scholarly journals Wintertime subarctic new particle formation from Kola Peninsula sulfur emissions

2021 ◽  
Vol 21 (23) ◽  
pp. 17559-17576
Author(s):  
Mikko Sipilä ◽  
Nina Sarnela ◽  
Kimmo Neitola ◽  
Totti Laitinen ◽  
Deniz Kemppainen ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Kola Peninsula ◽  
Cloud Condensation Nuclei ◽  
Particle Formation ◽  
Negative Ion ◽  
The Arctic ◽  
Size Distributions ◽  
New Particle Formation ◽  
So2 Emissions ◽  
Finnish Lapland

Abstract. The metallurgical industry in the Kola Peninsula, north-west Russia, form, after Norilsk, Siberia, the second largest source of air pollution in the Arctic and subarctic domain. Sulfur dioxide (SO2) emissions from the ore smelters are transported to wide areas, including Finnish Lapland. We performed investigations on concentrations of SO2, aerosol precursor vapours, aerosol and ion cluster size distributions together with chemical composition measurements of freshly formed clusters at the SMEAR I station in Finnish Lapland relatively close (∼ 300 km) to the Kola Peninsula industrial sites during the winter 2019–2020. We show that highly concentrated SO2 from smelter emissions is converted to sulfuric acid (H2SO4) in sufficient concentrations to drive new particle formation hundreds of kilometres downwind from the emission sources, even at very low solar radiation intensities. Observed new particle formation is primarily initiated by H2SO4–ammonia (negative-)ion-induced nucleation. Particle growth to cloud condensation nuclei (CCN) sizes was concluded to result from sulfuric acid condensation. However, air mass advection had a large role in modifying aerosol size distributions, and other growth mechanisms and condensation of other compounds cannot be fully excluded. Our results demonstrate the dominance of SO2 emissions in controlling wintertime aerosol and CCN concentrations in the subarctic region with a heavily polluting industry.

scholarly journals Wintertime sub-arctic new particle formation from Kola Peninsula sulphur emissions

2021 ◽  
Author(s):  
Mikko Sipilä ◽  
Nina Sarnela ◽  
Kimmo Neitola ◽  
Totti Laitinen ◽  
Deniz Kemppainen ◽  
...  
Keyword(s):  
Kola Peninsula ◽  
Sulphuric Acid ◽  
Cloud Condensation Nuclei ◽  
Particle Formation ◽  
Negative Ion ◽  
The Arctic ◽  
Size Distributions ◽  
New Particle Formation ◽  
So2 Emissions ◽  
Finnish Lapland

Abstract. Metallurgical industry in Kola peninsula, North-West Russia, form a second largest source of air pollution in the Arctic and sub-Arctic domain. Sulphur dioxide emissions from the ore smelters are transported to wide areas including Finnish Lapland. We performed investigations on concentrations of SO2 and aerosol precursor vapours, aerosol and ion cluster size distributions together with chemical composition measurements of freshly formed clusters at SMEAR I station in Finnish Lapland relatively close (~300 km) to Kola peninsula industrial sites during winter 2019–2020. We show that highly concentrated SO2 from smelter emissions is converted to sulphuric acid (H2SO4) with sufficient concentrations to drive new particle formation hundreds of kilometres downwind of the emission sources even with very low solar radiation intensities. Observed new particle formation is primarily initiated by H2SO4 – ammonia (negative-) ion induced nucleation. Particle growth to cloud condensation nuclei (CCN) sizes was concluded to result from sulphuric acid condensation. However, airmass advection had a large role in modifying aerosol size distributions and other growth mechanisms cannot be fully excluded. Our results demonstrate the dominance of SO2 emissions in controlling winter-time aerosol and CCN concentrations in the subarctic region with heavily polluting industry.

scholarly journals Trends in new particle formation in eastern Lapland, Finland: effect of decreasing sulfur emissions from Kola Peninsula

