scholarly journals Comprehensive modelling study on observed new particle formation at the SORPES station in Nanjing, China

2016 ◽  
Vol 16 (4) ◽  
pp. 2477-2492 ◽  
Author(s):  
Xin Huang ◽  
Luxi Zhou ◽  
Aijun Ding ◽  
Ximeng Qi ◽  
Wei Nie ◽  
...  
Keyword(s):  
Transport Model ◽  
Anthropogenic Activities ◽  
Lower Troposphere ◽  
Particle Formation ◽  
Oxidation Products ◽  
New Particle Formation ◽  
Aerosol Formation ◽  
The Yrd ◽  
Modelling System ◽  
Modelling Study

Abstract. New particle formation (NPF) has been investigated intensively during the last 2 decades because of its influence on aerosol population and the possible contribution to cloud condensation nuclei. However, intensive measurements and modelling activities on this topic in urban metropolitan areas in China with frequent high-pollution episodes are still very limited. This study provides results from a comprehensive modelling study on the occurrence of NPF events in the western part of the Yangtze River Delta (YRD) region, China. The comprehensive modelling system, which combines the WRF-Chem (the Weather Research and Forecasting model coupled with Chemistry) regional chemical transport model and the MALTE-BOX sectional box model (the model to predict new aerosol formation in the lower troposphere), was shown to be capable of simulating atmospheric nucleation and subsequent growth. Here we present a detailed discussion of three typical NPF days, during which the measured air masses were notably influenced by either anthropogenic activities, biogenic emissions, or mixed ocean and continental sources. Overall, simulated NPF events were generally in good agreement with the corresponding measurements, enabling us to get further insights into NPF processes in the YRD region. Based on the simulations, we conclude that biogenic organic compounds, particularly monoterpenes, play an essential role in the initial condensational growth of newly formed clusters through their low-volatility oxidation products. Although some uncertainties remain in this modelling system, this method provides a possibility to better understand particle formation and growth processes.

scholarly journals First comprehensive modelling study on observed new particle formation at the SORPES station in Nanjing, China

2015 ◽  
Vol 15 (19) ◽  
pp. 27501-27538 ◽  
Author(s):  
X. Huang ◽  
L. X. Zhou ◽  
A. J. Ding ◽  
X. M. Qi ◽  
W. Nie ◽  
...  
Keyword(s):  
Transport Model ◽  
Anthropogenic Activities ◽  
Lower Troposphere ◽  
Particle Formation ◽  
Oxidation Products ◽  
New Particle Formation ◽  
Aerosol Formation ◽  
The Yrd ◽  
Modelling System ◽  
Modelling Study

Abstract. New particle formation (NPF) has been investigated intensively during the last two decades because of its influence on aerosol population and the possible contribution to cloud condensation nuclei. However, intensive measurements and modelling activities on this topic in urban metropolitans in China with frequently high pollution episodes are still very limited. This study provides results from a comprehensive modelling study on the occurrence of new particle formation events in the western part of the Yangtze River Delta region (YRD), China. The comprehensive modelling system, which combines regional chemical transport model WRF-Chem (the Weather Research and Forecasting model coupled with Chemistry) and the sectional box model MALTE-BOX (the model to predict new aerosol formation in the lower troposphere), was shown to be capable of simulating atmospheric nucleation and subsequent growth. Here we present a detailed discussion of three typical NPF days, during which the measured air masses were notably influenced by either anthropogenic activities, biogenic emissions, or mixed ocean and continental sources. Overall, simulated NPF events were generally in good agreement with the corresponding measurements, enabling us to get further insights into NPF processes in the YRD region. Based on the simulations, we conclude that besides gas-phase sulphuric acid, biogenic organic compounds, particularly monoterpenes, play an essential role in condensational growth of newly formed clusters and probably also in the particle formation process through their low volatile oxidation products. Although some uncertainties remain in this modelling system, this method provides a possibility to better understand the NPF processes.

