scholarly journals Apportioning aerosol natural and anthropogenic sources thorough simultaneous aerosol size distributions and chemical composition in the European high Arctic

2018 ◽  
Author(s):  
Manuel Dall'Osto ◽  
David C. S. Beddows ◽  
Peter Tunved ◽  
Roy M. Harrison ◽  
Angelo Lupi ◽  
...  

Abstract. Understanding aerosol size distributions is crucial to our ability to predict aerosol number concentrations. When of favourable size and composition, both long range transported particles as well as locally formed ones may serve as Cloud Condensation Nuclei (CCN); small changes may have a large impact on the low CCN concentrations currently characteristic of the Arctic environment. Here, we present a cluster analysis of particle size distributions (PSD, size range 8–500 nm) simultaneously collected from three high Arctic sites across Europe during a three year period (2013–2015). Two sites are located in the Svalbard archipelago: Zeppelin research station (474 m above ground), and the nearby Gruvebadet Observatory (about 2 km distance from Zepplelin, 67 m above ground). The third site (Villum Research Station – Station Nord, 30 m above ground) is 600 km to the west-northwest of Zeppelin, at the tip of north-eastern Greenland. An inter-site comparison exercise is carried out for the first time including the Gruvebadet site. K-means analysis provided eight specific aerosol categories, further combined into broad PSD with similar characteristics, namely: pristine low concentrations (12–14 %), 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 shows PSD 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, associated with sea spray (largest detectable sizes), Arctic haze (main mode at 150 nm) and aged accumulation mode (main mode at 220 nm) aerosols. In contrast, locally produced and most likely of marine biogenic origin particles exhibit size distributions dominated by the nucleation and Atiken mode aerosol during summer months. The obtained data and analysis set now the stage for future studies; including apportioning the relative contribution of primary and secondary aerosol formation processes to the aerosol size distribution in high Arctic, and elucidating anthropogenic aerosol dynamics, transport and removal processes across the Greenland sea. In a region of enormous importance for future climate on Earth, it is imperative to continue strengthening international scientific cooperation, in order to address important research questions on scales beyond singular station or measurement events.

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 ◽  
Vol 17 (13) ◽  
pp. 8101-8128 ◽  
Author(s):  
Eyal Freud ◽  
Radovan Krejci ◽  
Peter Tunved ◽  
Richard Leaitch ◽  
Quynh T. Nguyen ◽  
...  

Abstract. The Arctic environment has an amplified response to global climatic change. It is sensitive to human activities that mostly take place elsewhere. For this study, a multi-year set of observed aerosol number size distributions in the diameter range of 10 to 500 nm from five sites around the Arctic Ocean (Alert, Villum Research Station – Station Nord, Zeppelin, Tiksi and Barrow) was assembled and analysed.A cluster analysis of the aerosol number size distributions revealed four distinct distributions. Together with Lagrangian air parcel back-trajectories, they were used to link the observed aerosol number size distributions with a variety of transport regimes. This analysis yields insight into aerosol dynamics, transport and removal processes, on both an intra- and an inter-monthly scale. For instance, the relative occurrence of aerosol number size distributions that indicate new particle formation (NPF) event is near zero during the dark months, increases gradually to  ∼ 40 % from spring to summer, and then collapses in autumn. Also, the likelihood of Arctic haze aerosols is minimal in summer and peaks in April at all sites.The residence time of accumulation-mode particles in the Arctic troposphere is typically long enough to allow tracking them back to their source regions. Air flow that passes at low altitude over central Siberia and western Russia is associated with relatively high concentrations of accumulation-mode particles (Nacc) at all five sites – often above 150 cm−3. There are also indications of air descending into the Arctic boundary layer after transport from lower latitudes.The analysis of the back-trajectories together with the meteorological fields along them indicates that the main driver of the Arctic annual cycle of Nacc, on the larger scale, is when atmospheric transport covers the source regions for these particles in the 10-day period preceding the observations in the Arctic. The scavenging of these particles by precipitation is shown to be important on a regional scale and it is most active in summer. Cloud processing is an additional factor that enhances the Nacc annual cycle.There are some consistent differences between the sites that are beyond the year-to-year variability. They are the result of differences in the proximity to the aerosol source regions and to the Arctic Ocean sea-ice edge, as well as in the exposure to free-tropospheric air and in precipitation patterns – to mention a few. Hence, for most purposes, aerosol observations from a single Arctic site cannot represent the entire Arctic region. Therefore, the results presented here are a powerful observational benchmark for evaluation of detailed climate and air chemistry modelling studies of aerosols throughout the vast Arctic region.


