scholarly journals Traffic-originated nanocluster emission exceeds H<sub>2</sub>SO<sub>4</sub>-driven photochemical new particle formation in an urban area

2020 ◽  
Vol 20 (1) ◽  
pp. 1-13 ◽  
Author(s):  
Miska Olin ◽  
Heino Kuuluvainen ◽  
Minna Aurela ◽  
Joni Kalliokoski ◽  
Niina Kuittinen ◽  
...  
Keyword(s):  
Solar Radiation ◽  
Particle Formation ◽  
Urban Environments ◽  
Urban Traffic ◽  
Photochemical Oxidation ◽  
Traffic Density ◽  
Formation Mechanisms ◽  
New Particle Formation ◽  
Aerosol Formation ◽  
Vehicle Exhaust

Abstract. Elevated ambient concentrations of sub-3 nm particles (nanocluster aerosol, NCA) are generally related to atmospheric new particle formation events, usually linked with gaseous sulfuric acid (H2SO4) produced via photochemical oxidation of sulfur dioxide. According to our measurement results of H2SO4 and NCA concentrations, traffic density, and solar irradiance at an urban traffic site in Helsinki, Finland, the view of aerosol formation in traffic-influenced environments is updated by presenting two separate and independent pathways of traffic affecting the atmospheric NCA concentrations: by acting as a direct nanocluster source and by influencing the production of H2SO4. As traffic density in many areas is generally correlated with solar radiation, it is likely that the influence of traffic-related nanoclusters has been hidden in the diurnal variation and is thus underestimated because new particle formation events also follow the diurnal cycle of sunlight. Urban aerosol formation studies should, therefore, be updated to include the proposed formation mechanisms. The formation of H2SO4 in urban environments is here separated into two routes: primary H2SO4 is formed in hot vehicle exhaust and is converted rapidly to the particle phase; secondary H2SO4 results from the combined effect of emitted gaseous precursors and available solar radiation. A rough estimation demonstrates that ∼85 % of the total NCA and ∼68 % of the total H2SO4 in urban air at noontime at the measurement site are contributed by traffic, indicating the importance of traffic emissions.

scholarly journals Traffic-originated nanocluster emission exceeds H<sub>2</sub>SO<sub>4</sub>-driven photochemical new particle formation in an urban area

2019 ◽  
Author(s):  
Miska Olin ◽  
Heino Kuuluvainen ◽  
Minna Aurela ◽  
Joni Kalliokoski ◽  
Niina Kuittinen ◽  
...  
Keyword(s):  
Solar Radiation ◽  
Particle Formation ◽  
Urban Environments ◽  
Urban Traffic ◽  
Photochemical Oxidation ◽  
Traffic Density ◽  
Formation Mechanisms ◽  
New Particle Formation ◽  
Aerosol Formation ◽  
Vehicle Exhaust

Abstract. Elevated ambient concentrations of sub-3 nm particles (nanocluster aerosol, NCA) are generally related to atmospheric new particle formation events, usually linked with gaseous sulfuric acid (H2SO4) produced via photochemical oxidation of sulfur dioxide. According to our measurement results of H2SO4 and NCA concentrations, traffic density, and solar irradiance at an urban traffic site in Helsinki, Finland, the view of aerosol formation in traffic-influenced environments is updated by presenting two separate and independent pathways of traffic affecting the atmospheric NCA concentrations: by acting as a direct nanocluster source, and by influencing the production of H2SO4. As traffic density is frequently correlated with solar radiation, it is likely that the influence of traffic-related nanoclusters has been hidden in the diurnal variation, and is thus underestimated because new particle formation events also follow the diurnal cycle of sunlight. Urban aerosol formation studies should, therefore, be updated to include the proposed formation mechanisms. Additionally, the directly emitted NCA poses a potentially elevated health risk, highlighting the need for quantifying the source and loadings in populated areas. The formation of H2SO4 in urban environments is here separated in two routes: primary H2SO4 is formed in hot vehicle exhaust and is converted rapidly to particle phase; secondary H2SO4 results from the combined effect of emitted gaseous precursors and available solar radiation.

