scholarly journals Chemical characterization of atmospheric ions at the High Altitude Research Station Jungfraujoch (Switzerland)

2016 ◽  
Author(s):  
Carla Frege ◽  
Federico Bianchi ◽  
Ugo Molteni ◽  
Jasmin Tröstl ◽  
Heikki Junninen ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
High Altitude ◽  
Methanesulfonic Acid ◽  
Particle Formation ◽  
Back Trajectory ◽  
Research Station ◽  
New Particle Formation ◽  
Night Time ◽  
Negative Spectrum ◽  
Air Masses

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.

scholarly journals Chemical characterization of atmospheric ions at the high altitude research station Jungfraujoch (Switzerland)

2017 ◽  
Vol 17 (4) ◽  
pp. 2613-2629 ◽  
Author(s):  
Carla Frege ◽  
Federico Bianchi ◽  
Ugo Molteni ◽  
Jasmin Tröstl ◽  
Heikki Junninen ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
High Altitude ◽  
Methanesulfonic Acid ◽  
Chemical Characterization ◽  
Solar Irradiation ◽  
Back Trajectory ◽  
High Signal ◽  
Research Station ◽  
Negative Spectrum ◽  
Air Masses

Abstract. The ion composition at high altitude (3454 m a.s.l.) was measured with an atmospheric pressure interface time-of-flight mass spectrometer (APi-TOF) during a period of 9 months, from August 2013 to April 2014. 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 solar irradiation. On many occasions we also saw a high signal of sulfuric acid during nighttime when 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 found I2O5 clustered with an ion, a species that was proposed from laboratory and modeling studies. All halogenated ions exhibited an unexpected diurnal behavior with low values during daytime. 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 NPF events at the Jungfraujoch take place within a restricted period of time of 24–48 h after air masses have had contact with the boundary layer. This time frame appears to be crucial to reach an optimal oxidation state and concentration of organic molecules necessary to facilitate nucleation.

scholarly journals Atmospheric new particle formation at the research station Melpitz, Germany: connection with gaseous precursors and meteorological parameters

2018 ◽  
Vol 18 (3) ◽  
pp. 1835-1861 ◽  
Author(s):  
Johannes Größ ◽  
Amar Hamed ◽  
André Sonntag ◽  
Gerald Spindler ◽  
Hanna Elina Manninen ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Solar Radiation ◽  
Gas Phase ◽  
Meteorological Parameters ◽  
Particle Formation ◽  
Number Concentration ◽  
Independent Effect ◽  
Research Station ◽  
New Particle Formation ◽  
Automated Method

Abstract. This paper revisits the atmospheric new particle formation (NPF) process in the polluted Central European troposphere, focusing on the connection with gas-phase precursors and meteorological parameters. Observations were made at the research station Melpitz (former East Germany) between 2008 and 2011 involving a neutral cluster and air ion spectrometer (NAIS). Particle formation events were classified by a new automated method based on the convolution integral of particle number concentration in the diameter interval 2–20 nm. To study the relevance of gaseous sulfuric acid as a precursor for nucleation, a proxy was derived on the basis of direct measurements during a 1-month campaign in May 2008. As a major result, the number concentration of freshly produced particles correlated significantly with the concentration of sulfur dioxide as the 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. 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. Based on the diurnal evolution of aerosol, gas-phase, and meteorological parameters near the ground, we further conclude that the particle formation process is likely to start in elevated parts of the boundary layer rather than near ground level.

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 (4) ◽  
pp. 11361-11399 ◽  
Author(s):  
J. Boulon ◽  
K. Sellegri ◽  
H. Venzac ◽  
D. Picard ◽  
E. Weingartner ◽  
...  
Keyword(s):  
High Altitude ◽  
Particle Formation ◽  
Swiss Alps ◽  
Aerosol Size Distribution ◽  
New Particle Formation ◽  
High Concentration ◽  
Air Masses ◽  
Charged Aerosol ◽  
Smog Chambers ◽  
The Many

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.