2010 ◽  
Vol 10 (16) ◽  
pp. 7891-7906 ◽  
Author(s):  
Z. Jurányi ◽  
M. Gysel ◽  
E. Weingartner ◽  
P. F. DeCarlo ◽  
L. Kammermann ◽  
...  

Abstract. Atmospheric aerosol particles are able to act as cloud condensation nuclei (CCN) and are therefore important for the climate and the hydrological cycle, but their properties are not fully understood. Total CCN number concentrations at 10 different supersaturations in the range of SS=0.12–1.18% were measured in May 2008 at the remote high alpine research station, Jungfraujoch, Switzerland (3580 m a.s.l.). In this paper, we present a closure study between measured and predicted CCN number concentrations. CCN predictions were done using dry number size distribution (scanning particle mobility sizer, SMPS) and bulk chemical composition data (aerosol mass spectrometer, AMS, and multi-angle absorption photometer, MAAP) in a simplified Köhler theory. The predicted and the measured CCN number concentrations agree very well and are highly correlated. A sensitivity study showed that the temporal variability of the chemical composition at the Jungfraujoch can be neglected for a reliable CCN prediction, whereas it is important to know the mean chemical composition. The exact bias introduced by using a too low or too high hygroscopicity parameter for CCN prediction was further quantified and shown to be substantial for the lowest supersaturation. Despite the high average organic mass fraction (~45%) in the fine mode, there was no indication that the surface tension was substantially reduced at the point of CCN activation. A comparison between hygroscopicity tandem differential mobility analyzer (HTDMA), AMS/MAAP, and CCN derived κ values showed that HTDMA measurements can be used to determine particle hygroscopicity required for CCN predictions if no suitable chemical composition data are available.


2013 ◽  
Vol 13 (12) ◽  
pp. 32353-32389 ◽  
Author(s):  
G. P. Almeida ◽  
J. Brito ◽  
C. A. Morales ◽  
M. F. Andrade ◽  
P. Artaxo

Abstract. Measurements of cloud condensation nuclei (CCN), aerosol size distribution and non-refractory chemical composition were performed from 16 to 31 October 2012 in the São Paulo Metropolitan Area (SPMA), Brazil. CCN measurements were performed at 0.2%, 0.4%, 0.6%, 0.8% and 1.0% water supersaturation and were subsequently compared with Köhler theory, considering the chemical composition. Real-time chemical composition has been obtained deploying for the first time in SPMA an Aerosol Chemical Ionization Monitor (ACSM). CCN closure analyses were performed considering internal mixture. Average aerosol composition during the studied period yielded 4.81 ± 3.05, 3.26 ± 2.10, 0.30 ± 0.27, 0.52 ± 0.32, 0.37 ± 0.21 and 0.04 ± 0.04 μg m−3 for organics, BC, NH4, SO4, NO3 and Cl, respectively. Particle number concentration was 12 813 ± 5350 cm−3, being a large fraction in the nucleation mode. CCN concentrations were on average 1090 ± 328 cm−3 and 3570 ± 1695 cm−3 at SS = 0.2% and SS = 1.0%, respectively. Results show an increase in aerosol hygroscopicity in the afternoon as a result of aerosol photochemical processing, leading to an enhancement of both organic and inorganic secondary aerosols in the atmosphere, as well as an increase in aerosol average diameter. Considering the bulk composition alone, CCN concentrations were substantially overpredicted (29.6 ± 45.1% at 0.2% supersaturation and 57.3 ± 30.0% at 1.0% supersaturation). Overall, the impact of composition on the calculated NCCN decreases with decreasing supersaturation, partially because using bulk composition introduces less bias for large diameters and lower critical supersaturations. Results suggest that the consideration of only inorganic fraction improves the calculated NCCN. Introducing a size-dependent chemical composition based on filter measurements from previous campaigns has considerably improved simulated values for NCCN (average overprediction error 3.0 ± 33.4% at 0.20% supersaturation and average under prediction error 2.4 ± 20.5% at 1.0% supersaturation). This study provides the first insight on aerosol real-time composition and hygroscopicity on a~site strongly impacted by emissions of a unique vehicular fleet due to the extensive biofuel usage.