2014 ◽  
Vol 14 (9) ◽  
pp. 4383-4396 ◽  
Author(s):  
E.-M. Kyrö ◽  
R. Väänänen ◽  
V.-M. Kerminen ◽  
A. Virkkula ◽  
T. Petäjä ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Kola Peninsula ◽  
Formation Rate ◽  
Particle Formation ◽  
The Arctic ◽  
Late Winter ◽  
Rapid Decline ◽  
New Particle Formation ◽  
Sulfur Species ◽  
Sulfur Emissions

Abstract. The smelter industry in Kola Peninsula is the largest source of anthropogenic SO2 in the Arctic part of Europe and one of the largest within the Arctic domain. Due to socio-economic changes in Russia, the emissions have been decreasing especially since the late 1990s resulting in decreased SO2 concentrations close to Kola in eastern Lapland, Finland. At the same time, the frequency of new particle formation days has been decreasing distinctively at SMEAR I station in eastern Lapland, especially during spring and autumn. We show that sulfur species, namely sulfur dioxide and sulfuric acid, have an important role in both new particle formation and subsequent growth and that the decrease in new particle formation days is a result of the reduction of sulfur emissions originating from Kola Peninsula. In addition to sulfur species, there are many other quantities, such as formation rate of aerosol particles, condensation sink and nucleation mode particle number concentration, which are related to the number of observed new particle formation (NPF) days and need to be addressed when linking sulfur emissions and NPF. We show that while most of these quantities exhibit statistically significant trends, the reduction in Kola sulfur emissions is the most obvious reason for the rapid decline in NPF days. Sulfuric acid explains approximately 20–50% of the aerosol condensational growth observed at SMEAR I, and there is a large seasonal variation with highest values obtained during spring and autumn. We found that (i) particles form earlier after sunrise during late winter and early spring due to high concentrations of SO2 and H2SO4; (ii) several events occurred during the absence of light, and they were connected to higher than average concentrations of SO2; and (iii) high SO2 concentrations could advance the onset of nucleation by several hours. Moreover, air masses coming over Kola Peninsula seemed to favour new particle formation.

Composition and concentrations of aerosol precursor gases in the sub-Arctic boreal forest

2021 ◽  
Author(s):  
Tuija Jokinen ◽  
Katrianne Lehtipalo ◽  
Kimmo Neitola ◽  
Nina Sarnela ◽  
Totti Laitinen ◽  
...  
Keyword(s):  
Seasonal Variation ◽  
Sulfuric Acid ◽  
Ambient Air ◽  
Particle Formation ◽  
The Arctic ◽  
New Particle Formation ◽  
Aerosol Formation ◽  
Iodic Acid ◽  
Field Station

<p>One way to form aerosol particles is the condensation of oxidized atmospheric trace gases, such as sulfuric acid (SA) into small molecular clusters. After growing to larger particles by condensation of low volatile gases, they can affect the planets climate directly by scattering light and indirectly by acting as cloud condensation nuclei. Observations of low-volatility aerosol precursor gases have been reported around the world but long-term measurement series and Arctic data sets showing seasonal variation are close to non-existent. In here, we present ~7 months of aerosol precursor gas measurements performed with the nitrate based chemical ionization mass spectrometer (CI-APi-TOF). We deployed our measurements ~250 km above the Arctic Circle at the Finnish sub-Arctic field station, SMEAR I in Värriö. We report concentration measurements of the most common new particle formation related compounds; sulfuric acid, methanesulfonic acid (MSA), iodic acid (IA) and highly oxygenated organic compounds, HOMs. At this remote measurement site, surrounded by a strict nature preserve, that gets occasional pollution from a Russian city of Murmansk, SA is originated both from anthropogenic and biological sources and has a clear diurnal cycle but no significant seasonal variation, while MSA as an oxidation product of purely biogenic sources is showing a more distinct seasonal cycle. Iodic acid concentrations are the most stable throughout the measurement period, showing almost identical peak concentrations for spring, summer and autumn. HOMs are abundant during the summer months and due to their high correlation with ambient air temperature, we suggest that most of HOMs are products of monoterpene oxidation. New particle formation events at SMEAR I happen under relatively low temperatures, low relative humidity, high ozone concentration, high SA concentration in the morning and high MSA concentrations in the afternoon. The role of HOMs in aerosol formation will be discussed. All together, these are the first long term measurements of aerosol forming precursor from the sub-arctic region helping us to understand atmospheric chemical processes and aerosol formation in the rapidly changing Arctic.</p><p> </p><p> </p>

scholarly journals Molecular insights into new particle formation in Barcelona, Spain

