Search

We investigated long-term changes using a harmonised 22-year data set of aerosol light absorption measurements, in conjunction with air mass history and aerosol source analysis. The measurements were performed at Zeppelin Observatory, Svalbard, from 2002 to 2023. We report a statistically significant decreasing long-term trend for the light absorption coefficient. However, the last 8 years of 2016–2023 showed a slight increase in the magnitude of the light absorption coefficient for the Arctic haze season. In addition, we observed an increasing trend in the single-scattering albedo from 2002 to 2023. Five distinct source regions, representing different transport pathways, were identified. The trends involving air masses from the five regions showed decreasing absorption coefficients, except for the air masses from Eurasia. We show that the changes in the occurrences of each transport pathway cannot explain the reductions in the absorption coefficient observed at the Zeppelin station. An increase in contributions of air masses from more marine regions, with lower absorption coefficients, is compensated for by an influence from high-emission regions. The proportion of air masses en route to Zeppelin, which have been influenced by active fires, has undergone a noticeable increase starting in 2015. However, this increase has not impacted the long-term trends in the concentration of light-absorbing aerosol. Along with aerosol optical properties, we also show an increasing trend in accumulated surface precipitation experienced by air masses en route to the Zeppelin Observatory. We argue that the increase in precipitation, as experienced by air masses arriving at the station, can explain a quarter of the long-term reduction in the light absorption coefficient. We emphasise that meteorological conditions en route to the Zeppelin Observatory are critical for understanding the observed trends. [ABSTRACT FROM AUTHOR]

Black carbon (BC), the most efficient atmospheric aerosol for absorbing light in the visible spectrum, exerts a warming effect on a region undergoing unprecedented climatic changes. Here, BC is studied indirectly using filter-based methods to ascertain aerosol light absorption parameters. We investigated long-term changes using a harmonised 21-year data set of light absorption measurements, in conjunction with air mass source analysis. The measurements were performed at Zeppelin Observatory (ZEP), Svalbard, from 2002 to 2022. We report a statistically significant (s.s.) decreasing long-term trend for the light absorption coefficient, measured at the site for the entirety of the data set. However, the last 7 years, 2016–2022, showed a slightly increasing s.s. trend for the haze season. In addition, we observed an increasing trend in the single scattering albedo from 2002 to 2022. Five distinct source regions were identified; the trends involving air masses from the five regions showed decreasing absorption coefficients, except for the air masses influenced by emissions from Eurasia. We show that the changes in the occurrences of each transport pathway cannot explain the reductions in the absorption coefficient observed at the Zeppelin station; an increase in contributions of air masses from more marine regions, with lower absorption coefficients, is compensated by the influence from high-emission regions. Along with aerosol optical properties, we also show an increasing trend in accumulated surface precipitation experienced by air masses en route to the Zeppelin Observatory. We argue that rainfall, as a sink of aerosol, plays a role in the long-term trends in the absorption coefficient, explaining approximately a quarter of the overall trend. A decreasing trend in the scavenging ratio further suggests an increase in the aerosol removal processes. We note that there is an increasing potential influence from active forest fires, particularly in the last few summers (i.e. 2015–2022). Active fires have been shown to have a significant impact on the mean seasonal absorption coefficient especially during northern hemispheric summer. However, no noticeable alteration in annual long-term trends can be observed. [ABSTRACT FROM AUTHOR]

As explained in the latest Arctic Monitoring and Assessment Programme (AMAP) report released in early 2021, the Arctic has warmed 3 times more quickly than the planet as a whole, as well as faster than previously thought. The Siberian Arctic is of great interest mainly because observations are sparse or largely lacking. A research aerosol station has been developed on Bely Island (Kara Sea) in western Siberia. Measurements of equivalent black carbon (EBC) concentrations were carried out at the "Island Bely" station continuously from August 2019 to November 2020. The source origin of the measured EBC and the main contributing sources were assessed using atmospheric transport modeling coupled with the most updated emission inventories for anthropogenic and biomass burning sources of BC. The obtained climatology for BC during the period of measurements showed an apparent seasonal variation with the highest concentrations between December and April (60 ± 92 ng m -3) and the lowest between June and September (18 ± 72 ng m -3), typical of the Arctic haze seasonality reported elsewhere. When air masses arrived at the station through the biggest oil and gas extraction regions of Kazakhstan, Volga-Ural, Komi, Nenets and western Siberia, BC contribution from gas flaring dominated over domestic, industrial and traffic sectors, ranging from 47 % to 68 %, with a maximum contribution in January. When air was transported from Europe during the cold season, emissions from transportation were more important. Accordingly, shipping emissions increased due to the touristic cruise activities and the ice retreat in summertime. Biomass burning (BB) played the biggest role between April and October, contributing 81 % at maximum in July. Long-range transport of BB aerosols appeared to induce large variability to the absorption Ångström exponent (AAE) with values > 1.0 (excluding outliers). As regards the continental contribution to surface BC at the Island Bely station, Russian emissions dominated during the whole year, while European and Asian ones contributed up to 20 % in the cold period. Quantification of several pollution episodes showed an increasing trend in surface concentrations and frequency during the cold period as the station is directly in the Siberian gateway of the highest anthropogenic pollution sources to the Russian Arctic. [ABSTRACT FROM AUTHOR]

