scholarly journals New Particle Formation in the South Aegean Sea during the Etesians: importance for CCN production and cloud droplet number

Author(s):  
P. Kalkavouras ◽  
E. Bossioli ◽  
S. Bezantakos ◽  
A. Bougiatioti ◽  
N. Kalivitis ◽  
...  

Abstract. We examine the concentration levels and size distribution of submicron aerosol particles along with the concentration of trace gases and meteorological variables over the central (Santorini) and south Aegean Sea (Crete) from 15 to 28 July 2013, a period that includes Etesian events and moderate northern winds. Particle nucleation bursts were recorded during the Etesian flow at both stations, with those observed at Santorini reaching up to 1.5 × 104 particles cm−3. On Crete (at Finokalia station), the fraction of nucleation-mode particles was diminished, but a higher number of Aitken-mode was observed as a result of the downward mixing and photochemistry. Aerosol and photochemical pollutants covaried throughout the measurement period: lower concentrations were observed during the period of strong Etesian flow (e.g. 43–70 ppbv for ozone, 1.5–5.7 μg m−3 for sulfate), but were substantially enhanced during the period of moderate winds (i.e., increase of up to 32 % for ozone, and 140 % for sulfate). To understand how new particle formation (NPF) affects cloud formation, we quantify its impact on the CCN levels and cloud droplet number concentration. We find that NPF can double CCN number (at 0.1 % supersaturation) but the resulting strong competition for water vapor in cloudy updrafts decreases maximum supersaturation by 14 % and augments the potential droplet number only by 12 %. Therefore, although NPF events may strongly elevate CCN numbers, the relative impacts on cloud droplet number (compared to pre-event levels) is eventually limited by water vapor availability and depends on the prevailing cloud formation dynamics and the aerosol levels associated with the background in the region.

2017 ◽  
Vol 17 (1) ◽  
pp. 175-192 ◽  
Author(s):  
Panayiotis Kalkavouras ◽  
Elissavet Bossioli ◽  
Spiros Bezantakos ◽  
Aikaterini Bougiatioti ◽  
Nikos Kalivitis ◽  
...  

Abstract. This study examines how new particle formation (NPF) in the eastern Mediterranean in summer affects CCN (cloud condensation nuclei) concentrations and cloud droplet formation. For this, the concentration and size distribution of submicron aerosol particles, along with the concentration of trace gases and meteorological variables, were studied over the central (Santorini) and southern Aegean Sea (Finokalia, Crete) from 15 to 28 July 2013, a period that includes Etesian events and moderate northern surface winds. Particle nucleation bursts were recorded during the Etesian flow at both stations, with those observed at Santorini reaching up to 1.5  ×  104 particles cm−3; the fraction of nucleation-mode particles over Crete was relatively diminished, but a higher number of Aitken-mode particles were observed as a result of aging. Aerosol and photochemical pollutants covaried throughout the measurement period; lower concentrations were observed during the period of Etesian flow (e.g., 43–70 ppbv for ozone and 1.5–5.7 µg m−3 for sulfate) but were substantially enhanced during the period of moderate surface winds (i.e., increase of up to 32 for ozone and 140 % for sulfate). We find that NPF can double CCN number (at 0.1 % supersaturation), but the resulting strong competition for water vapor in cloudy updrafts decreases maximum supersaturation by 14 % and augments the potential droplet number only by 12 %. Therefore, although NPF events may strongly elevate CCN numbers, the relative impacts on cloud droplet number (compared to pre-event levels) is eventually limited by water vapor availability and depends on the prevailing cloud formation dynamics and the aerosol levels associated with the background of the region.


2021 ◽  
Vol 21 (18) ◽  
pp. 14293-14308
Author(s):  
Sihui Jiang ◽  
Fang Zhang ◽  
Jingye Ren ◽  
Lu Chen ◽  
Xing Yan ◽  
...  