2020 ◽  
Vol 20 (16) ◽  
pp. 10029-10045 ◽  
Author(s):  
James Brean ◽  
David C. S. Beddows ◽  
Zongbo Shi ◽  
Brice Temime-Roussel ◽  
Nicolas Marchand ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Organic Compounds ◽  
Radiative Forcing ◽  
Cloud Condensation Nuclei ◽  
Sulfuric Acid Concentration ◽  
Particle Growth ◽  
Particle Formation ◽  
Necessary Condition ◽  
New Particle Formation ◽  
High Concentrations

Abstract. Atmospheric aerosols contribute some of the greatest uncertainties to estimates of global radiative forcing and have significant effects on human health. New particle formation (NPF) is the process by which new aerosols of sub-2 nm diameter form from gas-phase precursors and contributes significantly to particle numbers in the atmosphere, accounting for approximately 50 % of cloud condensation nuclei globally. Here, we study summertime NPF in urban Barcelona in north-eastern Spain utilising particle counting instruments down to 1.9 nm and a Nitrate Chemical Ionisation Atmospheric Pressure interface Time of Flight Mass Spectrometer (CI-APi-ToF). The rate of formation of new particles is seen to increase linearly with sulfuric acid concentration, although particle formation rates fall short of chamber studies of H2SO4–DMA–H2O while exceeding those of H2SO4–BioOxOrg–H2O nucleation, although a role of highly oxygenated molecules (HOMs) cannot be ruled out. The sulfuric acid dimer : monomer ratio is significantly lower than that seen in experiments involving sulfuric acid and dimethylamine (DMA) in chambers, indicating that stabilisation of sulfuric acid clusters by bases is weaker in this dataset than in chambers, either due to rapid evaporation due to high summertime temperatures or limited pools of stabilising amines. Such a mechanism cannot be verified in these data, as no higher-order H2SO4–amine clusters nor H2SO4–HOM clusters were measured. The high concentrations of HOMs arise from isoprene, alkylbenzene, monoterpene and polycyclic aromatic hydrocarbon (PAH) oxidation, with alkylbenzenes providing greater concentrations of HOMs due to significant local sources. The concentration of these HOMs shows a dependence on temperature. The organic compounds measured primarily fall into the semivolatile organic compound (SVOC) volatility class arising from alkylbenzene and isoprene oxidation. Low-volatility organic compounds (LVOCs) largely arise from oxidation of alkylbenzenes, PAHs and monoterpenes, whereas extremely low-volatility organic compounds (ELVOCs) arise from primarily PAH and monoterpene oxidation. New particle formation without growth past 10 nm is also observed, and on these days oxygenated organic concentrations are lower than on days with growth by a factor of 1.6, and thus high concentrations of low-volatility oxygenated organics which primarily derive from traffic-emitted volatile organic compounds (VOCs) appear to be a necessary condition for the growth of newly formed particles in Barcelona. These results are consistent with prior observations of new particle formation from sulfuric acid–amine reactions in both chambers and the real atmosphere and are likely representative of the urban background of many European Mediterranean cities. A role for HOMs in the nucleation process cannot be confirmed or ruled out, and there is strong circumstantial evidence of the participation of HOMs across multiple volatility classes in particle growth.

