scholarly journals Long-term analysis of clear-sky new particle formation events and nonevents in Hyytiälä

2017 ◽  
Vol 17 (10) ◽  
pp. 6227-6241 ◽  
Author(s):  
Lubna Dada ◽  
Pauli Paasonen ◽  
Tuomo Nieminen ◽  
Stephany Buenrostro Mazon ◽  
Jenni Kontkanen ◽  
...  

Abstract. New particle formation (NPF) events have been observed all around the world and are known to be a major source of atmospheric aerosol particles. Here we combine 20 years of observations in a boreal forest at the SMEAR II station (Station for Measuring Ecosystem–Atmosphere Relations) in Hyytiälä, Finland, by building on previously accumulated knowledge and by focusing on clear-sky (noncloudy) conditions. We first investigated the effect of cloudiness on NPF and then compared the NPF event and nonevent days during clear-sky conditions. In this comparison we considered, for example, the effects of calculated particle formation rates, condensation sink, trace gas concentrations and various meteorological quantities in discriminating NPF events from nonevents. The formation rate of 1.5 nm particles was calculated by using proxies for gaseous sulfuric acid and oxidized products of low volatile organic compounds, together with an empirical nucleation rate coefficient. As expected, our results indicate an increase in the frequency of NPF events under clear-sky conditions in comparison to cloudy ones. Also, focusing on clear-sky conditions enabled us to find a clear separation of many variables related to NPF. For instance, oxidized organic vapors showed a higher concentration during the clear-sky NPF event days, whereas the condensation sink (CS) and some trace gases had higher concentrations during the nonevent days. The calculated formation rate of 3 nm particles showed a notable difference between the NPF event and nonevent days during clear-sky conditions, especially in winter and spring. For springtime, we are able to find a threshold equation for the combined values of ambient temperature and CS, (CS (s−1) > −3.091  ×  10−5  ×  T (in Kelvin) + 0.0120), above which practically no clear-sky NPF event could be observed. Finally, we present a probability distribution for the frequency of NPF events at a specific CS and temperature.

2016 ◽  
Author(s):  
Lubna Dada ◽  
Pauli Paasonen ◽  
Tuomo Nieminen ◽  
Stephany Buenrostro Mazon ◽  
Jenni Kontkanen ◽  
...  

Abstract. New particle formation (NPF) events have been observed all around the world and are known to be a major source of atmospheric aerosol particles. Here we combine 20 years of observations in a boreal forest at the SMEAR II station (Station for Measuring Ecosystem-Atmosphere Relations) in Hyytiälä, Finland, by utilizing previously accumulated knowledge, and by focusing on clear-sky (non-cloudy) conditions. We first investigated the effect of cloudiness on NPF and then compared the NPF event and non-event days during clear-sky conditions. In this comparison we considered, for example, the effects of calculated particle formation rates, condensation sink, trace gas concentrations and various meteorological quantities. The formation rate of 1.5 nm particles was calculated by using proxies for gaseous sulfuric acid and oxidized products of low volatile organic compounds. As expected, our results indicate an increase in the frequency of NPF events under clear-sky conditions. Also, focusing on clearsky conditions enabled us to find a clear separation of many variables related to NPF. For instance, oxidized organic vapors showed higher concentration during the clear-sky NPF event days, whereas the condensation sink (CS) and some trace gases had higher concentrations during the non-event days. The calculated formation rate of 3 nm particles showed a notable difference between the NPF event and non-event days during clear-sky conditions, especially in winter and spring. For spring time, we are able to find a threshold value for the combined values of ambient temperature and CS, above which practically no clear-sky NPF event could be observed. Finally, we present a probability distribution for the frequency of NPF events at a specific CS and temperature.


2021 ◽  
Vol 21 (4) ◽  
pp. 2457-2468
Author(s):  
Runlong Cai ◽  
Chao Yan ◽  
Dongsen Yang ◽  
Rujing Yin ◽  
Yiqun Lu ◽  
...  