Abstract. The effect of new particle formation (NPF) on cloud condensation nuclei (CCN) varies widely in diverse environments. CCN or cloud droplets from NPF sources remain highly uncertain in the urban atmosphere; they are greatly affected by the high background aerosols and frequent local emissions. In this study, we quantified the effect of NPF on cloud droplet number concentration (CDNC, or Nd) at typical updraft velocities (V) in clouds based on field observations on 25 May–18 June 2017 in urban Beijing. We show that NPF increases the Nd by 32 %–40 % at V=0.3–3 m s−1 during the studied period. The Nd is reduced by 11.8 ± 5.0 % at V=3 m s−1 and 19.0 ± 4.5 % at V=0.3 m s−1 compared to that calculated from constant supersaturations due to the water vapor competition effect, which suppresses the cloud droplet formation by decreasing the environmental maximum supersaturation (Smax). The effect of water vapor competition becomes smaller at larger V that can provide more sufficient water vapor. However, under extremely high aerosol particle number concentrations, the effect of water vapor competition becomes more pronounced. As a result, although a larger increase of CCN-sized particles by NPF events is derived on clean NPF days when the number concentration of preexisting background aerosol particles is very low, no large discrepancy is presented in the enhancement of Nd by NPF between clean and polluted NPF days. We finally reveal a considerable impact of the primary sources on the evaluation of the contribution of NPF to CCN number concentration (NCCN) and Nd based on a case study. Our study highlights the importance of full consideration of both the environmental meteorological conditions and multiple sources (i.e., secondary and primary) to evaluate the effect of NPF on clouds and the associated climate effects in polluted regions.


2015 ◽  
Vol 15 (21) ◽  
pp. 12283-12313 ◽  
Author(s):  
A. Lupascu ◽  
R. Easter ◽  
R. Zaveri ◽  
M. Shrivastava ◽  
M. Pekour ◽  
...  

Abstract. Accurate representation of the aerosol lifecycle requires adequate modeling of the particle number concentration and size distribution in addition to their mass, which is often the focus of aerosol modeling studies. This paper compares particle number concentrations and size distributions as predicted by three empirical nucleation parameterizations in the Weather Research and Forecast coupled with chemistry (WRF-Chem) regional model using 20 discrete size bins ranging from 1 nm to 10 μm. Two of the parameterizations are based on H2SO4, while one is based on both H2SO4 and organic vapors. Budget diagnostic terms for transport, dry deposition, emissions, condensational growth, nucleation, and coagulation of aerosol particles have been added to the model and are used to analyze the differences in how the new particle formation parameterizations influence the evolving aerosol size distribution. The simulations are evaluated using measurements collected at surface sites and from a research aircraft during the Carbonaceous Aerosol and Radiative Effects Study (CARES) conducted in the vicinity of Sacramento, California. While all three parameterizations captured the temporal variation of the size distribution during observed nucleation events as well as the spatial variability in aerosol number, all overestimated by up to a factor of 2.5 the total particle number concentration for particle diameters greater than 10 nm. Using the budget diagnostic terms, we demonstrate that the combined H2SO4 and low-volatility organic vapor parameterization leads to a different diurnal variability of new particle formation and growth to larger sizes compared to the parameterizations based on only H2SO4. At the CARES urban ground site, peak nucleation rates are predicted to occur around 12:00 Pacific (local) standard time (PST) for the H2SO4 parameterizations, whereas the highest rates were predicted at 08:00 and 16:00 PST when low-volatility organic gases are included in the parameterization. This can be explained by higher anthropogenic emissions of organic vapors at these times as well as lower boundary-layer heights that reduce vertical mixing. The higher nucleation rates in the H2SO4-organic parameterization at these times were largely offset by losses due to coagulation. Despite the different budget terms for ultrafine particles, the 10–40 nm diameter particle number concentrations from all three parameterizations increased from 10:00 to 14:00 PST and then decreased later in the afternoon, consistent with changes in the observed size and number distribution. We found that newly formed particles could explain up to 20–30 % of predicted cloud condensation nuclei at 0.5 % supersaturation, depending on location and the specific nucleation parameterization. A sensitivity simulation using 12 discrete size bins ranging from 1 nm to 10 μm diameter gave a reasonable estimate of particle number and size distribution compared to the 20 size bin simulation, while reducing the associated computational cost by ~ 36 %.