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 ◽  
...  
Keyword(s):  
High Altitude ◽  
Particle Formation ◽  
Ion Source ◽  
Swiss Alps ◽  
Aerosol Size Distribution ◽  
New Particle Formation ◽  
Data Set ◽  
Air Mass ◽  
Air Masses ◽  
Charged Aerosol

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.

scholarly journals New Particle Formation at a High Altitude Site in India: Impact of Fresh Emissions and Long Range Transport

2018 ◽  
Author(s):  
Vyoma Singla ◽  
Subrata Mukherjee ◽  
Adam Kristensson ◽  
Govindan Pandithurai ◽  
Kundan K. Dani ◽  
...  
Keyword(s):  
High Altitude ◽  
Cloud Condensation Nuclei ◽  
Particle Formation ◽  
Western India ◽  
New Particle Formation ◽  
Condensation Nuclei ◽  
Air Masses ◽  
North East ◽  
The North ◽  
Inorganic Species

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.

scholarly journals Observation of new particle formation and measurement of sulfuric acid, ammonia, amines and highly oxidized molecules using nitrate CI-APi-TOF at a rural site in central Germany

2016 ◽  
Author(s):  
Andreas Kürten ◽  
Anton Bergen ◽  
Martin Heinritzi ◽  
Markus Leiminger ◽  
Verena Lorenz ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Mass Spectrometer ◽  
Field Measurements ◽  
Proton Transfer Reaction ◽  
Particle Formation ◽  
Rural Site ◽  
New Particle Formation ◽  
Iodic Acid ◽  
Night Time ◽  
Central Germany

Abstract. The exact mechanisms for new particle formation (NPF) under different boundary layer conditions are not known yet. One important question is if amines and sulfuric acid lead to efficient NPF in the atmosphere. Furthermore, it is not clear to what extent highly oxidized organic molecules (HOM) are involved in NPF. We conducted field measurements at a rural site in central Germany in the proximity of three larger dairy farms to investigate if there is a connection between NPF and the presence of amines and/or ammonia due to the local emissions from the farms. Comprehensive measurements using a nitrate Chemical Ionization-Atmospheric Pressure interface-Time Of Flight (CI-APi-TOF) mass spectrometer, a Proton Transfer Reaction-Mass Spectrometer (PTR-MS), particle counters and Differential Mobility Analyzers (DMAs) as well as measurements of trace gases and meteorological parameters were performed. It is shown that the nitrate CI-APi-TOF is suitable for sensitive measurements of sulfuric acid, amines, a nitrosamine, ammonia, iodic acid and HOM. NPF was found to correlate with sulfuric acid, while an anti-correlation with RH, amines and ammonia is observed. The anti-correlation between NPF and amines could be due to the efficient uptake of these compounds by nucleating clusters and small particles. Much higher HOM dimer (C19/C20 compounds) concentrations during the night than during the day indicate that these HOM do not efficiently self-nucleate as no night-time NPF is observed. Observed iodic acid probably originates from an iodine-containing reservoir substance but the iodine signals are very likely too low to have a significant effect on NPF.

scholarly journals High concentrations of sub-3 nm clusters and frequent new particle formation observed in the Po Valley, Italy, during the PEGASOS 2012 campaign

2015 ◽  
Vol 15 (22) ◽  
pp. 33077-33119
Author(s):  
J. Kontkanen ◽  
E. Järvinen ◽  
H. E. Manninen ◽  
K. Lehtipalo ◽  
J. Kangasluoma ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Formation Rate ◽  
Particle Formation ◽  
Back Trajectory ◽  
New Particle Formation ◽  
Neutral Cluster ◽  
Po Valley ◽  
High Concentrations ◽  
Condensation Sink ◽  
Measurement Period

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.

scholarly journals Open ocean and coastal new particle formation from sulfuric acid and amines around the Antarctic Peninsula

2021 ◽  
Author(s):  
James Brean ◽  
Manuel Dall’Osto ◽  
Rafel Simó ◽  
Zongbo Shi ◽  
David C. S. Beddows ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Antarctic Peninsula ◽  
Particle Formation ◽  
Open Ocean ◽  
New Particle Formation ◽  
The Antarctic

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.

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