scholarly journals Size-segregated aerosol chemical composition at a boreal site in southern Finland, during the QUEST project

2005 ◽  
Vol 5 (5) ◽  
pp. 8851-8877
Author(s):  
F. Cavalli ◽  
M. C. Facchini ◽  
S. Decesari ◽  
L. Emblico ◽  
M. Mircea ◽  
...  
Keyword(s):  
Total Mass ◽  
Chemical Properties ◽  
Particle Formation ◽  
Water Soluble ◽  
Oxidation Products ◽  
Forest Site ◽  
New Particle Formation ◽  
Anthropogenic Aerosol ◽  
Photo Oxidation ◽  
Mass Concentrations

Abstract. Size-segregated aerosol samples were collected during the QUEST field campaign at Hyytiälä, a boreal forest site in Southern Finland, during spring 2003. Aerosol samples were selectively collected during both particle formation events and periods in which no particle formation occurred. A comprehensive characterisation of the aerosol chemical properties (water-soluble inorganic and organic fraction) and an analysis of the relevant meteorological parameters revealed how aerosol chemistry and meteorology combine to determine a favorable "environment" for new particle formation. The results indicated that all events, typically favored during northerly air mass advection, were background aerosols (total mass concentrations range between 1.97 and 4.31 μg m−3), with an increasingly pronounced marine character as the northerly air flow arrived progressively from the west and, in contrast, with a moderate SO2-pollution influence as the air arrived from more easterly directions. Conversely, the non-event aerosol, transported from the south, exhibited the chemical features of European continental sites, with a marked increase in the concentrations of all major anthropogenic aerosol constituents. The higher non-event mass concentration (total mass concentrations range between 6.88 and 16.30 μg m−3) and, thus, a larger surface area, tended to suppress new particle formation, more efficiently depleting potential gaseous precursors for nucleation. The analysis of water-soluble organic compounds showed that clean nucleation episodes were dominated by aliphatic biogenic species, while non-events were characterised by a large abundance of anthropogenic oxygenated species. Interestingly, a significant content of α-pinene photo-oxidation products was observed in the events aerosol, accounting for, on average, 72% of their WSOC; while only moderate amounts of these species were found in the non-event aerosol. If the organic vapors condensing onto accumulation mode particles are responsible also for the growth of newly formed thermodynamically stable clusters, our finding allows one to postulate that, at the site, α-pinene photo-oxidation products (and probably also photo-oxidation products from other terpenes) are the most likely species to contribute to the growth of nanometer-sized particles.

scholarly journals Size-segregated aerosol chemical composition at a boreal site in southern Finland, during the QUEST project

2006 ◽  
Vol 6 (4) ◽  
pp. 993-1002 ◽  
Author(s):  
F. Cavalli ◽  
M. C. Facchini ◽  
S. Decesari ◽  
L. Emblico ◽  
M. Mircea ◽  
...  
Keyword(s):  
Total Mass ◽  
Chemical Properties ◽  
Particle Formation ◽  
Water Soluble ◽  
Oxidation Products ◽  
Forest Site ◽  
New Particle Formation ◽  
Anthropogenic Aerosol ◽  
Photo Oxidation ◽  
Mass Concentrations

Abstract. Size-segregated aerosol samples were collected during the QUEST field campaign at Hyytiälä, a boreal forest site in Southern Finland, during spring 2003. Aerosol samples were selectively collected during both particle formation events and periods in which no particle formation occurred. A comprehensive characterisation of the aerosol chemical properties (water-soluble inorganic and organic fraction) and an analysis of the relevant meteorological parameters revealed how aerosol chemistry and meteorology combine to determine a favorable "environment" for new particle formation. The results indicated that all events, typically favored during northerly air mass advection, were background aerosols (total mass concentrations range between 1.97 and 4.31 µg m-3), with an increasingly pronounced marine character as the northerly air flow arrived progressively from the west and, in contrast, with a moderate SO2-pollution influence as the air arrived from more easterly directions. Conversely, the non-event aerosol, transported from the south, exhibited the chemical features of European continental sites, with a marked increase in the concentrations of all major anthropogenic aerosol constituents. The higher non-event mass concentration (total mass concentrations range between 6.88 and 16.30 µg m-3) and, thus, a larger surface area, tended to suppress new particle formation, more efficiently depleting potential gaseous precursors for nucleation. The analysis of water-soluble organic compounds showed that clean nucleation episodes were dominated by aliphatic biogenic species, while non-events were characterised by a large abundance of anthropogenic oxygenated species. Interestingly, a significant content of α-pinene photo-oxidation products was observed in the events aerosol, accounting for, on average, 72% of their WSOC; while only moderate amounts of these species were found in the non-event aerosol. If the organic vapors condensing onto accumulation mode particles are responsible also for the growth of newly formed thermodynamically stable clusters, our finding allows one to postulate that, at the site, α-pinene photo-oxidation products (and probably also photo-oxidation products from other terpenes) are the most likely species to contribute to the growth of nanometer-sized particles.

