scholarly journals Airborne measurements of new particle formation in the free troposphere above the Mediterranean Sea during the HYMEX campaign

2015 ◽  
Vol 15 (17) ◽  
pp. 10203-10218 ◽  
Author(s):  
C. Rose ◽  
K. Sellegri ◽  
E. Freney ◽  
R. Dupuy ◽  
A. Colomb ◽  
...  
Keyword(s):  
Mediterranean Sea ◽  
Hydrological Cycle ◽  
Particle Growth ◽  
Particle Formation ◽  
Free Troposphere ◽  
New Particle Formation ◽  
Scanning Mobility Particle Sizer ◽  
Air Mass ◽  
Airborne Measurements ◽  
The Mediterranean

Abstract. While atmospheric new particle formation (NPF) has been observed in various environments and was found to contribute significantly to the total aerosol particle concentration, the production of new particles over open seas is poorly documented in the literature. Nucleation events were detected and analysed over the Mediterranean Sea using two condensation particle counters and a scanning mobility particle sizer on board the ATR-42 research aircraft during flights conducted between 11 September and 4 November 2012 in the framework of the HYMEX (HYdrological cycle in Mediterranean EXperiment) project. The main purpose of the present work was to characterize the spatial extent of the NPF process, both horizontally and vertically. Our findings show that nucleation is occurring over large areas above the Mediterranean Sea in all air mass types. Maximum concentrations of particles in the size range 5–10 nm (N5–10) do not systematically coincide with lower fetches (time spent by the air mass over the sea before sampling), and significant N5–10 values are found for fetches between 0 and 60 h depending on the air mass type. These observations suggest that nucleation events could be more influenced by local precursors originating from emission processes occurring above the sea, rather than linked to synoptic history. Vertical soundings were performed, giving the opportunity to examine profiles of the N5–10 concentration and to analyse the vertical extent of NPF. Our observations demonstrate that the process could be favoured above 1000 m, i.e. frequently in the free troposphere, and more especially between 2000 and 3000 m, where the NPF frequency is close to 50 %. This vertical distribution of NPF might be favoured by the gradients of several atmospheric parameters, together with the mixing of two air parcels, which could also explain the occurrence of the process at preferential altitudes. In addition, increased condensation sinks collocated with high concentrations of small particles suggest the occurrence of NPF events promoted by inputs from the boundary layer, most probably associated with convective clouds and their outflow. After their formation, particles slowly grow at higher altitudes to diameters of at least 30 nm while not being greatly depleted or affected by coagulation. Our analysis of the particle size distributions suggests that particle growth could decrease with increasing altitude.

scholarly journals Airborne measurements of new particle formation in the free troposphere above the Mediterranean Sea during the HYMEX campaign

2015 ◽  
Vol 15 (6) ◽  
pp. 8151-8189 ◽  
Author(s):  
C. Rose ◽  
K. Sellegri ◽  
E. Freney ◽  
R. Dupuy ◽  
A. Colomb ◽  
...  
Keyword(s):  
High Altitude ◽  
Mediterranean Sea ◽  
Hydrological Cycle ◽  
Particle Formation ◽  
Free Troposphere ◽  
New Particle Formation ◽  
Scanning Mobility Particle Sizer ◽  
Air Mass ◽  
Airborne Measurements ◽  
The Mediterranean

