scholarly journals New particle formation and ultrafine charged aerosol climatology at a high altitude site in the Alps (Jungfraujoch, 3580 m a.s.l., Switzerland)

2010 ◽  
Vol 10 (19) ◽  
pp. 9333-9349 ◽  
Author(s):  
J. Boulon ◽  
K. Sellegri ◽  
H. Venzac ◽  
D. Picard ◽  
E. Weingartner ◽  
...  

Abstract. We investigate the formation and growth of charged aerosols clusters at Jungfraujoch, in the Swiss Alps (3580 m a.s.l.), the highest altitude site of the European EUCAARI project intensive campaign. Charged particles and clusters (0.5–1.8 nm) were measured from April 2008 to April 2009 and allowed the detection of nucleation events in this very specific environment (presence of free tropospheric air and clouds). We found that the naturally charged aerosol concentrations, which are dominated by the cluster size class, shows a strong diurnal pattern likely linked to valley breezes transporting surface layer ion precursors, presumably radon. Cosmic rays were found not to be the major ion source at the measurement site. However, at night, when air masses are more representative of free tropospheric conditions, we found that the cluster concentrations are still high. The charged aerosol size distribution and concentration are strongly influenced by the presence of clouds at the station. Clouds should be taken into account when deriving high altitude nucleation statistics. New particle formation occurs on average 17.5% of the measurement period and shows a weak seasonality with a minimum of frequency during winter, but this seasonality is enhanced when the data set is screened for periods when the atmospheric station is out of clouds. The role of ions in the nucleation process was investigated and we found that the ion-mediated nucleation explains 22.3% of the particle formation. The NPF events frequency is correlated with UV radiation but not with calculated H2SO4 concentrations, suggesting that other compounds such as organic vapors are involved in the nucleation and subsequently growth process. In fact, NPF events frequency also surprisingly increases with the condensational sink (CS), suggesting that at Jungfraujoch, the presence of condensing vapours probably coupled with high CS are driving the occurrence of NPF events. A strong link to the air mass path was also pointed out and events were observed to be frequently occurring in Eastern European air masses, which present the highest condensational sink. In these air masses, pre-existing cluster concentrations are more than three time larger than in other air masses during event days, and no new clusters formation is observed, contrarily to what is happening in other air mass types.

2010 ◽  
Vol 10 (4) ◽  
pp. 11361-11399 ◽  
Author(s):  
J. Boulon ◽  
K. Sellegri ◽  
H. Venzac ◽  
D. Picard ◽  
E. Weingartner ◽  
...  

Abstract. Aerosol nucleation is an important source of atmospheric particles which have an effect both on the climatic system and on human health. The new particle formation (NPF) process is an ubiquitous phenomenon, yet poorly understood despite the many studies performed on this topic using various approaches (observation, experimentation in smog chambers and modeling). In this work, we investigate the formation of secondary charged aerosols and its climatology at Jungfraujoch, a high altitude site in Swiss Alps (3580 m a.s.l.). Charged particles and clusters (0.5–1.8 nm) were measured within the EUCAARI program from April 2008 to April 2009 and allowed the detection of nucleation events. We found that the aerosol concentration, which is dominated by cluster size class, shows a strong diurnal pattern and that the aerosol size distribution and concentration are strongly influenced by the presence of clouds either during daytime or nighttime conditions. New particle formation events have been investigated and it appears that new particle formation occurs 17.5% of measured days and that the nucleation frequency is strongly linked to air mass origin and path and negatively influenced by cloud presence. In fact, we show that NPF events depend on the occurrence of high concentration VOCs air masses which allowed clusters growing by condensation of organic vapors rather than nucleation of new clusters. Furthermore, the contribution of ions to nucleation process was studied and we found that ion-mediated nucleation (IMN) contribute to 26% of the total nucleation so that ions play an important role in the new particle formation and growth at Jungfraujoch.


2005 ◽  
Vol 5 (6) ◽  
pp. 11929-11963 ◽  
Author(s):  
M. Komppula ◽  
S.-L. Sihto ◽  
H. Korhonen ◽  
H. Lihavainen ◽  
V.-M. Kerminen ◽  
...  

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.


2020 ◽  
Author(s):  
Diego Aliaga ◽  
Victoria Sinclair ◽  
Zha Qiaozhi ◽  
Marcos Andrade ◽  
Claudia Mohr ◽  
...  