2017 ◽  
Author(s):  
Eyal Freud ◽  
Radovan Krejci ◽  
Peter Tunved ◽  
Richard Leaitch ◽  
Quynh T. Nguyen ◽  
...  

Abstract. The Arctic environment has an amplified response to global climatic change. It is sensitive to human activities that mostly take place elsewhere. For this study, a multi-year set of observed aerosol number size distributions in the diameter range of 10 to 500 nm from five sites around the Arctic Ocean (Alert, Villum Research Station – Station Nord, Zeppelin, Tiksi and Barrow) was assembled and analysed. A cluster analysis of the aerosol number size distributions, revealed four distinct distributions. Together with Lagrangian air parcel back-trajectories, they were used to link the observed aerosol number size distributions with a variety of transport regimes. This analysis yields insight into aerosol dynamics, transport and removal processes, on both an intra- and inter-monthly scales. For instance, the relative occurrence of aerosol number size distributions that indicate new particle formation (NPF) event is near zero during the dark months, and increases gradually to ~ 40 % from spring to summer, and then collapses in autumn. Also, the likelihood of Arctic Haze aerosols is minimal in summer and peaks in April at all sites. The residence time of accumulation-mode particles in the Arctic troposphere is typically long enough to allow tracking them back to their source regions. Air flow that passes at low altitude over central Siberia and Western Russia is associated with relatively high concentrations of accumulation-mode particles (Nacc) at all five sites – often above 150 cm−3. There are also indications of air descending into the Arctic boundary layer after transport from lower latitudes. The analysis of the back-trajectories together with the meteorological fields along them indicates that the main driver of the Arctic annual cycle of Nacc, on the larger scale, is when atmospheric transport covers the source regions for these particles in the 10-day period preceding the observations in the Arctic. The scavenging of these particles by precipitation is shown to be important on a regional scale and it is most active in summer. Cloud processing is an additional factor that enhances the Nacc annual cycle. There are some consistent differences between the sites that are beyond the year-to-year variability. They are the result of differences in the proximity to the aerosol source regions and to the Arctic Ocean sea-ice edge, as well as in the exposure to free tropospheric air and in precipitation patterns – to mention a few. Hence, for most purposes, aerosol observations from a single Arctic site cannot represent the entire Arctic region. Therefore, the results presented here are a powerful observational benchmark for evaluation of detailed climate and air chemistry modelling studies of aerosols throughout the vast Arctic region.