scholarly journals The role of VOC oxidation products in continental new particle formation

2008 ◽  
Vol 8 (10) ◽  
pp. 2657-2665 ◽  
Author(s):  
A. Laaksonen ◽  
M. Kulmala ◽  
C. D. O'Dowd ◽  
J. Joutsensaari ◽  
P. Vaattovaara ◽  
...  
Keyword(s):  
Gas Phase ◽  
Chemical Properties ◽  
High Volume ◽  
Particle Growth ◽  
Particle Formation ◽  
Oxidation Products ◽  
Chemical Compositions ◽  
New Particle Formation ◽  
Voc Oxidation

Abstract. Aerosol physical and chemical properties and trace gas concentrations were measured during the QUEST field campaign in March–April 2003, in Hyytiälä, Finland. Our aim was to understand the role of oxidation products of VOC's such as mono- and sesquiterpenes in atmospheric nucleation events. Particle chemical compositions were measured using the Aerodyne Aerosol Mass Spectrometer, and chemical compositions of aerosol samples collected with low-pressure impactors and a high volume sampler were analysed using a number of techniques. The results indicate that during and after new particle formation, all particles larger than 50 nm in diameter contained similar organic substances that are likely to be mono- and sesquiterpene oxidation products. The oxidation products identified in the high volume samples were shown to be mostly aldehydes. In order to study the composition of particles in the 10–50 nm range, we made use of Tandem Differential Mobility Analyzer results. We found that during nucleation events, both 10 and 50 nm particle growth factors due to uptake of ethanol vapour correlate strongly with gas-phase monoterpene oxidation product (MTOP) concentrations, indicating that the organic constituents of particles smaller than 50 nm in diameter are at least partly similar to those of larger particles. We furthermore showed that particle growth rates during the nucleation events are correlated with the gas-phase MTOP concentrations. This indicates that VOC oxidation products may have a key role in determining the spatial and temporal features of the nucleation events. This conclusion was supported by our aircraft measurements of new 3–10 nm particle concentrations, which showed that the nucleation event on 28 March 2003, started at the ground layer, i.e. near the VOC source, and evolved together with the mixed layer. Furthermore, no new particle formation was detected upwind away from the forest, above the frozen Gulf of Bothnia.

scholarly journals The role of VOC oxidation products in continental new particle formation

2007 ◽  
Vol 7 (3) ◽  
pp. 7819-7841 ◽  
Author(s):  
A. Laaksonen ◽  
M. Kulmala ◽  
C. D. O'Dowd ◽  
J. Joutsensaari ◽  
P. Vaattovaara ◽  
...  
Keyword(s):  
Gas Phase ◽  
Chemical Properties ◽  
High Volume ◽  
Particle Growth ◽  
Particle Formation ◽  
Oxidation Products ◽  
Chemical Compositions ◽  
New Particle Formation ◽  
Voc Oxidation

Abstract. Aerosol physical and chemical properties and trace gas concentrations were measured during the QUEST field campaign in March–April, 2003, in Hyytiälä, Finland. Our aim was to understand the role of oxidation products of VOC's such as mono- and sesquiterpenes in atmospheric nucleation events. Particle chemical compositions were measured using the Aerodyne Aerosol Mass Spectrometer, and chemical compositions of aerosol samples collected with low-pressure impactors and a high volume sampler were analysed using a number of techniques. The results indicate that during and after new particle formation, all particles larger than 50 nm in diameter contained similar organic substances that are likely to be mono- and sesquiterpene oxidation products. The oxidation products identified in the high volume samples were shown to be mostly aldehydes. In order to study the composition of particles in the 10–50 nm range, we made use of Tandem Differential Mobility Analyzer results. We found that during nucleation events, both 10 and 50 nm particle growth factors due to uptake of ethanol vapour correlate strongly with gas-phase monoterpene oxidation product (MTOP) concentrations, indicating that the organic constituents of particles smaller than 50 nm in diameter are at least partly similar to those of larger particles. We furthermore showed that particle growth rates during the nucleation events are correlated with the gas-phase MTOP concentrations. This indicates that VOC oxidation products may have a key role in determining the spatial and temporal features of the nucleation events. This conclusion was supported by our aircraft measurements of new 3–10 nm particle concentrations, which showed that the nucleation event on 28 March 2003, started at the ground layer, i.e. near the VOC source, and evolved together with the mixed layer. Furthermore, no new particle formation was detected upwind away from the forest, above the frozen Gulf of Bothnia.