<p>Measuring aerosol at high altitude sites is useful as it enables sampling of the free troposphere over long time frames. However, in order to draw conclusions from station measurement data, we need to determine which air mass sources are present at any given sampling time. This task is challenging at mountain sites, due to complex topography which in turn drives complex meteorology. Between December 2017 and May 2018, the Southern hemisphere high ALTitude Experiment on particle Nucleation And growth (SALTENA) campaign was conducted at Chacaltaya in Bolivia at 5240 m a.s.l. The data set obtained in this campaign contains records of nearly all relevant aerosol characteristics and aerosol precursors. To identify the source regions of the observed air masses we performed high resolution (down to 1 km) simulations with the Weather Research and Forecasting Model (WRF). The WRF model output is then used to as input to the Lagrangian particle dispersion model (FLEXPART). FLEXPART simulations are initialised every hour and 20 thousand particles are released per hour and track backwards in time for 96 hours. The FLEXPART footprint output is regridded onto a log-polar cylindrical grid where we perform a ‘K-means’ cluster analysis on the 3D cells defined by the grid. The cells are clustered based on the time series of their source receptor relationship (i.e. emission sensitivities), producing regions (clusters) resolved not only in the horizontal but also the vertical domain. Our results show that regions located close to the station (<100km) have a low but persistent influence with diurnal variations and close contact to the surface. Mid-range regions (100-800km) have the highest influence with a higher percentage of air masses from the free troposphere. Long-range regions (>800km) have a higher influence than the short-range regions but lower than the middle-range regions. Most of the air masses from these long-range regions come from the free troposphere. With this method we have successfully resolved the various air mass influences at the measurement site. The high meteorological resolution and the stochastic nature of FLEXPART are seminal for capturing the transport pathways.</p>


2018 ◽  
Vol 18 (2) ◽  
pp. 587-599 ◽  
Author(s):  
Xiaojing Shen ◽  
Junying Sun ◽  
Niku Kivekäs ◽  
Adam Kristensson ◽  
Xiaoye Zhang ◽  
...  

Abstract. In this work, the spatial extent of new particle formation (NPF) events and the relative probability of observing particles originating from different spatial origins around three rural sites in eastern China were investigated using the NanoMap method, using particle number size distribution (PNSD) data and air mass back trajectories. The length of the datasets used were 7, 1.5, and 3 years at rural sites Shangdianzi (SDZ) in the North China Plain (NCP), Mt. Tai (TS) in central eastern China, and Lin'an (LAN) in the Yangtze River Delta region in eastern China, respectively. Regional NPF events were observed to occur with the horizontal extent larger than 500 km at SDZ and TS, favoured by the fast transport of northwesterly air masses. At LAN, however, the spatial footprint of NPF events was mostly observed around the site within 100–200 km. Difference in the horizontal spatial distribution of new particle source areas at different sites was connected to typical meteorological conditions at the sites. Consecutive large-scale regional NPF events were observed at SDZ and TS simultaneously and were associated with a high surface pressure system dominating over this area. Simultaneous NPF events at SDZ and LAN were seldom observed. At SDZ the polluted air masses arriving over the NCP were associated with higher particle growth rate (GR) and new particle formation rate (J) than air masses from Inner Mongolia (IM). At TS the same phenomenon was observed for J, but GR was somewhat lower in air masses arriving over the NCP compared to those arriving from IM. The capability of NanoMap to capture the NPF occurrence probability depends on the length of the dataset of PNSD measurement but also on topography around the measurement site and typical air mass advection speed during NPF events. Thus the long-term measurements of PNSD in the planetary boundary layer are necessary in the further study of spatial extent and the probability of NPF events. The spatial extent, relative probability of occurrence, and typical evolution of PNSD during NPF events presented in this study provide valuable information to further understand the climate and air quality effects of new particle formation.


2020 ◽  
Author(s):  
Juan Andrés Casquero-Vera ◽  
Hassan Lyamani ◽  
Lubna Dada ◽  
Simo Hakala ◽  
Pauli Paasonen ◽  
...  

Abstract. A substantial fraction of the atmospheric aerosols originates from secondary new particle formation (NPF), where atmospheric vapours are transformed into particles that subsequently grow to larger sizes, affecting human health and the climate. In this study, we investigate aerosol size distributions at two stations located close to each other (~ 20 km), but at different altitudes: urban (UGR; 680 m a.s.l.) and high-altitude remote (SNS; 2500 m a.s.l.) site, both in the area of Granada, Spain, and part of AGORA observatory (Andalusian Global ObseRvatory of the Atmosphere). The analysis shows a significant contribution of nucleation mode aerosol particles to the total aerosol number concentration at both sites, with a contribution of 47 % and 48 % at SNS and UGR, respectively. Due to the important contribution of NPF events to the total aerosol number concentrations and their high occurrence frequency (> 70 %) during the study period, a detailed analysis of NPF events is done in order to get insight into the possible mechanisms and processes involved in NPF events at these contrastive sites. At SNS, NPF is found to be associated with the transport of gaseous precursors from lower altitudes by orographic buoyant upward flows. However, NPF events at SNS site are always observed from the smallest measured sizes of the aerosol size distribution (4 nm), implying that NPF takes place in or in the vicinity of the high-altitude SNS station rather than transported from lower altitudes. Although NPF events at the mountain site seem to be connected with those occurring at the urban site, growth rates (GR) at SNS are higher than those at UGR site (GR7–25 of 6.9 and 4.5 nm h−1 and GR4–7 of 4.1 and 3.6 nm h−1 at SNS and UGR, respectively). This fact could have a special importance on the production of cloud condensation nuclei (CCN) and therefore on cloud formations which may affect regional/global climate, since larger GR at mountain sites could be translated to larger survival probability of NPF particles to reach CCN sizes, due to shorter time needed for the growth. The analysis of sulfuric acid (H2SO4) shows that the contribution of H2SO4 is able to explain a minimal fraction contribution to the observed GRs at both sites (


2018 ◽  
Author(s):  
Vyoma Singla ◽  
Subrata Mukherjee ◽  
Adam Kristensson ◽  
Govindan Pandithurai ◽  
Kundan K. Dani ◽  
...  

