scholarly journals Summertime observations of ultrafine particles and cloud condensation nuclei from the boundary layer to the free troposphere in the Arctic

Author(s):  
Julia Burkart ◽  
Megan D. Willis ◽  
Heiko Bozem ◽  
Jennie L. Thomas ◽  
Kathy Law ◽  
...  

Abstract. The Arctic is extremely sensitive to climate change. Shrinking sea ice extent increases the area covered by open ocean during Arctic summer, which impacts the surface albedo and aerosol and cloud properties among many things. In this context extensive aerosol measurements (aerosol composition, particle number and size, cloud condensation nuclei, and trace gases) were made during 11 flights of the NETCARE July, 2014 airborne campaign conducted from Resolute Bay, Nunavut (74N, 94W). Flights routinely included vertical profiles from about 60 to 3000 m a.g.l. as well as several low-level horizontal transects over open ocean, fast ice, melt ponds, and polynyas. Here we discuss the vertical distribution of ultrafine particles (UFP, particle diameter, dp: 5–20 nm), size distributions of larger particles (dp: 20 nm to 1 μm), and cloud condensation nuclei (CCN, supersaturation = 0.6 %) in relation to meteorological conditions and underlying surfaces. UFPs were observed predominantly within the boundary layer, where concentrations were often several hundreds to a few thousand particles per cubic centimeter. Occasionally, particle concentrations below 10 cm−3 were found. The highest UFP concentrations were observed above open ocean and at the top of low-level clouds, whereas numbers over ice-covered regions were substantially lower. Overall, UFP formation events were frequent in a clean boundary layer with a low condensation sink. In a few cases this ultrafine mode extended to sizes larger than 40 nm, suggesting that these UFP can grow into a size range where they can impact clouds and therefore climate.

2017 ◽  
Vol 17 (8) ◽  
pp. 5515-5535 ◽  
Author(s):  
Julia Burkart ◽  
Megan D. Willis ◽  
Heiko Bozem ◽  
Jennie L. Thomas ◽  
Kathy Law ◽  
...  

Abstract. Motivated by increasing levels of open ocean in the Arctic summer and the lack of prior altitude-resolved studies, extensive aerosol measurements were made during 11 flights of the NETCARE July 2014 airborne campaign from Resolute Bay, Nunavut. Flights included vertical profiles (60 to 3000 m above ground level) over open ocean, fast ice, and boundary layer clouds and fogs. A general conclusion, from observations of particle numbers between 5 and 20 nm in diameter (N5 − 20), is that ultrafine particle formation occurs readily in the Canadian high Arctic marine boundary layer, especially just above ocean and clouds, reaching values of a few thousand particles cm−3. By contrast, ultrafine particle concentrations are much lower in the free troposphere. Elevated levels of larger particles (for example, from 20 to 40 nm in size, N20 − 40) are sometimes associated with high N5 − 20, especially over low clouds, suggestive of aerosol growth. The number densities of particles greater than 40 nm in diameter (N >  40) are relatively depleted at the lowest altitudes, indicative of depositional processes that will lower the condensation sink and promote new particle formation. The number of cloud condensation nuclei (CCN; measured at 0.6 % supersaturation) are positively correlated with the numbers of small particles (down to roughly 30 nm), indicating that some fraction of these newly formed particles are capable of being involved in cloud activation. Given that the summertime marine Arctic is a biologically active region, it is important to better establish the links between emissions from the ocean and the formation and growth of ultrafine particles within this rapidly changing environment.


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.


2019 ◽  
Vol 19 (22) ◽  
pp. 14339-14364 ◽  
Author(s):  
Simonas Kecorius ◽  
Teresa Vogl ◽  
Pauli Paasonen ◽  
Janne Lampilahti ◽  
Daniel Rothenberg ◽  
...  