Abstract. While atmospheric new particle formation (NPF) has been observed in various environments and was found to contribute significantly to the total aerosol particle concentration, the production of new particles over open seas is poorly documented in the literature. Nucleation events were detected and analysed over the Mediterranean Sea using two condensation particle counters and a Scanning Mobility Particle Sizer on-board the ATR-42 research aircraft during flights conducted between the 11 September and the 4 November 2012 in the framework of the HYMEX (HYdrological cycle in Mediterranean EXperiment) project. The main purpose of the present work was to characterize the spatial extent of the NPF process. Our findings show that nucleation is occurring over large areas above the Mediterranean Sea in all air mass types. Maximum concentrations of particles in the size range 5–10 nm (N5–10) do not systematically coincide with lower fetches (time spent by the air mass over the sea before sampling), and significant N5–10 values are found for fetches between 0 and 60 h depending on the air mass type. These observations suggest that nucleation events could be more influenced by processes occurring above the sea, rather than linked to synoptic history. The analysis of the vertical extent of nucleation demonstrates that the process is favoured at high altitude, above 1000 m, i.e. frequently in the free troposphere, and more especially between 2000 and 3000 m, where the nucleation frequency is close to 50%. This vertical distribution of nucleation is favoured by the gradients of several parameters, such as the condensation sink, the temperature and the relative humidity. The mixing of two air parcels could also explain the occurrence of nucleation at preferential altitudes. After they formed, particles slowly grow at high altitude to diameters of at least 30 nm while being poorly depleted by coagulation processes. Our analysis of the particle size distributions suggests that particle growth could decrease with increasing altitudes.

scholarly journals CCN production by new particle formation in the free troposphere

2017 ◽  
Vol 17 (2) ◽  
pp. 1529-1541 ◽  
Author(s):  
Clémence Rose ◽  
Karine Sellegri ◽  
Isabel Moreno ◽  
Fernando Velarde ◽  
Michel Ramonet ◽  
...  
Keyword(s):  
Particle Number ◽  
Particle Growth ◽  
Particle Formation ◽  
Number Concentration ◽  
Particle Number Concentration ◽  
Free Troposphere ◽  
New Particle Formation ◽  
Data Set ◽  
Radiative Processes ◽  
The Impact

Abstract. Global models predict that new particle formation (NPF) is, in some environments, responsible for a substantial fraction of the total atmospheric particle number concentration and subsequently contributes significantly to cloud condensation nuclei (CCN) concentrations. NPF events were frequently observed at the highest atmospheric observatory in the world, on Chacaltaya (5240 m a.s.l.), Bolivia. The present study focuses on the impact of NPF on CCN population. Neutral cluster and Air Ion Spectrometer and mobility particle size spectrometer measurements were simultaneously used to follow the growth of particles from cluster sizes down to ∼ 2 nm up to CCN threshold sizes set to 50, 80 and 100 nm. Using measurements performed between 1 January and 31 December 2012, we found that 61 % of the 94 analysed events showed a clear particle growth and significant enhancement of the CCN-relevant particle number concentration. We evaluated the contribution of NPF, relative to the transport and growth of pre-existing particles, to CCN size. The averaged production of 50 nm particles during those events was 5072, and 1481 cm−3 for 100 nm particles, with a larger contribution of NPF compared to transport, especially during the wet season. The data set was further segregated into boundary layer (BL) and free troposphere (FT) conditions at the site. The NPF frequency of occurrence was higher in the BL (48 %) compared to the FT (39 %). Particle condensational growth was more frequently observed for events initiated in the FT, but on average faster for those initiated in the BL, when the amount of condensable species was most probably larger. As a result, the potential to form new CCN was higher for events initiated in the BL (67 % against 53 % in the FT). In contrast, higher CCN number concentration increases were found when the NPF process initially occurred in the FT, under less polluted conditions. This work highlights the competition between particle growth and the removal of freshly nucleated particles by coagulation processes. The results support model predictions which suggest that NPF is an effective source of CCN in some environments, and thus may influence regional climate through cloud-related radiative processes.

scholarly journals New Particle Formation and impact on CCN concentrations in the boundary layer and free troposphere at the high altitude station of Chacaltaya (5240 m a.s.l.), Bolivia

2016 ◽  
Author(s):  
C. Rose ◽  
K. Sellegri ◽  
I. Moreno ◽  
F. Velarde ◽  
M. Ramonet ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Particle Number ◽  
Particle Growth ◽  
Particle Formation ◽  
Number Concentration ◽  
Particle Number Concentration ◽  
Free Troposphere ◽  
New Particle Formation ◽  
Radiative Processes ◽  
The Impact