Abstract. There is a lack of characterization of the aerosol population in Western India, how it is affected by meteorological parameters, and new particle formation and the influence on cloud condensation nuclei (CCN). For this reason, measurements of particle number size distribution, aerosol chemical composition, meteorology and cloud condensation nuclei number concentration were monitored at High Altitude Cloud Physics Laboratory (HACPL) in Mahabaleshwar mountain town in Western India between November 2016 and February 2017. Most air masses in this period originated from the Indian continent to the north-east of HACPL. New particle formation (NPF) events were observed on 47 days and mainly associated with these north-easterly air masses and high SO2 emissions and biomass burning activities, while weaker or non-NPF days were associated with westerly air masses and relatively higher influence of local air pollution. The growth of newly formed particles enhanced the mass concentration of secondary organic and inorganic species of aerosol particles. The mean growth rate, formation rate, condensation sink and coagulation loss for the 13 strongest events was found to be 2.58 ± 0.38 nm h−1, 2.82 ± 1.37 cm−3 s−1, 22.3 ± 2.87 * 10-3 s−1 and 1.62 ± 1.04 cm−3 s−1 respectively. A closer examination of 5 events showed that low relative humidity and solar radiation favoured new particle formation. These NPF events lead to a significant increase in CCN concentration (mean ~ 53 ± 36 %). The NanoMap method revealed that NPF took place up to several hundred kilometers upwind and to the north-east of HACPL.


2015 ◽  
Vol 15 (6) ◽  
pp. 8151-8189 ◽  
Author(s):  
C. Rose ◽  
K. Sellegri ◽  
E. Freney ◽  
R. Dupuy ◽  
A. Colomb ◽  
...  

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.


2006 ◽  
Vol 6 (10) ◽  
pp. 2811-2824 ◽  
Author(s):  
M. Komppula ◽  
S.-L. Sihto ◽  
H. Korhonen ◽  
H. Lihavainen ◽  
V.-M. Kerminen ◽  
...  

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.


2016 ◽  
Author(s):  
Carla Frege ◽  
Federico Bianchi ◽  
Ugo Molteni ◽  
Jasmin Tröstl ◽  
Heikki Junninen ◽  
...  

Abstract. The ion composition at high-altitude (3450 m a.s.l.) was measured with an Atmospheric Pressure interface Time of Flight mass spectrometer (APi-TOF) during a period of nine months. The negative mass spectra were dominated by the ions of sulfuric, nitric, malonic and methanesulfonic acid (MSA) as well as SO5−. The most prominent positive ion peaks were from amines. The other cations were mainly organic compounds clustered with a nitrogen-containing ion, which could be either NH4+ or an aminium. Occasionally the positive spectra were characterized by groups of compounds each differing by a methylene group. In the negative spectrum, sulfuric acid was always observed during clear sky conditions following the diurnal cycle of sun irradiation. We also measured many events during night time where the signal of sulfuric acid was high and clusters up to the tetramer were observed. A plausible reason for these events could be evaporation from particles at low relative humidity. A remarkably strong correlation between the signals of SO5− and CH3SO3− was observed for the full measurement period. The presence of these two ions during both the day and the night suggests a non-photochemical channel of formation which is possibly linked to halogen chemistry. Halogenated species, especially Br− and IO3−, were frequently observed in air masses that originated mainly from the Atlantic Ocean and occasionally from continental areas based on back trajectory analyses. We measured I2O5 clustered with an ion, a species that was proposed from laboratory and modelling studies. All halogenated species exhibited an unexpected diurnal behaviour with low values during day time. New particle formation (NPF) events were observed and characterized by 1) highly oxygenated molecules (HOMs) and low sulfuric acid or 2) ammonia-sulfuric acid clusters. We present characteristic spectra for each of these two event types based on 26 nucleation episodes. The mass spectrum of the ammonia-sulfuric acid nucleation event compares very well with laboratory measurements reported from the CLOUD chamber. A source receptor analysis indicates that new particle formation events at the Jungfraujoch take place within a restricted period of time of 24–48 hours after air masses have had contact with boundary layer. This time frame appears to be crucial to reach an optimal oxidation state and concentration of organic molecules necessary to facilitate nucleation.


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