Arctic Ocean water: A source of light absorbing particles to the atmosphere

Johan Ström (et al.).

Article

Comparison between summertime and wintertime Arctic Ocean primary marine aerosol properties

Julia Zábori (et al.). Atmospheric Chemistry and Physics Discussions

Article

Collective geographical ecoregions and precursor sources driving Arctic new particle formation

2023. James Brean (et al.). Atmospheric Chemistry And Physics 23 (3), 2183-2198

Article

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.

Organic Compounds, Radiocarbon, Trace Elements and Atmospheric Transport Illuminating Sources of Elemental Carbon in a 300-Year Svalbard Ice Core

2023. M. M. Ruppel (et al.). Journal of Geophysical Research - Atmospheres 128 (16)

Article

Black carbon (BC) particles produced by incomplete combustion of biomass and fossil fuels warm the atmosphere and decrease the reflectivity of snow and ice, hastening their melt. Although the significance of BC in Arctic climate change is widely acknowledged, observations on its deposition and sources are few. We present BC source types in a 300-year (1700-2005) Svalbard ice core by analysis of particle-bound organic compounds, radiocarbon, and trace elements. According to the radiocarbon results, 58% of the deposited elemental carbon (EC, thermal-optical proxy of BC) is of non-fossil origin throughout the record, while the organic compounds suggest a higher percentage (68%). The contribution of fossil fuels to EC is suggested to have been elevated between 1860 and 1920, particularly based on the organics and trace element data. A second increase in fossil fuel sources seems to have occurred near the end of the record: according to radiocarbon measurements between 1960 and 1990, while the organics and trace element data suggest that the contribution of fossil fuels has increased since the 1970s to the end of the record, along with observed increasing EC deposition. Modeled atmospheric transport between 1948 and 2004 shows that increasing EC deposition observed at the glacier during that period can be associated with increased atmospheric transport from Far East Asia. Further observational BC source data are essential to help target climate change mitigation efforts. The combination of robust radiocarbon with organic compound analyses requiring low sample amounts seems a promising approach for comprehensive Arctic BC source apportionment.

Airmass Analysis of Size-Resolved Black Carbon Particles Observed in the Arctic Based on Cluster Analysis

2022. Roxana S. Cremer, Peter Tunved, Johan Ström. Atmosphere 13 (5)

Article

Here we apply new analysis methods and approaches to existing long-term measurement series that provide additional insights into the atmospheric processes that control black carbon (BC) in the Arctic. Based on clustering size distribution data from Zeppelin Observatory for the years 2002–2010, observations classified as ‘Polluted’ were further investigated based on BC properties. The data were split into two subgroups, and while the microphysical and chemical fingerprints of the two subgroups are very similar, they show larger differences in BC concentration and correlation with the particle size distribution. Therefore, a source–receptor analysis was performed with HYSPLIT 10-days backward trajectories for both subsets. We demonstrate that within this ‘Polluted’ category, the airmasses that contributed to the largest BC signal at the Zeppelin station are not necessarily associated with traditional transport pathways from Eurasia. Instead, the strongest signal is from a region east of the Ural Mountains across the continent to the Kamchatka Peninsula.

Atmospheric composition in the European Arctic and 30 years of the Zeppelin Observatory, Ny-Ålesund

2022. Stephen M. Platt (et al.). Atmospheric Chemistry And Physics 22 (5), 3321-3369

Article

The Zeppelin Observatory (78.90^∘ N, 11.88^∘ E) is located on Zeppelin Mountain at 472 m a.s.l. on Spitsbergen, the largest island of the Svalbard archipelago. Established in 1989, the observatory is part of Ny-Ålesund Research Station and an important atmospheric measurement site, one of only a few in the high Arctic, and a part of several European and global monitoring programmes and research infrastructures, notably the European Monitoring and Evaluation Programme (EMEP); the Arctic Monitoring and Assessment Programme (AMAP); the Global Atmosphere Watch (GAW); the Aerosol, Clouds and Trace Gases Research Infrastructure (ACTRIS); the Advanced Global Atmospheric Gases Experiment (AGAGE) network; and the Integrated Carbon Observation System (ICOS). The observatory is jointly operated by the Norwegian Polar Institute (NPI), Stockholm University, and the Norwegian Institute for Air Research (NILU). Here we detail the establishment of the Zeppelin Observatory including historical measurements of atmospheric composition in the European Arctic leading to its construction. We present a history of the measurements at the observatory and review the current state of the European Arctic atmosphere, including results from trends in greenhouse gases, chlorofluorocarbons (CFCs) and hydrochlorofluorocarbons (HCFCs), other traces gases, persistent organic pollutants (POPs) and heavy metals, aerosols and Arctic haze, and atmospheric transport phenomena, and provide an outline of future research directions.

Snow albedo and its sensitivity to changes in deposited light-absorbing particles estimated from ambient temperature and snow depth observations at a high-altitude site in the Himalaya

2022. Johan Ström (et al.). Elementa 10 (1)

Article

Snow darkening by deposited light-absorbing particles (LAP) accelerates snowmelt and shifts the snow melt-out date (MOD). Here, we present a simple approach to estimate the snow albedo variability due to LAP deposition and test this method with data for 2 seasons (February–May 2016 and December 2016–June 2017) at a high-altitude valley site in the Central Himalayas, India. We derive a parameterization for the snow albedo that only depends on the daily observations of average ambient temperature and change in snow depth, as well as an assumed average concentration of LAP in snow precipitation. Linear regression between observed and parameterized albedo for the base case assuming an equivalent elemental carbon concentration [EC_eq] of 100 ng g^–1 in snow precipitation yields a slope of 0.75 and a Pearson correlation coefficient r² of 0.76. However, comparing the integrated amount of shortwave radiation absorbed during the winter season using observed albedo versus base case albedo resulted in rather small differences of 11% and 4% at the end of Seasons 1 and 2, respectively. The enhanced energy absorbed due to LAP at the end of the 2 seasons for the base case scenario (assuming an [EC_eq] of 100 ng g^–1 in snow precipitation) was 40% and 36% compared to pristine snow. A numerical evaluation with different assumed [EC_eq] in snow precipitation suggests that the relative sensitivity of snow albedo to changes in [EC_eq] remains rather constant for the 2 seasons. Doubling [EC_eq] augments the absorption by less than 20%, highlighting that the impact on a MOD is small even for a doubling of average LAP in snow precipitation.

Unmasking the Effects of Aerosols on Greenhouse Warming Over Europe

2022. Paul Glantz (et al.). Journal of Geophysical Research - Atmospheres 127 (22)

Article

Aerosol optical thickness (AOT) has decreased substantially in Europe in the summer half year (April–September) since 1980, with almost a 50% reduction in Central and Eastern Europe, according to Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2) reanalysis. At the same time, strong positive trends in ERA5 reanalysis surface solar radiation downward for all-sky and clear-sky conditions (SSRD and SSRDc, respectively) and temperature at 2 m are found for Europe in summer during the period 1979–2020. The GEBA observations show as well strong increases in SSRD during the latest four decades. Estimations of changes in SSRDc, using the Santa Barbara DISORT Atmospheric Radiative Transfer (SBDART) model, show similarly strong increases when fed by MERRA-2 AOT. The estimates of warming in this study, caused by increases in SSRD and SSRDc, are based on energy budget approximations and the Stefan Boltzmann law. The increases in near surface temperature, estimated both for clear-sky and all-sky conditions, are up to about 1°C for Central and Eastern Europe. The total warming over large parts of this region for clear-sky conditions is however nearly double the global mean temperature increase of 1.1°C, while somewhat less for all-sky conditions. The effects of aerosols on warming over the southerly Iberian Peninsula are weaker compared to countries further north. The rapid total warming over the Iberian Peninsula is probably caused by greenhouse warming, drier surface conditions, and to some degree decline in aerosols. Reduced cloud cover is found for large parts of Europe in summer during the latest four decades.

Deposition of light-absorbing particles in glacier snow of the Sunderdhunga Valley, the southern forefront of the central Himalayas

2021. Jonas Svensson (et al.). Atmospheric Chemistry And Physics 21 (4), 2931-2943

Article

Anthropogenic activities on the Indo-Gangetic Plain emit vast amounts of light-absorbing particles (LAPs) into the atmosphere, modifying the atmospheric radiation state. With transport to the nearby Himalayas and deposition to its surfaces the particles contribute to glacier melt and snowmelt via darkening of the highly reflective snow. The central Himalayas have been identified as a region where LAPs are especially pronounced in glacier snow but still remain a region where measurements of LAPs in the snow are scarce. Here we study the deposition of LAPs in five snow pits sampled in 2016 (and one from 2015) within 1 km from each other from two glaciers in the Sunderdhunga Valley, in the state of Uttarakhand, India, in the central Himalayas. The snow pits display a distinct enriched LAP layer interleaved by younger snow above and older snow below. The LAPs exhibit a distinct vertical distribution in these different snow layers. For the analyzed elemental carbon (EC), the younger snow layers in the different pits show similarities, which can be characterized by a deposition constant of about 50 µg m⁻² mm⁻¹ snow water equivalent (SWE), while the old-snow layers also indicate similar values, described by a deposition constant of roughly 150 µg m⁻² mm⁻¹ SWE. The enriched LAP layer, contrarily, displays no similar trends between the pits. Instead, it is characterized by very high amounts of LAPs and differ in orders of magnitude for concentration between the pits. The enriched LAP layer is likely a result of strong melting that took place during the summers of 2015 and 2016, as well as possible lateral transport of LAPs. The mineral dust fractional absorption is slightly below 50 % for the young- and old-snow layers, whereas it is the dominating light-absorbing constituent in the enriched LAP layer, thus, highlighting the importance of dust in the region. Our results indicate the problems with complex topography in the Himalayas but, nonetheless, can be useful in large-scale assessments of LAPs in Himalayan snow.

Dimethyl Sulfide-Induced Increase in Cloud Condensation Nuclei in the Arctic Atmosphere

2021. Ki-Tae Park (et al.). Global Biogeochemical Cycles 35 (7)

Article

Oceanic dimethyl sulfide (DMS) emissions have been recognized as a biological regulator of climate by contributing to cloud formation. Despite decades of research, the climatic role of DMS remains ambiguous largely because of limited observational evidence for DMS-induced cloud condensation nuclei (CCN) enhancement. Here, we report concurrent measurement of DMS, physiochemical properties of aerosol particles, and CCN in the Arctic atmosphere during the phytoplankton bloom period of 2010. We encountered multiple episodes of new particle formation (NPF) and particle growth when DMS mixing ratios were both low and high. The growth of particles to sizes at which they can act as CCN accelerated in response to an increase in atmospheric DMS. Explicitly, the sequential increase in all relevant parameters (including the source rate of condensable vapor, the growth rate of particles, Aitken mode particles, hygroscopicity, and CCN) was pronounced at the DMS-derived NPF and particle growth events. This field study unequivocally demonstrates the previously unconfirmed roles of DMS in the growth of particles into climate-relevant size and eventual CCN activation.

Elemental and water-insoluble organic carbon in Svalbard snow: a synthesis of observations during 2007-2018

2021. Christian Zdanowicz (et al.). Atmospheric Chemistry And Physics 21 (4), 3035-3057

Article

Light-absorbing carbonaceous aerosols emitted by biomass or fossil fuel combustion can contribute to amplifying Arctic climate warming by lowering the albedo of snow. The Svalbard archipelago, being near to Europe and Russia, is particularly affected by these pollutants, and improved knowledge of their distribution in snow is needed to assess their impact. Here we present and synthesize new data obtained on Svalbard between 2007 and 2018, comprising measurements of elemental (EC) and water-insoluble organic carbon (WIOC) in snow from 37 separate sites. We used these data, combined with meteorological data and snowpack modeling, to investigate the variability of EC and WIOC deposition in Svalbard snow across latitude, longitude, elevation and time. Overall, EC concentrations (C-snow(EC)) ranged from < 1.0 to 266.6 ng g(-1), while WIOC concentrations (C-snow(WIOC)) ranged from < 1 to 9426 ng g(-1), with the highest values observed near Ny-Alesund. Calculated snowpack loadings (L-snow(EC), L-snow(WIOC)) on glaciers surveyed in spring 2016 were 0.1 to 2.6 mg m(-2) and 2 to 173 mg m(-2), respectively. The median C-snow(EC) and the L-snow(EC) on those glaciers were close to or lower than those found in earlier (2007- 2009), comparable surveys. Both L-snow(EC) and L(snow)(WIOC )increased with elevation and snow accumulation, with dry deposition likely playing a minor role. Estimated area-averaged snowpack loads across Svalbard were 1.1 mg EC m(-2) and 38.3 mg WIOC m(-2) for the 2015-2016 winter. An similar to 11-year long dataset of spring surface snow measurements from the central BrOgger Peninsula was used to quantify the interannual variability of EC and WIOC deposition in snow. In most years, C-snow(EC) and C-snow(WIOC) at Ny-Alesund (50 m a.s.l.) were 2-5 times higher than on the nearby Austre Brogger-breen glacier (456 m a.s.l.), and the median EC/WIOC in Ny-Alesund was 6 times higher, suggesting a possible influence of local EC emission from Ny-Alesund. While no long-term trends between 2011 and 2018 were found, C-snow(EC) and C-snow(WIOC) showed synchronous variations at Ny-Alesund and Austre Broggerbreen. When compared with data from other circum-Arctic sites obtained by comparable methods, the median C(snow)(EC)on Svalbard falls between that found in central Greenland (lowest) and those in continental sectors of European Arctic (northern Scandinavia, Russia and Siberia; highest), which is consistent with large-scale patterns of BC in snow reported by surveys based on other methods.

Relationship between cloud condensation nuclei (CCN) concentration and aerosol optical depth in the Arctic region

2021. Seo H. Ahn (et al.). Atmospheric Environment 267

Article

To determine the direct and indirect effects of aerosols on climate, it is important to know the spatial and temporal variations in cloud condensation nuclei (CCN) concentrations. Although many types of CCN measurements are available, extensive CCN measurements are challenging because of the complexity and high operating cost, especially in remote areas. As aerosol optical depth (AOD) can be readily observed by remote sensing, many attempts have been made to estimate CCN concentrations from AOD. In this study, the CCN-AOD relationship is parameterized based on CCN ground measurements from the Zeppelin Observatory (78.91 degrees N, 11.89 degrees E, 474 m asl) in the Arctic region. The AOD measurements were obtained from the Ny-Alesund site (78.923 degrees N, 11.928 degrees E) and Modern-Era Retrospective Analysis for Research and Applications, Version 2 reanalysis. Our results show a CCN-AOD correlation with a coefficient of determination R-2 of 0.59. Three additional estimation models for CCN were presented based on the following data: (i) in situ aerosol chemical composition, (ii) in situ aerosol optical properties, and (iii) chemical composition of AOD obtained from reanalysis data. The results from the model using in situ aerosol optical properties reproduced the observed CCN concentration most efficiently, suggesting that the contribution of BC to CCN concentration should be considered along with that of sulfate.