While carbon dioxide is the main cause for global warming, modeling short-lived climate forcers (SLCFs) such as methane, ozone, and particles in the Arctic allows us to simulate near-term climate and health impacts for a sensitive, pristine region that is warming at 3 times the global rate. Atmospheric modeling is critical for understanding the long-range transport of pollutants to the Arctic, as well as the abundance and distribution of SLCFs throughout the Arctic atmosphere. Modeling is also used as a tool to determine SLCF impacts on climate and health in the present and in future emissions scenarios. In this study, we evaluate 18 state-of-the-art atmospheric and Earth system models by assessing their representation of Arctic and Northern Hemisphere atmospheric SLCF distributions, considering a wide range of different chemical species (methane, tropospheric ozone and its precursors, black carbon, sulfate, organic aerosol, and particulate matter) and multiple observational datasets. Model simulations over 4 years (2008–2009 and 2014–2015) conducted for the 2022 Arctic Monitoring and Assessment Programme (AMAP) SLCF assessment report are thoroughly evaluated against satellite, ground, ship, and aircraft-based observations. The annual means, seasonal cycles, and 3-D distributions of SLCFs were evaluated using several metrics, such as absolute and percent model biases and correlation coefficients. The results show a large range in model performance, with no one particular model or model type performing well for all regions and all SLCF species. The multi-model mean (mmm) was able to represent the general features of SLCFs in the Arctic and had the best overall performance. For the SLCFs with the greatest radiative impact (CH 4 , O 3 , BC, and SO 42-), the mmm was within ± 25 % of the measurements across the Northern Hemisphere. Therefore, we recommend a multi-model ensemble be used for simulating climate and health impacts of SLCFs. Of the SLCFs in our study, model biases were smallest for CH 4 and greatest for OA. For most SLCFs, model biases skewed from positive to negative with increasing latitude. Our analysis suggests that vertical mixing, long-range transport, deposition, and wildfires remain highly uncertain processes. These processes need better representation within atmospheric models to improve their simulation of SLCFs in the Arctic environment. As model development proceeds in these areas, we highly recommend that the vertical and 3-D distribution of SLCFs be evaluated, as that information is critical to improving the uncertain processes in models. [ABSTRACT FROM AUTHOR]

Even though the Arctic is remote, aerosol properties observed there are strongly influenced by anthropogenic emissions from outside the Arctic. This is particularly true for the so-called Arctic haze season (January through April). In summer (June through September), when atmospheric transport patterns change, and precipitation is more frequent, local Arctic sources, i.e., natural sources of aerosols and precursors, play an important role. Over the last few decades, significant reductions in anthropogenic emissions have taken place. At the same time a large body of literature shows evidence that the Arctic is undergoing fundamental environmental changes due to climate forcing, leading to enhanced emissions by natural processes that may impact aerosol properties. In this study, we analyze 9 aerosol chemical species and 4 particle optical properties from 10 Arctic observatories (Alert, Kevo, Pallas, Summit, Thule, Tiksi, Barrow/Utqiaġvik, Villum, and Gruvebadet and Zeppelin Observatory – both at Ny-Ålesund Research Station) to understand changes in anthropogenic and natural aerosol contributions. Variables include equivalent black carbon, particulate sulfate, nitrate, ammonium, methanesulfonic acid, sodium, iron, calcium and potassium, as well as scattering and absorption coefficients, single scattering albedo and scattering Ångström exponent. First, annual cycles are investigated, which despite anthropogenic emission reductions still show the Arctic haze phenomenon. Second, long-term trends are studied using the Mann–Kendall Theil–Sen slope method. We find in total 41 significant trends over full station records, i.e., spanning more than a decade, compared to 26 significant decadal trends. The majority of significantly declining trends is from anthropogenic tracers and occurred during the haze period, driven by emission changes between 1990 and 2000. For the summer period, no uniform picture of trends has emerged. Twenty-six percent of trends, i.e., 19 out of 73, are significant, and of those 5 are positive and 14 are negative. Negative trends include not only anthropogenic tracers such as equivalent black carbon at Kevo, but also natural indicators such as methanesulfonic acid and non-sea-salt calcium at Alert. Positive trends are observed for sulfate at Gruvebadet. No clear evidence of a significant change in the natural aerosol contribution can be observed yet. However, testing the sensitivity of the Mann–Kendall Theil–Sen method, we find that monotonic changes of around 5 % yr -1 in an aerosol property are needed to detect a significant trend within one decade. This highlights that long-term efforts well beyond a decade are needed to capture smaller changes. It is particularly important to understand the ongoing natural changes in the Arctic, where interannual variability can be high, such as with forest fire emissions and their influence on the aerosol population. To investigate the climate-change-induced influence on the aerosol population and the resulting climate feedback, long-term observations of tracers more specific to natural sources are needed, as well as of particle microphysical properties such as size distributions, which can be used to identify changes in particle populations which are not well captured by mass-oriented methods such as bulk chemical composition. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

