scholarly journals Atmospheric black carbon and sulfate concentrations in Northeast Greenland

2015 ◽  
Vol 15 (8) ◽  
pp. 11465-11493 ◽  
Author(s):  
A. Massling ◽  
I. E. Nielsen ◽  
D. Kristensen ◽  
J. H. Christensen ◽  
L. L. Sørensen ◽  
...  

Abstract. Measurements of Black Carbon (BC) in aerosols at the high Arctic field site Villum Research Station (VRS) at Station Nord in North Greenland showed a seasonal variation in BC concentrations with a maximum in winter and spring at ground level. The data was obtained using a Multi Angle Absorption Photometer (MAAP). A similar seasonal pattern was found for sulfate concentrations with a maximum level during winter and spring analyzed by ion chromatography. A correlation between BC and sulfate concentrations was observed over the years 2011 to 2013. This finding gives the hint that most likely transport of primary emitted BC particles to the Arctic was accompanied by aging of the aerosols through condensational processes. This process may have led to the formation of secondary inorganic matter and further transport of BC particles as cloud processing and further washout of particles is less likely based on the typically observed transport patterns of air masses arriving at VRS. Additionally, concentrations of EC (elemental carbon) based on a thermo-optical method were determined and compared to BC measurements. Model estimates of the climate forcing due to BC in the Arctic are based on contributions of long-range transported BC during spring and summer. The measured concentrations were here compared with model results obtained by the Danish Hemispheric Model, DEHM. Good agreement between measured and modeled concentrations of both BC and sulfate was observed. The dominant source is found to be combustion of fossil fuel with biomass burning as a minor though significant source. During winter and spring the Arctic atmosphere is known to be impacted by long-range transport of BC and associated with the Arctic haze phenomenon.

2015 ◽  
Vol 15 (16) ◽  
pp. 9681-9692 ◽  
Author(s):  
A. Massling ◽  
I. E. Nielsen ◽  
D. Kristensen ◽  
J. H. Christensen ◽  
L. L. Sørensen ◽  
...  

Abstract. Measurements of equivalent black carbon (EBC) in aerosols at the high Arctic field site Villum Research Station (VRS) at Station Nord in North Greenland showed a seasonal variation in EBC concentrations with a maximum in winter and spring at ground level. Average measured concentrations were about 0.067 ± 0.071 for the winter and 0.011 ± 0.009 for the summer period. These data were obtained using a multi-angle absorption photometer (MAAP). A similar seasonal pattern was found for sulfate concentrations with a maximum level during winter and spring analyzed by ion chromatography. Here, measured average concentrations were about 0.485 ± 0.397 for the winter and 0.112 ± 0.072 for the summer period. A correlation between EBC and sulfate concentrations was observed over the years 2011 to 2013 stating a correlation coefficient of R2 = 0.72. This finding gives the hint that most likely transport of primary emitted BC particles to the Arctic was accompanied by aging of the aerosols through condensational processes. BC and sulfate are known to have only partly similar sources with respect to their transport pathways when reaching the high Arctic. Aging processes may have led to the formation of secondary inorganic matter and further transport of BC particles as cloud processing and further washout of particles is less likely based on the typically observed transport patterns of air masses arriving at VRS. Additionally, concentrations of EC (elemental carbon) based on a thermo-optical method were determined and compared to EBC measurements. EBC measurements were generally higher, but a correlation between EC and EBC resulted in a correlation coefficient of R2 = 0.64. Model estimates of the climate forcing due to BC in the Arctic are based on contributions of long-range transported BC during spring and summer. The measured concentrations were here compared with model results obtained by the Danish Eulerian Hemispheric Model, DEHM. Good agreement between measured and modeled concentrations of both EBC/BC and sulfate was observed. Also, the correlation between BC and sulfate concentrations was confirmed based on the model results observed over the years 2011 to 2013 stating a correlation coefficient of R2 = 0.74. The dominant source is found to be combustion of fossil fuel with biomass burning as a minor, albeit significant source.