2021 ◽  
Author(s):  
Sihui Jiang ◽  
Fang Zhang ◽  
Jingye Ren ◽  
Lu Chen ◽  
Xing Yan ◽  
...  

Abstract. New particle formation (NPF) is a large source of cloud condensation nuclei (CCN) and cloud droplet in the troposphere. In this study, we quantified the contribution of NPF to cloud droplet number concentration (CDNC, or Nd) at typical updraft velocities (V) in clouds using a field campaign data of aerosol number size distribution and chemical composition observed on May 25–June 18, 2017 in urban Beijing. We show that the NPF drives the variations of CCN and cloud droplet and increases Nd by 30–33 % at V = 0.3–3 m s−1 in urban atmosphere. A markedly reduction in Nd is observed due to water vapor competition with consideration of actual environmental updraft velocity, decreasing by 11.8 ± 5.0 % at V = 3 m s−1 and 19.0 ± 4.5 % at V = 0.3 m s−1 compared to that from a prescribed supersaturation. The effect of water vapor competition becomes smaller at larger V that can provide more sufficient water vapor. Essentially, water vapor competition led to the reduction in Nd by decreasing the environmental maximum supersaturation (Smax) for the activation of aerosol particles. It is shown that Smax was decreased by 14.5–11.7 % for V = 0.3–3 m s−1. Particularly, the largest suppression of cloud droplet formation due to the water vapor competition is presented at extremely high aerosol particle number concentrations. As a result, although a larger increase of CCN-size particles by NPF event is derived on clean NPF day when pre-existing background aerosol particles are very low, there is no large discrepancy in the enhancement of Nd by NPF between the clean and polluted NPF day. We finally show a considerable impact of the primary sources when evaluating the NPF contribution to cloud droplet based on a case study. Our study highlights the importance of fully consideration of both the environmental meteorological conditions and multiple sources (i.e. secondary and primary) to evaluate the NPF effect on clouds and the associated climate effects in polluted regions.


2015 ◽  
Vol 15 (2) ◽  
pp. 2305-2353 ◽  
Author(s):  
J. Größ ◽  
W. Birmili ◽  
A. Hamed ◽  
A. Sonntag ◽  
A. Wiedensohler ◽  
...  

Abstract. This paper revisits the atmospheric new particle formation (NPF) process in the polluted Central European troposphere, focusing on the diurnal evolution of the meteorological and gas phase parameters involved. Atmospheric aerosol observations include Neutral cluster and Air Ion Spectrometer (NAIS) measurements at the research station Melpitz, East Germany between 2008 and 2011. Particle formation events were classified by a new automated method based on the convolution integral of particle number concentration in the diameter range 2–20 nm. To study the relationship with gaseous precursors, a proximity measure was calculated for the sulfuric acid concentration on the basis of a one month intensive measurement campaign in May 2008. A major result was that the number concentration of fresh produced neutral particles correlated significantly with the amount of sulfur dioxide available as a main precursor of sulfuric acid. The condensation sink, a factor potentially inhibiting NPF events, played a subordinate role only. The same held for experimentally determined ammonia concentrations, which also represent a recognised precursor of aerosol particle nucleation. The analysis of meteorological parameters confirmed the absolute need for solar radiation to induce NPF events, and demonstrated the presence of significant turbulence during those events. Due to its tight correlation with solar radiation, however, an independent effect of turbulence for NPF could not be established with certainty. On the basis of observed diurnal cycles of aerosol, gas phase, and meteorological parameters near the ground, we conclude that particle formation is likely to be induced aloft, rather than near the ground.


2019 ◽  
Vol 19 (9) ◽  
pp. 6185-6203 ◽  
Author(s):  
Panayiotis Kalkavouras ◽  
Aikaterini Bougiatioti ◽  
Nikos Kalivitis ◽  
Iasonas Stavroulas ◽  
Maria Tombrou ◽  
...  

