| 1. |
- Fountoukis, C., et al.
(author)
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Simulating ultrafine particle formation in Europe using a regional ctm : contribution of primary emissions versus secondary formation to aerosol number concentrations
- 2012
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In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:18, s. 8663-8677
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Journal article (peer-reviewed)abstract
- A three-dimensional regional chemical transport model (CTM) with detailed aerosol microphysics, PMCAMx-UF, was applied to the European domain to simulate the contribution of direct emissions and secondary formation to total particle number concentrations during May 2008. PMCAMx-UF uses the Dynamic Model for Aerosol Nucleation and the Two-Moment Aerosol Sectional (TOMAS) algorithm to track both aerosol number and mass concentration using a sectional approach. The model predicts nucleation events that occur over scales of hundreds up to thousands of kilometers especially over the Balkans and Southeast Europe. The model predictions were compared against measurements from 7 sites across Europe. The model reproduces more than 70% of the hourly concentrations of particles larger than 10 nm (N-10) within a factor of 2. About half of these particles are predicted to originate from nucleation in the lower troposphere. Regional nucleation is predicted to increase the total particle number concentration by approximately a factor of 3. For particles larger than 100 nm the effect varies from an increase of 20% in the eastern Mediterranean to a decrease of 20% in southern Spain and Portugal resulting in a small average increase of around 1% over the whole domain. Nucleation has a significant effect in the predicted N-50 levels (up to a factor of 2 increase) mainly in areas where there are condensable vapors to grow the particles to larger sizes. A semi-empirical ternary sulfuric acid-ammonia-water parameterization performs better than the activation or the kinetic parameterizations in reproducing the observations. Reducing emissions of ammonia and sulfur dioxide affects certain parts of the number size distribution.
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| 2. |
- Kerminen, V-M, et al.
(author)
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Cloud condensation nuclei production associated with atmospheric nucleation : a synthesis based on existing literature and new results
- 2012
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In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:24, s. 12037-12059
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Journal article (peer-reviewed)abstract
- This paper synthesizes the available scientific information connecting atmospheric nucleation with subsequent cloud condensation nuclei (CCN) formation. We review both observations and model studies related to this topic, and discuss the potential climatic implications. We conclude that CCN production associated with atmospheric nucleation is both frequent and widespread phenomenon in many types of continental boundary layers, and probably also over a large fraction of the free troposphere. The contribution of nucleation to the global CCN budget spans a relatively large uncertainty range, which, together with our poor understanding of aerosol-cloud interactions, results in major uncertainties in the radiative forcing by atmospheric aerosols. In order to better quantify the role of atmospheric nucleation in CCN formation and Earth System behavior, more information is needed on (i) the factors controlling atmospheric CCN production and (ii) the properties of both primary and secondary CCN and their interconnections. In future investigations, more emphasis should be put on combining field measurements with regional and large-scale model studies.
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| 3. |
- Kulmala, M., et al.
(author)
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General overview: European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) - integrating aerosol research from nano to global scales
- 2011
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In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:24, s. 13061-13143
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Journal article (peer-reviewed)abstract
- In this paper we describe and summarize the main achievements of the European Aerosol Cloud Climate and Air Quality Interactions project (EUCAARI). EUCAARI started on 1 January 2007 and ended on 31 December 2010 leaving a rich legacy including: (a) a comprehensive database with a year of observations of the physical, chemical and optical properties of aerosol particles over Europe, (b) comprehensive aerosol measurements in four developing countries, (c) a database of airborne measurements of aerosols and clouds over Europe during May 2008, (d) comprehensive modeling tools to study aerosol processes fron nano to global scale and their effects on climate and air quality. In addition a new Pan-European aerosol emissions inventory was developed and evaluated, a new cluster spectrometer was built and tested in the field and several new aerosol parameterizations and computations modules for chemical transport and global climate models were developed and evaluated. These achievements and related studies have substantially improved our understanding and reduced the uncertainties of aerosol radiative forcing and air quality-climate interactions. The EUCAARI results can be utilized in European and global environmental policy to assess the aerosol impacts and the corresponding abatement strategies.
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| 4. |
- Kulmala, M., et al.
(author)
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Introduction: European Integrated Project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) : integrating aerosol research from nano to global scales
- 2009
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In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 9, s. 2825-2841
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Journal article (peer-reviewed)abstract
- The European Aerosol Cloud Climate and Air Quality Interactions project EUCAARI is an EU Research Framework 6 integrated project focusing on understanding the interactions of climate and air pollution. EUCAARI works in an integrative and multidisciplinary way from nano-to global scale. EUCAARI brings together several leading European research groups, state-of-the-art infrastructure and some key scientists from third countries to investigate the role of aerosol on climate and air quality. Altogether 48 partners from 25 countries are participating in EUCAARI. During the first 16 months EUCAARI has built operational systems, e. g. established pan-European measurement network for Lagrangian studies and four stations in developing countries. Also an improved understanding of nanoscale processes (like nucleation) has been implemented in global models. Here we present the research methods, organisation, operations and first results of EUCAARI.