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 Air pollution control and decreasing new particle formation lead to strong climate warming

2011 ◽  
Vol 11 (9) ◽  
pp. 25991-26007 ◽  
Author(s):  
R. Makkonen ◽  
A. Asmi ◽  
V.-M. Kerminen ◽  
M. Boy ◽  
A. Arneth ◽  
...  
Keyword(s):  
Air Pollution ◽  
Pollution Control ◽  
Cloud Condensation Nuclei ◽  
Particle Formation ◽  
Control Measures ◽  
Air Pollution Control ◽  
New Particle Formation ◽  
Anthropogenic Aerosol ◽  
Aerosol Forcing ◽  
Year 2000

Abstract. The number of cloud droplets determines several climatically relevant cloud properties. A major cause for the high uncertainty in the indirect aerosol forcing is the availability of cloud condensation nuclei (CCN), which in turn is highly sensitive to atmospheric new particle formation. Here we present the effect of new particle formation on anthropogenic aerosol forcing in present-day (year 2000) and future (year 2100) conditions. The total aerosol forcing (−1.61 W m−2 in year 2000) is simulated to be greatly reduced in the future, to −0.23 W m−2, mainly due to decrease in SO2 emissions and resulting decrease in new particle formation. With the total aerosol forcing decreasing in response to air pollution control measures taking effect, warming from increased greenhouse gas concentrations can potentially increase at a very rapid rate.

scholarly journals New insights into nocturnal nucleation

2012 ◽  
Vol 12 (9) ◽  
pp. 4297-4312 ◽  
Author(s):  
I. K. Ortega ◽  
T. Suni ◽  
M. Boy ◽  
T. Grönholm ◽  
H. E. Manninen ◽  
...  
Keyword(s):  
Quantum Chemical ◽  
Aerosol Particles ◽  
Particle Formation ◽  
Nucleation And Growth ◽  
Oxidation Products ◽  
New Particle Formation ◽  
Aerosol Dynamics ◽  
Different Types ◽  
Consistent Manner ◽  
Dynamics Models

Abstract. Formation of new aerosol particles by nucleation and growth is a significant source of aerosols in the atmosphere. New particle formation events usually take place during daytime, but in some locations they have been observed also at night. In the present study we have combined chamber experiments, quantum chemical calculations and aerosol dynamics models to study nocturnal new particle formation. All our approaches demonstrate, in a consistent manner, that the oxidation products of monoterpenes play an important role in nocturnal nucleation events. By varying the conditions in our chamber experiments, we were able to reproduce the very different types of nocturnal events observed earlier in the atmosphere. The exact strength, duration and shape of the events appears to be sensitive to the type and concentration of reacting monoterpenes, as well as the extent to which the monoterpenes are exposed to ozone and potentially other atmospheric oxidants.

scholarly journals Secondary organic aerosol production from pinanediol, a semi-volatile surrogate for first-generation oxidation products of monoterpenes

2018 ◽  
Vol 18 (9) ◽  
pp. 6171-6186 ◽  
Author(s):  
Penglin Ye ◽  
Yunliang Zhao ◽  
Wayne K. Chuang ◽  
Allen L. Robinson ◽  
Neil M. Donahue
Keyword(s):  
Organic Compounds ◽  
First Generation ◽  
Secondary Organic Aerosol ◽  
Organic Aerosol ◽  
Particle Formation ◽  
Oxidation Products ◽  
Basis Set ◽  
New Particle Formation ◽  
Aerosol Mass ◽  
Volatile Precursor

Abstract. We have investigated the production of secondary organic aerosol (SOA) from pinanediol (PD), a precursor chosen as a semi-volatile surrogate for first-generation oxidation products of monoterpenes. Observations at the CLOUD facility at CERN have shown that oxidation of organic compounds such as PD can be an important contributor to new-particle formation. Here we focus on SOA mass yields and chemical composition from PD photo-oxidation in the CMU smog chamber. To determine the SOA mass yields from this semi-volatile precursor, we had to address partitioning of both the PD and its oxidation products to the chamber walls. After correcting for these losses, we found OA loading dependent SOA mass yields from PD oxidation that ranged between 0.1 and 0.9 for SOA concentrations between 0.02 and 20 µg m−3, these mass yields are 2–3 times larger than typical of much more volatile monoterpenes. The average carbon oxidation state measured with an aerosol mass spectrometer was around −0.7. We modeled the chamber data using a dynamical two-dimensional volatility basis set and found that a significant fraction of the SOA comprises low-volatility organic compounds that could drive new-particle formation and growth, which is consistent with the CLOUD observations.