2014 ◽  
Vol 14 (14) ◽  
pp. 7559-7572 ◽  
Author(s):  
G. P. Almeida ◽  
J. Brito ◽  
C. A. Morales ◽  
M. F. Andrade ◽  
P. Artaxo

Abstract. Measurements of cloud condensation nuclei (CCN), aerosol size distribution and non-refractory chemical composition were performed from 16 to 31 October 2012 in the São Paulo Metropolitan Area (SPMA), Brazil. CCN measurements were performed at 0.23, 0.45, 0.68, 0.90 and 1.13% water supersaturation and were subsequently compared with the Köhler theory, considering the chemical composition. Real-time chemical composition has been obtained by deploying, for the first time in the SPMA, an aerosol chemical ionization monitor (ACSM). CCN closure analyses were performed considering internal mixtures. Average aerosol composition during the studied period yielded (arithmetic mean~± standard deviation) 4.81 ± 3.05, 3.26 ± 2.10, 0.30 ± 0.27, 0.52 ± 0.32, 0.37 ± 0.21 and 0.04 ± 0.04 μg m−3 for organics, BC, NH4, SO4, NO3 and Cl, respectively. Particle number concentration was 12 813 ± 5350 cm−3, with a dominant nucleation mode. CCN concentrations were on average 1090 ± 328 and 3570 ± 1695 cm−3 at SS = 0.23% and SS = 1.13%, respectively. Results show an increase in aerosol hygroscopicity in the afternoon as a result of aerosol photochemical processing, leading to an enhancement of both organic and inorganic secondary aerosols in the atmosphere, as well as an increase in aerosol average diameter. Considering the bulk composition alone, observed CCN concentrations were substantially overpredicted when compared with the Köhler theory (44.1 ± 47.9% at 0.23% supersaturation and 91.4 ± 40.3% at 1.13% supersaturation). Overall, the impact of composition on the calculated CCN concentration (NCCN) decreases with decreasing supersaturation, partially because using bulk composition introduces less bias for large diameters and lower critical supersaturations, defined as the supersaturation at which the cloud droplet activation will take place. Results suggest that the consideration of only inorganic fraction improves the calculated NCCN. Introducing a size-dependent chemical composition based on filter measurements from previous campaigns has considerably improved simulated values for NCCN (average overprediction error 14.8 ± 38.6% at 0.23% supersaturation and 3.6 ± 21.6% at 1.13% supersaturation). This study provides the first insight on aerosol real-time composition and hygroscopicity at a site strongly impacted by emissions of a unique vehicular fleet due to the extensive biofuel usage.


2011 ◽  
Vol 11 (3) ◽  
pp. 8801-8840
Author(s):  
M. Martin ◽  
R. Y.-W. Chang ◽  
B. Sierau ◽  
S. Sjogren ◽  
E. Swietlicki ◽  
...  

Abstract. We present an aerosol – cloud condensation nuclei CCN) closure study on summer high Arctic aerosol based on measurements that were carried out in summer 2008 during the Arctic Summer Cloud Ocean Study (ASCOS) on board the Swedish ice breaker Oden. The data presented here were collected during a three-week time period in the pack ice (>85° N) when the icebreaker Oden was moored to an ice floe and drifted passively during the most biological active period into autumn freeze up conditions. CCN number concentrations were obtained using two CCN counters measuring at different supersaturations. The directly measured CCN number concentration is then compared with a CCN number concentration calculated using both bulk aerosol mass composition data from an aerosol mass spectrometer and aerosol number size distributions obtained from a differential mobility particle sizer, assuming κ-Köhler theory and an internally mixed aerosol. For the two highest measured supersaturations, 0.73 and 0.41%, closure could not be achieved with the investigated settings concerning hygroscopicity and density. The calculated CCN number concentration was always higher than the measured one. One possible explanation is that the smaller particles that activate at these supersaturations have a relative larger insoluble organic mass fraction and thus are less good CCN than the larger particles. At 0.20, 0.15 and 0.10% supersaturation, the measured CCN number can be represented with different parameters for the hygroscopicity and density of the particles. For the best agreement of the calculated CCNnumber concentration with the measured one the organic fraction of the aerosol needs to be nearly insoluble (қorg=0.02). However, this is not unambigious and қorg=0.2 is found as an upper limit at 0.1% supersaturation.


