lnstitut für Sensorik und Elektronik

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Evidence for the role of organics in aerosol particle formation under atmospheric conditions
(National Academy of Sciences, 19.01.2010) Metzger, Axel; Verheggen, Bart; Dommen, Josef; Duplissy, Jonathan; Prévôt, André S.H.; Weingartner, Ernest; Riipinen, Ilona; Kulmala, Markku; Spracklen, Dominick V.; Carslaw, Kenneth S.; Baltensperger, Urs
New particle formation in the atmosphere is an important parameter in governing the radiative forcing of atmospheric aerosols. However, detailed nucleation mechanisms remain ambiguous, as laboratory data have so far not been successful in explaining atmospheric nucleation. We investigated the formation of new particles in a smog chamber simulating the photochemical formation of H2SO4 and organic condensable species. Nucleation occurs at H2SO4 concentrations similar to those found in the ambient atmosphere during nucleation events. The measured particle formation rates are proportional to the product of the concentrations of H2SO4 and an organic molecule. This suggests that only one H2SO4 molecule and one organic molecule are involved in the rate-limiting step of the observed nucleation process. Parameterizing this process in a global aerosol model results in substantially better agreement with ambient observations compared to control runs.
01A - Beitrag in wissenschaftlicher Zeitschrift
Explaining global surface aerosol number concentrations in terms of primary emissions and particle formation
(Copernicus, 26.05.2010) Spracklen, Dominick V.; Carslaw, Kenneth S.; Merikanto, Joonas; Mann, Graham W.; Reddington, Carly L.; Pickering, S.; Ogren, John A.; Andrews, Elisabeth; Baltensperger, Urs; Weingartner, Ernest; Boy, Michael; Kulmala, Markku; Laakso, Lauri; Lihavainen, Heikki; Kivekäs, Niku; Komppula, Mika; Mihalopoulos, Ninolaos; Kouvarakis, Giorgos; Jennings, Stephen G.; O'Dowd, Collin D.; Birmili, Wolfram; Wiedensohler, Alfred; Weller, Rolf; Gras, John; Laj, Paolo; Sellegri, Karine; Bonn, Boris; Krejci, Radovan; Laaksonen, Ari; Hamed, Amar; Minikin, Andreas; Harrison, Roy Michael; Talbot, Robert; Sun, Junying
We synthesised observations of total particle number (CN) concentration from 36 sites around the world. We found that annual mean CN concentrations are typically 300–2000 cm−3 in the marine boundary layer and free troposphere (FT) and 1000–10 000 cm−3 in the continental boundary layer (BL). Many sites exhibit pronounced seasonality with summer time concentrations a factor of 2–10 greater than wintertime concentrations. We used these CN observations to evaluate primary and secondary sources of particle number in a global aerosol microphysics model. We found that emissions of primary particles can reasonably reproduce the spatial pattern of observed CN concentration (R2=0.46) but fail to explain the observed seasonal cycle (R2=0.1). The modeled CN concentration in the FT was biased low (normalised mean bias, NMB=−88%) unless a secondary source of particles was included, for example from binary homogeneous nucleation of sulfuric acid and water (NMB=−25%). Simulated CN concentrations in the continental BL were also biased low (NMB=−74%) unless the number emission of anthropogenic primary particles was increased or a mechanism that results in particle formation in the BL was included. We ran a number of simulations where we included an empirical BL nucleation mechanism either using the activation-type mechanism (nucleation rate, J, proportional to gas-phase sulfuric acid concentration to the power one) or kinetic-type mechanism (J proportional to sulfuric acid to the power two) with a range of nucleation coefficients. We found that the seasonal CN cycle observed at continental BL sites was better simulated by BL particle formation (R2=0.3) than by increasing the number emission from primary anthropogenic sources (R2=0.18). The nucleation constants that resulted in best overall match between model and observed CN concentrations were consistent with values derived in previous studies from detailed case studies at individual sites. In our model, kinetic and activation-type nucleation parameterizations gave similar agreement with observed monthly mean CN concentrations.