2021 ◽  
Vol 21 (17) ◽  
pp. 13287-13309
Author(s):  
Jakob Boyd Pernov ◽  
Bjarne Jensen ◽  
Andreas Massling ◽  
Daniel Charles Thomas ◽  
Henrik Skov

Abstract. While much research has been devoted to the subject of gaseous elemental mercury (GEM) and gaseous oxidized mercury (GOM) in the Arctic spring during atmospheric mercury depletion events, few studies have examined the behavior of GOM in the High Arctic summer. GOM, once deposited and incorporated into the ecosystem, can pose a threat to human and wildlife health, though there remain large uncertainties regarding the transformation, deposition, and assimilation of mercury into the food web. Therefore, to further our understanding of the dynamics of GOM in the High Arctic during the late summer, we performed measurements of GEM and GOM, along with meteorological parameters and atmospheric constituents, and utilized modeled air mass history during two summer campaigns in 2019 and 2020 at Villum Research Station (Villum) in northeastern Greenland. Seven events of enhanced GOM concentrations were identified and investigated in greater detail. In general, the common factors associated with event periods at ground level were higher levels of radiation and lower H2O mixing ratios, accumulated precipitation, and relative humidity (RH), although none were connected with cold temperatures. Non-event periods at ground level each displayed a different pattern in one or more parameters when compared to event periods. Generally, air masses during event periods for both campaigns were colder and drier, arrived from higher altitudes, and spent more time above the mixed layer and less time in a cloud compared to non-events, although some events deviated from this general pattern. Non-event air masses displayed a different pattern in one or more parameters when compared to event periods, although they were generally warmer and wetter and arrived from lower altitudes with little radiation. Coarse-mode aerosols were hypothesized to provide the heterogenous surface for halogen propagation during some of the events, while for others the source is unknown. While these general patterns were observed for event and non-event periods, analysis of individual events showed more specific origins. Five of the seven events were associated with air masses that experienced similar conditions: transported from the cold, dry, and sunlit free troposphere. However, two events experienced contrasting conditions, with air masses being warm and wet with surface layer contact under little radiation. Two episodes of extremely high levels of NCoarse and BC, which appear to originate from flaring emissions in Russia, did not contribute to enhanced GOM levels. This work aims to provide a better understanding of the dynamics of GOM during the High Arctic summer.


2019 ◽  
Author(s):  
Ingeborg E. Nielsen ◽  
Henrik Skov ◽  
Andreas Massling ◽  
Axel C. Eriksson ◽  
Manuel Dall'Osto ◽  
...  

Abstract. There are limited measurements of the chemical composition, abundance, and sources of black carbon (BC) containing particles in the high Arctic. To address this, we report 93 days of Soot Particle Aerosol Mass Spectrometer (SP-AMS) data collected in the high Arctic. The period spans from February 20th until May 23rd 2015 at Villum Research Station (VRS) in Northern Greenland (81°36' N). Particulate sulfate (SO42−) accounted for 66 % of the non-refractory PM1, which amounted to 2.3 µg m−3 as an average value observed during the campaign. The second most abundant species was organic matter (24 %), averaging 0.55 µg m3. Both organic aerosol (OA) and PM1, estimated from the sum of all collected species, showed a marked decrease throughout May in accordance with Arctic haze leveling off. The refractory black carbon (rBC) concentration averaged 0.1 µg m−3 over the entire campaign. Positive Matrix Factorization (PMF) of the OA mass spectra yielded three factors: (1) a Hydrocarbon-like Organic Aerosol (HOA) factor, which was dominated by primary aerosols and accounted for 12 % of OA mass; (2) an Arctic haze Organic Aerosol (AOA) factor, which accounted for 64 % of the OA and dominated until mid-April while being nearly absent from the end of May; and (3) a more oxygenated Marine Organic Aerosol (MOA) factor, which accounted for 22 % of OA. AOA correlated significantly with SO42−, suggesting the main part of that factor being secondary OA. The MOA emerged late at the end of March, where it increased with solar radiation and reduced sea ice extent, and dominated OA for the rest of the campaign until the end of May. Important differences are observed among the factors, including the highest O/C ratio (0.95) and S/C ratio (0.011) for MOA – the marine related factor. Our data supports current understanding of the Arctic summer aerosols, driven mainly by secondary aerosol formation, but with an important contribution from marine emissions. In view of a changing Arctic climate with changing sea-ice extent, biogenic processes, and corresponding source strengths, highly time-resolved data are urgently needed in order to elucidate the components dominating aerosol concentrations.


