Cu) at sites affected by emissions from nearby cities.

Multigenerational oxidation chemistry of atmospheric organic compounds and its effects on aerosol loadings and chemical composition is investigated by implementing the Two-Dimensional Volatility Basis Set (2-D-VBS) in a Lagrangian host chemical transport model. Three model formulations were chosen to explore the complex interactions between functionalization and fragmentation processes during gas-phase oxidation of organic compounds by the hydroxyl radical. The base case model employs a conservative transformation by assuming a reduction of one order of magnitude in effective saturation concentration and an increase of oxygen content by one or two oxygen atoms per oxidation generation. A second scheme simulates functionalization in more detail using group contribution theory to estimate the effects of oxygen addition to the carbon backbone on the compound volatility. Finally, a fragmentation scheme is added to the detailed functionalization scheme to create a functionalization-fragmentation parameterization. Two condensed-phase chemistry pathways are also implemented as additional sensitivity tests to simulate (1) heterogeneous oxidation via OH uptake to the particle-phase and (2) aqueous-phase chemistry of glyoxal and methylglyoxal. The model is applied to summer and winter periods at three sites where observations of organic aerosol (OA) mass and O:C were obtained during the European Integrated Project on Aerosol Cloud Climate and Air Quality Interactions (EUCAARI) campaigns. The base case model reproduces observed mass concentrations and O:C well, with fractional errors (FE) lower than 55% and 25%, respectively. The detailed functionalization scheme tends to overpredict OA concentrations, especially in the summertime, and also underpredicts O:C by approximately a factor of 2. The detailed functionalization model with fragmentation agrees well with the observations for OA concentration, but still underpredicts O:C. Both heterogeneous oxidation and aqueous-phase processing have small effects on OA levels but heterogeneous oxidation, as implemented here, does enhance O:C by about 0.1. The different schemes result in very different fractional attribution for OA between anthropogenic and biogenic sources.

Tidally exposed macroalgae emit large amounts of I2 and iodocarbons that produce hotspots of iodine chemistry and intense particle nucleation events in the coastal marine boundary layer. Current emission rates are poorly characterized, however,with reported emission rates varying by 3 orders of magnitude. In this study, I2 emissions from 25 Laminaria digitata samples were investigated in a simulation chamber using incoherent broadbandcavity-enhanced absorption spectroscopy (IBBCEAS). The chamber design allowed gradual extraction of seawater to simulate tidal emersion of algae. Samples were exposed to air with or without O3 and to varying irradiances. Emission of I2 occurred in four distinct stages: (1) moderate emissions from partially submerged samples;(2) a strong release by fully emerged samples; (3) slowing or stopping of I2 release; and (4) later pulses of I2 evident in some samples. Emission rates were highly variable and ranged from 7to 616 pmol min−1 gFW−1 in ozone-free air, with a median value of 55 pmol min−1 gFW−1 for 20 samples.

Laboratory studies into particle formation from Laminaria digitata macroalgae were undertaken to elucidate aerosol formation for a range of I(2) (0.3-76 ppb(v)) and O(3) (

The recent eruption of Iceland's Eyjafjallajokull volcano caused extensive disruption across Europe. In this paper, we describe the volcanic ash parameterisation incorporated in the regional climate model (REMOTE) for forecasting volcanic ash dispersion. We investigate model sensitivity to emission parameters including eruption column height and vertical release distribution. Model results over a number of key ash incursion events are assessed in terms of agreement with both ground based measurements and retrieved LIDAR data at a number of European sites.