Using correlations between observed equivalent black carbon and aerosol size distribution to derive size resolved BC mass concentration: a method applied on long-term observations performed at Zeppelin station, Ny-Ålesund, Svalbard

2021. Peter Tunved (et al.). Tellus. Series B, Chemical and physical meteorology 73 (1), 1-17

Article

The aim of this study was to explore particle size dependent properties by combining long-term observations of equivalent black carbon (eBC) and number size distributions to investigate their correlation as function of particle size. The work was conducted in two main parts. The first part consisted of a short laboratory experiment to compare observed total particle light absorption (σ_abs) with that observed according to particle size by using a combination of a Differential Mobility Analyzer (DMA) and a Particle Soot Absorption Photometer (PSAP). The laboratory study confirmed strong similarities between the observed and derived σ_abs. In the second part the statistical approach using correlation between the σ_abs and the dN of each bin of the number size distribution was tested on long-term data ranging from 2002 to 2010 observed at Zeppelin station, Ny-Ålesund Svalbard. The data was clustered according to the number size distribution and grouped in four major categories: Washout, Nucleation, Intermediate and Polluted. Each category presented different features with respect to the derived eBC mass distributions, the Intermediate category showed similarities to the few available Single Particle Soot Photometer (SP2) observations in the Arctic. Overall, the statistical distribution of eBC, according to particle size, presented a larger dynamical range in the location of the mode(s). To check for consistency, the eBC mass distributions were transformed into number based eBC size distribution and compared to the observed total number size distribution. Whereas the Washout, Nucleation and Intermediate categories presented plausible number distributions, the Polluted category displayed a mode at small sizes (about 50 nm) that was significantly exaggerated.

From a polar to a marine environment: has the changing Arctic led to a shift in aerosol light scattering properties?

2020. Dominic Heslin-Rees (et al.). Atmospheric Chemistry And Physics 20 (21), 13671-13686

Article

The study of long-term trends in aerosol optical properties is an important task to understand the underlying aerosol processes influencing the change of climate. The Arctic, as the place where climate change manifests most, is an especially sensitive region of the world. Within this work, we use a unique long-term data record of key aerosol optical properties from the Zeppelin Observatory, Svalbard, to ask the question of whether the environmental changes of the last 2 decades in the Arctic are reflected in the observations. We perform a trend analysis of the measured particle light scattering and backscattering coefficients and the derived scattering Angstrom exponent and hemispheric backscattering fraction. In contrast to previous studies, the effect of in-cloud scavenging and of potential sampling losses at the site are taken explicitly into account in the trend analysis. The analysis is combined with a back trajectory analysis and satellite-derived sea ice data to support the interpretation of the observed trends. We find that the optical properties of aerosol particles have undergone clear and significant changes in the past 2 decades. The scattering Angstrom exponent exhibits statistically significant decreasing of between -4.9 % yr(-1) and -6.5 % yr(-1) (using wavelengths of lambda = 450 and 550 nm), while the particle light scattering coefficient exhibits statistically significant increasing trends of between 2.6 % yr(-1) and 2.9 % yr(-1) (at a wavelength of lambda = 550 nm). The magnitudes of the trends vary depending on the season. These trends indicate a shift to an aerosol dominated more by coarse-mode particles, most likely the result of increases in the relative amount of sea spray aerosol. We show that changes in air mass circulation patterns, specifically an increase in air masses from the south-west, are responsible for the shift in aerosol optical properties, while the decrease of Arctic sea ice in the last 2 decades only had a marginal influence on the observed trends.

Physical and chemical properties of aerosol particles and cloud residuals on Mt. angstrom reskutan in Central Sweden during summer 2014

2020. Emelie Linnéa Graham (et al.). Tellus. Series B, Chemical and physical meteorology 72 (1)

Article

The size distribution, volatility and hygroscopicity of ambient aerosols and cloud residuals were measured with a differential mobility particle sizer (DMPS) and a volatility-hygroscopicity tandem differential mobility analyser (VHTDMA) coupled to a counterflow virtual impactor (CVI) inlet during the Cloud and Aerosol Experiment at Are (CAEsAR) campaign at Mt. Areskutan during summer 2014. The chemical composition of particulate matter (PM) and cloud water were analysed offline using thermo-optical OC/EC analysis and ion chromatography. The importance of aerosol particle size for cloud droplet activation and subsequent particle scavenging was clearly visible in the measured size distributions. Cloud residuals were shifted towards larger sizes compared to ambient aerosol, and the cloud events were followed by a size distribution dominated by smaller particles. Organics dominated both PM (62% organic mass fraction) and cloud water (63% organic mass fraction) composition. The volatility and hygroscopicity of the ambient aerosols were representative of homogeneous aged aerosol with contributions from biogenic secondary organics, with median volume fraction remaining (VFR) of 0.04-0.05, and median hygroscopicity parameter kappa of 0.16-0.24 for 100-300 nm particles. The corresponding VFR and kappa for the cloud residuals were 0.03-0.04 and 0.18-0.20. The chemical composition, hygroscopicity and volatility measurements thus showed no major differences between the ambient aerosol particles and cloud residuals. The VFR and kappa values predicted based on the chemical composition measurements agreed well with the VHTDMA measurements, indicating the bulk chemical composition to be a reasonable approximation throughout the size distribution. There were indications, however, of some more subtle changes in time scales not achievable by the offline chemical analysis applied here. Further, online observations of aerosol and cloud residual chemical composition are therefore warranted.

Composition, isotopic fingerprint and source attribution of nitrate deposition from rain and fog at a Sub-Arctic Mountain site in Central Sweden (Mt Åreskutan)

2019. Carmen P. Vega (et al.). Tellus. Series B, Chemical and physical meteorology 71

Article

While dry and rain deposition of nitrate (NO3-) and ammonium (NH4+) are regularly assessed, fog deposition is often overlooked. This work assesses summer fog events contribution to nitrogen deposition and availability for forest ecosystems. Rain and fog samples were collected at Mt Areskutan, Sweden, during CAEsAR (Cloud and Aerosol Characterization Experiment), in 2014. NH4+ + NO3- represent (31 +/- 25) % of total rain ion amount, and (31 +/- 42) % in fog. Based on ion concentrations and the nitrate stable isotope signatures delta(N-15) and delta(O-18), it was possible to detect the plume generated by the Vastmanland forest fire; NOx emissions from oil rigs and Kola Peninsula; and the plume of Bardarbunga volcano, Iceland. Scavenging of ions by fog was more efficient than by rain. Rain NH4+ and NO3- deposition was (26 +/- 36) mu mol m(-2) d(-1) and (23 +/- 27) mu mol m(-2) d(-1), respectively. Fog NH4+ and NO3- contributed (77 +/- 80) % to total wet deposition of these species. Upscaling rain deposition fluxes to 1 year gave an inorganic nitrogen deposition of (18 +/- 16) mmol m(-2) a(-1) ((252 +/- 224) mg m(-2) a(-1) N equivalents), whereas fog deposition was estimated as (59 +/- 47) mmol m(-2) a(-1) ((826 +/- 658) mg m(-2) a(-1) N equivalents). Annual fog deposition was four times higher than previously reported for the area which only considered rain deposition. However, great uncertainty on the calculation of fog deposition need to be bear in mind. These findings suggest that fog should be considered in deposition estimates of inorganic nitrogen and major ions. If fog deposition is not accounted for, ion wet deposition may be greatly underestimated. Further sampling of wet and dry deposition is important for understanding the influence of nitrogen deposition on forest and vegetation development, as well as soil major ion loads.

Interactions between the atmosphere, cryosphere, and ecosystems at northern high latitudes

2019. Michael Boy (et al.). Atmospheric Chemistry And Physics 19 (3), 2015-2061

Article

The Nordic Centre of Excellence CRAICC (Cryosphere-Atmosphere Interactions in a Changing Arctic Climate), funded by NordForsk in the years 2011-2016, is the largest joint Nordic research and innovation initiative to date, aiming to strengthen research and innovation regarding climate change issues in the Nordic region. CRAICC gathered more than 100 scientists from all Nordic countries in a virtual centre with the objectives of identifying and quantifying the major processes controlling Arctic warming and related feedback mechanisms, outlining strategies to mitigate Arctic warming, and developing Nordic Earth system modelling with a focus on short-lived climate forcers (SLCFs), including natural and anthropogenic aerosols. The outcome of CRAICC is reflected in more than 150 peer-reviewed scientific publications, most of which are in the CRAICC special issue of the journal Atmospheric Chemistry and Physics. This paper presents an overview of the main scientific topics investigated in the centre and provides the reader with a state-of-the-art comprehensive summary of what has been achieved in CRAICC with links to the particular publications for further detail. Faced with a vast amount of scientific discovery, we do not claim to completely summarize the results from CRAICC within this paper, but rather concentrate here on the main results which are related to feedback loops in climate change-cryosphere interactions that affect Arctic amplification.

Multiple-scattering correction factor of quartz filters and the effect of filtering particles mixed in water: implications for analyses of light absorption in snow samples

2019. Jonas Svensson, Johan Ström, Aki Virkkula. Atmospheric Measurement Techniques 12 (11), 5913-5925

Article

The deposition of light-absorbing aerosol (LAA) onto snow initiates processes that lead to increased snowmelt. Measurements of LAA, such as black carbon (BC) and mineral dust, have been observed globally to darken snow. Several measurement techniques of LAA in snow collect the particulates on filters for analysis. Here we investigate micro-quartz filters' optical response to BC experiments in which the particles are initially suspended in air or in a liquid. With particle soot absorption photometers (PSAPs) we observed a 20% scattering enhancement for quartz filters compared to the standard PSAP Pallflex filters. The multiple-scattering correction factor (C-ref) of the quartz filters for airborne soot aerosol is estimated to be similar to 3.4. In the next stage correction factors were determined for BC particles mixed in water and also for BC particles both mixed in water and further treated in an ultrasonic bath. Comparison of BC collected from airborne particles with BC mixed in water filters indicated a higher mass absorption cross section by approximately a factor of 2 for the liquid-based filters, which is probably due to the BC particles penetrating deeper in the filter matrix. The ultrasonic bath increased absorption still further, roughly by a factor of 1.5, compared to only mixing in water. Application of the correction functions to earlier published field data from the Himalaya and Finnish Lapland yielded mass absorption coefficient (MAC) values of similar to 7-10 m(2) g(-1) at lambda = 550 nm, which is in the range of the published MAC of airborne BC aerosol.

On the seasonal variation in observed size distributions in northern Europe and their changes with decreasing anthropogenic emissions in Europe: climatology and trend analysis based on 17 years of data from Aspvreten, Sweden

2019. Peter Tunved, Johan Ström. Atmospheric Chemistry And Physics 19 (23), 14849-14873

Article

Size-resolved aerosol trends were investigated based on a 17-year data set (2000-2017) from the rural background site Aspvreten located in southern Sweden (58.8 degrees N, 17.4 degrees E). Cluster analysis of the size distributions was performed to aid in the interpretation of the data. The results confirm previous findings of decreasing aerosol mass and number during the last decades as a result of reduced anthropogenic emissions in Europe. We show that both particle modal number concentration and size have substantially been reduced during the last 17 years. Negative trends in particle number concentration of about 10 cm(-3) yr(-1) are present for nuclei, Aitken, and accumulation modes. In total, integral particle number concentration has decreased by 30 %, from 1860 to ca. 1300 cm(-3). The reduction in modal number concentration is accompanied by a decrease in modal size, and this decrease is largest for the accumulation mode (2 nm yr(-1) or about 17 % for the whole period). These reductions have resulted in a decrease in submicron particle mass (< 390 nm) by more than 50 % over the period 2000-2017. These decreases are similar to observations found at other stations in northern Europe. Although all size classes show a downward trend as annual averages, we also show that observed trends are not evenly distributed over the year and that a rather complex picture emerges where both sign and magnitude of trends vary with season and size. The strongest negative trends are present during spring (accumulation mode) and autumn (Aitken mode). The strongest positive trends are present during summer months (Aitken mode). The combined trajectory and data analyses do not present evidence for an increase in new particle formation formed locally, although some evidence of increased new particle formation some distance away from the receptor is present. Observed aerosol size distribution data, together with an adiabatic cloud parcel model, were further used to estimate the change in cloud droplet concentration for various assumptions of updraught velocities and aerosol chemical composition. The results indicate a substantial increase in the atmospheric brightening effect due to a reduction in cloud reflectivity corresponding to 10 %-12 % reduction in cloud albedo over the period 2000-2017.

Simultaneous measurements of aerosol size distributions at three sites in the European high Arctic

2019. Manuel Dall'Osto (et al.). Atmospheric Chemistry And Physics 19 (11), 7377-7395

Article

Aerosols are an integral part of the Arctic climate system due to their direct interaction with radiation and indirect interaction through cloud formation. Understanding aerosol size distributions and their dynamics is crucial for the ability to predict these climate relevant effects. When of favourable size and composition, both long-rangetransported - and locally formed particles - may serve as cloud condensation nuclei (CCN). Small changes of composition or size may have a large impact on the low CCN concentrations currently characteristic of the Arctic environment. We present a cluster analysis of particle size distributions (PSDs; size range 8-500 nm) simultaneously collected from three high Arctic sites during a 3-year period (20132015). Two sites are located in the Svalbard archipelago: Zeppelin research station (ZEP; 474 m above ground) and the nearby Gruvebadet Observatory (GRU; about 2 km distance from Zeppelin, 67 m above ground). The third site (Villum Research Station at Station Nord, VRS; 30 m above ground) is 600 km west-northwest of Zeppelin, at the tip of northeastern Greenland. The GRU site is included in an inter-site comparison for the first time. K-means cluster analysis pro- vided eight specific aerosol categories, further combined into broad PSD classes with similar characteristics, namely pristine low concentrations (12 %-14 % occurrence), new particle formation (16 %-32 %), Aitken (21 %-35 %) and accumulation (20 %-50 %). Confined for longer time periods by consolidated pack sea ice regions, the Greenland site GRU shows PSDs with lower ultrafine-mode aerosol concentrations during summer but higher accumulation-mode aerosol concentrations during winter, relative to the Svalbard sites. By association with chemical composition and cloud condensation nuclei properties, further conclusions can be derived. Three distinct types of accumulation-mode aerosol are observed during winter months. These are associated with sea spray (largest detectable sizes, > 400 nm), Arctic haze (main mode at 150 nm) and aged accumulation-mode (main mode at 220 nm) aerosols. In contrast, locally produced particles, most likely of marine biogenic origin, exhibit size distributions dominated by the nucleation and Aitken mode during summer months. The obtained data and analysis point towards future studies, including apportioning the relative contribution of primary and secondary aerosol formation processes and elucidating anthropogenic aerosol dynamics and transport and removal processes across the Greenland Sea. In order to address important research questions in the Arctic on scales beyond a singular station or measurement events, it is imperative to continue strengthening international scientific cooperation.