Abstract. Global models predict that new particle formation (NPF) is, in some environments, responsible for a substantial fraction of the total atmospheric particle number concentration and subsequently contribute significantly to cloud condensation nuclei (CCN) concentrations. NPF events were frequently observed at the highest atmospheric observatory in the world, Chacaltaya (5240 m a.s.l.), Bolivia. The present study focuses on the impact of NPF on CCN population. Neutral cluster and Air Ion Spectrometer and mobility particle size spectrometer measurements were simultaneously used to follow the growth of particles from cluster sizes down to ~ 2 nm up to CCN threshold sizes set to 50, 80 and 100 nm. Using measurements performed between January 1 and December 31 2012, we found that 61% of the 94 analysed events showed a clear particle growth and significant enhancement of the CCN-relevant particle number concentration. We evaluated the contribution of NPF events relative to the transport of pre-existing particles to the site. The averaged production of 50 nm particles during those events was 5072 cm−3, and 1481 cm−3 for 100 nm particles, with a larger contribution of NPF compared to transport, especially during the wet season. The data set was further segregated into boundary layer (BL) and free troposphere (FT) conditions at the site. The NPF frequency of occurrence was higher in the BL (48 %) compared to the FT (39 %). Particle condensational growth was more frequently observed for events initiated in the FT, but on average faster for those initiated in the BL, when the amount of condensable species was most probably larger. As a result, the potential to form new CCN was higher for events initiated in the BL (67 % against 56 % in the FT). In contrast, higher CCN number concentration increases were found when the NPF process initially occurred in the FT, under less polluted conditions. This work highlights the competition between particle growth and the removal of freshly nucleated particles by coagulation processes. The results support model predictions which suggest that NPF is an effective source of CCN in some environments, and thus may influence regional climate through cloud related radiative processes.

scholarly journals New particle formation in air mass transported between two measurement sites in Northern Finland

2005 ◽  
Vol 5 (6) ◽  
pp. 11929-11963 ◽  
Author(s):  
M. Komppula ◽  
S.-L. Sihto ◽  
H. Korhonen ◽  
H. Lihavainen ◽  
V.-M. Kerminen ◽  
...  
Keyword(s):  
Growth Rates ◽  
Particle Growth ◽  
Particle Formation ◽  
Distribution Data ◽  
New Particle Formation ◽  
Air Mass ◽  
Air Masses ◽  
Aerosol Dynamics ◽  
Almost All ◽  
Distinct Features

Abstract. This study covers four years of aerosol number size distribution data from Pallas and Värriö sites 250 km apart from each other in Northern Finland and compares new particle formation events between these sites. In eastern air masses almost all events were observed to start earlier at the eastern station Värriö, whereas in western air masses most of the events were observed to start earlier at the western station Pallas. This demonstrates that particle formation in a certain air mass type depends not only on the diurnal variation of the parameters causing the phenomenon (such as photochemistry) but also on some properties carried by the air mass itself. The correlation in growth rates between the two sites was relatively good, which suggests that the amount of condensable vapour causing the growth must have been at about the same level in both sites. The value of condensation sink was frequently much higher at the downwind station. It seems that secondary particle formation related to biogenic sources dominate in many cases over the particle sinks during the air mass transport between the sites. Two cases of transport from Pallas to Värriö were further analysed with an aerosol dynamics model. The model was able to reproduce the observed nucleation events 250 km down-wind at Värriö but revealed some differences between the two cases. The simulated nucleation rates were in both cases similar but the organic concentration profiles that best reproduced the observations were different in the two cases indicating that divergent formation reactions may dominate under different conditions. The simulations also suggested that organic compounds were the main contributor to new particle growth, which offers a tentative hypothesis to the distinct features of new particles at the two sites: Air masses arriving from Atlantic Ocean typically spent approximately only ten hours over land before arriving at Pallas, and thus the time for the organic vapours to accumulate in the air and to interact with the particles is relatively short. This can lead to low nucleation mode growth rates and even to suppression of detectable particle formation event due to efficient scavenging of newly formed clusters, as was observed in the case studies.

scholarly journals Spatial extent of new particle formation events over the Mediterranean Basin from multiple ground-based and airborne measurements