scholarly journals The link between atmospheric radicals and newly formed particles at a spruce forest site in Germany

2014 ◽  
Vol 14 (19) ◽  
pp. 10823-10843 ◽  
Author(s):  
B. Bonn ◽  
E. Bourtsoukidis ◽  
T. S. Sun ◽  
H. Bingemer ◽  
L. Rondo ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Inorganic Compounds ◽  
Empirical Relationship ◽  
Particle Formation ◽  
Climate Feedback ◽  
Activation Process ◽  
Forest Site ◽  
Peroxy Radicals ◽  
New Particle Formation ◽  
The Impact

Abstract. It has been claimed for more than a century that atmospheric new particle formation is primarily influenced by the presence of sulfuric acid. However, the activation process of sulfuric acid related clusters into detectable particles is still an unresolved topic. In this study we focus on the PARADE campaign measurements conducted during August/September 2011 at Mt Kleiner Feldberg in central Germany. During this campaign a set of radicals, organic and inorganic compounds and oxidants and aerosol properties were measured or calculated. We compared a range of organic and inorganic nucleation theories, evaluating their ability to simulate measured particle formation rates at 3 nm in diameter (J3) for a variety of different conditions. Nucleation mechanisms involving only sulfuric acid tentatively captured the observed noon-time daily maximum in J3, but displayed an increasing difference to J3 measurements during the rest of the diurnal cycle. Including large organic radicals, i.e. organic peroxy radicals (RO2) deriving from monoterpenes and their oxidation products, in the nucleation mechanism improved the correlation between observed and simulated J3. This supports a recently proposed empirical relationship for new particle formation that has been used in global models. However, the best match between theory and measurements for the site of interest was found for an activation process based on large organic peroxy radicals and stabilised Criegee intermediates (sCI). This novel laboratory-derived algorithm simulated the daily pattern and intensity of J3 observed in the ambient data. In this algorithm organic derived radicals are involved in activation and growth and link the formation rate of smallest aerosol particles with OH during daytime and NO3 during night-time. Because the RO2 lifetime is controlled by HO2 and NO we conclude that peroxy radicals and NO seem to play an important role for ambient radical chemistry not only with respect to oxidation capacity but also for the activation process of new particle formation. This is supposed to have significant impact of atmospheric radical species on aerosol chemistry and should be taken into account when studying the impact of new particles in climate feedback cycles.

scholarly journals Modelling the formation of organic particles in the atmosphere

2003 ◽  
Vol 3 (6) ◽  
pp. 6147-6178 ◽  
Author(s):  
T. Anttila ◽  
V.-M. Kerminen ◽  
M. Kulmala ◽  
A. Laaksonen ◽  
C. O’Dowd
Keyword(s):  
Sulphuric Acid ◽  
Particle Formation ◽  
Water Soluble ◽  
Forest Site ◽  
Initial Growth ◽  
Aerosol Formation ◽  
Stable Clusters ◽  
Kohler Theory ◽  
Organic Particles ◽  
Organic Particle

Abstract. A modelling study investigating the formation of organic particles from inorganic, thermodynamically stable clusters was carried out. A recently-developed theory, the so-called nano-Köhler theory, which describes a thermodynamic equilibrium between a nanometer-size cluster, water and water-soluble organic compound, was implemented in a dynamical model along with a treatment of the appropriate aerosol and gas-phase processes. The obtained results suggest that both gaseous sulphuric acid and organic vapours contribute to organic particle formation. The initial growth of freshly-nucleated clusters having a diameter around 1 nm is driven by condensation of gaseous sulphuric acid and by a lesser extent cluster self-coagulation. After the clusters have reached sizes of around 2 nm in diameter, low-volatile organic vapours start to condense spontaneously into the clusters, thereby accelerating their growth to detectable sizes. A shortage of gaseous sulphuric acid or organic vapours limit, or suppress altogether, the particle formation, since freshly-nucleated clusters are rapidly coagulated away by pre-existing particles. The obtained modelling results were applied to explaining the observed seasonal cycle in the number of aerosol formation events in a continental forest site.

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