Year-Round In Situ Measurements of Arctic Low-Level Clouds: Microphysical Properties and Their Relationships With Aerosols

2019. M. Koike (et al.). Journal of Geophysical Research - Atmospheres 124 (3), 1798-1822

Article

Two years of continuous in situ measurements of Arctic low-level clouds have been made at the Mount Zeppelin Observatory (78 degrees 56N, 11 degrees 53E), in Ny-angstrom lesund, Spitsbergen. The monthly median value of the cloud particle number concentration (N-c) showed a clear seasonal variation: Its maximum appeared in May-July (658cm(-3)), and it remained low between October and March (87cm(-3)). At temperatures warmer than 0 degrees C, a clear correlation was found between the hourly N-c values and the number concentrations of aerosols with dry diameters larger than 70nm (N-70), which are proxies for cloud condensation nuclei (CCN). When clouds were detected at temperatures colder than 0 degrees C, some of the data followed the summertime N-c to N-70 relationship, while other data showed systematically lower N-c values. The lidar-derived depolarization ratios suggested that the former (CCN-controlled) and latter (CCN-uncontrolled) data generally corresponded to clouds consisting of supercooled water droplets and those containing ice particles, respectively. The CCN-controlled data persistently appeared throughout the year at Zeppelin. The aerosol-cloud interaction index (ACI=dlnN(c)/(3dlnN(70))) for the CCN-controlled data showed high sensitivities to aerosols both in the summer (clean air) and winter-spring (Arctic haze) seasons (0.220.03 and 0.250.02, respectively). The air parcel model calculations generally reproduced these values. The threshold diameters of aerosol activation (D-act), which account for the N-c of the CCN-controlled data, were as low as 30-50nm when N-70 was less than 30cm(-3), suggesting that new particle formation can affect Arctic cloud microphysics.

Cloud droplet activation of black carbon particles coated with organic compounds of varying solubility

2018. Maryam Dalirian (et al.). Atmospheric Chemistry and Physics Discussions 18 (16), 12477-12489

Article

Atmospheric black carbon (BC) particles are a concern due to their impact on air quality and climate. Their net climate effect 15 is, however, still uncertain. This uncertainty is partly related to the contribution of coated BC-particles to the global CCN budgets. In this study, laboratory measurements were performed to investigate cloud condensation nuclei (CCN) activity of BC (Regal black) particles, in pure state or coated through evaporating and subsequent condensation of glutaric acid, levoglucosan (both water-soluble organics) or oleic acid (an organic compound with low solubility). A combination of Soot Particle Aerosol Mass Spectrometer (SP-AMS) measurements and size distribution measurements with Scanning Mobility 20 Particle Sizer (SMPS) showed that the studied BC particles were nearly spherical agglomerates with a fractal dimension of 2.79 and that they were coated evenly by the organic species. The CCN activity of BC particles increased after coating with all the studied compounds and was governed by the fraction of organic material. The CCN activation of the BC particles coated by glutaric acid and levoglucosan were in good agreement with the theoretical calculations using shell-and-core model, which is based on a combination of the CCN activities of the pure compounds. The oleic acid coating enhanced the CCN 25 activity of the BC particles, even though the pure oleic acid particles were CCN inactive. The surprising effect of oleic acid might be related to the arrangement of the oleic acid molecules on the surface of the BC cores or other surface phenomena facilitating water condensation onto the coated particles. Our results show potential in accurately predicting the CCN activity of atmospheric BC coated with organic species by present theories, given that the identities and amount of the coating species are known. Furthermore, our results suggest that even relatively thin soluble coatings (around 2 nm for the compounds studied here) are enough to make the insoluble BC particles CCN active at typical atmospheric supersaturations and thus be efficiently taken up by cloud droplets. This highlights the need of an accurate description of the composition of atmospheric particles containing BC to unravel their net impact on climate.

Light-absorption of dust and elemental carbon in snow in the Indian Himalayas and the Finnish Arctic

2018. Jonas Svensson (et al.). Atmospheric Measurement Techniques 11 (3), 1403-1416

Article

Light-absorbing impurities (LAIs) deposited in snow have the potential to substantially affect the snow radiation budget, with subsequent implications for snow melt. To more accurately quantify the snow albedo, the contribution from different LAIs needs to be assessed. Here we estimate the main LAI components, elemental carbon (EC) (as a proxy for black carbon) and mineral dust in snow from the Indian Himalayas and paired the results with snow samples from Arctic Finland. The impurities are collected onto quartz filters and are analyzed thermal-optically for EC, as well as with an additional optical measurement to estimate the light-absorption of dust separately on the filters. Laboratory tests were conducted using substrates containing soot and mineral particles, especially prepared to test the experimental setup. Analyzed ambient snow samples show EC concentrations that are in the same range as presented by previous research, for each respective region. In terms of the mass absorption cross section (MAC) our ambient EC surprisingly had about half of the MAC value compared to our laboratory standard EC (chimney soot), suggesting a less light absorptive EC in the snow, which has consequences for the snow albedo reduction caused by EC. In the Himalayan samples, larger contributions by dust (in the range of 50% or greater for the light absorption caused by the LAI) highlighted the importance of dust acting as a light absorber in the snow. Moreover, EC concentrations in the Indian samples, acquired from a 120 cm deep snow pit (possibly covering the last five years of snow fall), suggest an increase in both EC and dust deposition. This work emphasizes the complexity in determining the snow albedo, showing that LAI concentrations alone might not be sufficient, but additional transient effects on the light-absorbing properties of the EC need to be considered and studied in the snow. Equally as imperative is the confirmation of the spatial and temporal representativeness of these data by comparing data from several and deeper pits explored at the same time.

The seasonal characteristics of cloud condensation nuclei (CCN) in the arctic lower troposphere

2018. Chang Hoon Jung (et al.). Tellus. Series B, Chemical and physical meteorology 70 (1), 1-13

Article

Cloud Condensation Nuclei (CCN) concentration and aerosol size distributions in the Arctic were collected during the period 2007-2013 at the Zeppelin observatory (78.91 degrees N, 11.89 degrees E, 474 masl). Annual median CCN concentration at a supersaturation (SS) of 0.4% show the ranges of 45 approximate to 81cm(-3). The monthly median CCN number density varied between 17cm(-3) in October 2007 and 198cm(-3) in March, 2008. The CCN spectra parameters C (83cm(-3)) and k (0.23) were derived. In addition, calculated annual median value of hygroscopicity parameter is 0.46 at SS of 0.4%. Particle number concentration of accumulation mode from aerosol size distribution measurements are well correlated with CCN concentration. The CCN to CN>10 nm (particle number concentration larger than 10nm in diameter) ratio shows a maximum during March and minimum during July. The springtime high CCN concentration is attributed to high load of accumulation mode aerosol transported from the mid-latitudes, known as Arctic Haze. CCN concentration remains high also during Arctic summer due to the source of new CCN through particle formation followed by consecutive aerosol growth. Lowest aerosol as well as CCN number densities were observed during Arctic autumn and early winter when aerosol formation in the Arctic and long-range transport into the Arctic are not effective.

A new aerosol wet removal scheme for the Lagrangian particle model FLEXPART

2017. Henrik Grythe (et al.). Geoscientific Model Development 10 (4), 1447-1466

Article

A new and more physically based treatment of how removal by precipitation is calculated by FLEXPART is introduced, to take into account more aspects of aerosol diversity. Also new, is the definition of clouds and cloud properties. Results from simulations show good agreement with observed atmospheric concentrations for distinctly different aerosols. Atmospheric lifetimes were found to vary from a few hours (large aerosol particles) up to a month (small non-soluble).

Arctic sea ice melt leads to atmospheric new particle formation

2017. M. Dall' Osto (et al.). Scientific Reports 7

Article

Atmospheric new particle formation (NPF) and growth significantly influences climate by supplying new seeds for cloud condensation and brightness. Currently, there is a lack of understanding of whether and how marine biota emissions affect aerosol-cloud-climate interactions in the Arctic. Here, the aerosol population was categorised via cluster analysis of aerosol size distributions taken at Mt Zeppelin (Svalbard) during a 11 year record. The daily temporal occurrence of NPF events likely caused by nucleation in the polar marine boundary layer was quantified annually as 18%, with a peak of 51% during summer months. Air mass trajectory analysis and atmospheric nitrogen and sulphur tracers link these frequent nucleation events to biogenic precursors released by open water and melting sea ice regions. The occurrence of such events across a full decade was anti-correlated with sea ice extent. New particles originating from open water and open pack ice increased the cloud condensation nuclei concentration background by at least ca. 20%, supporting a marine biosphere-climate link through sea ice melt and low altitude clouds that may have contributed to accelerate Arctic warming. Our results prompt a better representation of biogenic aerosol sources in Arctic climate models.

Chemical composition and source analysis of carbonaceous aerosol particles at a mountaintop site in central Sweden

2017. Vera Franke (et al.). Tellus. Series B, Chemical and physical meteorology 69

Article

The chemical composition of atmospheric particulate matter at Mt. angstrom reskutan, a mountaintop site in central Sweden, was analysed with a focus on its carbonaceous content. Filter samples taken during the Cloud and Aerosol Experiment at angstrom re (CAEsAR 2014) were analysed by means of a thermo-optical method and ion chromatography. Additionally, the particle light absorption and particle number size distribution measurements for the entire campaign were added to the analysis. Mean airborne concentrations of organic and elemental carbon during CAEsAR 2014 were OC= 0.85 +/- 0.8 mu gm(-3) and EC = 0.06 +/- 0.06 mu gm(-3), respectively. Elemental to organic carbon ratios varied between EC/OC = 0.02 and 0.19. During the study a large wildfire occurred in Vastmanland, Sweden, with the plume reaching our study site. This led to significant increases in OC and EC concentrations (OC = 3.04 +/- 0.03 mu gm(-3) and EC = 0.24 +/- 0.00 mu gm(-3)). The mean mass-specific absorption coefficient observed during the campaign was sigma(BC)(abs) = 9.1 +/- 7.3 m(2)g(-1) (at wavelength lambda= 637 nm). In comparison to similarly remote European sites, Mt. angstrom reskutan experienced significantly lower carbonaceous aerosol loadings with a clear dominance of organic carbon. A mass closure study revealed a missing chemical mass fraction that likely originated from mineral dust. Potential regional source contributions of the carbonaceous aerosol were investigated using modelled air mass back trajectories. This source apportionment pointed to a correlation between high EC concentrations and air originating from continental Europe. Particles rich in organic carbon most often arrived from highly vegetated continental areas. However, marine regions were also a source of these aerosol particles. The source contributions derived during this study were compared to emission inventories of an Earth system model. This comparison highlighted a lack of OC and EC point-sources in the model's emission inventory which could potentially lead to an underestimation of the carbonaceous aerosol reaching Mt. angstrom reskutan in the simulation of this Earth system model.

Do contemporary (1980-2015) emissions determine the elemental carbon deposition trend at Holtedahlfonna glacier, Svalbard?

2017. Meri M. Ruppel (et al.). Atmospheric Chemistry And Physics 17 (20), 12779-12795

Article

The climate impact of black carbon (BC) is notably amplified in the Arctic by its deposition, which causes albedo decrease and subsequent earlier snow and ice spring melt. To comprehensively assess the climate impact of BC in the Arctic, information on both atmospheric BC concentrations and deposition is essential. Currently, Arctic BC deposition data are very scarce, while atmospheric BC concentrations have been shown to generally decrease since the 1990s. However, a 300-year Svalbard ice core showed a distinct increase in EC (elemental carbon, proxy for BC) deposition from 1970 to 2004 contradicting atmospheric measurements and modelling studies. Here, our objective was to decipher whether this increase has continued in the 21st century and to investigate the drivers of the observed EC deposition trends. For this, a shallow firn core was collected from the same Svalbard glacier, and a regional-to-meso-scale chemical transport model (SILAM) was run from 1980 to 2015. The ice and firn core data indicate peaking EC deposition values at the end of the 1990s and lower values thereafter. The modelled BC deposition results generally support the observed glacier EC variations. However, the ice and firn core results clearly deviate from both measured and modelled atmospheric BC concentration trends, and the modelled BC deposition trend shows variations seemingly independent from BC emission or atmospheric BC concentration trends. wet-deposited at this Svalbard glacier, indicating that meteorological processes such as precipitation and scavenging efficiency have most likely a stronger influence on the BC deposition trend than BC emission or atmospheric concentration trends. BC emission source sectors contribute differently to the modelled atmospheric BC concentrations and BC deposition, which further supports our conclusion that different processes affect atmospheric BC concentration and deposition trends. Consequently, Arctic BC deposition trends should not directly be inferred based on atmospheric BC measurements, and more observational BC deposition data are required to assess the climate impact of BC in Arctic snow.

Trends in black carbon and size-resolved particle number concentrations and vehicle emission factors under real-world conditions

2017. Patricia Krecl (et al.). Atmospheric Environment 165, 155-168

Article

Kerbside concentrations of NOx, black carbon (BC), total number of particles (diameter > 4 nm) and number size distribution (28-410 nm) were measured at a busy street canyon in Stockholm in 2006 and 2013. Over this period, there was an important change in the vehicle fleet due to a strong dieselisation process of light-duty vehicles and technological improvement of vehicle engines. This study assesses the impact of these changes on ambient concentrations and particle emission factors (EF). EF were calculated by using a novel approach which combines the NOx tracer method with positive matrix factorisation (PMF) applied to particle number size distributions. NOx concentrations remained rather constant between these two years, whereas a large decrease in particle concentrations was observed, being on average 60% for BC, 50% for total particle number, and 53% for particles in the range 28-100 nm. The PMF analysis yielded three factors that were identified as contributions from gasoline vehicles, diesel fleet, and urban background. This separation allowed the calculation of the average vehicle EF for each particle metric per fuel type. In general, gasoline EF were lower than diesel EF, and EF for 2013 were lower than the ones derived for 2006. The EFBC decreased 77% for both gasoline and diesel fleets, whereas the particle number EF reduction was higher for the gasoline (79%) than for the diesel (37%) fleet. Our EF are consistent with results from other on-road studies, which reinforces that the proposed methodology is suitable for EF determination and to assess the effectiveness of policies implemented to reduce vehicle exhaust emissions. However, our EF are much higher than EF simulated with traffic emission models (HBEFA and COPERT) that are based on dynamometer measurements, except for EFBC for diesel vehicles. This finding suggests that the EF from the two leading models in Europe should be revised for BC (gasoline vehicles) and particle number (all vehicles), since they are used to compile national inventories for the road transportation sector and also to assess their associated health effects. Using the calculated kerbside EF, we estimated that the traffic emissions were lower in 2013 compared to 2006 with a 61% reduction for BC (due to decreases in both gasoline and diesel emissions), and 34-45% for particle number (reduction only in gasoline emissions). Limitations of the application of these EF to other studies are also discussed.

Multi-seasonal ultrafine aerosol particle number concentration measurements at the Gruvebadet observatory, Ny-lesund, Svalbard Islands

2016. Angelo Lupi (et al.). Rendiconti lincei scienze fisiche e naturali 27, 59-71

Article

The object of this study was to investigate the different modal behavior of ultrafine aerosol particles collected at the Gruvebadet observatory located in Ny-lesund (Svalbard Islands, 78A degrees 55'N, 11A degrees 56'E). Aerosol particle size distribution was measured in the size range from 10 to 470 nm typically from the beginning of spring to the beginning of fall during four (non-consecutive) years (2010, 2011, 2013 and 2014). The median concentration for the whole period taken into account was 214 particles cm(-3), oscillating between the median maximum in July with a concentration of 257 particles cm(-3) and a median minimum in April with 197 particles cm(-3). The median total number concentration did not present a well-defined seasonal behavior, as shown by contrast looking at the sub/modal number concentration, where distinct trends appeared in the predominant accumulation concentration recorded during April/May and the preponderant concentration of Aitken particles during the summer months. Lastly, the short side-by-side spring 2013 campaign performed at the Zeppelin observatory with a differential mobility particle sizer was characterized by an aerosol concentration mean steady difference between the two instruments of around 14 %, thereby supporting the reliability of the device located at Gruvebadet.