This study focuses on the dispersion of the Eyjafjallajokull volcanic ash plume over the west of Ireland, at the Mace Head Supersite, and its influence on cloud formation and microphysics during one significant event spanning May 16th and May 17th, 2010. Ground-based remote sensing of cloud microphysics was performed using a Ka-band Doppler cloud RADAR, a LIDAR-ceilometer and a multi-channel microwave-radiometer combined with the synergistic analysis scheme SYRSOC (Synergistic Remote Sensing Of Cloud). For this case study of volcanic aerosol interaction with clouds, cloud droplet number concentration (CDNC), liquid water content (LWC), and droplet effective radius (reff) and the relative dispersion were retrieved. A unique cloud type formed over Mace Head characterized by layer-averaged maximum, mean and standard deviation values of the CDNC, reff and LWC: Nmax = 948 cm−3, N ¯ = 297 cm − 3 , σ N = 250 cm − 3 , reff max = 35.5 μm, r e f f ¯ = 4.8 μm , σ r e f f = 4.4 μm , L W C max = 0.23 g m − 3 , L W C ¯ = 0.055 g m − 3 , σ L W C = 0.054 g m − 3 , respectively. The high CDNC, for marine clean air, were associated with large accumulation mode diameter (395 nm) and a hygroscopic growth factor consistent with sulphuric acid aerosol, despite being almost exclusively internally mixed in submicron sizes. Additionally, the Condensation Nuclei (CN, d > 10 nm) to Cloud Condensation Nuclei (CCN) ratio, CCN:CN ∼1 at the moderately low supersaturation of 0.25%. This case study illustrates the influence of volcanic aerosols on cloud formation and microphysics and shows that volcanic aerosol can be an efficient CCN.

The Eyjafjallajokull ash plume was detected at the Mace Head Atmospheric Research Station numerous times from April 19th till 18th May 2010 following subsidence into, and dilution in, the boundary layer. The three strongest of these events, lasting 12–18 h, are analysed in detail in terms of physical, chemical and optical properties. The ash size distribution was bimodal with a supermicron mode of 2.5 μm diameter for the one case where it was measured. The submicron mode varied from 185 nm during the high-explosive phase to 395 nm during the low-explosive phase. Non-sea-salt (nss)-sulphate mass was 2.5 times higher during the low-explosive phase. Total particle concentrations ranged from 760 cm −3 to 1247 cm −3 and were typical of clean air in the region. Between 30% and 39% of submicron chemical mass (i.e. exclusive of water content) was ash primarily composed of silicon dioxide while accounting for the water content, the submicron aerosol was composed of primary ash (15%), nss-sulphate (25%) and water (55%). Hygroscopic growth factors were characteristic of sulphate aerosol but revealed an internally-mixed aerosol pointing to a mix of predominantly primary ash, nss-sulphate and water. For the majority of the ash plumes, all condensation nuclei (CN, diameter > 10 nm) were activated into cloud condensation nuclei (CCN) at a supersaturation of 0.25%. Aerosol absorption increased by about a factor of two in the plume, compared to background levels, while aerosol scattering coefficients increased by an order of magnitude.

Aerosol loading in the marine environment is investigated using aerosol composition measurements from several research ship campaigns (ICEALOT, MAP, RHaMBLe, VOCALS and OOMPH), observations of total AOD column from satellite (MODIS) and ship-based instruments (Maritime Aerosol Network, MAN), and a global chemical transport model (GEOS-Chem). This work represents the most comprehensive evaluation of oceanic OM emission inventories to date, by employing aerosol composition measurements obtained from campaigns with wide spatial and temporal coverage. The model underestimates AOD over the remote ocean on average by 0.02 (21 %), compared to satellite observations, but provides an unbiased simulation of ground-based Maritime Aerosol Network (MAN) observations. Comparison with cruise data demonstrates that the GEOS-Chem simulation of marine sulfate, with the mean observed values ranging between 0.22 μg m−3 and 1.34 μg m−3, is generally unbiased, however surface organic matter (OM) concentrations, with the mean observed concentrations between 0.07 μg m−3 and 0.77 μg m−3, are underestimated by a factor of 2–5 for the standard model run. Addition of a sub-micron marine OM source of approximately 9 TgC yr−1 brings the model into agreement with the ship-based measurements, however this additional OM source does not explain the model underestimate of marine AOD. The model underestimate of marine AOD is therefore likely the result of a combination of satellite retrieval bias and a missing marine aerosol source (which exhibits a different spatial pattern than existing aerosol in the model).