scholarly journals Ternary homogeneous nucleation of H<sub>2</sub>SO<sub>4</sub>, NH<sub>3</sub>, and H<sub>2</sub>O under conditions relevant to the lower troposphere

2010 ◽  
Vol 10 (9) ◽  
pp. 22395-22414 ◽  
Author(s):  
D. Benson ◽  
A. Markovich ◽  
S.-H. Lee
Keyword(s):  
Nucleation Rate ◽  
Homogeneous Nucleation ◽  
Enhancement Factor ◽  
Lower Troposphere ◽  
Global Scale ◽  
Particle Formation ◽  
New Particle Formation ◽  
Aerosol Formation ◽  
Laboratory Measurements ◽  
Atmospheric Observations

Abstract. Ternary homogeneous nucleation (THN) of H2SO4, NH3 and H2O has been used to explain new particle formation in various atmospheric regions, yet laboratory measurements have failed to reproduce atmospheric observations. Here, we report laboratory observations of THN made under conditions relevant to the lower troposphere (H2SO4 of 106–107 cm−3, NH3 of 0.08–20 ppbv, and 288 K). Our observations show that NH3 can enhance atmospheric H2SO4 aerosol nucleation and the enhancement factor (EF) in nucleation rate due to NH3 increases linearly with increasing NH3 and increases exponentially with decreasing H2SO4 and RH. The critical clusters of ternary homogeneous nucleation contain 3–5 molecules of H2SO4, 1–4 molecules of H2O, and only 1 molecule of NH3. The composition of H2SO4 and H2O in critical clusters and the threshold of H2SO4 concentrations required for the unit nucleation rate both do not vary in the presence and absence of NH3. These observations can be directly used to improve aerosol nucleation models to correctly assess how man-made SO2 and NH3 affect aerosol formation and CCN production at the global scale.

scholarly journals The simulations of sulfuric acid concentration and new particle formation in an urban atmosphere in China

2013 ◽  
Vol 13 (6) ◽  
pp. 14977-15005
Author(s):  
Z. B. Wang ◽  
M. Hu ◽  
D. Mogensen ◽  
D. L. Yue ◽  
J. Zheng ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Acid Concentration ◽  
Sulfuric Acid Concentration ◽  
Lower Troposphere ◽  
Particle Formation ◽  
Urban Atmosphere ◽  
Chemical Mechanism ◽  
New Particle Formation ◽  
Aerosol Formation ◽  
Surrounding Areas

Abstract. Simulations of sulfuric acid concentration and new particle formation are performed by using the zero-dimensional version of the model MALTE (Model to predict new Aerosol formation in the Lower TropospherE) and measurements from the Campaign of Air Quality Research in Beijing and Surrounding areas (CAREBeijing) in 2008. Chemical reactions from the Master Chemical Mechanism Version 3.2 (MCM v3.2) are used in the model. High correlation (slope = 0.72, R = 0.74) between the modelled and observed sulfuric acid concentrations is found during daytime (06:00–18:00). The aerosol dynamics are simulated by the University of Helsinki Multicomponent Aerosol (UHMA) model including several nucleation mechanisms. The results indicate that the model is able to predict the on- and offset of new particle formation in an urban atmosphere in China. In addition, the number concentrations of newly formed particles in kinetic-type nucleation including homogenous homomolecular (J=K[H2SO4]2) and homogenous heteromolecular nucleation involving organic vapours (J=Khet[H2SO4][Org]) are in satisfactory agreement with the observations. However, the specific organic compounds possibly participate in the nucleation process should be investigated in further studies.

scholarly journals The simulations of sulfuric acid concentration and new particle formation in an urban atmosphere in China

2013 ◽  
Vol 13 (21) ◽  
pp. 11157-11167 ◽  
Author(s):  
Z. B. Wang ◽  
M. Hu ◽  
D. Mogensen ◽  
D. L. Yue ◽  
J. Zheng ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Acid Concentration ◽  
Sulfuric Acid Concentration ◽  
Lower Troposphere ◽  
Particle Growth ◽  
Particle Formation ◽  
Urban Atmosphere ◽  
Chemical Mechanism ◽  
New Particle Formation ◽  
Aerosol Formation