01A - Beitrag in wissenschaftlicher Zeitschrift
EUCAARI ion spectrometer measurements at 12 European sites – analysis of new particle formation events
(Copernicus, 25.08.2010) Manninen, Hanna E.; Nieminen, Tuomo; Asmi, Eija; Gagné, Stéphanie; Häkkinen, Silja; Lehtipalo, Katrianne; Aalto, Pasi Pekka; Vana, Marko; Mirme, Aadu; Mirme, Sander; Hõrrak, Urmas; Plass-Dülmer, Christian; Stange, Gert; Kiss, Gyula; Hoffer, András; Törő, N.; Moerman, Marcel; Henzing, Bas; de Leeuw, Gerrit; Brinkenberg, Marcel; Kouvarakis, Giorgos N.; Bougiatioti, Aikaterini; Mihalopoulos, Nikolaos; O'Dowd, Colin D.; Ceburnis, Darius; Arneth, Almut; Svenningsson, Brigitta; Swietlicki, Erik; Tarozzi, Leone; Decesari, Stefano; Facchini, Maria Cristina; Birmili, Wolfram; Sonntag, André; Wiedensohler, Alfred; Boulon, Julien; Sellegri, Karine; Laj, Paolo; Gysel, Martin; Bukowiecki, Nicolas; Weingartner, Ernest; Wehrle, Günther; Laaksonen, Ari; Hamed, Amar; Joutsensaari, Jorma; Petäjä, Tuukka; Kerminen, Veli-Matti; Kulmala, Markku
We present comprehensive results on continuous atmospheric cluster and particle measurements in the size range ~1–42 nm within the European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) project. We focused on characterizing the spatial and temporal variation of new particle formation events and relevant particle formation parameters across Europe. Different types of air ion and cluster mobility spectrometers were deployed at 12 field sites across Europe from March 2008 to May 2009. The measurements were conducted in a wide variety of environments, including coastal and continental locations as well as sites at different altitudes (both in the boundary layer and the free troposphere). New particle formation events were detected at all of the 12 field sites during the year-long measurement period. From the data, nucleation and growth rates of newly formed particles were determined for each environment. In a case of parallel ion and neutral cluster measurements, we could also estimate the relative contribution of ion-induced and neutral nucleation to the total particle formation. The formation rates of charged particles at 2 nm accounted for 1–30% of the corresponding total particle formation rates. As a significant new result, we found out that the total particle formation rate varied much more between the different sites than the formation rate of charged particles. This work presents, so far, the most comprehensive effort to experimentally characterize nucleation and growth of atmospheric molecular clusters and nanoparticles at ground-based observation sites on a continental scale.