Horizontal resolution sensitivity can significantly contribute to the uncertainty in predictions of meteorology and air-quality from a regional climate model. In the study presented here, a state-of-the-art regional scale atmospheric climate-chemistry-aerosol model REMOTE is used to understand the influence of spatial model resolutions of 1.0°, 0.5° and 0.25° on predicted meteorological and aerosol parameters for June 2003 for the European domain comprising North-east Atlantic and Western Europe. Model precipitation appears to improve with resolution while wind speed has shown best results for 0.25° resolution for most of the stations compared with ECAD data. Low root mean square error and spatial bias for surface pressure, precipitation and surface temperature show that the model is very reliable. Spatial and temporal variation in black carbon, primary organic carbon, sea-salt and sulphate concentrations and their burden are presented. In most cases, chemical species concentrations at the surface show no particular trend or improvement with increase in resolution. There has been a pronounced influence of horizontal resolution on the vertical distribution pattern of some aerosol species. Some of these effects are due to the improvement in topographical details, flow characteristics and associated vertical and horizontal dynamic processes. The different sink processes have contributed very differently to the various aerosol species in terms of deposition (wet and dry) and sedimentation which are strongly linked to the meteorological processes. Overall, considering the performance of meteorological parameters and chemical species concentrations, a horizontal model resolution of 0.5° is suggested to achieve reasonable results within the limitations of this model.

Thyroid hormone levels sufficient for brain development and normal metabolism require a minimal supply of iodine, mainly dietary. Living near the sea may confer advantages for iodine intake. Iodine (I2 )g as released from seaweeds may, through respiration, supply a significant fraction of daily iodine require- ments. Gaseous iodine released over seaweed beds was measured by a new gas chromatography-mass spec- trometry (GC-MS)-based method and iodine intake assessed by measuring urinary iodine (UI) excretion. Urine samples were obtained from female schoolchil- dren living in coastal seaweed rich and low seaweed abundance and inland areas of Ireland. Median I2 ranged 154-905 pg/L (daytime downwind), with higher values (*1,287 pg/L) on still nights, 1,145-3,132 pg/L (over seaweed). A rough estimate of daily gaseous iodine intake in coastal areas, based upon an arbitrary respiration of 10,000L, ranged from 1 to 20 lg/day. Despite this relatively low potential I2 intake, UI in populations living near a seaweed hotspot were much higher than in lower abundance seaweed coastal or inland areas (158, 71 and 58 lg/L, respectively). Higher values(150 lg/L were observed in 45.6% of (seaweed rich), 3.6% (lower seaweed), 2.3% (inland)) supporting the hypothesis that iodine intake in coastal regions may be dependent on seaweed abundance rather than proximity to the sea. The findings do not exclude the possibility of a significant role for iodine inhalation in influencing iodine status. Despite lacking iodized salt, coastal communities in seaweed-rich areas can maintain an adequate iodine supply. This observation brings new meaning to the expression ''Sea air is good for you!''

Mineral dust is an important aerosol species in the Earth’s atmosphere and has a major source within North Africa, of which the Sahara forms the major part. Aerosol Time of Flight Mass Spectrometry (ATOFMS) is first used to determine the mixing state of dust particles collected from the land surface in the Saharan region, showing low abundance of species such as nitrate and sulphate internally mixed with the dust mineral matrix. These data are then compared with the ATOFMS single particle mass spectra of Saharan dust particles detected in the marine atmosphere in the vicinity of the Cape Verde islands, which are further compared with those from particles with longer atmospheric residence sampled at a coastal station at Mace Head, Ireland. Saharan dust particles collected near the Cape Verde Islands showed increased internally mixed nitrate but no sulphate, whilst Saharan dust particles collected on the coast of Ireland showed a very high degree of internally mixed secondary species including nitrate, sulphate and methanesulphonate. This uptake of secondary species will change the pH and hygroscopic properties of the aerosol dust and thus can influence the budgets of other reactive gases, as well as influencing the radiative properties of the particles and the availability of metals for dissolution.