Abstract. Simulations of sulfuric acid concentration and new particle formation are performed by using the zero-dimensional version of the model MALTE (Model to predict new Aerosol formation in the Lower TropospherE) and measurements from the Campaign of Air Quality Research in Beijing and Surrounding areas (CAREBeijing) in 2008. Chemical reactions from the Master Chemical Mechanism version 3.2 (MCM v3.2) are used in the model. High correlation (slope = 0.72, R = 0.74) between the modelled and observed sulfuric acid concentrations is found during daytime (06:00–18:00). The aerosol dynamics are simulated by the University of Helsinki Multicomponent Aerosol (UHMA) model including several nucleation mechanisms. The results indicate that the model is able to predict the on- and offset of new particle formation in an urban atmosphere in China. In addition, the number concentrations of newly formed particles in kinetic-type nucleation including homogenous homomolecular (J=K[H2SO4]2) and homogenous heteromolecular nucleation involving organic vapours (J=Khet[H2SO4][Org]) are in satisfactory agreement with the observations. However, the specific organic compounds that possibly participate in the nucleation process should be investigated in further studies. For the particle growth, only a small fraction of the oxidized total organics condense onto the particles in polluted environments. Meanwhile, the OH and O3 oxidation mechanism contribute 5.5% and 94.5% to the volume concentration of small particles, indicating the particle growth is more controlled by the precursor gases and their oxidation by O3.

scholarly journals Implementation of state-of-the-art ternary new-particle formation scheme to the regional chemical transport model PMCAMx-UF in Europe

2016 ◽  
Vol 9 (8) ◽  
pp. 2741-2754 ◽  
Author(s):  
Elham Baranizadeh ◽  
Benjamin N. Murphy ◽  
Jan Julin ◽  
Saeed Falahat ◽  
Carly L. Reddington ◽  
...  
Keyword(s):  
Transport Model ◽  
Three Dimensional ◽  
Chemical Transport ◽  
Particle Formation ◽  
Radiative Transfer Model ◽  
Transfer Model ◽  
New Particle Formation ◽  
Chemical Transport Model ◽  
Order Of Magnitude ◽  
Adjustment Scheme

Abstract. The particle formation scheme within PMCAMx-UF, a three-dimensional chemical transport model, was updated with particle formation rates for the ternary H2SO4–NH3–H2O pathway simulated by the Atmospheric Cluster Dynamics Code (ACDC) using quantum chemical input data. The model was applied over Europe for May 2008, during which the EUCAARI-LONGREX (European Aerosol Cloud Climate and Air Quality Interactions–Long-Range Experiment) campaign was carried out, providing aircraft vertical profiles of aerosol number concentrations. The updated model reproduces the observed number concentrations of particles larger than 4 nm within 1 order of magnitude throughout the atmospheric column. This agreement is encouraging considering the fact that no semi-empirical fitting was needed to obtain realistic particle formation rates. The cloud adjustment scheme for modifying the photolysis rate profiles within PMCAMx-UF was also updated with the TUV (Tropospheric Ultraviolet and Visible) radiative-transfer model. Results show that, although the effect of the new cloud adjustment scheme on total number concentrations is small, enhanced new-particle formation is predicted near cloudy regions. This is due to the enhanced radiation above and in the vicinity of the clouds, which in turn leads to higher production of sulfuric acid. The sensitivity of the results to including emissions from natural sources is also discussed.

scholarly journals Secondary organic aerosol in the global aerosol – chemistry transport model Oslo CTM2

2007 ◽  
Vol 7 (3) ◽  
pp. 9053-9092 ◽  
Author(s):  
C. R. Hoyle ◽  
T. Berntsen ◽  
G. Myhre ◽  
I. S. A. Isaksen
Keyword(s):  
Ammonium Sulphate ◽  
Secondary Organic Aerosol ◽  
Transport Model ◽  
Model Simulation ◽  
Anthropogenic Activities ◽  
Organic Aerosol ◽  
Oxidation Products ◽  
Total Production ◽  
Chemical Transport Model ◽  
Sulphate Aerosol