Long-term measurements of atmospheric mass concentrations of black carbon (BC) are needed to investigate changes in its emission, transport, and deposition. However, depending on instrumentation, parameters related to BC such as aerosol absorption coefficient (babs) have been measured instead. Most ground-based measurements of babs in the Arctic have been made by filter-based absorption photometers, including particle soot absorption photometers (PSAPs), continuous light absorption photometers (CLAPs), Aethalometers, and multi-angle absorption photometers (MAAPs). The measured babs can be converted to mass concentrations of BC (MBC) by assuming the value of the mass absorption cross section (MAC; MBC= babs/ MAC). However, the accuracy of conversion of babs to MBC has not been adequately assessed. Here, we introduce a systematic method for deriving MAC values from babs measured by these instruments and independently measured MBC. In this method, MBC was measured with a filter-based absorption photometer with a heated inlet (COSMOS). COSMOS-derived MBC (MBC (COSMOS)) is traceable to a rigorously calibrated single particle soot photometer (SP2), and the absolute accuracy of MBC (COSMOS) has been demonstrated previously to be about 15 % in Asia and the Arctic. The necessary conditions for application of this method are a high correlation of the measured babs with independently measured MBC and long-term stability of the regression slope, which is denoted as MAC cor (MAC derived from the correlation). In general, babs – MBC (COSMOS) correlations were high (r2= 0.76–0.95 for hourly data) at Alert in Canada, Ny-Ålesund in Svalbard, Barrow (NOAA Barrow Observatory) in Alaska, Pallastunturi in Finland, and Fukue in Japan and stable for up to 10 years. We successfully estimated MAC cor values (10.8–15.1 m 2 g -1 at a wavelength of 550 nm for hourly data) for these instruments, and these MAC cor values can be used to obtain error-constrained estimates of MBC from babs measured at these sites even in the past, when COSMOS measurements were not made. Because the absolute values of MBC at these Arctic sites estimated by this method are consistent with each other, they are applicable to the study of spatial and temporal variation in MBC in the Arctic and to evaluation of the performance of numerical model calculations. [ABSTRACT FROM AUTHOR]

Seasonal to interannual variations in the concentrations of sulfur aerosols (< 2.5 µ m in diameter; non sea-salt sulfate: NSS-SO 42- ; anthropogenic sulfate: Anth-SO 42- ; biogenic sulfate: Bio-SO 42- ; methanesulfonic acid: MSA) in the Arctic atmosphere were investigated using measurements of the chemical composition of aerosols collected at Ny-Ålesund, Svalbard (78.9 ∘ N, 11.9 ∘ E) from 2015 to 2019. In all measurement years the concentration of NSS-SO 42- was highest during the pre-bloom period and rapidly decreased towards summer. During the pre-bloom period we found a strong correlation between NSS-SO 42- (sum of Anth-SO 42- and Bio-SO 42-) and Anth-SO 42-. This was because more than 50 % of the NSS-SO 42- measured during this period was Anth-SO 42- , which originated in northern Europe and was subsequently transported to the Arctic in Arctic haze. Unexpected increases in the concentration of Bio-SO 42- aerosols (an oxidation product of dimethylsulfide: DMS) were occasionally found during the pre-bloom period. These probably originated in regions to the south (the North Atlantic Ocean and the Norwegian Sea) rather than in ocean areas in the proximity of Ny-Ålesund. Another oxidation product of DMS is MSA, and the ratio of MSA to Bio-SO 42- is extensively used to estimate the total amount of DMS-derived aerosol particles in remote marine environments. The concentration of MSA during the pre-bloom period remained low, primarily because of the greater loss of MSA relative to Bio-SO 42- and the suppression of condensation of gaseous MSA onto particles already present in air masses being transported northwards from distant ocean source regions (existing particles). In addition, the low light intensity during the pre-bloom period resulted in a low concentration of photochemically activated oxidant species including OH radicals and BrO; these conditions favored the oxidation pathway of DMS to Bio-SO 42- rather than to MSA, which acted to lower the MSA concentration at Ny-Ålesund. The concentration of MSA peaked in May or June and was positively correlated with phytoplankton biomass in the Greenland and Barents seas around Svalbard. As a result, the mean ratio of MSA to the DMS-derived aerosols was low (0.09 ± 0.07) in the pre-bloom period but high (0.32 ± 0.15) in the bloom and post-bloom periods. There was large interannual variability in the ratio of MSA to Bio-SO 42- (i.e., 0.24 ± 0.11 in 2017, 0.40 ± 0.14 in 2018, and 0.36 ± 0.14 in 2019) during the bloom and post-bloom periods. This was probably associated with changes in the chemical properties of existing particles, biological activities surrounding the observation site, and air mass transport patterns. Our results indicate that MSA is not a conservative tracer for predicting DMS-derived particles, and the contribution of MSA to the growth of newly formed particles may be much larger during the bloom and post-bloom periods than during the pre-bloom period. [ABSTRACT FROM AUTHOR]