2011 ◽  
Vol 11 (12) ◽  
pp. 32499-32534 ◽  
Author(s):  
M. T. Lund ◽  
T. Berntsen

Abstract. A critical parameter for the atmospheric lifetime of black carbon (BC) aerosols, and hence for the range over which the particles can be transported, is the aging time, i.e. the time before the aerosols become available for removal by wet deposition. This study compares two different parameterizations of BC aging in the chemistry transport model OsloCTM2: (i) a bulk parameterization (BULK) where aging is represented by a constant transfer to hydrophilic mode and (ii) a microphysical module (M7) where aging occurs through particle interaction and where the particle size distribution is accounted for. We investigate the effect of including microphysics on the distribution of BC globally and in the Arctic. We also focus on the impact on estimated contributions to Arctic BC from selected emission source regions. With more detailed microphysics (M7) there are regional and seasonal variations in aging. The aging is slower during high-latitude winter, when the production of sulfate is lower, than in lower latitudes and during summer. High-latitude concentrations of BC are significantly increased during winter compared to BULK. Furthermore, M7 improves the model performance at high Arctic surface stations, especially the accumulation of BC during winter. A proper representation of vertical BC load is important because the climate effects of the aerosols depend on their altitude in the atmosphere. Comparisons with measured vertical profiles indicate that the model generally overestimates the BC load, particularly at higher altitudes, and this overestimation is exacerbated with M7 compared to BULK. Both parameterizations show that north of 65° N emissions in Europe contribute most to atmospheric BC concentration and to BC in snow and ice. M7 leads to a pronounced seasonal pattern in contributions and contributions from Europe and Russia increase strongly during winter compared to BULK. There is generally a small increase in the amount of BC in snow and ice with M7 compared to BULK, but concentrations are still underestimated relative to measurements.


2010 ◽  
Vol 10 (2) ◽  
pp. 2221-2244 ◽  
Author(s):  
L. Huang ◽  
S. L. Gong ◽  
S. Sharma ◽  
D. Lavoué ◽  
C. Q. Jia

Abstract. Black carbon (BC) particles accumulated in the Arctic troposphere and deposited over snow have significant effects on radiative forcing of the Arctic regional climate. Applying cluster analysis technique on 10-day backward trajectories, transport pathways affecting Alert (82.5° N, 62.5° W), Nunavut in Canada are identified in this work, along with the associated transport frequency. Based on the atmospheric transport frequency and the estimated BC emission intensity from surrounding regions, a linear regression model is constructed to investigate the inter-annual variations of BC observed at Alert in January and April, representative of winter and spring respectively, between 1990 and 2005. Strong correlations are found between BC concentrations predicted with the regression model and measured at Alert for both seasons (R2 equals 0.77 and 0.81 for winter and spring, respectively). Results imply that atmospheric transport and BC emission are the major contributors to the inter-annual variations in BC concentrations observed at Alert in the cold seasons for the 16-year period. Based on the regression model the relative contributions of regional BC emissions affecting Alert are attributed to the Eurasian sector, composed of the European Union and the former USSR, and the North American sector. Considering both seasons, the model suggests that Eurasia is the major contributor to the near-surface BC levels at the Canadian High Arctic site with an average contribution of over 85% during the 16-year period. In winter, the atmospheric transport of BC aerosols from Eurasia is found to be even more predominant with a multi-year average of 94%. The model estimates smaller contribution from the Eurasian sector in spring (70%) than that in winter. It is also found that the change in Eurasian contributions depends mainly on the reduction of emission intensity, while the changes in both emission and atmospheric transport contributed to the inter-annual variation of North American contributions.


2019 ◽  
Vol 19 (11) ◽  
pp. 7377-7395 ◽  
Author(s):  
Manuel Dall'Osto ◽  
David C. S. Beddows ◽  
Peter Tunved ◽  
Roy M. Harrison ◽  
Angelo Lupi ◽  
...  