Abstract. A significant fraction of atmospheric particles that serve as cloud condensation nuclei (CCN) are thought to originate from the condensational growth of new particle formation (NPF) from the gas phase. Here, 7 years of continuous aerosol and meteorological measurements (June 2008 to May 2015) at a remote background site of the eastern Mediterranean were recorded and analyzed to assess the impact of NPF (of 162 episodes identified) on CCN and cloud droplet number concentration (CDNC) formation in the region. A new metric is introduced to quantitatively determine the initiation and duration of the influence of NPF on the CCN spectrum. NPF days were found to increase CCN concentrations (from 0.10 % to 1.00 % supersaturation) between 29 % and 77 %. Enhanced CCN concentrations from NPF are mostly observed, as expected, under low preexisting particle concentrations and occur in the afternoon, relatively later in the winter and autumn than in the summer. Potential impacts of NPF on cloud formation were quantified by introducing the observed aerosol size distributions and chemical composition into an established cloud droplet parameterization. We find that the supersaturations that develop are very low (ranging between 0.03 % and 0.27 %) for typical boundary layer dynamics (σw ∼0.3 m s−1) and NPF is found to enhance CDNC by a modest 13 %. This considerable contrast between CCN and CDNC response is in part from the different supersaturation levels considered, but also because supersaturation drops from increasing CCN because of water vapor competition effects during the process of droplet formation. The low cloud supersaturation further delays the appearance of NPF impacts on CDNC to clouds formed in the late evening and nighttime – which has important implications for the extent and types of indirect effects induced by NPF events. An analysis based on CCN concentrations using prescribed supersaturation can provide very different, even misleading, conclusions and should therefore be avoided. The proposed approach here offers a simple, yet highly effective way for a more realistic impact assessment of NPF events on cloud formation.


2013 ◽  
Vol 13 (24) ◽  
pp. 12495-12506 ◽  
Author(s):  
Z. B. Wang ◽  
M. Hu ◽  
J. Y. Sun ◽  
Z. J. Wu ◽  
D. L. Yue ◽  
...  

Abstract. Long-term measurements of particle number size distributions were carried out both at an urban background site (Peking University, PKU) and a regional Global Atmospheric Watch station (Shangdianzi, SDZ) from March to November in 2008. In total, 52 new particle formation (NPF) events were observed simultaneously at both sites, indicating that this is a regional phenomenon in the North China Plain. On average, the mean condensation sink value before the nucleation events started was 0.025 s−1 in the urban environment, which was 1.6 times higher than that at regional site. However, higher particle formation and growth rates were observed at PKU (10.8 cm−3 s−1 and 5.2 nm h−1) compared with those at SDZ (4.9 cm−3 s−1 and 4.0 nm h−1). These results implied that precursors were much more abundant in the polluted urban environment. Different from the observations in cleaner environments, the background conditions of the observed particle homogeneous nucleation events in the North China Plain could be characterized as the co-existing of a stronger source of precursor gases and a higher condensational sink of pre-existing aerosol particles. Secondary aerosol formation following nucleation events results in an increase of particle mass concentration, particle light scattering coefficient, and cloud condensation nuclei (CCN) number concentration, with consequences on visibility, radiative effects, and air quality. Typical regional NPF events with significant particle nucleation rates and subsequent particle growth over a sufficiently long time period at both sites were chosen to investigate the influence of NPF on the number concentration of "potential" CCN. As a result, the NPF and the subsequent condensable growth increased the CCN number concentration in the North China Plain by factors in the range from 5.6 to 8.7. Moreover, the potential contribution of anthropogenic emissions to the CCN number concentration was more than 50%, to which more attention should be drawn in regional and global climate modeling, especially in the polluted urban areas.


2019 ◽  
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 have been done 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 of 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. It 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 on Arctic cloud formation.


2015 ◽  
Vol 15 (14) ◽  
pp. 19729-19801
Author(s):  
A. Lupascu ◽  
R. Easter ◽  
R. Zaveri ◽  
M. Shrivastava ◽  
M. Pekour ◽  
...  