01A - Beitrag in wissenschaftlicher Zeitschrift
Ion-induced nucleation of pure biogenic particles
(Springer, 26.05.2016) Kirby, Jasper; Duplissy, Jonathan; Sengupta, Kamalika; Frege, Carla; Gordon, Hamish; Williamson, Christina; Heinritzi, Martin; Simon, Mario; Yan, Chao; Almeida, João; Tröstl, Jasmin; Nieminen, Tuomo; Ortega, Ismael K.; Wagner, Robert; Adamov, Alexey; Amorim, Antonio; Bernhammer, Anne-Kathrin; Bianchi, Federico; Breitenlechner, Martin; Brilke, Sophia; Chen, Xuemeng; Craven, Jill; Dias, Antonio; Ehrhart, Sebastian; Flagan, Richard C.; Franchin, Alessandro; Fuchs, Claudia; Guida, Roberto; Hakala, Jani; Hoyle, Christopher R.; Jokinen, Tuija; Junninen, Heikki; Kangasluoma, Juha; Kim, Jaeseok; Krapf, Manuel; Kürten, Andreas; Laaksonen, Ari; Lehtipalo, Katrianne; Makhmutov, Vladimir; Mathot, Serge; Molteni, Ugo; Onnela, Antti; Peräkylä, Otso; Piel, Felix; Petäjä, Tuukka; Praplan, Arnaud P.; Pringle, Kirsty; Rap, Alexandru; Richards, Nigel A.D.; Riipinen, Ilona; Rissanen, Matti P.; Rondo, Linda; Sarnela, Nina; Schobesberger, Siegfried; Scott, Catherine E.; Seinfeld, John H.; Sipilä, Mikko; Steiner, Gerhard; Stozhkov, Yuri; Stratmann, Frank; Tomé, Antonio; Virtanen, Annele; Vogel, Alexander L.; Wagner, Andrea C.; Wagner, Paul E.; Weingartner, Ernest; Wimmer, Daniela; Winkler, Paul M.; Ye, Penglin; Zhang, Xuan; Hansel, Armin; Dommen, Josef; Donahue, Neil M.; Worsnop, Douglas R.; Baltensperger, Urs; Kulmala, Markku; Carslaw, Kenneth S.; Curtius, Joachim
Atmospheric aerosols and their effect on clouds are thought to be important for anthropogenic radiative forcing of the climate, yet remain poorly understood. Globally, around half of cloud condensation nuclei originate from nucleation of atmospheric vapours. It is thought that sulfuric acid is essential to initiate most particle formation in the atmosphere, and that ions have a relatively minor role. Some laboratory studies, however, have reported organic particle formation without the intentional addition of sulfuric acid, although contamination could not be excluded. Here we present evidence for the formation of aerosol particles from highly oxidized biogenic vapours in the absence of sulfuric acid in a large chamber under atmospheric conditions. The highly oxygenated molecules (HOMs) are produced by ozonolysis of α-pinene. We find that ions from Galactic cosmic rays increase the nucleation rate by one to two orders of magnitude compared with neutral nucleation. Our experimental findings are supported by quantum chemical calculations of the cluster binding energies of representative HOMs. Ion-induced nucleation of pure organic particles constitutes a potentially widespread source of aerosol particles in terrestrial environments with low sulfuric acid pollution.
01A - Beitrag in wissenschaftlicher Zeitschrift
Number size distributions and seasonality of submicron particles in Europe 2008–2009
(Copernicus, 15.06.2011) Asmi, Ari; Wiedensohler, Alfred; Laj, Paolo; Fjaeraa, Ann Mari; Sellegri, Karine; Birmili, Wolfram; Weingartner, Ernest; Baltensperger, Urs; Zdimal, Vladimir; Zikova, Nadezda; Putaud, Jean-Philippe; Marinoni, Angela; Tunved, Peter; Hansson, Hans-Christen; Fiebig, Markus; Kivekäs, Niku; Lihavainen, Heikki; Asmi, Eija; Ulevicius, Vidmantas; Aalto, Pasi Pekka; Swietlicki, Erik; Kristensson, Adam; Mihalopoulos, Nikolaos; Kalivitis, Nikos; Kalapov, Ivo; Kiss, Gyula; de Leeuw, Gerrit; Henzing, Bas; Harrison, Roy; Beddows, David; O'Dowd, Colin; Jennings, Stephen G.; Flentje, Harald; Weinhold, Kay; Meinhardt, Frank; Ries, Ludwig; Kulmala, Markku
Two years of harmonized aerosol number size distribution data from 24 European field monitoring sites have been analysed. The results give a comprehensive overview of the European near surface aerosol particle number concentrations and number size distributions between 30 and 500 nm of dry particle diameter. Spatial and temporal distribution of aerosols in the particle sizes most important for climate applications are presented. We also analyse the annual, weekly and diurnal cycles of the aerosol number concentrations, provide log-normal fitting parameters for median number size distributions, and give guidance notes for data users. Emphasis is placed on the usability of results within the aerosol modelling community. We also show that the aerosol number concentrations of Aitken and accumulation mode particles (with 100 nm dry diameter as a cut-off between modes) are related, although there is significant variation in the ratios of the modal number concentrations. Different aerosol and station types are distinguished from this data and this methodology has potential for further categorization of stations aerosol number size distribution types. The European submicron aerosol was divided into characteristic types: Central European aerosol, characterized