Characterisation and Source Apportionment of Submicron Particle Number Size Distributions in a Busy Street Canyon

2015. Patricia Krecl (et al.). Aerosol and Air Quality Research 15 (1), 220-233

Article

Street canyons are well-known hot spots due to the harmful exposure to high concentrations of atmospheric pollutants emitted mainly by motor vehicles. We report on measurements of air pollutants conducted in a street canyon in Stockholm (Sweden) in spring 2006. Particle number size distributions (PNSD) were measured in the 25-606 nm range, along with total particle number, light-absorbing carbon mass concentration (M-LAC), PM10, NOx, CO, traffic rate (TR), vehicle speed and meteorological variables. We used PNSD as input to the positive matrix factorisation (PMF) analysis to identify and apportion the pollutant sources. All pollutants showed distinct diurnal patterns, with highest concentrations in weekday mornings (08:00-09:00). TR was always higher on weekdays, except for the early hours (00:00-06:00). The raise in the weekend early-hour TR was accompanied by the largest MLAC of the day, a higher NOx/CO ratio compared to weekdays and a modal shift of PNSD towards larger diameters (47-56 nm), indicates a change in the vehicle fleet share to being dominated by diesel-run taxis. The largest contribution to the submicron particles was observed for winds blowing along the canyon, transporting particles emitted by vehicles accelerating from the traffic lights at the intersection, uphill towards the measurement site, and from the nearby streets. Three PMF factors were identified: local emissions from a mixed fleet dominated by gasoline engines, local traffic emissions highly impacted by diesel vehicles, and urban background aerosol. On average, gasoline-fuelled vehicles largely contributed to NOx, and particle number concentrations (54-65%), whereas M-LAC sources were dominated by diesel emissions, especially at weekends in the early hours (73%). The urban background contribution was rather low (4-13%) and with little dependence on the weekday. This work demonstrated how particle size distribution measurements, together with M-LAC, NOx and CO can be used to quantify the contribution from diesel and gasoline vehicles.

In situ observations of black carbon in snow and the corresponding spectral surface albedo reduction

2015. C. A. Pedersen (et al.). Journal of Geophysical Research - Atmospheres 120 (4), 1476-1489

Article

Black carbon (BC) particles emitted from incomplete combustion of fossil fuel and biomass and deposited on snow and ice darken the surface and reduce the surface albedo. Even small initial surface albedo reductions may have larger adjusted effects due to snow morphology changes and changes in the sublimation and snow melt rate. Most of the literature on the effect of BC on snow surface albedo is based on numerical models, and few in situ field measurements exist to confirm this reduction. Here we present an extensive set of concurrent in situ measurements of spectral surface albedo, BC concentrations in the upper 5 cm of the snowpack, snow physical parameters (grain size and depth), and incident solar flux characteristics from the Arctic. From this data set (with median BC concentrations ranging from 5 to 137 ng BC per gram of snow) we are able to separate the BC signature on the snow albedo from the natural snow variability. Our measurements show a significant correlation between BC in snow and spectral surface albedo. Based on these measurements, parameterizations are provided, relating the snow albedo, as a function of wavelength, to the equivalent BC content in the snowpack. The term equivalent BC used here is the elemental carbon concentration inferred from the thermo-optical method adjusted for the fraction of non-BC constituents absorbing sunlight in the snow. The first parameterization is a simple equation which efficiently describes the snow albedo reduction due to the equivalent BC without including details on the snow or BC microphysics. This can be used in models when a simplified description is needed. A second parameterization, including snow grain size information, shows enhanced correspondence with the measurements. The extracted parameterizations are valid for wavelength bands 400-900 nm, constrained for BC concentrations between 1 and 400 ng g(-1), and for an optically thick snowpack. The parameterizations are purely empirical, and particular focus was on the uncertainties associated with the measurements, and how these uncertainties propagate in the parameterizations. Integrated, the first parameterization (based only on the equivalent BC) gives a broadband (400-900 nm) snow albedo reduction of 0.004 due to 10 ng equivalent BC per gram of snow, while the effect is almost 5 times larger for BC concentrations 1 order of magnitude higher. The study shows that the reconstructed albedo from the second parameterization (including information on the snow grain size) corresponds better to the radiative transfer model Snow, Ice, and Aerosol Radiation albedo than the reconstructed albedo from the first parameterization (excluding grain size information).

Size-resolved cloud condensation nuclei concentration measurements in the Arctic: two case studies from the summer of 2008

2015. Julia Zabori (et al.). Atmospheric Chemistry And Physics 15 (23), 13803-13817

Article

The Arctic is one of the most vulnerable regions affected by climate change. Extensive measurement data are needed to understand the atmospheric processes governing this vulnerability. Among these, data describing cloud formation potential are of particular interest, since the indirect effect of aerosols on the climate system is still poorly understood. In this paper we present, for the first time, size-resolved cloud condensation nuclei (CCN) data obtained in the Arctic. The measurements were conducted during two periods in the summer of 2008: one in June and one in August, at the Zeppelin research station (78 degrees 54'N, 11 degrees 53'E) in Svalbard. Trajectory analysis indicates that during the measurement period in June 2008, air masses predominantly originated from the Arctic, whereas the measurements from August 2008 were influenced by mid-latitude air masses. CCN supersaturation (SS) spectra obtained on the 27 June, before size-resolved measurements were begun, and spectra from the 21 and 24 August, conducted before and after the measurement period, revealed similarities between the 2 months. From the ratio between CCN concentration and the total particle number concentration (CN) as a function of dry particle diameter (D-p) at a SS of 0.4 %, the activation diameter (D-50), corresponding to CCN / CN = 0.50, was estimated. D-50 was found to be 60 and 67 nm for the examined periods in June and August 2008, respectively. Corresponding D-50 hygroscopicity parameter (kappa) values were estimated to be 0.4 and 0.3 for June and August 2008, respectively. These values can be compared to hygroscopicity values estimated from bulk chemical composition, where kappa was calculated to be 0.5 for both June and August 2008. While the agreement between the 2 months is reasonable, the difference in kappa between the different methods indicates a size dependence in the particle composition, which is likely explained by a higher fraction of inorganics in the bulk aerosol samples.

The relationship between cloud condensation nuclei (CCN) concentration and light extinction of dried particles: indications of underlying aerosol processes and implications for satellite-based CCN estimates

2015. Y. Shinozuka (et al.). Atmospheric Chemistry And Physics 15 (13), 7585-7604

Article

We examine the relationship between the number concentration of boundary-layer cloud condensation nuclei (CCN) and light extinction to investigate underlying aerosol processes and satellite-based CCN estimates. For a variety of airborne and ground-based observations not dominated by dust, regression identifies the CCN (cm(-3)) at 0.4 +/- 0.1% supersaturation with 10(0.3 alpha+1.3)sigma(0.75) where sigma (Mm(-1)) is the 500 nm extinction coefficient by dried particles and alpha is the Angstrom exponent. The deviation of 1 km horizontal average data from this approximation is typically within a factor of 2.0. partial derivative logCCN / partial derivative log sigma is less than unity because, among other explanations, growth processes generally make aerosols scatter more light without increasing their number. This, barring special meteorology-aerosol connections, associates a doubling of aerosol optical depth with less than a doubling of CCN, contrary to previous studies based on heavily averaged measurements or a satellite algorithm.

A feasibility study of mapping light-absorbing carbon using a taxi fleet as a mobile platform

2014. Patricia Krecl (et al.). Tellus. Series B, Chemical and physical meteorology 66, 23533

Article

Carbon-containing particles are associated with adverse health effects, and their light-absorbing fractions were recently estimated to be the second largest contributor to global warming after carbon dioxide. Knowledge on the spatiotemporal variability of light-absorbing carbon (LAC) particles in urban areas is relevant for air quality management and to better diagnose the population exposure to these particles. This work reports on the first mobile LAC mass concentrations (M-LAC) measured on-board four taxis in the Stockholm metropolitan area in November 2011. On average, concentrations were higher and more variable during daytime (median of 1.9 mu g m(-3) and median absolute deviation of 2.3 mu g m(-3)). Night-time (21:00-05:00) measurements were very similar for all road types and also compared to levels monitored at an urban background fixed site (median of 0.9 mu g m(-3)). We observed a large intra-urban variability in concentrations, with maxima levels inside road tunnels (median and 95th percentile of 7.5 and 40.1 mu g m(-3), respectively). Highways presented the second ranked concentrations (median and 95th percentile of 3.2 and 9.7 mu g m(-3), respectively) associated with highest vehicle speed (median of 65 km h(-1)), traffic rates (median of 62 000 vehicles day(-1) and 1500 vehicles h(-1)) and diesel vehicles share (7-10%) when compared to main roads, canyon streets, and local roads. Multiple regression modelling identified hourly traffic rate and M-LAC concentration measured at an urban background site as the best predictors of on-road concentrations, but explained only 25% of the observed variability. This feasibility study proved to be a time-and cost-effective approach to map out ambient M-LAC concentrations in Stockholm and more research is required to represent the distribution in other periods of the year. Simultaneous monitoring of other pollutants, closely correlated to M-LAC levels in traffic-polluted environments, and including video recording of road and traffic changes would be an asset.

A review of sea-spray aerosol source functions using a large global set of sea salt aerosol concentration measurements

2014. Henrik Grythe (et al.). Atmospheric Chemistry And Physics 14 (3), 1277-1297

Article

Sea-spray aerosols (SSA) are an important part of the climate system because of their effects on the global radiative budget - both directly as scatterers and absorbers of solar and terrestrial radiation, and indirectly as cloud condensation nuclei (CCN) influencing cloud formation, lifetime, and precipitation. In terms of their global mass, SSA have the largest uncertainty of all aerosols. In this study we review 21 SSA source functions from the literature, several of which are used in current climate models. In addition, we propose a new function. Even excluding outliers, the global annual SSA mass produced spans roughly 3-70 Pg yr(-1) for the different source functions, for particles with dry diameter D-p < 10 mu m, with relatively little interannual variability for a given function. The FLEXPART Lagrangian particle dispersion model was run in backward mode for a large global set of observed SSA concentrations, comprised of several station networks and ship cruise measurement campaigns. FLEXPART backward calculations produce gridded emission sensitivity fields, which can subsequently be multiplied with gridded SSA production fluxes in order to obtain modeled SSA concentrations. This allowed us to efficiently and simultaneously evaluate all 21 source functions against the measurements. Another advantage of this method is that source-region information on wind speed and sea surface temperatures (SSTs) could be stored and used for improving the SSA source function parameterizations. The best source functions reproduced as much as 70% of the observed SSA concentration variability at several stations, which is comparable with state of the art aerosol models. The main driver of SSA production is wind, and we found that the best fit to the observation data could be obtained when the SSA production is proportional to U-10(3.5), where U-10 is the source region averaged 10m wind speed. A strong influence of SST on SSA production, with higher temperatures leading to higher production, could be detected as well, although the underlying physical mechanisms of the SST influence remains unclear. Our new source function with wind speed and temperature dependence gives a global SSA production for particles smaller than D-p < 10 mu m of 9 Pg yr(-1), and is the best fit to the observed concentrations.

Elemental carbon in snow at Changbai Mountain, northeastern China: concentrations, scavenging ratios, and dry deposition velocities

2014. Z. W. Wang (et al.). Atmospheric Chemistry And Physics 14 (2), 629-640

Article

Light-absorbing aerosol - particularly elemental carbon (EC) - while mixed with snow and ice is an important climate driver from the enhanced absorption of solar radiation. Currently, considerable efforts are being made to estimate its radiative forcing on a global scale, but several uncertainties remain, particularly those regarding its deposition processes. In this study, concurrent measurements of EC in air and snow are performed for three years (2009-2012) at Changbai station, northeastern China. The scavenging ratio and the wet-and dry-deposition fluxes of EC over the snow surface are estimated. The mean EC concentration in the surface snow is 1000 +/- 1500 ng g(-1), ranging from 7 to 7640 ng g(-1). The mean value of the scavenging ratio of EC by snow is 140 +/- 100, with a median value of 150, which is smaller than that reported in Arctic areas. A non-rimed snow process is a significant factor in interpreting differences with Arctic areas. Wet-deposition fluxes of EC are estimated to be 0.47 +/- 0.37 mu g cm(-2) month(-1) on average over the three snow seasons studied. Dry deposition is more than five times higher, with an average of 2.65 +/- 1.93 mu g cm(-2) month(-1); however, only winter period estimation is possible (December-February). During winter in Changbai, 87% of EC in snow is estimated to be due to dry deposition, with a mean dry deposition velocity of 6.44 x 10(-3) ms(-1) and median of 8.14 x 10(-3) ms(-1). Finally, the calculation of the radiative effect shows that 500 ng g(-1) of dry-deposited EC to a snow surface absorbs three times more incoming solar energy than the same mass mixed in the snow through wet deposition. Deposition processes of an EC-containing snow surface are, therefore, crucial to estimate its radiative forcing better, particularly in northeastern China, where local emission strongly influences the level and gradient of EC in the snowpack, and snow-covered areas are cold and dry due to the atmospheric general circulation. Furthermore, this study builds on the knowledge to characterize the conditions in the snow-laden Chinese rural areas better as well as to constrain transport of EC to the Arctic better.

Hygroscopic growth and cloud forming potential of Arctic aerosol based on observed chemical and physical characteristics (a 1 year study 2007-2008)

2014. S. Silvergren (et al.). Journal of Geophysical Research - Atmospheres 119 (24), 14080-14097

Article

Aerosol particle samples were collected, and the particle size distribution was measured during 1 year at the Zeppelin station (474 m asl) on Svalbard. The chemical constituents, hygroscopicity, and cloud forming properties of the aerosol were analyzed. The aerosol contained mostly sulfate and nitrate during the summer, whereas from September to February the main components were sodium and chloride. The highest concentration (20%) of water-soluble organic matter was sampled in December. The hygroscopic growth factors for the water-soluble fraction were 1.56-2.01 at 90% relative humidity, peaking in October, when the measured supersaturations needed for cloud drop formation were also the lowest. Sea-salt components showed a positive correlation with the cloud forming capability, whereas the organic content had no correlation. The hygroscopicity factors, or kappa values, were determined in three ways for each month: (1)kappa(H-TDMA) from measurements of the hygroscopic growth of particles produced from atomization of the filter extracts, (2)kappa(CCNC) from measurements of the critical supersaturation as a function of size for these particles, and (3)kappa(chem) was modeled based on the organic and inorganic composition of the filter samples. Using the measured particle size distributions and the critical activation diameters from the Cloud Condensation Nuclei Counter (CCNC) measurements, it was found that the number of CCN varied more with supersaturation during the summer months. The best agreement between all three kappa values was in December and January. Comparisons with earlier studies do not suggest any trend in the Arctic aerosol seasonal variability over the last decade.