Atmospheric aging promotes internal mixing of black carbon (BC), leading to an enhancement of light absorption and radiative forcing. The relationship between BC mixing state and consequent absorption enhancement was never estimated for BC found in the Arctic region. In the present work, we aim to quantify the absorption enhancement and its impact on radiative forcing as a function of microphysical properties and mixing state of BC observed in situ at the Zeppelin Arctic station (78° N) in the spring of 2012 during the CLIMSLIP (Climate impacts of short-lived pollutants in the polar region) project. Single-particle soot photometer (SP2) measurements showed a mean mass concentration of refractory black carbon (rBC) of 39 ngm-3, while the rBC mass size distribution was of lognormal shape, peaking at an rBC mass-equivalent diameter (DrBC) of around 240 nm. On average, the number fraction of particles containing a BC core with DrBC>80 nm was less than 5% in the size range (overall optical particle diameter) from 150 to 500 nm. The BC cores were internally mixed with other particulate matter. The median coating thickness of BC cores with 220 nm < DrBC < 260 nm was 52 nm, resulting in a core--shell diameter ratio of 1.4, assuming a coated sphere morphology. Combining the aerosol absorption coefficient observed with an Aethalometer and the rBC mass concentration from the SP2, a mass absorption cross section (MAC) of 9.8m² g-1 was inferred at a wavelength of 550 nm. Consistent with direct observation, a similar MAC value (8.4m² g-1 at 550 nm) was obtained indirectly by using Mie theory and assuming a coated-sphere morphology with the BC mixing state constrained from the SP2 measurements. According to these calculations, the lensing effect is estimated to cause a 54% enhancement of the MAC compared to that of bare BC particles with equal BC core size distribution. Finally, the ARTDECO radiative transfer model was used to estimate the sensitivity of the radiative balance to changes in light absorption by BC as a result of a varying degree of internal mixing at constant total BC mass. The clear-sky noontime aerosol radiative forcing over a surface with an assumed wavelength-dependent albedo of 0.76-0.89 decreased, when ignoring the absorption enhancement, by -0.12 W in m-2 compared to the base case scenario, which was constrained with mean observed aerosol properties for the Zeppelin site in Arctic spring. The exact magnitude of this forcing difference scales with environmental conditions such as the aerosol optical depth, solar zenith angle and surface albedo. Nevertheless, our investigation suggests that the absorption enhancement due to internal mixing of BC, which is a systematic effect, should be considered for quantifying the aerosol radiative forcing in the Arctic region. [ABSTRACT FROM AUTHOR]

Understanding the role of short-lived climate forcers such as black carbon (BC) at high northern latitudes in climate change is hampered by the scarcity of surface observations in the Russian Arctic. In this study, highly time-resolved Equivalent BC (EBC) measurements during a ship campaign in the White, Barents, and Kara Seas in October 2015 are presented. The measured EBC concentrations are compared with BC concentrations simulated with a Lagrangian particle dispersion model coupled with a recently completed global emission inventory to quantify the origin of the Arctic BC. EBC showed increased values (100-400 ng m-3) in the Kara Strait, Kara Sea, and Kola Peninsula and an extremely high concentration (1000 ng m-3) in the White Sea. Assessment of BC origin throughout the expedition showed that gas-flaring emissions from the Yamal-Khanty-Mansiysk and Nenets-Komi regions contributed the most when the ship was close to the Kara Strait, north of 70° N. Near Arkhangelsk (White Sea), biomass burning in mid-latitudes, surface transportation, and residential and commercial combustion from Central and Eastern Europe were found to be important BC sources. The model reproduced observed EBC concentrations efficiently, building credibility in the emission inventory for BC emissions at high northern latitudes. [ABSTRACT FROM AUTHOR]