Abstract. The global chemical transport model Oslo CTM2 has been extended to include the formation, transport and deposition of secondary organic aerosol (SOA). Precursor hydrocarbons which are oxidised to form condensible species include both biogenic species such as terpenes and isoprene, as well as species emitted predominantly by anthropogenic activities (toluene, m-xylene, methylbenzene and other aromatics). A model simulation for 2004 gives an annual global SOA production of approximately 55 Tg. Of this total, 2.5 Tg is found to consist of the oxidation products of anthropogenically emitted hydrocarbons, and about 15 Tg is formed by the oxidation products of isoprene. The global production of SOA is increased to about 76 Tg yr−1 by allowing semi-volatile species to condense on ammonium sulphate aerosol. This brings modelled organic aerosol values closer to those observed, however observations in Europe remain significantly underestimated, raising the possibility of an unaccounted for SOA source. Allowing SOA to form on ammonium sulphate aerosol increases the contribution of anthropogenic SOA from about 4.5% to almost 9% of the total production. The importance of NO3 as an oxidant of SOA precursors is found to vary regionally, causing up to 50%–60% of the total amount of SOA near the surface in polluted regions and less than 25% in more remote areas. This study underscores the need for SOA to be represented in a more realistic way in global aerosol models in order to better reproduce observations of organic aerosol burdens in industrialised and biomass burning regions.

scholarly journals The importance of sesquiterpene oxidation products for secondary organic aerosol formation in a spring-time hemi-boreal forest

2021 ◽  
Author(s):  
Luis M. F. Barreira ◽  
Arttu Ylisirniö ◽  
Iida Pullinen ◽  
Angela Buchholz ◽  
Zijun Li ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Boreal Forest ◽  
Organic Compounds ◽  
Field Experiments ◽  
Complex Mixture ◽  
Particle Formation ◽  
Oxidation Products ◽  
Ionization Mass ◽  
Particle Phase ◽  
Aerosol Formation

Abstract. Secondary organic aerosols (SOA) formed from biogenic volatile organic compounds (BVOCs) constitute a significant fraction of atmospheric particulate matter and have been recognized to affect significantly the climate and air quality. Many laboratory and field experiments have studied SOA particle formation and growth in the recent years. Most of them have focused on a few monoterpenes and isoprene. However, atmospheric SOA particulate mass yields and chemical composition result from a much more complex mixture of oxidation products originating from many BVOCs, including terpenes other than isoprene and monoterpenes. Thus, a large uncertainty still remains regarding the contribution of BVOCs to SOA. In particular, organic compounds formed from sesquiterpenes have not been thoroughly investigated, and their contribution to SOA remains poorly characterized. In this study, a Filter Inlet for Gases and Aerosols (FIGAERO) combined with a high-resolution time-of-flight chemical ionization mass spectrometer (CIMS), with iodide ionization, was used for the simultaneous measurement of gas and particle phase atmospheric SOA. The aim of the study was to evaluate the relative contribution of sesquiterpene oxidation products to SOA in a spring-time hemi-boreal forest environment. Our results revealed that monoterpene and sesquiterpene oxidation products were the main contributors to SOA particles. The chemical composition of SOA particles was compared for times when either monoterpene or sesquiterpene oxidation products were dominant and possible key oxidation products for SOA particle formation were identified. Surprisingly, sesquiterpene oxidation products were the predominant fraction in the particle phase at some periods, while their gas phase concentrations remained much lower than those of monoterpene products. This can be explained by quick and effective partitioning of sesquiterpene products into the particle phase or their efficient removal by dry deposition. The SOA particle volatility determined from measured thermograms increased when the concentration of sesquiterpene oxidation products in SOA particles was higher than that of monoterpenes. Overall, this study demonstrates the important role of sesquiterpenes in atmospheric chemistry and suggests that the contribution of their products to SOA particles is being underestimated in comparison to the most studied terpenes.

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.

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;

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