Abstract. New particle formation (NPF) is one of the major sources of atmospheric ultrafine particles. Due to the high aerosol and trace gas concentrations, the mechanism and governing factors for NPF in the polluted atmospheric boundary layer may be quite different from those in clean environments, which is however less understood. Herein, based on long-term atmospheric measurements from January 2018 to March 2019 in Beijing, the nucleation mechanism and the influences of H2SO4 concentration, amine concentrations, and aerosol concentration on NPF are quantified. The collision of H2SO4–amine clusters is found to be the dominating mechanism to initialize NPF in urban Beijing. The coagulation scavenging due to the high aerosol concentration is a governing factor as it limits the concentration of H2SO4–amine clusters and new particle formation rates. The formation of H2SO4–amine clusters in Beijing is sometimes limited by low amine concentrations. Summarizing the synergistic effects of H2SO4 concentration, amine concentrations, and aerosol concentration, we elucidate the governing factors for H2SO4–amine nucleation for various conditions.


2013 ◽  
Author(s):  
Ella-Maria Kyrö ◽  
Riikka Väänänen ◽  
Miikka Dal Maso ◽  
Veli-Matti Kerminen ◽  
Aki Virkkula ◽  
...  

2015 ◽  
Vol 15 (22) ◽  
pp. 33077-33119
Author(s):  
J. Kontkanen ◽  
E. Järvinen ◽  
H. E. Manninen ◽  
K. Lehtipalo ◽  
J. Kangasluoma ◽  
...  

Abstract. The concentrations of neutral and charged sub-3 nm clusters and their connection to new particle formation (NPF) were investigated during the PEGASOS campaign (7 June–9 July 2012) at the San Pietro Capofiume measurement station in the Po Valley, Italy. Continuous high concentrations of sub-3 nm clusters were detected during the measurement period, although the condensation sink was relatively high (median value 1.1 × 10-2 s-1). The median cluster concentrations were 2140 and 7980 cm-3 in the size bins of 1.5–1.8 nm and 1.8–3 nm, and the majority of them were electrically neutral. NPF events were observed during the measurement period frequently, on 86 % of the days. The median growth rates of clusters during the events were 4.3, 6.0 and 7.2 nm h-1 in the size ranges of 1.5–3, 3–7 and 7–20 nm. The median formation rate of 1.6 nm clusters was high, 45 cm-3 s-1, and it exceeded the median formation rate of 2 nm clusters by one order of magnitude. The ion-induced nucleation fraction was low; the median values were 0.7 % at 1.6 nm and 3.0 % at 2 nm. On NPF event days the neutral cluster concentration had a maximum around 9 a.m. (local winter time), which was absent on a non-event day. The increase in the cluster concentrations in the morning coincided with the increase in the boundary layer height. At the same time radiation and temperature increased and RH and condensation sink decreased. The concentration of neutral clusters was observed to have apositive correlation with sulfuric acid proxy, indicating the significance of sulfuric acid for the cluster formation in San Pietro Capofiume. The condensation sink had anegative correlation with the concentration of charged clusters but no clear relation to the neutral cluster concentration. This finding, together with back-trajectory analysis, suggests that the precursor vapors of the clusters and background aerosol particles, acting as their sink, have possibly originated from the same sources, including e.g. power plants and industrial areas in the Po Valley.


2016 ◽  
Vol 16 (4) ◽  
pp. 1919-1935 ◽  
Author(s):  
Jenni Kontkanen ◽  
Emma Järvinen ◽  
Hanna E. Manninen ◽  
Katrianne Lehtipalo ◽  
Juha Kangasluoma ◽  
...  