by single mode median size distributions, unimodal number concentration histograms and low variability in CCN-sized aerosol number concentrations; Nordic aerosol with low number concentrations, although showing pronounced seasonal variation of especially Aitken mode particles; Mountain sites (altitude over 1000 m a.s.l.) with a strong seasonal cycle in aerosol number concentrations, high variability, and very low median number concentrations. Southern and Western European regions had fewer stations, which decreases the regional coverage of these results. Aerosol number concentrations over the Britain and Ireland had very high variance and there are indications of mixed air masses from several source regions; the Mediterranean aerosol exhibit high seasonality, and a strong accumulation mode in the summer. The greatest concentrations were observed at the Ispra station in Northern Italy with high accumulation mode number concentrations in the winter. The aerosol number concentrations at the Arctic station Zeppelin in Ny-Ålesund in Svalbard have also a strong seasonal cycle, with greater concentrations of accumulation mode particles in winter, and dominating summer Aitken mode indicating more recently formed particles. Observed particles did not show any statistically significant regional work-week or weekday related variation in number concentrations studied. Analysis products are made for open-access to the research community, available in a freely accessible internet site. The results give to the modelling community a reliable, easy-to-use and freely available comparison dataset of aerosol size distributions.
01A - Beitrag in wissenschaftlicher Zeitschrift
Primary versus secondary contributions to particle number concentrations in the European boundary layer
(Copernicus, 05.12.2011) Reddington, Carly L.; Carslaw, Ken S.; Spracklen, Dominick V.; Frontoso, Maria Grazia; Collins, Lisa M.; Merikanto, Joonas; Minikin, Andreas; Hamburger, Thomas; Coe, Hugh; Kulmala, Markku; Aalto, Pasi Pekka; Flentje, Harald; Plass-Dülmer, Christian; Birmili, Wolfram; Wiedensohler, Alfred; Wehner, Birgit; Tuch, Thomas; Sonntag, Alfred; O'Dowd, Collin D.; Jennings, Stephen G.; Dupuy, Regis; Baltensperger, Urs; Weingartner, Ernest; Hansson, Hans-Christen; Tunved, Peter; Laj, Paolo; Sellegri, Karine; Boulon, Julien; Putaud, Jean-Philippe; Gruening, Carsten; Swietlicki, Erik; Roldin, Pontus; Henzing, J.S.; Moerman, Marcel; Mihalopoulos, Nikolaos; Kouvarakis, Giorgos; Ždímal, Vladimir; Zíková, Nadezda; Marinoni, Angela; Bonasoni, Paolo; Duchi, Rocco
It is important to understand the relative contribution of primary and secondary particles to regional and global aerosol so that models can attribute aerosol radiative forcing to different sources. In large-scale models, there is considerable uncertainty associated with treatments of particle formation (nucleation) in the boundary layer (BL) and in the size distribution of emitted primary particles, leading to uncertainties in predicted cloud condensation nuclei (CCN) concentrations. Here we quantify how primary particle emissions and secondary particle formation influence size-resolved particle number concentrations in the BL using a global aerosol microphysics model and aircraft and ground site observations made during the May 2008 campaign of the European Integrated Project on Aerosol Cloud Climate Air Quality Interactions (EUCAARI). We tested four different parameterisations for BL nucleation and two assumptions for the emission size distribution of anthropogenic and wildfire carbonaceous particles. When we emit carbonaceous particles at small sizes (as recommended by the Aerosol Intercomparison project, AEROCOM), the spatial distributions of campaign-mean number concentrations of particles with diameter >50 nm (N50) and >100 nm (N100) were well captured by the model (R2≥0.8) and the normalised mean bias (NMB) was also small (−18% for N50 and −1% for N100). Emission of carbonaceous particles at larger sizes, which we consider to be more realistic for low spatial resolution global models, results in equally good correlation but larger bias (R2≥0.8, NMB = −52% and −29%), which could be partly but not entirely compensated by BL nucleation. Within the uncertainty of the observations and accounting for the uncertainty in the size of emitted primary particles, BL nucleation makes a statistically significant contribution to CCN-sized particles at less than a quarter of the ground sites. Our results show that a major source of uncertainty in CCN-sized particles in polluted European air is the emitted size of primary carbonaceous particles. New information is required not just from direct observations, but also to determine the "effective emission size" and composition of primary particles appropriate for different resolution models.