scholarly journals Particle concentration and flux dynamics in the atmospheric boundary layer as the indicator of formation mechanism

2011 ◽  
Vol 11 (12) ◽  
pp. 5591-5601 ◽  
Author(s):  
J. Lauros ◽  
A. Sogachev ◽  
S. Smolander ◽  
H. Vuollekoski ◽  
S.-L. Sihto ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Atmospheric Boundary Layer ◽  
Formation Mechanism ◽  
Turbulent Transport ◽  
Particle Formation ◽  
Formation Mechanisms ◽  
Forest Site ◽  
Aerosol Formation ◽  
Flux Dynamics ◽  
Layer Deposition

Abstract. We carried out column model simulations to study particle fluxes and deposition and to evaluate different particle formation mechanisms at a boreal forest site in Finland. We show that kinetic nucleation of sulphuric acid cannot be responsible for new particle formation alone as the simulated vertical profile of particle number concentration does not correspond to observations. Instead organic induced nucleation leads to good agreement confirming the relevance of the aerosol formation mechanism including organic compounds emitted by the biosphere. The simulation of aerosol concentration within the atmospheric boundary layer during nucleation event days shows a highly dynamical picture, where particle formation is coupled with chemistry and turbulent transport. We have demonstrated the suitability of our turbulent mixing scheme in reproducing the most important characteristics of particle dynamics within the boundary layer. Deposition and particle flux simulations show that deposition affects noticeably only the smallest particles in the lowest part of the atmospheric boundary layer.

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 SO<sub>2</sub> and NH<sub>3</sub> emissions enhance organosulfur compounds and fine particle formation from the photooxidation of a typical aromatic hydrocarbon

2021 ◽  
Vol 21 (10) ◽  
pp. 7963-7981
Author(s):  
Zhaomin Yang ◽  
Li Xu ◽  
Narcisse T. Tsona ◽  
Jianlong Li ◽  
Xin Luo ◽  
...  
Keyword(s):  
Mass Spectrometry ◽  
Oxidation Mechanism ◽  
Particle Formation ◽  
Urban Atmosphere ◽  
Mass Spectrometry Analysis ◽  
Formation Mechanisms ◽  
Chemical Compositions ◽  
Organosulfur Compounds ◽  
Aerosol Formation ◽  
Secondary Aerosol

Abstract. Aromatic hydrocarbons can dominate the volatile organic compound budget in the urban atmosphere. Among them, 1,2,4-trimethylbenzene (TMB), mainly emitted from solvent use, is one of the most important secondary organic aerosol (SOA) precursors. Although atmospheric SO2 and NH3 levels can affect secondary aerosol formation, the influenced extent of their impact and their detailed driving mechanisms are not well understood. The focus of the present study is to examine the chemical compositions and formation mechanisms of SOA from TMB photooxidation influenced by SO2 and/or NH3. Here, we show that SO2 emission could considerably enhance aerosol particle formation due to SO2-induced sulfate generation and acid-catalyzed heterogeneous reactions. Orbitrap mass spectrometry measurements revealed the generation of not only typical TMB products but also hitherto unidentified organosulfates (OSs) in SO2-added experiments. The OSs designated as being of unknown origin in earlier field measurements were also detected in TMB SOA, indicating that atmospheric OSs might also be originated from TMB photooxidation. For NH3-involved experiments, results demonstrated a positive correlation between NH3 levels and particle volume as well as number concentrations. The effects of NH3 on SOA composition were slight under SO2-free conditions but stronger in the presence of SO2. A series of multifunctional products with carbonyl, alcohols, and nitrate functional groups were tentatively characterized in NH3-involved experiments based on infrared spectra and mass spectrometry analysis. Plausible formation pathways were proposed for detected products in the particle phase. The volatility distributions of products, estimated using parameterization methods, suggested that the detected products gradually condense onto the nucleation particles to contribute to aerosol formation and growth. Our results suggest that strict control of SO2 and NH3 emissions might remarkably reduce organosulfates and secondary aerosol burden in the atmosphere. Updating the aromatic oxidation mechanism in models could result in more accurate treatment of particle formation for urban regions with considerable SO2, NH3, and aromatics emissions.