2017 ◽  
Vol 17 (15) ◽  
pp. 9567-9583 ◽  
Author(s):  
Kevin Berland ◽  
Clémence Rose ◽  
Jorge Pey ◽  
Anais Culot ◽  
Evelyn Freney ◽  
...  
Keyword(s):  
Size Distribution ◽  
Regional Scale ◽  
Particle Formation ◽  
Spatial Extent ◽  
Aerosol Size Distribution ◽  
Spatial And Temporal Variability ◽  
New Particle Formation ◽  
Airborne Measurements ◽  
Synoptic Conditions ◽  
The Mediterranean

Abstract. Over the last two decades, new particle formation (NPF), i.e., the formation of new particle clusters from gas-phase compounds followed by their growth to the 10–50 nm size range, has been extensively observed in the atmosphere at a given location, but their spatial extent has rarely been assessed. In this work, we use aerosol size distribution measurements performed simultaneously at Ersa (Corsica) and Finokalia (Crete) over a 1-year period to analyze the occurrence of NPF events in the Mediterranean area. The geographical location of these two sites, as well as the extended sampling period, allows us to assess the spatial and temporal variability in atmospheric nucleation at a regional scale. Finokalia and Ersa show similar seasonalities in the monthly average nucleation frequencies, growth rates, and nucleation rates, although the two stations are located more than 1000 km away from each other. Within this extended period, aerosol size distribution measurements were performed during an intensive campaign (3 July to 12 August 2013) from a ground-based station on the island of Mallorca, as well as onboard the ATR-42 research aircraft. This unique combination of stationary and mobile measurements provides us with detailed insights into the horizontal and vertical development of the NPF process on a daily scale. During the intensive campaign, nucleation events occurred simultaneously both at Ersa and Mallorca over delimited time slots of several days, but different features were observed at Finokalia. The results show that the spatial extent of the NPF events over the Mediterranean Sea might be as large as several hundreds of kilometers, mainly determined by synoptic conditions. Airborne measurements gave additional information regarding the origin of the clusters detected above the sea. The selected cases depicted contrasting situations, with clusters formed in the marine boundary layer or initially nucleated above the continent or in the free troposphere (FT) and further transported above the sea.

scholarly journals Aerosol spectral optical depths and size characteristics at a coastal industriallocation in India - effect of synoptic and mesoscale weather

2004 ◽  
Vol 22 (6) ◽  
pp. 1851-1860 ◽  
Author(s):  
K. Niranjan ◽  
B. Malleswara Rao ◽  
A. Saha ◽  
K. S. R. Murty
Keyword(s):  
Wind Speed ◽  
Size Range ◽  
Surface Wind ◽  
Particle Growth ◽  
Particle Formation ◽  
Size Distributions ◽  
New Particle Formation ◽  
Atmospheric Humidity ◽  
Air Mass ◽  
Micron Size

Abstract. The aerosol spectral optical depths at ten discrete channels in the visible and near IR bands, obtained from a ground-based passive multi-wavelength solar radiometer at a coastal industrial location, Visakhapatnam, on the east coast of India, are used to study the response of the aerosol optical properties and size distributions to the changes in atmospheric humidity, wind speed and direction. It is observed that during high humidity conditions, the spectral optical depths show about 30% higher growth factors, and the size distributions show the generation of a typical new mode around 0.4 microns. The surface wind speed and direction also indicate the formation of new particles when the humid marine air mass interacts with the industrial air mass. This is interpreted in terms of new particle formation and subsequent particle growth by condensation and self-coagulation. The results obtained on the surface-size segregated aerosol mass distribution from a co-located Quartz Crystal Microbalance during different humidity conditions also show a large mass increase in the sub-micron size range with an increase in atmospheric humidity, indicating new particle formation at the sub-micron size range.

scholarly journals New particle formation in air mass transported between two measurement sites in Northern Finland

2006 ◽  
Vol 6 (10) ◽  
pp. 2811-2824 ◽  
Author(s):  
M. Komppula ◽  
S.-L. Sihto ◽  
H. Korhonen ◽  
H. Lihavainen ◽  
V.-M. Kerminen ◽  
...  
Keyword(s):  
Growth Rates ◽  
Particle Growth ◽  
Particle Formation ◽  
Distribution Data ◽  
New Particle Formation ◽  
Air Mass ◽  
Air Masses ◽  
Aerosol Dynamics ◽  
Almost All ◽  
Distinct Features