Increase in elemental carbon values between 1970 and 2004 observed in a 300-year ice core from Holtedahlfonna (Svalbard)

2014. M. M. Ruppel (et al.). Atmospheric Chemistry And Physics 14 (20), 11447-11460

Article

Black carbon (BC) is a light-absorbing particle that warms the atmosphere-Earth system. The climate effects of BC are amplified in the Arctic, where its deposition on light surfaces decreases the albedo and causes earlier melt of snow and ice. Despite its suggested significant role in Arctic climate warming, there is little information on BC concentrations and deposition in the past. Here we present results on BC (here operationally defined as elemental carbon (EC)) concentrations and deposition on a Svalbard glacier between 1700 and 2004. The inner part of a 125m deep ice core from Holtedahlfonna glacier (79 degrees 8'N, 13 degrees 16'E, 1150 m a.s.l.) was melted, filtered through a quartz fibre filter and analysed for EC using a thermal-optical method. The EC values started to increase after 1850 and peaked around 1910, similar to ice core records from Greenland. Strikingly, the EC values again increase rapidly between 1970 and 2004 after a temporary low point around 1970, reaching unprecedented values in the 1990s. This rise is not seen in Greenland ice cores, and it seems to contradict atmospheric BC measurements indicating generally decreasing atmospheric BC concentrations since 1989 in the Arctic. For example, changes in scavenging efficiencies, post-depositional processes and differences in the vertical distribution of BC in the atmosphere are discussed for the differences between the Svalbard and Greenland ice core records, as well as the ice core and atmospheric measurements in Svalbard. In addition, the divergent BC trends between Greenland and Svalbard ice cores may be caused by differences in the analytical methods used, including the operational definitions of quantified particles, and detection efficiencies of different-sized BC particles. Regardless of the cause of the increasing EC values between 1970 and 2004, the results have significant implications for the past radiative energy balance at the coring site.

Mixing State of Size-Selected Submicrometer Particles in the Arctic in May and September 2012

2014. Kihong Park (et al.). Environmental Science and Technology 48 (2), 909-919

Article

Aerosols have been associated with large uncertainties in estimates of the radiation budget and cloud formation processes in the Arctic. This paper reports the results of a study of in situ measurements of hygroscopicity, fraction of volatile species, mixing state, and off-line morphological and elemental analysis of Aitken and accumulation mode particles in the Arctic (Ny-Alesund, Svalbard) in May and September 2012. The accumulation mode particles were more abundant in May than in September. This difference was due to more air mass flow from lower latitude continental areas, weaker vertical mixing, and less wet scavenging in May than in September, which may have led to a higher amount of long-range transport aerosols entering the Arctic in the spring. The Aitken mode particles observed intermittently in May were produced by nucleation, absent significant external mixing, whereas the accumulation mode particles displayed significant external mixing. The occurrence of an external mixing state was observed often in May than in September and more often in accumulation mode particles than in Aitken mode particles, and it was associated more with continental air masses (Siberian) than with other air masses. The external mixing of the accumulation mode particles in May may have been caused by multiple sources (i.e., long-range transport aerosols with aging and marine aerosols). These groups of externally mixed particles were subdivided into different mixing structures (internal mixtures of predominantly sulfates and volatile organics without nonvolatile species and internal mixtures of sulfates and nonvolatile components, such as sea salts, minerals, and soot). The variations in the mixing states and chemical species of the Arctic aerosols in terms of their sizes, air masses, and seasons suggest that the continuous size-dependent measurements observed in this study are useful for obtaining better estimates of the effects of these aerosols on climate change.

Organosulfates and organic acids in Arctic aerosols: speciation, annual variation and concentration levels

2014. A. M. K. Hansen (et al.). Atmospheric Chemistry And Physics 14 (15), 7807-7823

Article

Sources, composition and occurrence of secondary organic aerosols in the Arctic were investigated at Zeppelin Mountain, Svalbard, and Station Nord, northeastern Greenland, during the full annual cycle of 2008 and 2010, respectively. Speciation of organic acids, organosulfates and nitrooxy organosulfates - from both anthropogenic and biogenic precursors were in focus. A total of 11 organic acids (terpenylic acid, benzoic acid, phthalic acid, pinic acid, suberic acid, azelaic acid, adipic acid, pimelic acid, pinonic acid, diaterpenylic acid acetate and 3-methyl-1,2,3-butanetricarboxylic acid), 12 organosulfates and 1 nitrooxy organosulfate were identified in aerosol samples from the two sites using a high-performance liquid chromatograph (HPLC) coupled to a quadrupole Time-of-Flight mass spectrometer. At Station Nord, compound concentrations followed a distinct annual pattern, where high mean concentrations of organosulfates (47 +/- 14 ng m(-3)) and organic acids (11.5 +/- 4 ng m(-3)) were observed in January, February and March, contrary to considerably lower mean concentrations of organosulfates (2 +/- 3 ng m(3-)) and organic acids (2.2 +/- 1 ng m(-3)) observed during the rest of the year. At Zeppelin Mountain, organosulfate and organic acid concentrations remained relatively constant during most of the year at a mean concentration of 15 +/- 4 ng m(-3) and 3.9 +/- 1 ng m(-3), respectively. However during four weeks of spring, remarkably higher concentrations of total organosulfates (23-36 ng m(-3)) and total organic acids (7-10 ngm(-3)) were observed. Elevated organosulfate and organic acid concentrations coincided with the Arctic haze period at both stations, where northern Eurasia was identified as the main source region. Air mass transport from northern Eurasia to Zeppelin Mountain was associated with a 100% increase in the number of detected organosulfate species compared with periods of air mass transport from the Arctic Ocean, Scandinavia and Greenland. The results from this study suggested that the presence of organic acids and organosulfates at Station Nord was mainly due to long-range transport, whereas indications of local sources were found for some compounds at Zeppelin Mountain. Furthermore, organosulfates contributed significantly to organic matter throughout the year at Zeppelin Mountain (annual mean of 13 +/- 8 %) and during Arctic haze at Station Nord (7 +/- 2 %), suggesting organosulfates to be important compounds in Arctic aerosols.

Quantifying black carbon from biomass burning by means of levoglucosan - a one-year time series at the Arctic observatory Zeppelin

2014. K. E. Yttri (et al.). Atmospheric Chemistry And Physics 14 (12), 6427-6442

Article

Levoglucosan, a highly specific tracer of particulate matter from biomass burning, has been used to study the influence of residential wood burning, agricultural waste burning and Boreal forest fire emissions on the Arctic atmosphere black carbon (BC) concentration. A one-year time series from March 2008 to March 2009 of levoglucosan has been established at the Zeppelin observatory in the European Arctic. Elevated concentrations of levoglucosan in winter (mean: 1.02 ng m(-3)) compared to summer (mean: 0.13 ng m(-3)) were observed, resembling the seasonal variation seen for e.g. sulfate and BC. The mean concentration in the winter period was 2-3 orders of magnitude lower than typical values reported for European urban areas in winter, and 1-2 orders of magnitude lower than European rural background concentrations. Episodes of elevated levoglucosan concentration lasting from 1 to 6 days were more frequent in winter than in summer and peak values were higher, exceeding 10 ng m(-3) at the most. Concentrations of elemental carbon from biomass burning (ECbb) were obtained by combining measured concentrations of levoglucosan and emission ratios of levoglucosan and EC for wildfires/agricultural fires and for residential wood burning. Neglecting chemical degradation by OH provides minimum levoglucosan concentrations, corresponding to a mean ECbb concentration of 3.7 +/- 1.2 ng m(-3) in winter (October-April) and 0.8 +/- 0.3 ng m(-3) in summer (May-September), or 8.8 +/- 4.5% of the measured equivalent black carbon (EBC) concentration in winter and 6.1 +/- 3.4% in summer. When accounting for chemical degradation of levoglucosan by OH, an upper estimate of 31-45% of EBC could be attributed to ECbb* (ECbb adjusted for chemical degradation) in winter, whereas no reliable (< 100%) upper estimate could be provided for summer for the degradation rates applied. Hence, fossil fuel sources appear to dominate the European Arctic BC concentrations in winter, whereas the very wide range obtained for summer does not allow us to conclude upon this for the warm season. Calculations using the Lagrangian particle dispersion model FLEXPART show that the seasonal variation of the modeled ECbb (ECbb,m) concentration compared relatively well with observationally derived ECbb from agricultural fires/wildfires during summer, and residential wood burning in winter. The model overestimates by a factor of 2.2 in winter and 4.4 in summer when compared to the observationally derived mean ECbb concentration, which provides the minimum estimate, whereas it underestimates by a factor of 2.3-3.3 in winter and a factor of 4.5 in summer when compared to ECbb*, which provides the upper estimate. There are indications of too-low emissions of residential wood burning in northern Russia, a region of great importance with respect to observed concentrations of BC in the European Arctic.

Seasonal variation of aerosol water uptake and its impact on the direct radiative effect at Ny-Alesund, Svalbard

2014. Narges Rastak (et al.). Atmospheric Chemistry And Physics 14 (14), 7445-7460

Article

In this study we investigated the impact of water uptake by aerosol particles in ambient atmosphere on their optical properties and their direct radiative effect (ADRE, W m(-2)) in the Arctic at Ny-Alesund, Svalbard, during 2008. To achieve this, we combined three models, a hygroscopic growth model, a Mie model and a radiative transfer model, with an extensive set of observational data. We found that the seasonal variation of dry aerosol scattering coefficients showed minimum values during the summer season and the beginning of fall (July-August-September), when small particles (< 100 nm in diameter) dominate the aerosol number size distribution. The maximum scattering by dry particles was observed during the Arctic haze period (March-April-May) when the average size of the particles was larger. Considering the hygroscopic growth of aerosol particles in the ambient atmosphere had a significant impact on the aerosol scattering coefficients: the aerosol scattering coefficients were enhanced by on average a factor of 4.30 +/- 2.26 (mean +/- standard deviation), with lower values during the haze period (March-April-May) as compared to summer and fall. Hygroscopic growth of aerosol particles was found to cause 1.6 to 3.7 times more negative ADRE at the surface, with the smallest effect during the haze period (March-April-May) and the highest during late summer and beginning of fall (July-August-September).

Arctic aerosol life cycle: linking aerosol size distributions observed between 2000 and 2010 with air mass transport and precipitation at Zeppelin station, Ny-Alesund, Svalbard

2013. Peter Tunved, Johan Ström, Radovan Krejci. Atmospheric Chemistry And Physics 13 (7), 3643-3660

Article

In this study we present a qualitative and quantitative assessment of more than 10 yr of aerosol number size distribution data observed in the Arctic environment (Mt. Zeppelin (78 degrees 56' N, 11 degrees 53' E, 474 m a.s.l.), Ny Alesund, Svalbard). We provide statistics on both seasonal and diurnal characteristics of the aerosol observations and conclude that the Arctic aerosol number size distribution and related parameters such as integral mass and surface area exhibit a very pronounced seasonal variation. This seasonal variation seems to be controlled by both dominating source as well as meteorological conditions. Three distinctly different periods can be identified during the Arctic year: the haze period characterized by a dominating accumulation mode aerosol (March-May), followed by the sunlit summer period with low abundance of accumulation mode particles but high concentration of small particles which are likely to be recently and locally formed (June-August). The rest of the year is characterized by a comparably low concentration of accumulation mode particles and negligible abundance of ultrafine particles (September-February). A minimum in aerosol mass and number concentration is usually observed during September/October. We further show that the transition between the different regimes is fast, suggesting rapid change in the conditions defining their appearance. A source climatology based on trajectory analysis is provided, and it is shown that there is a strong seasonality of dominating source areas, with Eurasia dominating during the Autumn-Winter period and dominance of North Atlantic air during the summer months. We also show that new-particle formation events are rather common phenomena in the Arctic during summer, and this is the result of photochemical production of nucleating/condensing species in combination with low condensation sink. It is also suggested that wet removal may play a key role in defining the Arctic aerosol year, via the removal of accumulation mode size particles, which in turn have a pivotal role in facilitating the conditions favorable for new-particle formation events. In summary the aerosol Arctic year seems to be at least qualitatively predictable based on the knowledge of seasonality of transport paths and associated source areas, meteorological conditions and removal processes.

Comparison between summertime and wintertime Arctic Ocean primary marine aerosol properties

2013. Julia Zabori (et al.). Atmospheric Chemistry And Physics 13 (9), 4783-4799

Article

Primary marine aerosols (PMAs) are an important source of cloud condensation nuclei, and one of the key elements of the remote marine radiative budget. Changes occurring in the rapidly warming Arctic, most importantly the decreasing sea ice extent, will alter PMA production and hence the Arctic climate through a set of feedback processes. In light of this, laboratory experiments with Arctic Ocean water during both Arctic winter and summer were conducted and focused on PMA emissions as a function of season and water properties. Total particle number concentrations and particle number size distributions were used to characterize the PMA population. A comprehensive data set from the Arctic summer and winter showed a decrease in PMA concentrations for the covered water temperature (T-w) range between - 1 degrees C and 15 degrees C. A sharp decrease in PMA emissions for a T-w increase from -1 degrees C to 4 degrees C was followed by a lower rate of change in PMA emissions for T-w up to about 6 degrees C. Near constant number concentrations for water temperatures between 6 degrees C to 10 degrees C and higher were recorded. Even though the total particle number concentration changes for overlapping T-w ranges were consistent between the summer and winter measurements, the distribution of particle number concentrations among the different sizes varied between the seasons. Median particle number concentrations for a dry diameter (D-p) < 0.125 mu m measured during winter conditions were similar (deviation of up to 3 %), or lower (up to 70 %) than the ones measured during summer conditions (for the same water temperature range). For D-p > 0.125 mu m, the particle number concentrations during winter were mostly higher than in summer (up to 50 %). The normalized particle number size distribution as a function of water temperature was examined for both winter and summer measurements. An increase in T-w from -1 degrees C to 10 degrees C during winter measurements showed a decrease in the peak of relative particle number concentration at about a D-p of 0.180 mu m, while an increase was observed for particles with D-p > 1 mu m. Summer measurements exhibited a relative shift to smaller particle sizes for an increase of T-w in the range 7-11 degrees C. The differences in the shape of the number size distributions between winter and summer may be caused by different production of organic material in water, different local processes modifying the water masses within the fjord (for example sea ice production in winter and increased glacial meltwater inflow during summer) and different origin of the dominant sea water mass. Further research is needed regarding the contribution of these factors to the PMA production.