A more realistic estimation of the scattering and hemispheric backscattering coefficients, σ sp and σ bsp , and their respective optical cross section, C sca and C bk, of aerosol particles is presented on the basis of the exact resolution of the width of the size bins of the particle counter instruments when size distribution measurements are used, and, with the exact optical detector instruments ability. The scattering and hemispheric backscattering cross sections, C sca and C bk , of the particles are averaged over the full size bins of the particle counter instrument, while these quantities are usually estimated only on the value of the mean geometric diameter of each size bin. Six instruments, the APS, ASASP-X, DMPS, FSSP-100, ELPI, and SMPS frequently used in particle size distribution measurements are reviewed, for spherical sea-salt particles at a wavelength λ =0.55 μm. The comparison using the conventional geometric mean diameter versus the use of the full size bin leads to large amount of errors for the optical cross section with non-negligible effects on their respective optical coefficients. The maximal accuracy expected for these optical quantities depend on the particle diameter as well as on the channel width of the instruments, and are also function of the angular detector probe used to measure them.

Twelve case studies of multilayer cloud-base height (CBH) retrievals from two collocated ceilometers (Vaisala CL31 and Jenoptik CHM15K) have been analyzed. The studies were performed during the period from September to December 2008 at the Mace Head Atmospheric Research Station in Ireland. During the period of measurement, the two instruments provided vertical profiles of backscattered laser signal as well as the manufacturer’s operational cloud-base product. The cases selected covered a diverse range of cloud-cover conditions, ranging from single to multiple cloud layers and from cloud-base heights varying from only a few hundreds meters per day up to 3–5 km in a few hours. The results show significant offsets between the two manufacturer-derived CBHs along with a considerable degree of scatter. Using a newly developed temporal height-tracking (THT) algorithm applied to both ceilometers, significant improvement in the correlation between CBH derived from both instruments results in a correlation coefficient increasing to R2 = 0.997 (with a slope of 0.998) from R2 = 0.788 (with an associated slope of 0.925). Also, the regression intercept (offset) is reduced from 160 m to effectively zero (−3 m). For the worst individual case study, using the THT algorithm resulted in the correlation coefficient improving from R2 = 0.52, using the manufacturer’s output, to R2 = 0.97 with a reduction in the offset reducing from 569 to 32 m. Applying the THT algorithm to the backscatter profiles of both instruments led to retrieved cloud bases that are statistically consistent with each other and ensured reliable detection of CBH, particularly when inhomogeneous cloud fields were present and changing rapidly in time. The THT algorithm also overcomes multiple false cloud-base detections associated with the manufacturer’s output of the two instruments.

Secondary organic aerosol (SOA) formation through isoprene oxidation was investigated with the regional-scale climate model REMOTE. The applied modeling scheme includes a treatment for marine primary organic aerosol emissions, aerosol microphysics, and SOA formation through the gas/particle partitioning of semivolatile, water-soluble oxidation products. The focus was on SOA formation taking place over the North-East Atlantic during a period of high biological activity. Isoprene SOA concentrations were up to ~5 ngm−3over North Atlantic in the base case model runs, and isoprene oxidation made a negligible contribution to the marine organic aerosol (OA) mass. In particular, isoprene SOA did not account for the observed water-soluble organic carbon (WSOC) concentrations over North Atlantic. The performed model calculations, together with results from recent field measurements, imply a missing source of SOA over remote marine areas unless the isoprene oxidation products are considerably less volatile than the current knowledge indicates.