Abstract. 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-range-transported – 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 (2013–2015). 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 north-eastern Greenland. The GRU site is included in an inter-site comparison for the first time. K-means cluster analysis provided 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.


2017 ◽  
Author(s):  
Kohei Ikeda ◽  
Hiroshi Tanimoto ◽  
Takafumi Sugita ◽  
Hideharu Akiyoshi ◽  
Yugo Kanaya ◽  
...  

Abstract. We implemented a tagged tracer method of black carbon (BC) into a global chemistry-transport model GEOS-Chem, examined the pathways and efficiency of long-range transport from a variety of anthropogenic and biomass burning emission sources to the Arctic, and quantified the source contributions of individual emissions. Firstly, we evaluated the simulated BC by comparing it with observations at the Arctic sites and found that the simulated seasonal variations were improved by implementing an aging parameterization and reducing the wet scavenging rate by ice clouds. For tagging BC, we added BC tracers distinguished by source types (anthropogenic and biomass burning) and regions; the global domain was divided into 16 and 27 regions for anthropogenic and biomass burning emissions, respectively. Our simulations showed that BC emitted from Europe and Russia was transported to the Arctic mainly in the lower troposphere during winter and spring. In particular, BC transported from Russia was widely spread over the Arctic in winter and spring, leading to a dominant contribution of 62 % to the Arctic BC near the surface as the annual mean. In contrast, BC emitted from East Asia was found to be transported in the middle troposphere into the Arctic mainly over the Okhotsk Sea and East Siberia during winter and spring. We identified an important window area, which allowed a strong incoming of East Asian BC to the Arctic (130°–180° E and 3–8 km altitude at 66° N). The model demonstrated that the contribution from East Asia to the Arctic had a maximum at about 5 km altitude due to uplifting during the long-range transport in early spring. The efficiency of BC transport from East Asia to the Arctic was smaller than that from other large source regions such as Europe, Russia and North America. However, the East Asian contribution was most important for BC in the middle troposphere (41 %) and BC burden over the Arctic (27 %) because of the large emissions from this region. These results suggested that the main sources of the Arctic BC differed with altitude. The contribution of all the anthropogenic sources to Arctic BC concentrations near the surface was dominant (90 %) on an annual basis. The contributions of biomass burning in boreal regions (Siberia, Alaska and Canada) to the annual total BC deposition onto the Arctic were estimated to be 12–15 %, which became the maximum during summer.


2019 ◽  
Vol 19 (15) ◽  
pp. 10239-10256 ◽  
Author(s):  
Ingeborg E. Nielsen ◽  
Henrik Skov ◽  
Andreas Massling ◽  
Axel C. Eriksson ◽  
Manuel Dall'Osto ◽  
...  

Abstract. There are limited measurements of the chemical composition, abundance and sources of atmospheric particles in the High Arctic To address this, we report 93 d of soot particle aerosol mass spectrometer (SP-AMS) data collected from 20 February to 23 May 2015 at Villum Research Station (VRS) in northern Greenland (81∘36′ N). During this period, we observed the Arctic haze phenomenon with elevated PM1 concentrations ranging from an average of 2.3, 2.3 and 3.3 µg m−3 in February, March and April, respectively, to 1.2 µg m−3 in May. Particulate sulfate (SO42-) accounted for 66 % of the non-refractory PM1 with the highest concentration until the end of April and decreasing in May. The second most abundant species was organic aerosol (OA) (24 %). Both OA and PM1, estimated from the sum of all collected species, showed a marked decrease throughout May in accordance with the polar front moving north, together with changes in aerosol removal processes. The highest refractory black carbon (rBC) concentrations were found in the first month of the campaign, averaging 0.2 µg m−3. In March and April, rBC averaged 0.1 µg m−3 while decreasing to 0.02 µg m−3 in May. Positive matrix factorization (PMF) of the OA mass spectra yielded three factors: (1) a hydrocarbon-like organic aerosol (HOA) factor, which was dominated by primary aerosols and accounted for 12 % of OA mass, (2) an Arctic haze organic aerosol (AOA) factor and (3) a more oxygenated marine organic aerosol (MOA) factor. AOA dominated until mid-April (64 %–81 % of OA), while being nearly absent from the end of May and correlated significantly with SO42-, suggesting the main part of that factor is secondary OA. The MOA emerged late at the end of March, where it increased with solar radiation and reduced sea ice extent and dominated OA for the rest of the campaign until the end of May (24 %–74 % of OA), while AOA was nearly absent. The highest O∕C ratio (0.95) and S∕C ratio (0.011) was found for MOA. Our data support the current understanding that Arctic aerosols are highly influenced by secondary aerosol formation and receives an important contribution from marine emissions during Arctic spring in remote High Arctic areas. In view of a changing Arctic climate with changing sea-ice extent, biogenic processes and corresponding source strengths, highly time-resolved data are needed in order to elucidate the components dominating aerosol concentrations and enhance the understanding of the processes taking place.