Elemental carbon measurements in European Arctic snow packs

2013. S. Forsström (et al.). Journal of Geophysical Research: Atmospheres 118 (24), 13614-13627

Article

Long-term in situ observations of biomass burning aerosol at a high altitude station in Venezuela - sources, impacts and interannual variability

2013. Thomas Hamburger (et al.). Atmospheric Chemistry And Physics 13 (19), 9837-9853

Article

First long-term observations of South American biomass burning aerosol within the tropical lower free troposphere are presented. The observations were conducted between 2007 and 2009 at a high altitude station (4765 m a.s.l.) on the Pico Espejo, Venezuela. Sub-micron particle volume, number concentrations of primary particles and particle absorption were observed. Orographic lifting and shallow convection leads to a distinct diurnal cycle at the station. It enables measurements within the lower free troposphere during night-time and observations of boundary layer air masses during daytime and at their transitional regions. The seasonal cycle is defined by a wet rainy season and a dry biomass burning season. The particle load of biomass burning aerosol is dominated by fires in the Venezuelan savannah. Increases of aerosol concentrations could not be linked to long-range transport of biomass burning plumes from the Amazon basin or Africa due to effective wet scavenging of particles. Highest particle concentrations were observed within boundary layer air masses during the dry season. Ambient sub-micron particle volume reached 1.4 +/- 1.3 mu m(3) cm(-3), refractory particle number concentrations (at 300 degrees C) 510+/-420 cm(-3) and the absorption coefficient 0.91+/-1.2 Mm(-1). The respective concentrations were lowest within the lower free troposphere during the wet season and averaged at 0.19+/-0.25 mu m(3) cm-3, 150+/-94 cm(-3) and 0.15+/-0.26 Mm(-1). A decrease of particle concentrations during the dry seasons from 2007-2009 could be connected to a decrease in fire activity in the wider region of Venezuela using MODIS satellite observations. The variability of biomass burning is most likely linked to the El Nino-Southern Oscillation (ENSO). Low biomass burning activity in the Venezuelan savannah was observed to follow La Nina conditions, high biomass burning activity followed El Nino conditions.

Modeling Aerosol Water Uptake in The Arctic Based on The kappa-Kohler Theory

2013. Narges Rastak (et al.). Nucleation and Atmospheric Aerosols, 702-705

Conference

Water uptake or hygroscopicity is one of the most fundamental properties of atmospheric aerosols. Aerosol particles containing soluble materials can grow in size by absorbing water in ambient atmosphere. This property is measured by a parameter known as growth factor (GF), which is defined as the ratio of the wet diameter to the dry diameter. Hygroscopicity controls the size of an aerosol particle and therefore its optical properties in the atmosphere. Hygroscopic growth depends on the dry size of the particle, its chemical composition and the relative humidity in the ambient air (Fitzgerald, 1975; Pilinis et al., 1995). One of the typical problems in aerosol studies is the lack of measurements of aerosol size distributions and optical properties in ambient conditions. The gap between dry measurements and the real humid atmosphere is filled in this study by utilizing a hygroscopic model which calculates the hygroscopic growth of aerosol particles at Mt Zeppelin station, Ny Alesund, Svalbard during 2008.

Nitrate dry deposition in svalbard

2013. Mats P. Björkman (et al.). Tellus. Series B, Chemical and physical meteorology 65, 19071

Article

Arctic regions are generally nutrient limited, receiving an extensive part of their bio-available nitrogen from the deposition of atmospheric reactive nitrogen. Reactive nitrogen oxides, as nitric acid (HNO3) and nitrate aerosols (p-NO3), can either be washed out from the atmosphere by precipitation or dry deposited, dissolving to nitrate (NO3-). During winter, NO3- is accumulated in the snowpack and released as a pulse during spring melt. Quantification of NO3- deposition is essential to assess impacts on Arctic terrestrial ecology and for ice core interpretations. However, the individual importance of wet and dry deposition is poorly quantified in the high Arctic regions where in-situ measurements are demanding. In this study, three different methods are employed to quantify NO3- dry deposition around the atmospheric and ecosystem monitoring site, Ny-Alesund, Svalbard, for the winter season (September 2009 to May 2010): (1) A snow tray sampling approach indicates a dry deposition of -10.27 +/- 3.84 mg m(-2) (+/- S.E.); (2) A glacial sampling approach yielded somewhat higher values -30.68 +/- 12.00 mg m(-2); and (3) Dry deposition was also modelled for HNO3 and p-NO3 using atmospheric concentrations and stability observations, resulting in a total combined nitrate dry deposition of -10.76 +/- 1.26 mg m(-2). The model indicates that deposition primarily occurs via HNO3 with only a minor contribution by p-NO3. Modelled median deposition velocities largely explain this difference: 0.63 cm s(-1) for HNO3 while p-NO3 was 0.0025 and 0.16 cm s(-1) for particle sizes 0.7 and 7 mm, respectively. Overall, the three methods are within two standard errors agreement, attributing an average 14% (total range of 2-44%) of the total nitrate deposition to dry deposition. Dry deposition events were identified in association with elevated atmospheric concentrations, corroborating recent studies that identified episodes of rapid pollution transport and deposition to the Arctic.

Observed metre scale horizontal variability of elemental carbon in surface snow

2013. J. Svensson (et al.). Environmental Research Letters 8 (3), 034012

Article

Surface snow investigated for its elemental carbon (EC) concentration, based on a thermal-optical method, at two different sites during winter and spring of 2010 demonstrates metre scale horizontal variability in concentration. Based on the two sites sampled, a clean and a polluted site, the clean site (Arctic Finland) presents the greatest variability. In side-by-side ratios between neighbouring samples, 5 m apart, a ratio of around two was observed for the clean site. The median for the polluted site had a ratio of 1.2 between neighbouring samples. The results suggest that regions exposed to snowdrift may be more sensitive to horizontal variability in EC concentration. Furthermore, these results highlight the importance of carefully choosing sampling sites and timing, as each parameter will have some effect on EC variability. They also emphasize the importance of gathering multiple samples from a site to obtain a representative value for the area.

Reactive nitrogen and sulphate wet deposition at Zeppelin Station, Ny-Alesund, Svalbard

2013. Rafael Kuhnel (et al.). Polar Research 32

Article

As a potent fertilizer, reactive nitrogen plays an important role in Arctic ecosystems. Since the Arctic is a nutrient-limited environment, changes in nitrogen deposition can have severe impacts on local ecosystems. To quantify the amount of nitrogen deposited through snow and rain events, precipitation sampling was performed at Zeppelin Station, Svalbard, from November 2009 until May 2011. The samples were analysed for NO3-; nss-SO42- and NH4+ concentrations, and the deposition of single precipitation events was calculated using precipitation measurements taken at nearby Ny-Alesund. The majority of observed events showed concentrations ranging from 0.01 to 0.1 mg L-1 N for NO3- and NH4+ and from 0.02 to 0.3 mg L-1 S for nss-SO42-. The majority of calculated depositions ranged from 0.01 to 0.1 mg m(-2) N for NO3- and NH4+ and from 0.02 to 0.3 mg m(-2) S for nss-SO42-. The budget was controlled by strong deposition events, caused by long-lasting precipitation episodes that lasted for several days and which had raised concentrations of nitrogen and sulphur. Three future scenarios of increasing precipitation in the Arctic were considered. The results showed that deposition is mainly controlled by the amount of precipitation, which leads to the conclusion that increased precipitation might cause increases in deposition of the same magnitude.

Artiﬁcial primary marine aerosol production: a laboratory study with varying water temperature, salinity, and succinic acid concentration

2012. Julia Zábori (et al.). Atmospheric Chemistry And Physics 12 (22), 10709-10724

Article

Primary marine aerosols are an important component of the climate system, especially in the remote marine environment. With diminishing sea-ice cover, better understanding of the role of sea spray aerosol on climate in the polar regions is required. As for Arctic Ocean water, laboratory experiments with NaCl water confirm that a few degrees change in the water temperature (T_w) gives a large change in the number of primary particles. Small particles with a dry diameter between 0.01 μm and 0.25 μm dominate the aerosol number density, but their relative dominance decreases with increasing water temperature from 0 °C where they represent 85–90% of the total aerosol number to 10 °C, where they represent 60–70% of the total aerosol number. This effect is most likely related to a change in physical properties and not to modification of sea water chemistry. A change of salinity between 15 g kg⁻¹ and 35 g kg⁻¹ did not influence the shape of a particle number size distribution. Although the magnitude of the size distribution for a water temperature change between 0 °C and 16 °C changed, the shape did not. An experiment where succinic acid was added to a NaCl water solution showed, that the number concentration of particles with 0.010 μm < D_p < 4.5 μm decreased on average by 10% when the succinic acid concentration in NaCl water at a water temperature of 0 °C was increased from 0 μmol L⁻¹ to 94 μmol L⁻¹. A shift to larger sizes in the particle number size distribution is observed from pure NaCl water to Arctic Ocean water. This is likely a consequence of organics and different inorganic salts present in Arctic Ocean water in addition to the NaCl.

Chemical composition and sources of aerosol particles at Zeppelin Mountain (Ny Alesund, Svalbard): An electron microscopy study

2012. Stephan Weinbruch (et al.). Atmospheric Environment 49, 142-150

Article

Aerosol particles were collected at the Zeppelin Mountain Atmospheric Research Station (474 m asl) near Ny Alesund (Svalbard, Norway) on 27 different days between July 2007 and December 2008. The size, morphology and chemical composition of 57,617 individual particles were studied by high-resolution scanning electron microscopy and energy-dispersive X-ray microanalysis. Based on chemical composition, morphology, mixing state and stability under electron bombardment, the particles were assigned to one of the following groups: sea salt, aged sea salt, Ca sulphates, Na sulphates, carbonates, soot, silicates, fly ashes, secondary aerosol, secondary aerosol plus sodium, secondary aerosol plus soot, mixed particles and others. Sea salt, aged sea salt, silicates and mixed particles (mixtures of sea salt, silicates and Ca sulphates) are the most abundant groups for particles with aerodynamic diameters > 0.5 mu m, secondary aerosol, mixed particles and secondary aerosol with soot inclusions below 0.5 mu m. Silicate fly ashes (major source coal burning) and metal fly ashes (from metallurgical high temperature processes) occur only at very low number concentrations. In contrast to previous work, the fly ash abundance is not correlated with air masses that crossed industrialized regions in Central and Eastern Europe, Scandinavia or Russia. These observations indicate a significant reduction of long-range transport of heavy metals to Svalbard. Soot (external and internally mixed with secondary aerosol) shows a pronounced seasonal pattern with a much lower abundance during summer compared to spring, autumn and winter. The soot abundance is not correlated with the air mass back-trajectories. During summer (July and August), soot was only observed when cruise ships were present in the area around Ny Alesund (Kongsfjorden). Pronounced seasonal patterns were observed for the abundance of the mineral dust component which is generally lower in summer compared to the other seasons. The observed seasonal dependence of anthropogenic primary particles (soot, fly ashes) is in good agreement with the Arctic circulation pattern.

Inclined Lidar Observations of Boundary Layer Aerosol Particles above the Kongsfjord, Svalbard

2012. Astrid Lampert (et al.). Acta geophysica 60 (5), 1287-1307

Article

An inclined lidar with vertical resolution of 0.4 m was used for detailed boundary layer studies and to link observations at Zeppelin Mountain (474 m) and Ny-Alesund, Svalbard. We report on the observation of aerosol layers directly above the Kongsfjord. On 29 April 2007, a layer of enhanced backscatter was observed in the lowest 25 m above the open water surface. The low depolarization ratio indicated spherical particles. In the afternoon, this layer disappeared. The ultrafine particle concentration at Zeppelin and Corbel station (close to the Kongsfjord) was low. On 1 May 2007, a drying process in the boundary layer was observed. In the morning, the atmosphere up to Zeppelin Mountain showed enhanced values of the backscatter coefficient. Around noon, the top of the highly reflecting boundary layer decreased from 350 to 250 m. The top of the boundary layer observed by lidar was confirmed by radiosonde data.

Wintertime Arctic Ocean sea water properties and primary marine aerosol concentrations

2012. Julia Zábori (et al.). Atmospheric Chemistry And Physics 12 (21), 10405-10421

Article

Sea spray aerosols are an important part of the climate system through their direct and indirect effects. Due to the diminishing sea ice, the Arctic Ocean is one of the most rapidly changing sea spray aerosol source areas. However, the influence of these changes on primary particle production is not known.

In laboratory experiments we examined the influence of Arctic Ocean water temperature, salinity, and oxygen saturation on primary particle concentration characteristics. Sea water temperature was identified as the most important of these parameters. A strong decrease in sea spray aerosol production with increasing water temperature was observed for water temperatures between −1°C and 9°C. Aerosol number concentrations decreased from at least 1400 cm⁻³ to 350 cm⁻³. In general, the aerosol number size distribution exhibited a robust shape with one mode close to dry diameter D_p 0.2 μm with approximately 45% of particles at smaller sizes. Changes in sea water temperature did not result in pronounced change of the shape of the aerosol size distribution, only in the magnitude of the concentrations. Our experiments indicate that changes in aerosol emissions are most likely linked to changes of the physical properties of sea water at low temperatures. The observed strong dependence of sea spray aerosol concentrations on sea water temperature, with a large fraction of the emitted particles in the typical cloud condensation nuclei size range, provide strong arguments for a more careful consideration of this effect in climate models

Analysis of number size distributions of tropical free tropospheric = rosol particles observed at Pico Espejo (4765 m a.s.l.), Venezuela

2011. T. Schmeissner (et al.). Atmospheric Chemistry And Physics 11 (7), 3319-3332

Article

The first long-term measurements of aerosol number and size distributions in South-American tropical free troposphere (FT) were performed from March 2007 until March 2009. The measurements took place at the high altitude Atmospheric Research Station Alexander von Humboldt. The station is located on top of the Sierra Nevada mountain ridge at 4765 m a.s.l. nearby the city of Merida, Venezuela. Aerosol size distribution and number concentration data was obtained with a custom-built Differential Mobility Particle Sizer (DMPS) system and a Condensational Particle Counter (CPC). The analysis of the annual and diurnal variability of the tropical FT aerosol focused mainly on possible links to the atmospheric general circulation in the tropics. Considerable annual and diurnal cycles of the particle number concentration were observed. Highest total particle number concentrations were measured during the dry season (January-March, 519+/-613 cm(-3)), lowest during the wet season (July September, 318+/-194 cm(-3)). The more humid FT (relative humidity (RH) range 50-95 %) contained generally higher aerosol particle number concentrations (573+/-768 cm(-3) during dry season, 320+/-195 cm(-3) during wet season) than the dry FT (RH <50 %, 454+/-332 cm(-3) during dry season, 275+/-172 cm(-3) during wet season), indicating the importance of convection for aerosol distributions in the tropical FT. The diurnal cycle in the variability of the particle number concentration was mainly driven by local orography.

Elemental carbon deposition to Svalbard snow from Norwegian settlements and long-range transport

2011. Borgar Aamaas (et al.). Tellus. Series B, Chemical and physical meteorology 63 (3), 340-351

Article

The impact on snow pack albedo from local elemental carbon (EC) sources in Svalbard has been investigated for the winter of 2008. Highly elevated EC concentrations in the snow are observed around the settlements of Longyearbyen and Svea (locally > 1000 ng g(-1), about 200 times over the background level), while EC concentrations similar to the background level are seen around Ny-Alesund. Near Longyearbyen and Svea, darkened snow influenced by wind transported coal dust from open coal stockpiles is clearly visible from satellite images and by eye at the ground. As a first estimate, the reduction in snow albedo caused by local EC pollution from the Norwegian settlements has been compared to the estimated reduction caused by long-range transported EC for entire Svalbard. The effect of local EC from Longyearbyen, Svea and all Norwegian settlements are estimated to 2.1%, 7.9% and 10% of the total impact of EC, respectively. The EC particles tend to stay on the surface during melting, and elevated EC concentrations due to the spring melt was observed. This accumulation of EC enhances the positive albedo feedbacks. The EC concentrations were observed to be larger in metamorphosed snow than in fresh snow, and especially around ice lenses.