Abstract. The concentrations of neutral and charged sub-3nm clusters and their connection to new particle formation (NPF) were investigated during the PEGASOS campaign (7 June–9 July 2012) at the San Pietro Capofiume measurement station in the Po Valley, Italy. Continuous high concentrations of sub-3nm clusters were detected during the measurement period, although the condensation sink was relatively high (median value 1.1 × 10−2 s−1). The median cluster concentrations were 2140 and 7980 cm−3 in the size bins of 1.5–1.8 and 1.8–3 nm, and the majority of them were electrically neutral. NPF events were observed during the measurement period frequently, on 86 % of the days. The median growth rates of clusters during the events were 4.3, 6.0 and 7.2 nm h−1 in the size ranges of 1.5–3, 3–7 and 7–20 nm. The median formation rate of 1.6 nm clusters was high, 45 cm−3 s−1, and it exceeded the median formation rate of 2 nm clusters by 1 order of magnitude. The ion-induced nucleation fraction was low; the median values were 0.7 % at 1.6 nm and 3.0 % at 2 nm. On NPF event days the neutral cluster concentration had a maximum around 09:00 (local winter time), which was absent on a non-event day. The increase in the cluster concentrations in the morning coincided with the increase in the boundary layer height. At the same time radiation, temperature and SO2 concentration increased, and RH and condensation sink decreased. The concentrations of neutral and charged clusters were observed to have a positive correlation with sulfuric acid proxy, indicating the significance of sulfuric acid for the cluster formation in San Pietro Capofiume. The condensation sink had a negative correlation with the concentration of charged clusters but no clear relation to the neutral cluster concentration. This finding, together with back-trajectory analysis, suggests that the precursor vapors of the clusters and background aerosol particles, acting as their sink, have possibly originated from the same sources, including e.g., power plants and industrial areas in the Po Valley.


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 %.


2019 ◽  
Vol 19 (16) ◽  
pp. 10537-10555 ◽  
Author(s):  
Simo Hakala ◽  
Mansour A. Alghamdi ◽  
Pauli Paasonen ◽  
Ville Vakkari ◽  
Mamdouh I. Khoder ◽  
...  

Abstract. Atmospheric aerosols have significant effects on human health and the climate. A large fraction of these aerosols originates from secondary new particle formation (NPF), where atmospheric vapors form small particles that subsequently grow into larger sizes. In this study, we characterize NPF events observed at a rural background site of Hada Al Sham (21.802∘ N, 39.729∘ E), located in western Saudi Arabia, during the years 2013–2015. Our analysis shows that NPF events occur very frequently at the site, as 73 % of all the 454 classified days were NPF days. The high NPF frequency is likely explained by the typically prevailing conditions of clear skies and high solar radiation, in combination with sufficient amounts of precursor vapors for particle formation and growth. Several factors suggest that in Hada Al Sham these precursor vapors are related to the transport of anthropogenic emissions from the coastal urban and industrial areas. The median particle formation and growth rates for the NPF days were 8.7 cm−3 s−1 (J7 nm) and 7.4 nm h−1 (GR7−12 nm), respectively, both showing highest values during late summer. Interestingly, the formation and growth rates increase as a function of the condensation sink, likely reflecting the common anthropogenic sources of NPF precursor vapors and primary particles affecting the condensation sink. A total of 76 % of the NPF days showed an unusual progression, where the observed diameter of the newly formed particle mode started to decrease after the growth phase. In comparison to most long-term measurements, the NPF events in Hada Al Sham are exceptionally frequent and strong both in terms of formation and growth rates. In addition, the frequency of the decreasing mode diameter events is higher than anywhere else in the world.


2019 ◽  
Vol 76 (11) ◽  
pp. 3485-3504 ◽  
Author(s):  
Carsten Abraham ◽  
Adam H. Monahan

Abstract In a companion paper hidden Markov model (HMM) analyses have been conducted to classify the nocturnal stably stratified boundary layer (SBL) into weakly stable (wSBL) and very stable (vSBL) conditions at different tower sites on the basis of long-term Reynolds-averaged mean data. The resulting HMM regime sequences allow analysis of long-term (climatological) SBL regime statistics. In particular, statistical features of very persistent wSBL and vSBL nights, in which a single regime lasts for the entire night, are contrasted with those of nights with SBL regime transitions. The occurrence of very persistent nights is seasonally dependent and more likely in homogeneous surroundings than in regions with complex terrain. When transitions occur, their timing is not seasonally dependent, but transitions are enhanced close to sunset (for land-based sites). The regime event durations depict remarkably similar distributions across all stations with peaks in transition likelihood approximately 1–2 h after a preceding transition. At Cabauw in the Netherlands, very persistent wSBL and vSBL nights are usually accompanied by overcast conditions with strong geostrophic winds Ugeo or clear-sky conditions with weak Ugeo, respectively. In contrast, SBL regime transitions can neither be linked to magnitudes in Ugeo and cloud coverage nor to specific tendencies in Ugeo. However, regime transitions can be initiated by changes in low-level cloud cover.


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