Abstract. In a warming Arctic the increased occurrence of new particle formation (NPF) is believed to originate from the declining ice coverage during summertime. Understanding the physico-chemical properties of newly formed particles, as well as mechanisms that control both particle formation and growth in this pristine environment, is important for interpreting aerosol–cloud interactions, to which the Arctic climate can be highly sensitive. In this investigation, we present the analysis of NPF and growth in the high summer Arctic. The measurements were made on-board research vessel Polarstern during the PS106 Arctic expedition. Four distinctive NPF and subsequent particle growth events were observed, during which particle (diameter in a range 10–50 nm) number concentrations increased from background values of approx. 40 up to 4000 cm−3. Based on particle formation and growth rates, as well as hygroscopicity of nucleation and the Aitken mode particles, we distinguished two different types of NPF events. First, some NPF events were favored by negative ions, resulting in more-hygroscopic nucleation mode particles and suggesting sulfuric acid as a precursor gas. Second, other NPF events resulted in less-hygroscopic particles, indicating the influence of organic vapors on particle formation and growth. To test the climatic relevance of NPF and its influence on the cloud condensation nuclei (CCN) budget in the Arctic, we applied a zero-dimensional, adiabatic cloud parcel model. At an updraft velocity of 0.1 m s−1, the particle number size distribution (PNSD) generated during nucleation processes resulted in an increase in the CCN number concentration by a factor of 2 to 5 compared to the background CCN concentrations. This result was confirmed by the directly measured CCN number concentrations. Although particles did not grow beyond 50 nm in diameter and the activated fraction of 15–50 nm particles was on average below 10 %, it could be shown that the sheer number of particles produced by the nucleation process is enough to significantly influence the background CCN number concentration. This implies that NPF can be an important source of CCN in the Arctic. However, more studies should be conducted in the future to understand mechanisms of NPF, sources of precursor gases and condensable vapors, as well as the role of the aged nucleation mode particles in Arctic cloud formation.


2020 ◽  
Author(s):  
Jan Chylik ◽  
Stephan Mertes ◽  
Roel Neggers

<p>Arctic mixed-phase clouds are still not properly represented in weather forecast and climate models. Recent field campaigns in the Arctic have successfully probed low level mixed-phase clouds, however it remains difficult to gain understanding of this complex system from observational datasets alone. Complementary high-resolution simulations, properly constrained by relevant measurements, can serve as a virtual laboratory that provides a deeper insight into a developing boundary layer in the Arctic.</p><p><br>Our study focus on the impact of variability in cloud condensation nuclei (CCN) concentrations on the turbulence in Arctic mixed-phase clouds. Large-Eddy Simulations of convective mixed-phase clouds over open water were performed as observed during the ACLOUD campaign, which took place in Fram Strait west of Svalbard in May and June 2017. The Dutch Atmospheric Large Eddy Simulation (DALES) is used including a well-established double-moment mixed-phase microphysics scheme of Seifert & Beheng.</p><p><br>The results highlight various impact mechanisms of CCN on the boundary layer thermodynamic state, turbulence, and clouds. Lower CCN concentrations generally lead to decreased turbulence near the cloud top. However, they can also enhance the turbulence in the lower part of the boundary layer due to increased amount of sublimation of ice hydrometeors. Further implications for the role of mixed-phase clouds in the Arctic Amplification will be discussed.</p>


2015 ◽  
Vol 15 (4) ◽  
pp. 5079-5128 ◽  
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 characteristic of 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 two 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 two 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 sea salt in the bulk aerosol samples.


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.


2003 ◽  
Vol 3 (1) ◽  
pp. 949-982 ◽  
Author(s):  
P. Pradeep Kumar ◽  
K. Broekhuizen ◽  
J. P. D. Abbatt

Abstract. The ability of sub-micron-sized organic acid particles to act as cloud condensation nuclei (CCN) has been examined at room temperature using a newly constructed continuous-flow, thermal-gradient diffusion chamber (TGDC). The organic acids studied were: oxalic, malonic, glutaric, oleic and stearic. The CCN properties of the highly soluble acids – oxalic, malonic and glutaric – match very closely Kohler theory predictions which assume full dissolution of the dry particle and a surface tension of the growing droplet equal to that of water. In particular, for supersaturations between 0.3 and 0.6, agreement between the dry particle diameter which gives 50% activation and that calculated from Kohler theory is to within 3 nm on average. In the course of the experiments, considerable instability of glutaric acid particles was observed as a function of time and there is evidence that they fragment to some degree to smaller particles. Stearic acid and oleic acid, which are both highly insoluble in water, did not activate at supersaturations of 0.6% with dry diameters up to 140 nm. Finally, to validate the performance of the TGDC, we present results for the activation of ammonium sulfate particles that demonstrate good agreement with Kohler theory if solution non-ideality is considered. Our findings support earlier studies in the literature that showed highly soluble organics to be CCN active but insoluble species to be largely inactive.


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