01A - Beitrag in wissenschaftlicher Zeitschrift
Results from the CERN pilot CLOUD experiment
(Copernicus, 15.02.2010) Duplissy, Jonathan; Enghoff, Martin Bødker; Aplin, Karen L.; Arnold, Frank; Aufmhoff, Heinfried; Avngaard, Michael; Baltensperger, Urs; Bondo, Torsten; Bingham, Robert; Carslaw, Ken S.; Curtius, Joachim; David, A.; Fastrup, Bent; Gagné, Stéphanie; Hahn, F.; Harrison, Richerd Giles; Kellett, Barry; Kirkby, Jasper; Kulmala, Markku; Laakso, Lauri; Laaksonen, Ari; Lillestøl, Egil; Lockwood, Mike; Mäkelä, Jyrki Mikael; Makhmutov, Vladimir; Marsh, N. D.; Nieminen, Tuomo; Onnela, Antti; Pedersen, E.; Pedersen, Jens Olaf Pepke; Polny, Josef; Reichl, Udo; Seinfeld, John H.; Sipilä, Mikko; Stozhkov, Yuri; Stratmann, Frank; Svensmark, Henrik; Svensmark, Jacob; Veenhof, Rob; Verheggen, B.; Viisanen, Yrjö; Wagner, Paul E.; Wehrle, Günther; Weingartner, Ernest; Wex, Heike; Wilhelmsson, Mats; Winkler, Paul M.
During a 4-week run in October–November 2006, a pilot experiment was performed at the CERN Proton Synchrotron in preparation for the Cosmics Leaving OUtdoor Droplets (CLOUD) experiment, whose aim is to study the possible influence of cosmic rays on clouds. The purpose of the pilot experiment was firstly to carry out exploratory measurements of the effect of ionising particle radiation on aerosol formation from trace H2SO4 vapour and secondly to provide technical input for the CLOUD design. A total of 44 nucleation bursts were produced and recorded, with formation rates of particles above the 3 nm detection threshold of between 0.1 and 100 cm−3s−1, and growth rates between 2 and 37 nm h−1. The corresponding H2O concentrations were typically around 106 cm−3 or less. The experimentally measured formation rates and H2SO4 concentrations are comparable to those found in the atmosphere, supporting the idea that sulphuric acid is involved in the nucleation of atmospheric aerosols. However, sulphuric acid alone is not able to explain the observed rapid growth rates, which suggests the presence of additional trace vapours in the aerosol chamber, whose identity is unknown. By analysing the charged fraction, a few of the aerosol bursts appear to have a contribution from ion-induced nucleation and ion-ion recombination to form neutral clusters. Some indications were also found for the accelerator beam timing and intensity to influence the aerosol particle formation rate at the highest experimental SO2 concentrations of 6 ppb, although none was found at lower concentrations. Overall, the exploratory measurements provide suggestive evidence for ion-induced nucleation or ion-ion recombination as sources of aerosol particles. However, in order to quantify the conditions under which ion processes become significant, improvements are needed in controlling the experimental variables and in the reproducibility of the experiments. Finally, concerning technical aspects, the most important lessons for the CLOUD design include the stringent requirement of internal cleanliness of the aerosol chamber, as well as maintenance of extremely stable temperatures (variations below 0.1 °C).