Abstract. This study covers four years of aerosol number size distribution data from Pallas and Värriö sites 250 km apart from each other in Northern Finland and compares new particle formation events between these sites. In air masses of eastern origin almost all events were observed to start earlier at the eastern station Värriö, whereas in air masses of western origin most of the events were observed to start earlier at the western station Pallas. This demonstrates that particle formation in a certain air mass type depends not only on the diurnal variation of the parameters causing the phenomenon (such as photochemistry) but also on some properties carried by the air mass itself. The correlation in growth rates between the two sites was relatively good, which suggests that the amount of condensable vapour causing the growth must have been at about the same level in both sites. The condensation sink was frequently much higher at the downwind station. It seems that secondary particle formation related to biogenic sources dominate in many cases over the particle sinks during the air mass transport between the sites. Two cases of transport from Pallas to Värriö were further analysed with an aerosol dynamics model. The model was able to reproduce the observed nucleation events 250 km down-wind at Värriö but revealed some differences between the two cases. The simulated nucleation rates were in both cases similar but the organic concentration profiles that best reproduced the observations were different in the two cases indicating that divergent formation reactions may dominate under different conditions. The simulations also suggested that organic compounds were the main contributor to new particle growth, which offers a tentative hypothesis to the distinct features of new particles at the two sites: Air masses arriving from the Atlantic Ocean typically spent approximately only ten hours over land before arriving at Pallas, and thus the time for the organic vapours to accumulate in the air and to interact with the particles is relatively short. This can lead to low nucleation mode growth rates and even to suppression of detectable particle formation event due to efficient scavenging of newly formed clusters, as was observed in the case studies.

scholarly journals Modelling studies of HOMs and their contributions to new particle formation and growth: comparison of boreal forest in Finland and a polluted environment in China

2018 ◽  
Vol 18 (16) ◽  
pp. 11779-11791 ◽  
Author(s):  
Ximeng Qi ◽  
Aijun Ding ◽  
Pontus Roldin ◽  
Zhengning Xu ◽  
Putian Zhou ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Boreal Forest ◽  
Environmental Conditions ◽  
Eastern China ◽  
Particle Growth ◽  
Particle Formation ◽  
Forest Site ◽  
Polluted Environment ◽  
New Particle Formation ◽  
Multifunctional Compounds

Abstract. Highly oxygenated multifunctional compounds (HOMs) play a key role in new particle formation (NPF), but their quantitative roles in different environments of the globe have not been well studied yet. Frequent NPF events were observed at two “flagship” stations under different environmental conditions, i.e. a remote boreal forest site (SMEAR II) in Finland and a suburban site (SORPES) in polluted eastern China. The averaged formation rate of 6 nm particles and the growth rate of 6–30 nm particles were 0.3 cm−3 s−1 and 4.5 nm h−1 at SMEAR II compared to 2.3 cm−3 s−1 and 8.7 nm h−1 at SORPES, respectively. To explore the differences of NPF at the two stations, the HOM concentrations and NPF events at two sites were simulated with the MALTE-BOX model, and their roles in NPF and particle growth in the two distinctly different environments are discussed. The model provides an acceptable agreement between the simulated and measured concentrations of sulfuric acid and HOMs at SMEAR II. The sulfuric acid and HOM organonitrate concentrations are significantly higher but other HOM monomers and dimers from monoterpene oxidation are lower at SORPES compared to SMEAR II. The model simulates the NPF events at SMEAR II with a good agreement but underestimates the growth of new particles at SORPES, indicating a dominant role of anthropogenic processes in the polluted environment. HOMs from monoterpene oxidation dominate the growth of ultrafine particles at SMEAR II while sulfuric acid and HOMs from aromatics oxidation play a more important role in particle growth. This study highlights the distinct roles of sulfuric acid and HOMs in NPF and particle growth in different environmental conditions and suggests the need for molecular-scale measurements in improving the understanding of NPF mechanisms in polluted areas like eastern China.