Studying new particle formation from chemical emissions from sea surface using  ship-borne air-sea-interaction tanks

2021 ◽  
Author(s):  
Maija Peltola ◽  
Manon Rocco ◽  
Neill Barr ◽  
Erin Dunne ◽  
James Harnwell ◽  
...  
Keyword(s):  
Marine Biology ◽  
Cloud Condensation Nuclei ◽  
Aerosol Particles ◽  
Chemical Species ◽  
Particle Formation ◽  
Biological Properties ◽  
The European Union ◽  
New Particle Formation ◽  
Aerosol Formation ◽  
Horizon 2020

&lt;p&gt;Even though oceans cover over 70% of the Earth&amp;#8217;s surface, the ways in which oceans interact with climate are not fully known. Marine micro-organisms such as phytoplankton can play an important role in regulating climate by releasing different chemical species into air. In air these chemical species can react and form new aerosol particles. If grown to large enough sizes, aerosols can influence climate by acting as cloud condensation nuclei which influence the formation and properties of clouds. Even though a connection of marine biology and climate through aerosol formation was first proposed already over 30 years ago, the processes related to this connection are still uncertain.&lt;/p&gt;&lt;p&gt;To unravel how seawater properties affect aerosol formation and to identify which chemical species are responsible for aerosol formation, we built two Air-Sea-Interaction Tanks (ASIT) that isolate 1000 l of seawater and 1000 l of air directly above the water. The used seawater was collected from different locations during a ship campaign on board the R/V Tangaroa in the South West Pacific Ocean, close to Chatham Rise, east of New Zealand. Seawater from one location was kept in the tanks for 2-3 days and then changed. By using seawater collected from different locations, we could obtain water with different biological populations. To monitor the seawater, we took daily samples to determine its chemical and biological properties.&lt;/p&gt;&lt;p&gt;The air in the tanks was continuously flushed with particle filtered air. This way the air had on average 40 min to interact with the seawater surface before being sampled. Our air sampling was continuous and consisted of aerosol and air chemistry measurements. The instrumentation included measurements of aerosol number concentration from 1 to 500 nm and&amp;#160; chemical species ranging from ozone and sulphur dioxide to volatile organic compounds and chemical composition of molecular clusters.&lt;/p&gt;&lt;p&gt;Joining the seawater and atmospheric data together can give us an idea of what chemical species are emitted from the water into the atmosphere and whether these species can form new aerosol particles. Our preliminary results show a small number of particles in the freshly nucleated size range of 1-3 nm in the ASIT headspaces, indicating that new aerosol particles can form in the ASIT headspaces. In this presentation, we will also explore which chemical species could be responsible for aerosol formation and which plankton groups could be related to the emissions of these species. Combining these results with ambient data and modelling work can shed light on how important new particle formation from marine sources is for climate.&lt;/p&gt;&lt;p&gt;Acknowledgements: Sea2Cloud project is funded by European Research Council (ERC) under the European Union&amp;#8217;s Horizon 2020 research and innovation programme (Grant agreement No. 771369).&lt;/p&gt;

scholarly journals Formation and characteristics of ions and charged aerosol particles in a native Australian Eucalypt forest

2008 ◽  
Vol 8 (1) ◽  
pp. 129-139 ◽  
Author(s):  
T. Suni ◽  
M. Kulmala ◽  
A. Hirsikko ◽  
T. Bergman ◽  
L. Laakso ◽  
...  
Keyword(s):  
Growth Rates ◽  
Aerosol Particles ◽  
Particle Formation ◽  
Cluster Ions ◽  
Native Forest ◽  
New Particle Formation ◽  
Aerosol Formation ◽  
Eucalypt Forest ◽  
The World ◽  
Strong Source