01A - Beitrag in wissenschaftlicher Zeitschrift
Role of sulphuric acid, ammonia and galactic cosmic rays in atmospheric aerosol nucleation
(Springer, 24.08.2011) Kirkby, Jasper; Curtius, Joachim; Almeida, João; Dunne, Eimear; Duplissy, Jonathan; Ehrhart, Sebastian; Franchin, Alessandro; Gagné, Stéphanie; Ickes, Luisa; Kürten, Andreas; Kupc, Agnieszka; Metzger, Axel; Riccobono, Francesco; Rondo, Linda; Schobesberger, Siegfried; Tsagkogeorgas, Georgios; Wimmer, Daniela; Amorim, Antonio; Bianchi, Federico; Breitenlechner, Martin; David, André; Dommen, Josef; Downard, Andrew; Ehn, Mikael; Flagan, Richard C.; Haider, Stefan; Hansel, Armin; Hauser, Daniel; Jud, Werner; Junninen, Heikki; Kreissl, Fabian; Kvashin, Alexander; Laaksonen, Ari; Lehtipalo, Katrianne; Lima, Jorge; Lovejoy, Edward R.; Makhmutov, Vladimir; Mathot, Serge; Mikkilä, Jyri; Minginette, Pierre; Mogo, Sandra; Nieminen, Tuomo; Onnela, Antti; Pereira, Paulo; Petäjä, Tuukka; Schnitzhofer, Ralf; Seinfeld, John H.; Sipilä, Mikko; Stozhkov, Yuri; Stratmann, Frank; Tomé, Antonio; Vanhanen, Joonas; Viisanen, Yrjo; Vrtala, Aron; Wagner, Paul E.; Walther, Hansueli; Weingartner, Ernest; Wex, Heike; Winkler, Paul M.; Carslaw, Kenneth S.; Worsnop, Douglas R.; Baltensperger, Urs; Kulmala, Markku
Atmospheric aerosols exert an important influence on climate through their effects on stratiform cloud albedo and lifetime and the invigoration of convective storms. Model calculations suggest that almost half of the global cloud condensation nuclei in the atmospheric boundary layer may originate from the nucleation of aerosols from trace condensable vapours, although the sensitivity of the number of cloud condensation nuclei to changes of nucleation rate may be small. Despite extensive research, fundamental questions remain about the nucleation rate of sulphuric acid particles and the mechanisms responsible, including the roles of galactic cosmic rays and other chemical species such as ammonia. Here we present the first results from the CLOUD experiment at CERN. We find that atmospherically relevant ammonia mixing ratios of 100 parts per trillion by volume, or less, increase the nucleation rate of sulphuric acid particles more than 100–1,000-fold. Time-resolved molecular measurements reveal that nucleation proceeds by a base-stabilization mechanism involving the stepwise accretion of ammonia molecules. Ions increase the nucleation rate by an additional factor of between two and more than ten at ground-level galactic-cosmic-ray intensities, provided that the nucleation rate lies below the limiting ion-pair production rate. We find that ion-induced binary nucleation of H2SO4–H2O can occur in the mid-troposphere but is negligible in the boundary layer. However, even with the large enhancements in rate due to ammonia and ions, atmospheric concentrations of ammonia and sulphuric acid are insufficient to account for observed boundary-layer nucleation.