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| 5. |
- Murphy, Benjamin N., et al.
(author)
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A naming convention for atmospheric organic aerosol
- 2014
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In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 14:11, s. 5825-5839
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Journal article (peer-reviewed)abstract
- While the field of atmospheric organic aerosol scientific research has experienced thorough and insightful progress over the last half century, this progress has been accompanied by the evolution of a communicative and detailed yet, at times, complex and inconsistent language. The menagerie of detailed classification that now exists to describe organic compounds in our atmosphere reflects the wealth of observational techniques now at our disposal as well as the rich information provided by state-of-the-science instrumentation. However, the nomenclature in place to communicate these scientific gains is growing disjointed to the point that effective communication within the scientific community and to the public may be sacrificed. We propose standardizing a naming convention for organic aerosol classification that is relevant to laboratory studies, ambient observations, atmospheric models, and various stakeholders for air-quality problems. Because a critical aspect of this effort is to directly translate the essence of complex physico-chemical phenomena to a much broader, policy-oriented audience, we recommend a framework that maximizes comprehension among scientists and non-scientists alike. For example, to classify volatility, it relies on straightforward alphabetic terms (e.g., semivolatile, SV; intermediate volatility, IV; etc.) rather than possibly ambiguous numeric indices. This framework classifies organic material as primary or secondary pollutants and distinguishes among fundamental features important for science and policy questions including emission source, chemical phase, and volatility. Also useful is the addition of an alphabetic suffix identifying the volatility of the organic material or its precursor for when emission occurred. With this framework, we hope to introduce into the community a consistent connection between common notation for the general public and detailed nomenclature for highly specialized discussion. In so doing, we try to maintain consistency with historical, familiar naming schemes, unify much of the scattered nomenclature presented in recent literature, reduce the barrier of comprehension to outside audiences, and construct a scaffold into which insights from future scientific discoveries can be incorporated.
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| 6. |
- Patoulias, D., et al.
(author)
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The role of organic condensation on ultrafine particle growth during nucleation events
- 2015
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In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 15:11, s. 6337-6350
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Journal article (peer-reviewed)abstract
- A new aerosol dynamics model (DMANx) has been developed that simulates aerosol size/composition distribution and includes the condensation of organic vapors on nanoparticles through the implementation of the recently developed volatility basis set framework. Simulations were performed for Hyytiala (Finland) and Finokalia (Greece), two locations with different organic sources where detailed measurements were available to constrain the new model. We investigate the effect of condensation of organics and chemical aging reactions of secondary organic aerosol (SOA) precursors on ultrafine particle growth and particle number concentration during a typical springtime nucleation event in both locations. This work highlights the importance of the pathways of oxidation of biogenic volatile organic compounds and the production of extremely low volatility organics. At Hyytiala, organic condensation dominates the growth process of new particles. The low-volatility SOA contributes to particle growth during the early growth stage, but after a few hours most of the growth is due to semi-volatile SOA. At Finokalia, simulations show that organics have a complementary role in new particle growth, contributing 45% to the total mass of new particles. Condensation of organics increases the number concentration of particles that can act as CCN (cloud condensation nuclei) (N-100) by 13% at Finokalia and 25% at Hyytiala during a typical spring day with nucleation. The sensitivity of our results to the surface tension used is discussed.
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| 7. |
- Riipinen, Ilona, et al.