Abstract. Biogenic aerosol formation is likely to contribute significantly to the global aerosol load. In recent years, new-particle formation has been observed in various ecosystems around the world but hardly any measurements have taken place in the terrestrial Southern Hemisphere. Here, we report the first results of atmospheric ion and charged particle concentrations as well as of new-particle formation in a Eucalypt forest in Tumbarumba, South-East Australia, from July 2005 to October 2006. The measurements were carried out with an Air Ion Spectrometer (AIS) with a size range from 0.34 to 40 nm. The Eucalypt forest was a very strong source of new aerosol particles. Daytime aerosol formation took place on 52% of days with acceptable data, which is 2–3 times as often as in the Nordic boreal zone. Average growth rates for negative/positive 1.5–3 nm particles during these formation events were 2.89/2.68 nmh−1, respectively; for 3-7 nm particles 4.26/4.03, and for 7–20 nm particles 8.90/7.58 nmh−1, respectively. The growth rates for large ions were highest when the air was coming from the native forest which suggests that the Eucalypts were a strong source of condensable vapours. Average concentrations of cluster ions (0.34–1.8 nm) were 2400/1700 cm−3 for negative/positive ions, very high compared to most other measurements around the world. One reason behind these high concentrations could be the strong radon efflux from the soils around the Tumbarumba field site. Furthermore, comparison between night-time and daytime concentrations supported the view that cluster ions are produced close to the surface within the boundary layer also at night but that large ions are mostly produced in daytime. Finally, a previously unreported phenomenon, nocturnal aerosol formation, appeared in 32% of the analysed nights but was clustered almost entirely within six months from summer to autumn in 2006. From January to May, nocturnal formation was 2.5 times as frequent as daytime formation. Therefore, it appears that in summer and autumn, nocturnal production was the major mechanism for aerosol formation in Tumbarumba.

scholarly journals Cold oceans enhance terrestrial new-particle formation in near-coastal forests

2009 ◽  
Vol 9 (22) ◽  
pp. 8639-8650 ◽  
Author(s):  
T. Suni ◽  
L. Sogacheva ◽  
J. Lauros ◽  
H. Hakola ◽  
J. Bäck ◽  
...  
Keyword(s):  
Radiative Forcing ◽  
Vegetation Index ◽  
Climate Models ◽  
Particle Formation ◽  
New Particle Formation ◽  
Aerosol Formation ◽  
Coastal Forests ◽  
Organic Precursor ◽  
North East ◽  
The North

Abstract. The world's forests produce atmospheric aerosol by emitting volatile organic compounds (VOC) which, after being oxidized in the atmosphere, readily condense on the omnipresent nanometer-sized nuclei and grow them to climatically relevant sizes. The cooling effect of aerosols is the greatest uncertainty in current climate models and estimates of radiative forcing. Therefore, identifying the environmental factors influencing the biogenic formation of aerosols is crucial. In this paper, we connected biogenic aerosol formation events observed in a Eucalypt forest in South-East Australia during July 2005–December 2006 to air mass history using 96-h back trajectories. Formation of new particles was most frequent in the dry westerly and south-westerly air masses. According to NDVI (Normalized Difference Vegetation Index) measurements, photosynthesis was not significantly higher in this direction compared to the north-east direction. It is unlikely, therefore, that differences in photosynthesis-derived organic precursor emissions would have been significant enough to lead to the clear difference in NPF frequency between these two directions. Instead, the high evaporation rates above the Pacific Ocean resulted in humid winds from the north-east that effectively suppressed new-particle formation in the forest hundreds of kilometers inland. No other factor varied as significantly in tune with new-particle formation as humidity and we concluded that, in addition to local meteorological factors in the forest, the magnitude of evaporation from oceans hundreds of kilometers upwind can effectively suppress or enhance new-particle formation. Our findings indicate that, unlike warm waters, the cold polar oceans provide excellent clean and dry background air that enhances aerosol formation above near-coastal forests in Fennoscandia and South-East Australia.

scholarly journals New particle formation from sulfuric acid and ammonia: nucleation and growth model based on thermodynamics derived from CLOUD measurements for a wide range of conditions