A bioaerosol fluorescence detection system is being constructed using an ellipsoid reflector-based optical particle counter. The flux measuring device is to size submicron marine spray aerosol particles smaller than 100 nm in diameter. It will simultaneously non-destructively excite and detect fluorescence from organic matter contained in the aerosol. Chlorophyll-a is the primary fluorophor target, used as a marker for detecting phytoplankton (or derivatives thereof) in the particles. Particles have been sized to 500 nm in diameter and fluorescence detection testing is underway. The device will aid the quantification and identification of this organic material contained in marine spray aerosols, providing improved inputs into climate models and air quality assessments.

Airborne measurements of nucleation mode aerosol concentrations during nucleation events over the boreal forest of southern Finland are reported. Three case studies are analysis in an attempt to characterise the spatial scales over which these events occur and to identify the source region for particle production. For the cases presented, there is no evidence of nucleation mode particles in the Free Troposphere. Nucleation mode particles are first detected in the surface layer as the nocturnal inversion breaks up and develops into the current-day's new boundary layer. In terms of spatial variability, significant variability in the concentration of nucleation mode particles was observed and was attributed to changes in the topography which comprised a mix of forest canopy and frozen lakes. Measurements over the Gulf of Bothnia indicated no nucleation mode over the sea and confirm that the scale of the events is associated with the boreal forest scale and that the new particles are produced directly above the forest canopy.

Gas-to-particle conversion takes readily place in the atmosphere. Detecting the initial clusters, which act as embryos for the newly formed particles, is beyond traditional aerosol instrumentation. Charged atmospheric clusters can be measured with air ion spectrometers, but typical state-of-the-art condensation particle counters, which detect both neutral and charged clusters, only see particles larger than 2.5 nm in diameter. In this study we present a modified pulse-height condensation particle counter (PH-CPC) and confirm by laboratory verification that it is capable of detecting charged clusters with electrical mobility equivalent diameter down to ∼1 nm. We show how the detection efficiency and the pulse heights depend on the calibration particle size, polarity and composition. The effect of butanol supersaturation on the PH-CPC counting efficiency is also discussed. Furthermore, we developed an inversion method for the data to obtain true particle size distribution from the measurement signal.

Atmospheric new particle formation is generally thought to occur due to homogeneous or ion-induced nucleation of sulphuric acid. We compare ambient nucleation rates with laboratory data from nucleation experiments involving either sulphuric acid or oxidized SO2. Atmospheric nucleation occurs at H2SO4 concentrations 2–4 orders of magnitude lower than binary or ternary H2SO4 nucleation. In contrast, the atmospheric nucleation rates and H2SO4 concentrations are very well replicated in the SO2 oxidation experiments. We explain these features by the formation of free HSO5 radicals in pace with H2SO4 during the SO2 oxidation. We suggest that at temperatures above ~250 K these radicals produce nuclei of new aerosols much more efficiently than H2SO4. These nuclei are activated to further growth by H2SO4 and possibly other trace species. However, at lower temperatures the atmospheric relative acidity is high enough for the H2SO4–H2O nucleation to dominate.

This paper summarises the development and principal results of fifty years of research on aerosols in the marine atmosphere at Mace Head Atmospheric Research Station on the west coast of Ireland. It concentrates on the sources, physico-chemical properties, number and mass concentrations, size range, volatility and chemical composition of aerosols in different air masses. It also examines optical properties of the aerosols and their long-range transport.