Abstract. Accurate representation of the aerosol lifecycle requires adequate modeling of the particle number concentration and size distribution in addition to their mass, which is often the focus of aerosol modeling studies. This paper compares particle number concentrations and size distributions as predicted by three empirical nucleation parameterizations in the Weather Research and Forecast coupled with chemistry (WRF-Chem) regional model using 20 discrete size bins ranging from 1 nm to 10 μm. Two of the parameterizations are based on H2SO4 while one is based on both H2SO4 and organic vapors. Budget diagnostic terms for transport, dry deposition, emissions, condensational growth, nucleation, and coagulation of aerosol particles have been added to the model and are used to analyze the differences in how the new particle formation parameterizations influence the evolving aerosol size distribution. The simulations are evaluated using measurements collected at surface sites and from a research aircraft during the Carbonaceous Aerosol and Radiative Effects Study (CARES) conducted in the vicinity of Sacramento, California. While all three parameterizations captured the temporal variation of the size distribution during observed nucleation events as well as the spatial variability in aerosol number, all overestimated by up to a factor of 2.5 the total particle number concentration for particle diameters greater than 10 nm. Using the budget diagnostic terms, we demonstrate that the combined H2SO4 and low-volatility organic vapors parameterization leads to a different diurnal variability of new particle formation and growth to larger sizes compared to the parameterizations based on only H2SO4. At the CARES urban ground site, peak nucleation rates were predicted to occur around 12:00 Pacific (local) standard time (PST) for the H2SO4 parameterizations, whereas the highest rates were predicted at 08:00 and 16:00 PST when low-volatility organic gases are included in the parameterization. This can be explained by higher anthropogenic emissions of organic vapors at these times as well as lower boundary layer heights that reduce vertical mixing. The higher nucleation rates in the H2SO4-organic parameterization at these times were largely offset by losses due to coagulation. Despite the different budget terms for ultrafine particles, the 10–40 nm diameter particle number concentrations from all three parameterizations increased from 10:00 to 14:00 PST and then decreased later in the afternoon, consistent with changes in the observed size and number distribution. Differences among the three simulations for the 40–100 nm particle diameter range are mostly associated with the timing of the peak total tendencies that shift the morning increase and afternoon decrease in particle number concentration by up to two hours. We found that newly formed particles could explain up to 20–30 % of predicted cloud condensation nuclei at 0.5 % supersaturation, depending on location and the specific nucleation parameterization. A sensitivity simulation using 12 discrete size bins ranging from 1 nm to 10 μm diameter gave a reasonable estimate of particle number and size distribution compared to the 20 size bin simulation, while reducing the associated computational cost by ∼ 36 %.


2011 ◽  
Vol 11 (15) ◽  
pp. 7701-7713 ◽  
Author(s):  
R. H. H. Janssen ◽  
L. N. Ganzeveld ◽  
P. Kabat ◽  
M. Kulmala ◽  
T. Nieminen ◽  
...  

Abstract. Seasonal variations in cloud droplet number concentration (NCD) in low-level stratiform clouds over the boreal forest are estimated from MODIS observations of cloud optical and microphysical properties, using a sub-adiabatic cloud model to interpret vertical profiles of cloud properties. An uncertainty analysis of the cloud model is included to reveal the main sensitivities of the cloud model. We compared the seasonal cycle in NCD, obtained using 9 yr of satellite data, to surface concentrations of potential cloud activating aerosols, measured at the SMEAR II station at Hyytiälä in Finland. The results show that NCD and cloud condensation nuclei (CCN) concentrations have no clear correlation at seasonal time scale. The fraction of aerosols that actually activate as cloud droplet decreases sharply with increasing aerosol concentrations. Furthermore, information on the stability of the atmosphere shows that low NCD is linked to stable atmospheric conditions. Combining these findings leads to the conclusion that cloud droplet activation for the studied clouds over the boreal forest is limited by convection. Our results suggest that it is important to take the strength of convection into account when studying the influence of aerosols from the boreal forest on cloud formation, although they do not rule out the possibility that aerosols from the boreal forest affect other types of clouds with a closer coupling to the surface.


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