2021 ◽  
Author(s):  
Jakob Boyd Pernov ◽  
Bjarne Jensen ◽  
Andreas Massling ◽  
Daniel Charles Thomas ◽  
Henrik Skov

Abstract. While much research has been devoted to the subject of gaseous elemental mercury (GEM) and gaseous oxidized mercury (GOM) in the Arctic spring, during atmospheric mercury depletion events, few studies have examined the behavior of GOM in the High Arctic summer. GOM, once introduced into the ecosystem, can pose a threat to human and wildlife health, though there remain large uncertainties regarding the transformation, deposition, and assimilation of mercury into the ecosystem. Therefore, to further our understanding of the dynamics of gaseous oxidized mercury in the High Arctic during the late summer, we performed measurements of GEM and GOM along with meteorological parameters, atmospheric constituents, and air mass history during two summer campaigns in 2019 and 2020 at Villum Research Station (Villum) in Northeastern Greenland. Five events of enhanced GOM concentrations were identified and investigated in greater detail. The origin of these events was identified, through analysis of air mass back-trajectories, associated meteorological data, and other atmospheric constituents, to be the cold, dry free troposphere. These events were associated with low RH, limited precipitation, cold temperatures, and intense sunlight along the trajectory path. Events were positively correlated with ozone, aerosol particle number, and black carbon mass concentration, which were interpreted as an indication of tropospheric air masses. This work aims to provide a better understanding of the dynamics of GOM during the High Arctic summer.


2012 ◽  
Vol 12 (6) ◽  
pp. 14813-14836 ◽  
Author(s):  
M. Fenger ◽  
L. L. Sørensen ◽  
K. Kristensen ◽  
B. Jensen ◽  
Q. T. Nquyen ◽  
...  

Abstract. The knowledge of climate effects of atmospheric aerosols is associated with large uncertainty, and a better understanding of their physical and chemical properties is needed, especially in the Arctic environment. The objective of the present study is to improve our understanding of the processes affecting the composition of the aerosols in the high Arctic. Therefore size-segregated aerosols were sampled at a high Arctic site, Station Nord (Northeast Greenland), in March 2009 using a Micro Orifice Uniform Deposit Impactor. The aerosol samples were extracted in order to analyze the three water-soluble anions: chloride, nitrate and sulphate. The results are discussed based on possible chemical and physical transformations as well as transport patterns. The total concentrations of the ions at Station Nord were 53–507 ng m−3, 2–298 ng m−3 and 535–1087 ng m−3 for chloride (Cl−), nitrate (NO3-) and sulphate (SO42−), respectively. The aerosols in late winter/early spring, after polar sunrise, are found to be a mixture of long-range transported and regional to local originating aerosols. Fine particles, smaller than 1 μm, containing SO42−, Cl− and NO3−, are hypothesized to originate from long-range transport, where SO42− is by far the dominating anion accounting for 50–85% of the analyzed mass. The analysis suggests that Cl− and NO3− in coarser particles (>1.5 μm) originate from local/regional sources. Under conditions where the air mass is transported over sea-ice at high wind speeds, very coarse particles (>18 μm) are observed and it is hypothesized that frost flowers on the sea ice is a source of very coarse chloride particles in the Arctic.


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