Coastal nucleation events and behavior of cluster ions were characterized through the measurements of air ion mobility distributions at the Mace Head research station on the west coast of Ireland in 2006. We measured concentrations of cluster ions and charged aerosol particles in the size range of 0.34–40 nm. These measurements allow us to characterize freshly nucleated charged particles with diameters smaller than 3 nm. The analysis shows that bursts of intermediate ions (1.6–7 nm) are a frequent phenomenon in the marine coastal environment. Intermediate ion concentrations were generally close to zero, but during some nucleation episodes the concentrations increased to several hundreds per cm 3 . Nucleation events occurred during most of the measurement days. We classified all days into one of seven classes according to the occurrence and type of new particle formation. Nucleation events were observed during 207 days in 2006, most prominently in the spring and summer months. Rain-induced events, in turn, were observed during 132 days. Particle formation and growth events mostly coincided with the presence of low tide. Also small cluster ions (0.34–1.6 nm) were characterized. Average concentrations of small ions were 440 cm − 3 for the negative ions and 423 cm − 3 for the positive ions. Average mean mobilities of small ions were 1.86 cm 2 V − 1 s − 1 and 1.49 cm 2 V − 1 s − 1 for the negative and positive polarities, respectively. Concentrations of small ions were observed to be strongly dependent on the variations of meteorological parameters including wind speed and direction.

Frequency and intensity of cyclones over the North Atlantic are investigated using 2 data sets from simulations with the Rossby Centre regional climate model RCA3. The model domain comprises large parts of the North Atlantic and the adjacent continents. RCA3 is driven by ECHAM5- OM1 general circulation model data for May to December from 1985 to 2000 and May to December from 2085 to 2100 assuming the SRES-A2 emission scenario. We apply an objective algorithm to iden- tify and track tropical and extratropical cyclones, as well as extratropical transition. The simulation indicates increase in the count of strong hurricanes and extratropical cyclones. Contrasting, and gen- erally weaker, changes are seen for the less extreme events. Decreases of 18% in the count of extra- tropical cyclones and 13% in the count of tropical cyclones with wind speeds of ≥ 18 m s–1 can be found. Furthermore, there is a pronounced shift in the tracks of hurricanes and their extratropical transition in November and December—more hurricanes are seen over the Gulf of Mexico, the Caribbean Sea and the western Sargasso Sea and less over the southern North Atlantic.

The LAPBIAT measurement campaign took place in the Värriö SMEAR I measurement station located in Eastern Lapland in the spring of 2003 between 26 April and 11 May. In this paper we describe the measurement campaign, concentrations and fluxes of aerosol particles, air ions and trace gases, paying special attention to an aerosol particle formation event broken by a air mass change from a clean Arctic air mass with new particle formation to polluted one approaching from industrial areas of Kola Peninsula, Russia, lacking new particle formation. Aerosol particle number flux measurements show strong downward fluxes during that time. Concentrations of coarse aerosol particles were high for 1–2 days before the nucleation event (i.e. 28–29 April), very low immediately before and during the observed aerosol particle formation event (30 April) and increased moderately from the moment of sudden break of the event. In general particle deposition measurements based on snow samples show the same changes. Measurements of the mobility distribution of air ions showed elevated concentrations of intermediate air ions during the particle formation event. We estimated the growth rates in the nucleation mode size range. For particles

Four periods of EMEP (European Monitoring and Evaluation Programme) intensive measurement campaigns (June 2006, January 2007, September–October 2008 and February–March 2009) were modelled using the regional air quality model CAMx with VBS (Volatility Basis Set) approach for the first time in Europe within the framework of the EURODELTA-III model intercomparison exercise. More detailed analysis and sensitivity tests were performed for the period of February–March 2009 and June 2006 to investigate the uncertainties in emissions as well as to improve the modelling of organic aerosols (OA). Model performance for selected gas phase species and PM2.5 was evaluated using the European air quality database Airbase. Sulfur dioxide (SO2) and ozone (O3) were found to be overestimated for all the four periods with O3 having the largest mean bias during June 2006 and January–February 2007 periods (8.93 and 12.30 ppb mean biases, respectively). In contrast, nitrogen dioxide (NO2) and carbon monoxide (CO) were found to be underestimated for all the four periods. CAMx reproduced both total concentrations and monthly variations of PM2.5 very well for all the four periods with average biases ranging from −2.13 to 1.04 μg m-3. Comparisons with AMS (Aerosol Mass Spectrometer) measurements at different sites in Europe during February–March 2009, showed that in general the model over-predicts the inorganic aerosol fraction and under-predicts the organic one, such that the good agreement for PM2.5 is partly due to compensation of errors. The effect of the choice of volatility basis set scheme (VBS) on OA was investigated as well. Two sensitivity tests with volatility distributions based on previous chamber and ambient measurements data were performed. For February–March 2009 the chamber-case reduced the total OA concentrations by about 43 % on average. On the other hand, a test based on ambient measurement data increased OA concentrations by about 47 % for the same period bringing model and observations into better agreement. Comparison with the AMS data at the rural Swiss site Payerne in June 2006 shows no significant improvement in modelled OA concentration. Further sensitivity tests with increased biogenic and anthropogenic emissions suggest that OA in Payerne was largely dominated by residential heating emissions during the February–March 2009 period and by biogenic precursors in June 2006.