Observations of New Particle Formation events during summertime in Helsinki

2021 ◽  
Author(s):  
Roseline Thakur ◽  
Lubna Dada ◽  
Lisa Beck ◽  
Tommy Chan ◽  
Juha Sulo ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Urban Areas ◽  
Boreal Forests ◽  
Cloud Condensation Nuclei ◽  
Cyanobacterial Bloom ◽  
Particle Formation ◽  
Capital City ◽  
Atmospheric Conditions ◽  
New Particle Formation ◽  
Iodic Acid

<p>Aerosols can originate from different sources and undergo various formation pathways. New Particle formation (NPF) events occur when precursor vapors nucleate and vapors with low volatility condense on the critical nuclei enabling them to grow to cloud condensation nuclei (CCN) relevant sizes. As CCN, these aerosols affect the occurrence of clouds and their lifetime on local, regional and global level.  Many studies have investigated new particle formation events from various sites ranging from urban areas, boreal forests to pristine locations; however, there is still a dearth of studies investigating coastal new particle formation, which is a complex phenomenon due to the dynamic and ever-changing atmospheric conditions at the coast.  A comprehensive study of particle number distributions and aerosol forming precursor vapors was carried out in a coastal capital city of Finland, Helsinki, during the summer of 2019. The experimental setup comprising of a nitrate-based chemical ionization atmospheric pressure interface time of flight mass spectrometer (CI-APi-TOF), a neutral cluster-air ion spectrometer (NAIS) and a particle size magnifier (PSM) were housed in and around the SMEAR III station in Kumpula Science campus. SMEAR III is a unique site situated in a semi-urban yet coastal location. The period of experiment coincided with the cyanobacterial bloom in the coastal areas of Finland and in the Baltic Sea region. Our study recorded several regional NPF and aerosol burst events during this period. High concentrations of sulfuric acid was found to be associated with the regional NPF events whereas increasing iodic acid concentrations was mostly associated with the initiation of burst events. The sources of sulfuric acid and iodic acid has been carefully evaluated in this study.</p><p> </p>

Studies of the connection between condensable trace gases and aerosol particles in Svalbard

2021 ◽  
Author(s):  
Tuuli Lehmusjärvi ◽  
Roseline Thakur ◽  
Lisa Beck ◽  
Mikko Sipilä ◽  
Tuija Jokinen
Keyword(s):  
Cloud Condensation Nuclei ◽  
Regional Climate ◽  
High Arctic ◽  
Particle Formation ◽  
Urban Environments ◽  
The Arctic ◽  
New Particle Formation ◽  
Iodic Acid ◽  
Summer Time

<p>In the high Arctic, the climate is warming faster than in the lower latitudes due to the Arctic amplification. Sea ice is melting and permafrost is thawing, and the scarce vegetation of the Arctic is changing rapidly. All these varying conditions will have an impact on possible emission sources of aerosol precursor gases, thus affecting the New Particle Formation (NPF) in the Arctic atmosphere, of which we still know very little. It is important to study the NPF events, which parameters affect the aerosol phase and how these newly formed aerosols can grow into cloud condensation nuclei sizes. Only then, it is possible to understand how climate change is affecting the aerosol population, clouds and regional climate of the pristine Arctic. The role of the precursor gases like Sulphuric Acid (SA), Iodic Acid (IA), Methane Sulphonic Acid (MSA) and Highly Oxygenated organic Molecules (HOM) in NPF in boreal and urban environments has been explored to a great extent. However, the role of these precursor gases in NPF events in remote locations - devoid of pollution sources and the vegetation - is still ambiguous. Therefore, it is crucial to conduct long-term measurements to study the composition and concentrations of aerosol precursors molecules, nanoparticles and air ions in remote and climatically fragile place like Ny-Ålesund in the Arctic. This research location is not only a natural pristine laboratory to understand the atmospheric processes but also acts as a climate mirror reflecting the most drastic changes happening in the atmosphere and cryosphere. In this study, we aim to enhance the understanding of the role of aerosol precursor gases in new particle formation in Ny-Ålesund, Svalbard.</p><p>            We have studied aerosol particle formation now for almost three years in the Ny-Ålesund research village in Svalbard (78° 55' 24.7368'' N, 11° 54' 35.6220'' E.) with the Neutral cluster and Air Ion Spectrometer (NAIS) measuring ~1-40 nm particles and ions. We have conducted measurements with a Chemical Ionization Atmospheric Pressure interface Time Of Flight (CI-APi-TOF) mass spectrometer to understand the chemical composition of organic precursors vapours and abundance of inorganic aerosol precursor gases such as SA, MSA and IA. Additionally,  we have studied the emission and composition of volatile organic compounds on the site during summer-time.</p><p>            In this study, we report the time series concentrations of the most common aerosol precursor gases like SA, MSA, IA and HOM from the period 28.6.-25.7.2019, which are responsible for the initiation and/or growth of particles. The variability in the concentrations of these vapours is compared between NPF event and non-event days. The study explores also the role of meteorological parameters like wind speed, wind direction, temperature and humidity on NPF processes.</p>