scholarly journals New particle formation during α- and β-pinene oxidation by O<sub>3</sub>, OH and NO<sub>3</sub>, and the influence of water vapour: particle size distribution studies

2002 ◽  
Vol 2 (2) ◽  
pp. 469-506 ◽  
Author(s):  
B. Bonn ◽  
G. K. Moortgat
Keyword(s):  
Particle Size ◽  
Water Vapour ◽  
Particle Formation ◽  
New Particle Formation ◽  
Oxidation Reactions ◽  
Scanning Mobility Particle Sizer ◽  
Volume Yield ◽  
Influence Of Water ◽  
The Individual ◽  
Aerosol Volume

Abstract. New particle formation during the oxidation of a- and b-pinene (C10H16) by ozone, OH and NO3 was studied by measuring the particle size distributions with a scanning mobility particle sizer (TSI 3936). The results indicate a drastically higher nucleation potential of the ozonolysis than in the reaction with either OH or NO3. On the contrary, the contribution of the individual oxidation reactions to form new aerosol volume was found to depend on the location of the carbon double bond to be oxidized: for the endocyclic a-pinene reactions the ozonolysis contributed mostly to the aerosol volume yield, whereas for the exocyclic b-pinene reactions the oxidation by O3, OH and NO3 yielded a similar aerosol volume. In a second part of this study the influence of water vapour on the nucleation in all three possible oxidation routes was examined. The observations revealed only an effect of water vapour during the ozonolysis reactions.

scholarly journals Quantifying aerosol size distributions and their temporal variability in the Southern Great Plains, USA

2019 ◽  
Vol 19 (18) ◽  
pp. 11985-12006 ◽  
Author(s):  
Peter J. Marinescu ◽  
Ezra J. T. Levin ◽  
Don Collins ◽  
Sonia M. Kreidenweis ◽  
Susan C. van den Heever
Keyword(s):  
Size Distribution ◽  
Great Plains ◽  
Diurnal Cycle ◽  
Particle Formation ◽  
Aerosol Size Distribution ◽  
Size Distributions ◽  
New Particle Formation ◽  
Scanning Mobility Particle Sizer ◽  
Southern Great Plains ◽  
Particle Sizer

Abstract. A quality-controlled, 5-year dataset of aerosol number size distributions (particles with diameters (Dp) from 7 nm through 14 µm) was developed using observations from a scanning mobility particle sizer, aerodynamic particle sizer, and a condensation particle counter at the Department of Energy's Southern Great Plains (SGP) site. This dataset was used for two purposes. First, typical characteristics of the aerosol size distribution (number, surface area, and volume) were calculated for the SGP site, both for the entire dataset and on a seasonal basis, and size distribution lognormal fit parameters are provided. While the median size distributions generally had similar shapes (four lognormal modes) in all the seasons, there were some significant differences between seasons. These differences were most significant in the smallest particles (Dp<30 nm) and largest particles (Dp>800 nm). Second, power spectral analysis was conducted on this long-term dataset to determine key temporal cycles of total aerosol concentrations, as well as aerosol concentrations in specified size ranges. The strongest cyclic signal was associated with a diurnal cycle in total aerosol number concentrations that was driven by the number concentrations of the smallest particles (Dp<30 nm). This diurnal cycle in the smallest particles occurred in all seasons in ∼50 % of the observations, suggesting a persistent influence of new particle formation events on the number concentrations observed at the SGP site. This finding is in contrast with earlier studies that suggest new particle formation is observed primarily in the springtime at this site. The timing of peak concentrations associated with this diurnal cycle was shifted by several hours depending on the season, which was consistent with seasonal differences in insolation and boundary layer processes. Significant diurnal cycles in number concentrations were also found for particles with Dp between 140 and 800 nm, with peak concentrations occurring in the overnight hours, which were primarily associated with both nitrate and organic aerosol cycles. Weaker cyclic signals were observed for longer timescales (days to weeks) and are hypothesized to be related to the timescales of synoptic weather variability. The strongest periodic signals (3.5–5 and 7 d cycles) for these longer timescales varied depending on the season, with no cyclic signals and the lowest variability in the summer.

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