9 pages, 3 figures, 1 table, supporting information http://pubs.acs.org/doi/suppl/10.1021/acs.est.5b02922, A number of field observations employing aerosol mass spectrometers (AMS) have demonstrated that organic matter rich in monocarboxylic acids and aliphatic carbonyls originating from cooking activities (the COA factor) contributes significantly to ambient organic matter (OM) in urban environments. Little is known about the contribution and nature of COA in rural localities. We studied the correlation of COA with chemical tracers at a rural site in the Po Valley, Italy. Our statistical approach, based on positive matrix factorization (PMF) shows that the COA factor was clearly linked to local emissions of chloride and methanesulfonic acid (MSA), chemical tracers not associated with cooking emissions, or with combustion sources. While the association with Cl is not understood at this stage, the emission of reduced sulfur compounds, aliphatic carbonyls and monocarboxylic acids is consistent with several agricultural practices (e.g., manure storage) and waste disposal systems (e.g., landfills) which characterize the suburban and rural areas of the Po Valley and of other many populated environments. It is concluded that the nature and origins of the AMS COA factor measured at a rural site are complex and include far more than the emissions from food cooking, This work was funded by European integrated project on aerosol cloud climate and air quality interactions (no. 036833-2, EUCAARI). Manuel Dall’Osto and Roy M. Harrison thank the UK National Centre for Atmospheric Science for financial support. We acknowledge funding from the EU FP7-ENV-2013 programme “impact of Biogenic vs. Anthropogenic emissions on Clouds and Climate: towards a Holistic UnderStanding” (BACCHUS), project no. 603445. Programme Ramon y Cajal (RYC-2012-11922) also provided financial support

Direct climate radiative forcing depends on the aerosol optical depth τ, the single scattering albedo ϖ, and the up-scatter fraction β; these quantities are functions of the refractive index of the particles, their size relative to the incident wavelength, and their shape. Sea-salt aerosols crystallize into cubic shapes or in agglomerates of cubic particles under low relative humidity conditions. The present study investigates the effects of the shape of dried sea-salt particles on the detection of light scattering from the particles. Ground-based measurements of scattering and backscattering coefficients have been performed with an integrating nephelometer instrument for a wavelength λ = 0.55 μ m . The measurements are compared to two models: the Mie theory assuming a spherical shape for the particles and the Discrete Dipole Approximation (DDA) model for the hypothesis of cubic shape of the sea-salt aerosols. The comparison is made accurately by taking into account the actual range of the scattering angles measured by the nephelometer in both models that is from 7° to 170° for the scattering coefficient and from 90° to 170° for the backscattering coefficient. Modeled scattering and backscattering coefficients increase for nonspherical particles compared to spherical shape of particles with diameter larger than about 1 μm. However, the comparison of the modeling results with the measurements gives best agreement for particles diameter less than about 1 μm. The size distribution of the particles is measured with two instruments with different size bins: an electrical low-pressure impactor (ELPI) and an aerodynamic particle sizer (APS). It is found that the size of the bins of the instruments to determine the number concentration of the particles in accordance with their diameter is critical in the comparison of measurements with modeling.