Measurements of black carbon aerosol washout ratio on Svalbard

2011. Dean A. Hegg (et al.). Tellus. Series B, Chemical and physical meteorology 63 (5), 891-900

Article

Simultaneous measurements of aerosol black carbon (BC) in both fresh snow and in air on Svalbard are presented. From these, washout ratios for BC are calculated and compared to sparse previous measurements of this metric in the arctic. The current ratios are significantly higher than previously found measured values. We argue that the degree of snow riming within the accretion zone can explain most of this difference. Using an analytical model of the scavenging process, BC scavenging efficiencies are estimated to lie in the range 0.25-0.5, comparable to measured values.

Spatial and temporal variability of snow accumulation rate on the East Antarctic ice divide between Dome Fuji and EPICA DML

2011. S. Fujita (et al.). The Cryosphere 5 (4), 1057-1081

Article

To better understand the spatio-temporal variability of the glaciological environment in Dronning Maud Land (DML), East Antarctica, a 2800-km-long Japanese-Swedish traverse was carried out. The route includes ice divides between two ice-coring sites at Dome Fuji and EPICA DML. We determined the surface mass balance (SMB) averaged over various time scales in the late Holocene based on studies of snow pits and firn cores, in addition to radar data. We find that the large-scale distribution of the SMB depends on the surface elevation and continentality, and that the SMB differs between the windward and leeward sides of ice divides for strong-wind events. We suggest that the SMB is highly influenced by interactions between the large-scale surface topography of ice divides and the wind field of strong-wind events that are often associated with high-precipitation events. Local variations in the SMB are governed by the local surface topography, which is influenced by the bedrock topography. In the eastern part of DML, the accumulation rate in the second half of the 20th century is found to be higher by similar to 15% than averages over longer periods of 722 a or 7.9 ka before AD 2008. A similar increasing trend has been reported for many inland plateau sites in Antarctica with the exception of several sites on the leeward side of the ice divides.

Seven years of recent European net terrestrial carbon dioxide exchange constrained by atmospheric observations

2010. W. Peters (et al.). Global Change Biology 16 (4), 1317-1337

Article

We present an estimate of net ecosystem exchange (NEE) of CO2 in Europe for the years 2001-2007. It is derived with a data assimilation that uses a large set of atmospheric CO2 mole fraction observations (similar to 70 000) to guide relatively simple descriptions of terrestrial and oceanic net exchange, while fossil fuel and fire emissions are prescribed. Weekly terrestrial sources and sinks are optimized (i.e., a flux inversion) for a set of 18 large ecosystems across Europe in which prescribed climate, weather, and surface characteristics introduce finer scale gradients. We find that the terrestrial biosphere in Europe absorbed a net average of -165 Tg C yr-1 over the period considered. This uptake is predominantly in non-EU countries, and is found in the northern coniferous (-94 Tg C yr-1) and mixed forests (-30 Tg C yr-1) as well as the forest/field complexes of eastern Europe (-85 Tg C yr-1). An optimistic uncertainty estimate derived using three biosphere models suggests the uptake to be in a range of -122 to -258 Tg C yr-1, while a more conservative estimate derived from the a-posteriori covariance estimates is -165 +/- 437 Tg C yr-1. Note, however, that uncertainties are hard to estimate given the nature of the system and are likely to be significantly larger than this. Interannual variability in NEE includes a reduction in uptake due to the 2003 drought followed by 3 years of more than average uptake. The largest anomaly of NEE occurred in 2005 concurrent with increased seasonal cycles of observed CO2. We speculate these changes to result from the strong negative phase of the North Atlantic Oscillation in 2005 that lead to favorable summer growth conditions, and altered horizontal and vertical mixing in the atmosphere. All our results are available through http://www.carbontracker.eu.

Spatiotemporal Variability of Light-Absorbing Carbon Concentration in a Residential Area Impacted by Woodsmoke

2010. Patricia Krecl, Christer Johansson, Johan Ström. Journal of the Air & Waste Management Association 60 (3), 356-368

Article

Residential wood combustion (RWC) is responsible for 33% of the total carbon mass emitted in Europe. With the new European targets to increase the use of renewable energy, there is a growing concern that the population exposure to woodsmoke will also increase. This study investigates observed and simulated light-absorbing carbon mass (M-LAC) concentrations in a residential neighborhood (Lycksele, Sweden) where RWC is a major air pollution source during winter. The measurement analysis included descriptive statistics, correlation coefficient, coefficient of divergence, linear regression, concentration roses, diurnal pattern, and weekend versus weekday concentration ratios. Hourly RWC and road traffic contributions to M-LAC were simulated with a Gaussian dispersion model to assess whether the model was able to mimic the observations. Hourly mean and standard deviation concentrations measured at six sites ranged from 0.58 to 0.74 mu g m(-3) and from 0.59 to 0.79 mu g m(-3), respectively. The temporal and spatial variability decreased with increasing averaging time. Low-wind periods with relatively high M-LAC concentrations correlated more strongly than high-wind periods with low concentrations. On average, the model overestimated the observations by 3- to 5-fold and explained less than 10% of the measured hourly variability at all sites. Large residual concentrations were associated with weak winds and relatively high M-LAC loadings. The explanation of the observed variability increased to 31-45% when daily mean concentrations were compared. When the contribution from the boilers within the neighborhood was excluded from the simulations, the model overestimation decreased to 16-71%. When assessing the exposure to light-absorbing carbon particles using this type of model, the authors suggest using a longer averaging period (i.e., daily concentrations) in a larger area with an updated and very detailed emission inventory.

Elemental carbon distribution in Svalbard snow

2009. S. Forsstrom (et al.). Journal of Geophysical Research 114

Article

The concentration of apparent elemental carbon (ECa, based on a thermal-optical method) in the snow was investigated in Svalbard (European Arctic) during spring 2007. The median ECa concentration of 81 samples was 4.1 mu g l(-1) and the values ranged from 0 to 80.8 mu g l(-1) of melt water. The median concentration is nearly an order of magnitude lower than the previously published data of equivalent black carbon (BCe, based on an optical method), obtained from Svalbard snow in the 1980s. A systematic regional difference was evident: ECa concentrations were higher in east Svalbard compared to west Svalbard. The observations of snow ECa cover spatial scales up to several hundred kilometers, which is comparable to the resolution of many climate models. Measurements of atmospheric carbonaceous aerosol (2002-2008) at Zeppelin station in Ny-Alesund, Svalbard, were divided to air mass sectors based on calculated back trajectories. The results show that air originating from the eastern sector contains more than two and half times higher levels of soot than air arriving from south to west. The observed east-west gradient of ECa concentrations in snow may be because of a combination of the atmospheric concentration gradient, the orographic effect of the archipelago, and the efficient scavenging of the carbonaceous particles through precipitation

On small particles in the Arctic summer boundary layer: observations at two different heights near Ny-Ålesund, Svalbard

2009. Johan Ström (et al.). Tellus. Series B, Chemical and physical meteorology 61 (2), 473-482

Article

Concurrent observations of particle number densities and size distributions observed at two different heights (near ocean level and 475 m above sea level) in Ny-Ålesund, Svalbard were studied with respect to the diurnal variation during a summer period in June 2004. The results show that observed variation in particle number density in the Arctic boundary layer may be strongly modulated by vertical mixing and dilution. The particles appeared to be formed in the early morning when solar intensity reached about 30% of the mid-day intensity. Based on differences in the observed number densities at the two heights it appears as if particles are formed in the lower part of the boundary layer. The formation rate of 10 nm diameter particles is estimated to be 0.11 cm⁻³ s⁻¹ and the growth rate is in a range between 1 and 2 nm h⁻¹.

A global model study of processes controlling aerosol size distributions in the Arctic spring and summer.

2008. H. Korhonen (et al.). J. Geophys. Res. (D Atmos.)

Article

Chemical properties of Arctic aerosol particles collected at the Zeppelin station during the aerosol transition period in May and June of 2004

2008. Ulrika Behrenfeldt (et al.). Tellus. Series B: Chemical and Physical Meteorology 60 (3), 405-415

Article

Contribution of residential wood combustion to hourly winter aerosol in Northern Sweden determined by positive matrix factorization

2008. Patricia Krecl (et al.). Atmospheric Chemistry And Physics 8 (13), 3639-3653

Article

The combined effect of residential wood combustion (RWC) emissions with stable atmospheric conditions. which frequently occurs in Northern Sweden during wintertime, can deteriorate the air quality even in small towns. To estimate the contribution of RWC to the total atmospheric aerosol loading, positive matrix factorization (PMF) was applied to hourly mean particle number size distributions measured in a residential area in Lycksele during winter 2005/2006. The sources were identified based on the particle number size distribution profiles of the PMF factors., the diurnal contributions patterns estimated by PMF for both weekends and weekdays, and correlation of the modeled particle number concentration per factor with measured aerosol mass concentrations (PM10, PM1, and light-absorbing carbon M-LAC). Through these analyses. the factors were identified as local traffic (factor 1), local RWC (factor 2), and local RWC plus Ion-range transport (LRT) of aerosols (factor 3). In some occasions, the PMF model could not separate the contributions of local RWC from background concentrations since their particle number size distributions partially overlapped. As a consequence, we report the contribution of RWC as a range of values, being the minimum determined by factor 2 and the possible maximum as the contributions of both factors 2 and 3. A multiple linear regression (MLR) of observed PM10, PM1, total particle number, and M-LAC concentrations is carried out to determine the source contribution to these aerosol variables. The results reveal RWC is an important source of atmospheric particles in the size range 25-606 nm (44-57%), PM10 (36-82%), PM1 (31-83%), and M-LAC (40-76%) mass concentrations in the winter season.

Diurnal variation of atmospheric aerosol during the wood combustion season in Northern Sweden

2008. Patricia Krecl, Johan Ström, Christer Johansson. Atmospheric Environment 42 (18), 4113-4125

Article

A set of aerosol measurements was conducted in the residential area of Forsdala in Lycksele, Northern Sweden, during winter 2005/2006. This article describes the temporal and diurnal variation of the aerosol physical properties (concentrations of PM₁₀, PM₁, light-absorbing carbon, and particle number, and number size distributions), and the relationship among aerosol concentrations and meteorological variables. A large day-to-day and hour-to-hour variability in aerosol concentrations was observed during the intensive study period. Evening aerosol concentrations were statistically significantly higher on weekends than on weekdays. On weekdays, particle size distribution and concentrations varied diurnally with small particles (diameter <30 nm) associated mainly with morning motor vehicle emissions. The results suggest that a combination of emissions from residential wood combustion and traffic sources might explain the high evening concentrations of PM₁₀, PM₁, particle number, and light-absorbing carbon as well as large geometric mean diameters observed during weekdays and weekends. Strong correlations of PM₁₀ and PM₁ with particle size distributions are found in the diameter range 130–500 nm and are remarkably high on weekend evenings when larger particles are sampled. The correlation between light-absorbing carbon mass concentration and particle size distribution is high regarding both particle number and mass for particle diameters >95 nm. High aerosol concentrations were associated with low air temperatures and very stable atmospheric conditions close to the ground.

Do organics contribute to new particle formation in the Amazonian upper troposphere?

2008. Annica Ekman (et al.). Geophysical Research Letters 35, L17810

Article

3-D cloud-resolving model simulations including explicit aerosol physics and chemistry are compared with observations of upper tropospheric (12 km) aerosol size distributions over the Amazon Basin. The model underestimates the aerosol number concentration for all modes, especially the nucleation mode (d< 18nm). We show that a boundary layer SO2 mixing ratio of approximately 5 ppb would be needed in order to reproduce the high nucleation mode number concentrations observed. This high SO2 mixing ratio is very unlikely for the pristine Amazon Basin at this time of the year. Hence, it is suggested that vapours other than H2SO4 participate in the formation and growth of small aerosols. Using activation nucleation theory together with a small (0.4-10%) secondary organic aerosol mass yield, we show that isoprene has the potential of substantially increasing the number of small particles formed as well as reducing the underestimate for the larger aerosol modes.

Do organics contribute to small particle formation in the Amazonian upper troposphere?

2008. Annica Ekman (et al.). Geophysical Research Letters 35 (L17810), 5

Article

3-D cloud-resolving model simulations including explicit aerosol physics and chemistry are compared with observations of upper tropospheric (12 km) aerosol size distributions over the Amazon Basin. The model underestimates the aerosol number concentration for all modes, especially the nucleation mode (d < 18 nm). We show that a boundary layer SO₂ mixing ratio of approximately 5 ppb would be needed in order to reproduce the high nucleation mode number concentrations observed. This high SO₂ mixing ratio is very unlikely for the pristine Amazon Basin at this time of the year. Hence, it is suggested that vapours other than H₂SO₄ participate in the formation and growth of small aerosols. Using activation nucleation theory together with a small (0.4–10%) secondary organic aerosol mass yield, we show that isoprene has the potential of substantially increasing the number of small particles formed as well as reducing the underestimate for the larger aerosol modes.

Estimates of black carbon and size resolved particle number emission factors from residential wood burning based on ambient monitoring and model simulations.

2008. G Olivares (et al.). J. Air & Waste Manage. Assoc. 58, 838-848

Article

Feasibility of analyzing fine particulate matter in air using solid-phase extraction membranes and dynamic subcritical water extraction

2008. Johanna Tollbäck (et al.). Analytical chemistry 80 (9), 3159-67

Article

We have evaluated the feasibility of using Empore solid-phase extraction (SPE) membranes as an alternative to conventional techniques for sampling fine airborne particulate matter (PM), including nanoparticles, utilizing a scanning mobility particle sizer (SMPS) and a condensation particle counter to evaluate their efficiency for trapping fine particles in the 10-800 nm size range. The results demonstrate that the membranes can efficiently trap these particles and can then be conveniently packed into an extraction cell and extracted under matrix solid-phase dispersion (MSPD) conditions. The potential utility of sampling PM using Empore membranes followed by dynamic subcritical water extraction (DSWE) for fast, efficient, class-selective extraction of polycyclic aromatic hydrocarbons (PAHs) associated with the particles, prior to changing the solvent and analysis by GC/MS, was then explored. The performance of the method was tested using National Institute of Standards and Technology (NIST)-certified "urban dust" reference material (SRM 1649a) and real samples collected at a site in central Rome with heavy road traffic. The method appears to provide comparable extraction efficiency to that of conventional techniques and with using GC/MS, detection limits ranged in the few picograms per cubic meter level. Sampling PM by Empore membranes may reduce the risks of losses of semivolatile compounds, while allowing relatively high sampling flow rates and safe sample storage. Moreover, the combination of MSPD with DSWE permits specific fractions of the PM components to be eluted, thereby generating clean extracts and reducing both analysis time and sample manipulation.