(author)
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Connecting the solubility and CCN activation of complex organic aerosols : a theoretical study using solubility distributions
- 2015
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In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 15:11, s. 6305-6322
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Journal article (peer-reviewed)abstract
- We present a theoretical study investigating the cloud activation of multicomponent organic particles. We modeled these complex mixtures using solubility distributions (analogous to volatility distributions in the VBS, i.e., volatility basis set, approach), describing the mixture as a set of surrogate compounds with varying water solubilities in a given range. We conducted Khler theory calculations for 144 different mixtures with varying solubility range, number of components, assumption about the organic mixture thermodynamics and the shape of the solubility distribution, yielding approximately 6000 unique cloud condensation nucleus (CCN)-activation points. The results from these comprehensive calculations were compared to three simplifying assumptions about organic aerosol solubility: (1) complete dissolution at the point of activation; (2) combining the aerosol solubility with the molar mass and density into a single effective hygroscopicity parameter kappa; and (3) assuming a fixed water-soluble fraction eff. The complete dissolution was able to reproduce the activation points with a reasonable accuracy only when the majority (70-80 %) of the material was dissolved at the point of activation. The single-parameter representations of complex mixture solubility were confirmed to be powerful semi-empirical tools for representing the CCN activation of organic aerosol, predicting the activation diameter within 10% in most of the studied supersaturations. Depending mostly on the condensedphase interactions between the organic molecules, material with solubilities larger than about 0.1-100 g L-1 could be treated as soluble in the CCN activation process over atmospherically relevant particle dry diameters and supersaturations. Our results indicate that understanding the details of the solubility distribution in the range of 0.1-100 g L-1 is thus critical for capturing the CCN activation, while resolution outside this solubility range will probably not add much information except in some special cases. The connections of these results to the previous observations of the CCN activation and the molecular properties of complex organic mixture aerosols are discussed. The presented results help unravel the mechanistic reasons behind observations of hygroscopic growth and CCN activation of atmospheric secondary organic aerosol (SOA) particles. The proposed solubility distribution framework is a promising tool for modeling the interlinkages between atmospheric aging, volatility and water uptake of atmospheric organic aerosol.
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| 8. |
- Skyllakou, K., et al.
(author)
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Contributions of local and regional sources to fine PM in the megacity of Paris
- 2014
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In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 14:5, s. 2343-2352
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Journal article (peer-reviewed)abstract
- The particulate matter source apportionment technology (PSAT) is used together with PMCAMx, a regional chemical transport model, to estimate how local emissions and pollutant transport affect primary and secondary particulate matter mass concentration levels in Paris. During the summer and the winter periods examined, only 13% of the PM2.5 is predicted to be due to local Paris emissions, with 36% coming from mid-range (50-500 km from the center of the Paris) sources and 51% from long range transport ( more than 500 km from Paris). The local emissions contribution to simulated elemental carbon (EC) is significant, with almost 60% of the EC originating from local sources during both summer and winter. Approximately 50% of the simulated fresh primary organic aerosol (POA) originated from local sources and another 45% from areas 100-500 km from the receptor region during summer. Regional sources dominated the secondary PM components. During summer more than 70% of the simulated sulfate originated from SO2 emitted more than 500 km away from the center of the Paris. Also more than 45% of secondary organic aerosol (SOA) was due to the oxidation of VOC precursors that were emitted 100-500 km from the center of the Paris. The model simulates more contribution from long range secondary PM sources during winter because the timescale for its production is longer due to the slower photochemical activity. PSAT results for contributions of local and regional sources were compared with observation-based estimates from field campaigns that took place during the MEGAPOLI project. PSAT simulations are in general consistent ( within 20%) with these estimates for OA and sulfate. The only exception is that PSAT simulates higher local EC contribution during the summer compared to that estimated from observations.
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| 9. |
- van der Gon, Hacd, et al.
(author)
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Particulate emissions from residential wood combustion in Europe revised estimates and an evaluation
- 2015
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In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 15:11, s. 6503-6519
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Journal article (peer-reviewed)abstract
- Currently residential wood combustion (RWC) is increasing in Europe because of rising fossil fuel prices but also due to climate change mitigation policies. However, especially in small-scale applications, RWC may cause high emissions of particulate matter (PM). Recently we have developed a new high-resolution (7 x 7 km) anthropogenic carbonaceous aerosol emission inventory for Europe. The inventory indicated that about half of the total PM2.5 emission in Europe is carbonaceous aerosol and identified RWC as the largest organic aerosol source in Europe. The inventory was partly based on national reported PM emissions. Use of this organic aerosol inventory as input for two chemical transport models (CTMs), PMCAMx and EMEP MSC-W, revealed major underestimations of organic aerosol in winter time, especially for regions dominated by RWC. Interestingly, this was not universal but appeared to differ by country. In the present study we constructed a revised bottom-up emission inventory for RWC accounting for the semivolatile components of the emissions. The revised RWC emissions are higher than those in the previous inventory by a factor of 2-3 but with substantial inter-country variation. The new emission inventory served as input for the CTMs and a substantially improved agreement between measured and predicted organic aerosol was found. The revised RWC inven-tory improves the model-calculated organic aerosol significantly. Comparisons to Scandinavian source apportionment studies also indicate substantial improvements in the modelled wood-burning component of organic aerosol. This suggests that primary organic aerosol emission inventories need to be revised to include the semivolatile organic aerosol that is formed almost instantaneously due to dilution and cooling of the flue gas or exhaust. Since RWC is a key source of fine PM in Europe, a major revision of the emission estimates as proposed here is likely to influence source-receptor matrices and modelled source apportionment. Since usage of biofuels in small combustion units is a globally significant source, the findings presented here are also relevant for regions outside of Europe.
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