2014 ◽  
Vol 7 (8) ◽  
pp. 2615-2629 ◽  
Author(s):  
M. L. Krüger ◽  
S. Mertes ◽  
T. Klimach ◽  
Y. F. Cheng ◽  
H. Su ◽  
...  

Abstract. In this study we show how size-resolved measurements of aerosol particles and cloud condensation nuclei (CCN) can be used to characterize the supersaturation of water vapor in a cloud. The method was developed and applied during the ACRIDICON-Zugspitze campaign (17 September to 4 October 2012) at the high-Alpine research station Schneefernerhaus (German Alps, 2650 m a.s.l.). Number size distributions of total and interstitial aerosol particles were measured with a scanning mobility particle sizer (SMPS), and size-resolved CCN efficiency spectra were recorded with a CCN counter system operated at different supersaturation levels. During the evolution of a cloud, aerosol particles are exposed to different supersaturation levels. We outline and compare different estimates for the lower and upper bounds (Slow, Shigh) and the average value (Savg) of peak supersaturation encountered by the particles in the cloud. A major advantage of the derivation of Slow and Savg from size-resolved CCN efficiency spectra is that it does not require the specific knowledge or assumptions about aerosol hygroscopicity that are needed to derive estimates of Slow, Shigh, and Savg from aerosol size distribution data. For the investigated cloud event, we derived Slow ≈ 0.07–0.25%, Shigh ≈ 0.86–1.31% and Savg ≈ 0.42–0.68%.


2010 ◽  
Vol 10 (4) ◽  
pp. 8859-8897 ◽  
Author(s):  
Z. Jurányi ◽  
M. Gysel ◽  
E. Weingartner ◽  
P. F. DeCarlo ◽  
L. Kammermann ◽  
...  

Abstract. Atmospheric aerosol particles are able to act as cloud condensation nuclei (CCN) and are therefore important for the climate and the hydrological cycle, but their properties are not fully understood. Total CCN number concentrations at 10 different supersaturations in the range of SS = 0.12–1.18% were measured in May 2008 at the remote high alpine research station, Jungfraujoch, Switzerland (3580 m asl.). In this paper, we present a closure study between measured and predicted CCN number concentrations. CCN predictions were done using number size distribution (scanning particle mobility sizer, SMPS) and bulk chemical composition data (aerosol mass spectrometer, AMS, and multi-angle absorption photometer, MAAP) in a simplified Köhler theory. The predicted and the measured CCN concentrations agree very well and are highly correlated. A sensitivity study showed that the temporal variability of the chemical composition at the Jungfraujoch can be neglected for a reliable CCN prediction, whereas it is important to know the mean chemical composition. The exact bias introduced by using a too low or too high hygroscopicity parameter for CCN prediction was further quantified and shown to be substantial for the lowest supersaturation. Despite the high average organic mass fraction (45%) during the measurement campaign, there was no indication that the surface tension was substantially reduced at the point of CCN activation. A comparison between hygroscopicity tandem differential mobility analyzer (HTDMA), AMS/MAAP, and CCN derived κ values showed that HTDMA measurements can be used as a chemical composition proxy for CCN predictions if no suitable chemical composition data are available.


2015 ◽  
Vol 15 (23) ◽  
pp. 13803-13817 ◽  
Author(s):  
J. Zábori ◽  
N. Rastak ◽  
Y. J. Yoon ◽  
I. Riipinen ◽  
J. Ström

Abstract. 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°54´ N, 11°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 (Dp) at a SS of 0.4 %, the activation diameter (D50), corresponding to CCN / CN = 0.50, was estimated. D50 was found to be 60 and 67 nm for the examined periods in June and August 2008, respectively. Corresponding D50 hygroscopicity parameter (κ) 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 κ was calculated to be 0.5 for both June and August 2008. While the agreement between the 2 months is reasonable, the difference in κ 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.


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