scholarly journals New particle formation and its effect on CCN abundance in the summer Arctic: a case study during PS106 cruise

2019 ◽  
Author(s):  
Simonas Kecorius ◽  
Teresa Vogl ◽  
Pauli Paasonen ◽  
Janne Lampilahti ◽  
Daniel Rothenberg ◽  
...  
Keyword(s):  
Cloud Condensation Nuclei ◽  
Particle Diameter ◽  
Negative Ions ◽  
Particle Formation ◽  
Number Concentration ◽  
Cloud Formation ◽  
The Arctic ◽  
New Particle Formation ◽  
Nucleation Mode ◽  
Particle Formation And Growth

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.

scholarly journals Ion-induced sulfuric acid–ammonia nucleation drives particle formation in coastal Antarctica

2018 ◽  
Vol 4 (11) ◽  
pp. eaat9744 ◽  
Author(s):  
T. Jokinen ◽  
M. Sipilä ◽  
J. Kontkanen ◽  
V. Vakkari ◽  
P. Tisler ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Cloud Condensation Nuclei ◽  
Aerosol Particles ◽  
Particle Growth ◽  
Field Studies ◽  
Particle Formation ◽  
New Particle Formation ◽  
Aerosol Formation ◽  
Radiative Balance ◽  
Secondary Aerosol

Formation of new aerosol particles from trace gases is a major source of cloud condensation nuclei (CCN) in the global atmosphere, with potentially large effects on cloud optical properties and Earth’s radiative balance. Controlled laboratory experiments have resolved, in detail, the different nucleation pathways likely responsible for atmospheric new particle formation, yet very little is known from field studies about the molecular steps and compounds involved in different regions of the atmosphere. The scarcity of primary particle sources makes secondary aerosol formation particularly important in the Antarctic atmosphere. Here, we report on the observation of ion-induced nucleation of sulfuric acid and ammonia—a process experimentally investigated by the CERN CLOUD experiment—as a major source of secondary aerosol particles over coastal Antarctica. We further show that measured high sulfuric acid concentrations, exceeding 107 molecules cm−3, are sufficient to explain the observed new particle growth rates. Our findings show that ion-induced nucleation is the dominant particle formation mechanism, implying that galactic cosmic radiation plays a key role in new particle formation in the pristine Antarctic atmosphere.

scholarly journals New particle formation and its effect on cloud condensation nuclei abundance in the summer Arctic: a case study in the Fram Strait and Barents Sea

2019 ◽  
Vol 19 (22) ◽  
pp. 14339-14364 ◽  
Author(s):  
Simonas Kecorius ◽  
Teresa Vogl ◽  
Pauli Paasonen ◽  
Janne Lampilahti ◽  
Daniel Rothenberg ◽  
...  
Keyword(s):  
Cloud Condensation Nuclei ◽  
Particle Diameter ◽  
Negative Ions ◽  
Particle Formation ◽  
Number Concentration ◽  
The Arctic ◽  
New Particle Formation ◽  
Condensation Nuclei ◽  
Nucleation Mode ◽  
Particle Formation And Growth

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 were made 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 in 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. This 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 in Arctic cloud formation.

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