Observational and modelling evidence of tropical deep convective clouds as a source of mid-tropospheric accumulation mode aerosols

2008. Anders Engström (et al.). Geophysical Research Letters 35, L23813

Article

High concentrations (up to 550 cm−3 STP) of aerosols in the accumulation mode (>0.12 μm) were observed by aircraft above 7.5 km altitude in the dynamically active regions of several deep convective clouds during the INDOEX campaign. Using a coupled 3-D aerosol-cloud-resolving model, we find that significant evaporation of hydrometeors due to strong updrafts and exchange with ambient air occurs at the boundaries and within the cloud tower. Assuming that each evaporated hydrometeor release an aerosol, an increase in the aerosol concentration by up to 600 cm−3 STP is found in the model at altitudes between 6 and 10 km. The evaporation and release of aerosols occur as the cloud develops, suggesting that deep convective clouds are important sources of mid-tropospheric aerosols during their active lifetime. This source may significantly impact the vertical distribution as well as long-range transport of aerosols in the free troposphere.

On small particles in the Arctic summer boundary layer: observations at two different heights near Ny-Ålesund, Svalbard

2008. J Ström (et al.). Tellus B

Article

Aerosols in Polar Regions: An Historical Overview on the Basis of Optical Depth and In-Situ Observations

2007. C. Tomasi (et al.). J. Geophys. Res. (D Atmos.)

Article

Anthropogenic aerosol effects on convective cloud microphysical properties in southern Sweden

2007. E. Freud (et al.). Tellus B

Article

Arctic smoke – aerosol characteristics during a record air pollution event in the European Arctic and its radiative impact

2007. Renatte Treffeisen (et al.). Atmospheric Chemistry and Physics 7, 3035-3053

Article

Arctic smoke-record high air pollution levels in the European Arctic due to agrecultural fires in Eastern Europe in spring 2006

2007. A. Stohl (et al.). Atmos. Chem. Phys. 7, 511-534

Article

Carbon content of atmospheric aerosols in a residential area during the wood combustion season in Sweden.

2007. Patricia Krecl, Johan Ström, Christer Johansson. Atmos. Environ. 41, 6974-6985

Article

Humidity observations in the Arctic troposphere over Ny-Ålesund, Svalbard based on 14 years of radiosonde data.

2007. R. Treffeisen (et al.). Atmos. Chem. Phys. Discuss. 7, 1261-1293

Article

Relationerna mellan halterna av PM10, PM1 och sot i Sverige.

2007. Christer Johansson (et al.).

Report

The role of ambient temperature for particle number concentrations in a street canyon.

2007. Gustavo Olivares (et al.). Atmos. Environ. 41, 2145-2155

Article

Aerosol characteristics of air masses in Northern Europe – influences of location, transport, sinks and sources

2005. Peter Tunved (et al.). Journal of Geophysical Research 110 (D7), D07201

Article

Synoptic-scale air masses at different stations were classified following a definition based on Berliner Wetterkarte. This air mass classification has been related to 1 year of aerosol number size distributions measurements performed at four different stations extending from Aspvreten in Sweden (58.8 degrees N) to Pallas in northern Finland (68 degrees N). The air mass classification describes both class of air mass, based on the origin of the air mass, and character of air in terms of marine, mixed, and continental air masses. The aerosol size distribution properties were evaluated in relation to the air masses. Emphasis was put on the differences between marine, mixed, and continental character air masses. It is shown that continental air masses exceed marine and mixed character air masses both in number and mass concentration. Different classes of air masses were further associated with different aerosol size distribution properties. It is also shown that although serving as a somewhat good qualifier for the aerosol at individual stations, the air mass classification cannot be used to estimate the aerosol burden over large geographical areas. Instead, a sharp gradient was shown to exist between different stations, although aerosol properties were observed in equal air masses according to the definition by Berliner Wetterkarte. This gradient manifests as a south-northerly decrease in aerosol total number and volume, indicating that the aerosol properties including the aerosol size distribution are less conservative than the thermodynamic properties (e.g., pseudo-potential temperature and humidity profiles) that characterize the different air masses. Further, using a pseudo-Lagrangian approach, the aerosol turnover time was estimated for different sized aerosols in air moving from south to north (i.e., depletion of aerosols in air arriving from the continent). Turnover time of Aitken particles was found to be in the range of 1-2 days, while accumulation mode turnover time was estimated to be in the order of 2-3 days

A pseudo-Lagrangian model study of the size distribution properties over Scandinavia: Transport from Aspvreten to Värriö

2004. Peter Tunved (et al.). Atmospheric Chemistry and Physics Discussions (4), 7757-7794

Article

The evolution of the aerosol size distribution during transport between Aspvreten (58.8° N, 17.4° E) and Värriö (67.46° N, 29.35° E) was studied using a pseudo-Lagrangian approach. Aerosol dynamic processes were studied and interpreted utilizing a state-of-the-art aerosol dynamic box model UHMA (University of Helsinki Multicomponent Aerosol model) complemented with OH, NO₃, O₃ and terpene chemistry. In the model simulations, the growth and formation of aerosol particles was controlled by sulphuric acid, ammonia, water and an unidentified low volatile organic compound. This organic compound was assumed to be a product of terpene oxidation with a yield of 13% in the base case conditions. Changes of aerosol size distribution properties during transport between the stations were examined in twelve clear sky cases. On average, the modelled number agreed fairly well with observations. Mass concentration was overestimated by 10%. Apart from dilution, the only removal mechanism for aerosol mass is dry deposition. A series of sensitivity tests performed revealed that the absolute magnitude of dry deposition effects on the aerosol size distribution is slow overall. Furthermore, nucleation does not leave a significant contribution to aerosol number in the selected cases. The sensitivity of the modelled size distribution to concentration of precursor gases and oxidants is, however, obvious. In order to explain observed mass increase during transport we conclude that a yield of low volatile products from oxidation of terpenes of 10–15% is required to explain observed growth rates. Coagulation is acknowledged to be highly important in modelled cases.

An investigation of processes controlling the evolution of the boundary layer aerosol size distribution properties at the Swedish background station Aspvreten

2004. Peter Tunved, Johan Ström, Hans-Christen Hansson. Atmospheric Chemistry and Physics Discussions 4 (4), 4507-4543

Article

Aerosol size distributions have been measured at the Swedish background station Aspvreten (58.8° N, 17.4° E). Different states of the aerosol were determined using a novel application of cluster analysis. The analysis resulted in eight different clusters capturing the different stages of the aerosol lifecycle. The aerosol was interpreted as belonging to fresh, intermediate and aged type of size distribution and different magnitudes thereof. With aid of back trajectory analysis we present statistics concerning the relation of source area and different meteorological parameters using a non-lagrangian approach. Source area is argued to be important although not sufficient to describe the observed aerosol properties. Especially processing by clouds and precipitation is shown to be crucial for the evolution of the aerosol size distribution. As much as 60% of the observed size distributions present features likely related to cloud processes or wet deposition. The lifetime properties of different sized aerosols are discussed by means of measured variability. Processing by non-precipitating clouds most obviously affect aerosols in the size range 100 nm and larger. This indicates an approximate limit for activation in clouds to 100 nm in this type of environment. The aerosol lifecycle is discussed. Size distributions bearing signs of recent new particle formation (~30% of the observed size distributions) represent the first stage in the lifecycle. Aging may proceed in two directions: either growth by condensation and coagulation or processing by non-precipitating clouds. In both cases mass is accumulated. Wet removal is the main process capable of removing aerosol mass. Wet deposition is argued to be an important mechanism in reaching a state where nucleation may occur (i.e. sufficiently low aerosol surface area) in environments similar to the one studied

Johan Ström

Publications

Arctic Ocean water: A source of light absorbing particles to the atmosphere

Comparison between summertime and wintertime Arctic Ocean primary marine aerosol properties

Collective geographical ecoregions and precursor sources driving Arctic new particle formation

Organic Compounds, Radiocarbon, Trace Elements and Atmospheric Transport Illuminating Sources of Elemental Carbon in a 300-Year Svalbard Ice Core

Airmass Analysis of Size-Resolved Black Carbon Particles Observed in the Arctic Based on Cluster Analysis

Atmospheric composition in the European Arctic and 30 years of the Zeppelin Observatory, Ny-Ålesund

Snow albedo and its sensitivity to changes in deposited light-absorbing particles estimated from ambient temperature and snow depth observations at a high-altitude site in the Himalaya

Unmasking the Effects of Aerosols on Greenhouse Warming Over Europe

Deposition of light-absorbing particles in glacier snow of the Sunderdhunga Valley, the southern forefront of the central Himalayas

Dimethyl Sulfide-Induced Increase in Cloud Condensation Nuclei in the Arctic Atmosphere

Elemental and water-insoluble organic carbon in Svalbard snow: a synthesis of observations during 2007-2018

Relationship between cloud condensation nuclei (CCN) concentration and aerosol optical depth in the Arctic region

Using correlations between observed equivalent black carbon and aerosol size distribution to derive size resolved BC mass concentration: a method applied on long-term observations performed at Zeppelin station, Ny-Ålesund, Svalbard

From a polar to a marine environment: has the changing Arctic led to a shift in aerosol light scattering properties?

Physical and chemical properties of aerosol particles and cloud residuals on Mt. angstrom reskutan in Central Sweden during summer 2014

Composition, isotopic fingerprint and source attribution of nitrate deposition from rain and fog at a Sub-Arctic Mountain site in Central Sweden (Mt Åreskutan)

Interactions between the atmosphere, cryosphere, and ecosystems at northern high latitudes

Multiple-scattering correction factor of quartz filters and the effect of filtering particles mixed in water: implications for analyses of light absorption in snow samples

On the seasonal variation in observed size distributions in northern Europe and their changes with decreasing anthropogenic emissions in Europe: climatology and trend analysis based on 17 years of data from Aspvreten, Sweden

Simultaneous measurements of aerosol size distributions at three sites in the European high Arctic

Year-Round In Situ Measurements of Arctic Low-Level Clouds: Microphysical Properties and Their Relationships With Aerosols

Cloud droplet activation of black carbon particles coated with organic compounds of varying solubility

Light-absorption of dust and elemental carbon in snow in the Indian Himalayas and the Finnish Arctic

The seasonal characteristics of cloud condensation nuclei (CCN) in the arctic lower troposphere

A new aerosol wet removal scheme for the Lagrangian particle model FLEXPART

Arctic sea ice melt leads to atmospheric new particle formation

Chemical composition and source analysis of carbonaceous aerosol particles at a mountaintop site in central Sweden

Do contemporary (1980-2015) emissions determine the elemental carbon deposition trend at Holtedahlfonna glacier, Svalbard?

Trends in black carbon and size-resolved particle number concentrations and vehicle emission factors under real-world conditions

Multi-seasonal ultrafine aerosol particle number concentration measurements at the Gruvebadet observatory, Ny-lesund, Svalbard Islands

Characterisation and Source Apportionment of Submicron Particle Number Size Distributions in a Busy Street Canyon

In situ observations of black carbon in snow and the corresponding spectral surface albedo reduction

Size-resolved cloud condensation nuclei concentration measurements in the Arctic: two case studies from the summer of 2008

The relationship between cloud condensation nuclei (CCN) concentration and light extinction of dried particles: indications of underlying aerosol processes and implications for satellite-based CCN estimates

A feasibility study of mapping light-absorbing carbon using a taxi fleet as a mobile platform

A review of sea-spray aerosol source functions using a large global set of sea salt aerosol concentration measurements

Elemental carbon in snow at Changbai Mountain, northeastern China: concentrations, scavenging ratios, and dry deposition velocities

Hygroscopic growth and cloud forming potential of Arctic aerosol based on observed chemical and physical characteristics (a 1 year study 2007-2008)

Increase in elemental carbon values between 1970 and 2004 observed in a 300-year ice core from Holtedahlfonna (Svalbard)

Mixing State of Size-Selected Submicrometer Particles in the Arctic in May and September 2012

Organosulfates and organic acids in Arctic aerosols: speciation, annual variation and concentration levels

Quantifying black carbon from biomass burning by means of levoglucosan - a one-year time series at the Arctic observatory Zeppelin

Seasonal variation of aerosol water uptake and its impact on the direct radiative effect at Ny-Alesund, Svalbard

Arctic aerosol life cycle: linking aerosol size distributions observed between 2000 and 2010 with air mass transport and precipitation at Zeppelin station, Ny-Alesund, Svalbard

Comparison between summertime and wintertime Arctic Ocean primary marine aerosol properties

Elemental carbon measurements in European Arctic snow packs

Long-term in situ observations of biomass burning aerosol at a high altitude station in Venezuela - sources, impacts and interannual variability

Modeling Aerosol Water Uptake in The Arctic Based on The kappa-Kohler Theory

Nitrate dry deposition in svalbard

Observed metre scale horizontal variability of elemental carbon in surface snow

Reactive nitrogen and sulphate wet deposition at Zeppelin Station, Ny-Alesund, Svalbard

Artiﬁcial primary marine aerosol production: a laboratory study with varying water temperature, salinity, and succinic acid concentration

Chemical composition and sources of aerosol particles at Zeppelin Mountain (Ny Alesund, Svalbard): An electron microscopy study

Inclined Lidar Observations of Boundary Layer Aerosol Particles above the Kongsfjord, Svalbard

Wintertime Arctic Ocean sea water properties and primary marine aerosol concentrations

Analysis of number size distributions of tropical free tropospheric = rosol particles observed at Pico Espejo (4765 m a.s.l.), Venezuela

Elemental carbon deposition to Svalbard snow from Norwegian settlements and long-range transport

Measurements of black carbon aerosol washout ratio on Svalbard

Spatial and temporal variability of snow accumulation rate on the East Antarctic ice divide between Dome Fuji and EPICA DML

Seven years of recent European net terrestrial carbon dioxide exchange constrained by atmospheric observations

Spatiotemporal Variability of Light-Absorbing Carbon Concentration in a Residential Area Impacted by Woodsmoke

Elemental carbon distribution in Svalbard snow

On small particles in the Arctic summer boundary layer: observations at two different heights near Ny-Ålesund, Svalbard

A global model study of processes controlling aerosol size distributions in the Arctic spring and summer.

Chemical properties of Arctic aerosol particles collected at the Zeppelin station during the aerosol transition period in May and June of 2004

Contribution of residential wood combustion to hourly winter aerosol in Northern Sweden determined by positive matrix factorization

Diurnal variation of atmospheric aerosol during the wood combustion season in Northern Sweden

Do organics contribute to new particle formation in the Amazonian upper troposphere?

Do organics contribute to small particle formation in the Amazonian upper troposphere?

Estimates of black carbon and size resolved particle number emission factors from residential wood burning based on ambient monitoring and model simulations.

Feasibility of analyzing fine particulate matter in air using solid-phase extraction membranes and dynamic subcritical water extraction

Observational and modelling evidence of tropical deep convective clouds as a source of mid-tropospheric accumulation mode aerosols

On small particles in the Arctic summer boundary layer: observations at two different heights near Ny-Ålesund, Svalbard

Aerosols in Polar Regions: An Historical Overview on the Basis of Optical Depth and In-Situ Observations

Anthropogenic aerosol effects on convective cloud microphysical properties in southern Sweden

Arctic smoke – aerosol characteristics during a record air pollution event in the European Arctic and its radiative impact

Arctic smoke-record high air pollution levels in the European Arctic due to agrecultural fires in Eastern Europe in spring 2006

Carbon content of atmospheric aerosols in a residential area during the wood combustion season in Sweden.