01A - Beitrag in wissenschaftlicher Zeitschrift
The regional aerosol-climate model REMO-HAM
(Copernicus, 01.11.2012) Pietikäinen, Joni-Pekka; O'Donnell, Denis; Teichmann, Christopher; Karstens, Ute; Pfeifer, Samuel; Kazil, Jan; Podzun, Ralf; Fiedler, Susann; Kokkola, Harri; Birmili, Wolfram; O'Dowd, Colin D.; Baltensperger, Urs; Weingartner, Ernest; Gehrig, Robert; Spindler, Gerald; Kulmala, Markku; Feichter, Johann; Jacob, Daniela; Laaksonen, Aatto
REMO-HAM is a new regional aerosol-climate model. It is based on the REMO regional climate model and includes most of the major aerosol processes. The structure for aerosol is similar to the global aerosol-climate model ECHAM5-HAM, for example the aerosol module HAM is coupled with a two-moment stratiform cloud scheme. On the other hand, REMO-HAM does not include an online coupled aerosol-radiation nor a secondary organic aerosol module. In this work, we evaluate the model and compare the results against ECHAM5-HAM and measurements. Four different measurement sites were chosen for the comparison of total number concentrations, size distributions and gas phase sulfur dioxide concentrations: Hyytiälä in Finland, Melpitz in Germany, Mace Head in Ireland and Jungfraujoch in Switzerland. REMO-HAM is run with two different resolutions: 50 × 50 km2 and 10 × 10 km2. Based on our simulations, REMO-HAM is in reasonable agreement with the measured values. The differences in the total number concentrations between REMO-HAM and ECHAM5-HAM can be mainly explained by the difference in the nucleation mode. Since we did not use activation nor kinetic nucleation for the boundary layer, the total number concentrations are somewhat underestimated. From the meteorological point of view, REMO-HAM represents the precipitation fields and 2 m temperature profile very well compared to measurement. Overall, we show that REMO-HAM is a functional aerosol-climate model, which will be used in further studies.
01A - Beitrag in wissenschaftlicher Zeitschrift
Contribution of sulfuric acid and oxidized organic compounds to particle formation and growth
(Copernicus, 2012) Riccobono, Francesco; Rondo, Linda; Sipilä, Mikko; Barmet, Peter; Curtius, Joachim; Dommen, Josef; Ehn, Mikael; Ehrhart, Sebastian; Kulmala, Markku; Kürten, Andreas; Mikkilä, Jyri; Paasonen, Pauli; Petäjä, Tuukka; Weingartner, Ernest; Baltensperger, Urs
Abstract. Lack of knowledge about the mechanisms underlying new particle formation and their subsequent growth is one of the main causes for the large uncertainty in estimating the radiative forcing of atmospheric aerosols in global models. We performed chamber experiments designed to study the contributions of sulfuric acid and organic vapors to the formation and early growth of nucleated particles. Distinct experiments in the presence of two different organic precursors (1,3,5-trimethylbenzene and α-pinene) showed the ability of these compounds to reproduce the formation rates observed in the low troposphere. These results were obtained measuring the sulfuric acid concentrations with two chemical ionization mass spectrometers confirming the results of a previous study which modeled the sulfuric acid concentrations in presence of 1,3,5-trimethylbenzene. New analysis methods were applied to the data collected with a condensation particle counter battery and a scanning mobility particle sizer, allowing the assessment of the size resolved growth rates of freshly nucleated particles. The effect of organic vapors on particle growth was investigated by means of the growth rate enhancement factor (Γ), defined as the ratio between the measured growth rate in the presence of α-pinene and the kinetically limited growth rate of the sulfuric acid and water system. The observed Γ values indicate that the growth is already dominated by organic compounds at particle diameters of 2 nm. Both the absolute growth rates and Γ showed a strong dependence on particle size, supporting the nano-Köhler theory. Moreover, the separation of the contributions from sulfuric acid and organic compounds to particle growth reveals that the organic contribution seems to be enhanced by the sulfuric acid concentration. Finally, the size resolved growth analysis indicates that both condensation of oxidized organic compounds and reactive uptake contribute to particle growth.
01A - Beitrag in wissenschaftlicher Zeitschrift

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