2019 ◽  
Author(s):  
Andreas Kürten
Keyword(s):  
Sulfuric Acid ◽  
Growth Model ◽  
Thermodynamic Data ◽  
Particle Formation ◽  
Nucleation And Growth ◽  
Aerosol Size Distribution ◽  
Formation Mechanisms ◽  
Strong Impact ◽  
New Particle Formation ◽  
Wide Range

Abstract. Understanding new particle formation and growth is important because of the strong impact of these processes on climate and air quality. Measurements to elucidate the main new particle formation mechanisms are essential; however, these mechanisms have to be implemented in models to estimate their impact on the regional and global scale. Parameterizations are computationally cheap ways of implementing nucleation schemes in models but they have their limitations, as they do not necessarily include all relevant parameters. Process models using sophisticated nucleation schemes can be useful for the generation of look-up tables in large-scale models or for the analysis of individual new particle formation events. In addition, some other important properties can be derived from a process model that implicitly calculates the evolution of the full aerosol size distribution, e.g., the particle growth rates. Within this study, a model (SANTIAGO, Sulfuric acid Ammonia NucleaTIon And GrOwth model) is constructed that simulates new particle formation starting from the monomer of sulfuric acid up to a particle size of several hundred nanometers. The smallest sulfuric acid clusters containing one to four acid molecules and varying amount of base (ammonia) are allowed to evaporate in the model, whereas growth beyond the pentamer (5 sulfuric acid molecules) is assumed to be entirely collision-controlled. The main goal of the present study is to derive appropriate thermodynamic data needed to calculate the cluster evaporation rates as a function of temperature. These data are derived numerically from CLOUD (Cosmics Leaving OUtdoor Droplets) chamber new particle formation rates for neutral sulfuric acid-water-ammonia nucleation at temperatures between 208 K and 292 K. The numeric methods include an optimization scheme to derive the best estimates for the thermodynamic data (dH and dS) and a Monte Carlo method to derive their probability density functions. The derived data are compared to literature values. Using different data sets for dH and dS in SANTIAGO detailed comparison between model results and measured CLOUD new particle formation rates is discussed.

scholarly journals Frequency of new particle formation events in the urban Mediterranean climate

2014 ◽  
Vol 14 (19) ◽  
pp. 26463-26494 ◽  
Author(s):  
M. Brines ◽  
M. Dall'Osto ◽  
D. C. S. Beddows ◽  
R. M. Harrison ◽  
F. Gómez-Moreno ◽  
...  
Keyword(s):  
Los Angeles ◽  
Ultrafine Particles ◽  
Mediterranean Climate ◽  
Particle Number ◽  
Road Traffic ◽  
Particle Formation ◽  
Urban Environments ◽  
Urban Atmosphere ◽  
Size Distributions ◽  
New Particle Formation

Abstract. Road traffic emissions are often considered the main source of ultrafine particles (UFP, diameter smaller than 100 nm) in urban environments. However, recent studies have shown that – in southern European urban regions at least – new particle formation events can also contribute to UFP. In order to quantify such events we systematically studied four cities with a Mediterranean climate: Barcelona, Madrid, Rome and Los Angeles. The city of Brisbane is also included in our study due to its similar climate. Five long term datasets (from 3 months to 2 years) of fine and ultrafine particle number size distributions (measured by SMPS, Scanning Mobility Particle Sizer) were analysed. By applying k-Means clustering analysis, we categorized the collected aerosol size distributions in four main classes: "Traffic" (prevailing 41–63% of the time), "Background Pollution" (6–53%), "Nucleation" (6–33%) and "Specific case" (7–20%) the latter being site specific. The daily variation of the average UFP concentrations for a typical nucleation day at each site revealed a similar pattern for all cities, with three distinct particle bursts. A morning and an evening spike reflected traffic rush hours, whereas a third one at midday showed new particle formation events. This work shows that the average occurrence of particle size spectra dominated by new particle formation events was 18% of the time, showing the importance of this process as a source of UFP in the Mediterranean urban atmosphere. Furthermore, in a number of the studied cities, particle number concentration averaged daily profiles for the whole study periods clearly showed the same three particle bursts. This reveals nucleation events as a relevant contributor to the average daily urban exposure to UFP in Mediterranean urban environments.

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