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- ItemAerosol number size distributions from 3 to 500 nm diameter in the arctic marine boundary layer during summer and autumn(Copenhagen : Blackwell Munksgaard, 1996) Covert, D.S.; Wiedensohler, A.; Aalto, P.; Heintzenberg, J.; Mcmurry, P.H.; Leck, C.Aerosol physics measurements made onboard the Swedish icebreaker Oden in the late Summer and early Autumn of 1991 during the International Arctic Ocean Expedition (IAOE-91) have provided the first data on the size distribution of particles in the Arctic marine boundary layer (MBL) that cover both the number and mass modes of the size range from 3 to 500 nm diameter. These measurements were made in conjunction with atmospheric gas and condensed phase chemistry measurements in an effort to understand a part of the ocean-atmosphere sulfur cycle. Analysis of the particle physics data showed that there were three distinct number modes in the submicrometric aerosol in the Arctic MBL. These modes had geometric mean diameters of around 170 nm. 45 nm and 14 nm referred to as accumulation, Aitken and ultrafine modes, respectively. There were clear minima in number concentrations between the modes that appeared at 20 to 30 nm and at 80 to 100 nm. The total number concentration was most frequently between 30 and 60 particles cm-3 with a mean value of around 100 particles cm-3, but the hourly average concentration varied over two to three orders of magnitude during the 70 days of the expedition. On average, the highest concentration was in the accumulation mode that contained about 45% of the total number, while the Aitken mode contained about 40%. The greatest variability was in the ultrafine mode concentration which is indicative of active, earby sources (nucleation from the gas phase) and sinks; the Aitken and accumulation mode concentrations were much less variable. The ultrafine mode was observed about two thirds of the time and was dominant 10% of the time. A detailed description and statistical analysis of the modal aerosol parameters is presented here.
- ItemEUCAARI ion spectrometer measurements at 12 European sites – analysis of new particle formation events(München : European Geopyhsical Union, 2010) Manninen, H.E.; Nieminen, T.; Asmi, E.; Gagné, S.; Häkkinen, S.; Lehtipalo, K.; Aalto, P.; Vana, M.; Mirme, A.; Mirme, S.; Hõrrak, U.; Plass-Dülmer, C.; Stange, G.; Kiss, G.; Hoffer, A.; Törő, N.; Moerman, M.; Henzing, B.; de Leeuw, G.; Brinkenberg, M.; Kouvarakis, G.N.; Bougiatioti, A.; Mihalopoulos, N.; O'Dowd, C.; Ceburnis, D.; Arneth, A.; Svenningsson, B.; Swietlicki, E.; Tarozzi, L.; Decesari, S.; Facchini, M.C.; Birmili, W.; Sonntag, A.; Wiedensohler, A.; Boulon, J.; Sellegri, K.; Laj, P.; Gysel, M.; Bukowiecki, N.; Weingartner, E.; Wehrle, G.; Laaksonen, A.; Hamed, A.; Joutsensaari, J.; Petäjä, T.; Kerminen, V.-M.; Kulmala, M.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.
- ItemPrimary versus secondary contributions to particle number concentrations in the European boundary layer(München : European Geopyhsical Union, 2011) Reddington, C.L.; Carslaw, K.S.; Spracklen, D.V.; Frontoso, M.G.; Collins, L.; Merikanto, J.; Minikin, A.; Hamburger, T.; Coe, H.; Kulmala, M.; Aalto, P.; Flentje, H.; Plass-Dülmer, C.; Birmili, W.; Wiedensohler, A.; Wehner, B.; Tuch, T.; Sonntag, A.; O'Dowd, C.D.; Jennings, S.G.; Dupuy, R.; Baltensperger, U.; Weingartner, E.; Hansson, H.-C.; Tunved, P.; Laj, P.; Sellegri, K.; Boulon, J.; Putaud, J.-P.; Gruening, C.; Swietlicki, E.; Roldin, P.; Henzing, J.S.; Moerman, M.; Mihalopoulos, N.; Kouvarakis, G.; Ždímal, V.; Zíková, N.; Marinoni, A.; Bonasoni, P.; Duchi, R.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.
- ItemMobility particle size spectrometers: Harmonization of technical standards and data structure to facilitate high quality long-term observations of atmospheric particle number size distributions(München : European Geopyhsical Union, 2012) Wiedensohler, A.; Birmili, W.; Nowak, A.; Sonntag, A.; Weinhold, K.; Merkel, M.; Wehner, B.; Tuch, T.; Pfeifer, S.; Fiebig, M.; Fjäraa, A.M.; Asmi, E.; Sellegri, K.; Depuy, R.; Venzac, H.; Villani, P.; Laj, P.; Aalto, P.; Ogren, J.A.; Swietlick, E.; Williams, P.; Roldin, P.; Quincey, P.; Hüglin, C.; Fierz-Schmidhauser, R.; Gysel, M.; Weingartner, E.; Riccobono, F.; Santos, S.; Grüning, C.; Faloon, K.; Beddows, D.; Harrison, R.; Monahan, C.; Jennings, S.G.; O'Dowd, C.D.; Marinoni, A.; Horn, H.-G.; Keck, L.; Jiang, J.; Scheckman, J.; McMurry, P.H.; Deng, Z.; Zhao, C.S.; Moerman, M.; Henzing, B.; de Leeuw, G.; Löschau, G.; Bastian, S.Mobility particle size spectrometers often referred to as DMPS (Differential Mobility Particle Sizers) or SMPS (Scanning Mobility Particle Sizers) have found a wide range of applications in atmospheric aerosol research. However, comparability of measurements conducted world-wide is hampered by lack of generally accepted technical standards and guidelines with respect to the instrumental set-up, measurement mode, data evaluation as well as quality control. Technical standards were developed for a minimum requirement of mobility size spectrometry to perform long-term atmospheric aerosol measurements. Technical recommendations include continuous monitoring of flow rates, temperature, pressure, and relative humidity for the sheath and sample air in the differential mobility analyzer. We compared commercial and custom-made inversion routines to calculate the particle number size distributions from the measured electrical mobility distribution. All inversion routines are comparable within few per cent uncertainty for a given set of raw data. Furthermore, this work summarizes the results from several instrument intercomparison workshops conducted within the European infrastructure project EUSAAR (European Supersites for Atmospheric Aerosol Research) and ACTRIS (Aerosols, Clouds, and Trace gases Research InfraStructure Network) to determine present uncertainties especially of custom-built mobility particle size spectrometers. Under controlled laboratory conditions, the particle number size distributions from 20 to 200 nm determined by mobility particle size spectrometers of different design are within an uncertainty range of around ±10% after correcting internal particle losses, while below and above this size range the discrepancies increased. For particles larger than 200 nm, the uncertainty range increased to 30%, which could not be explained. The network reference mobility spectrometers with identical design agreed within ±4% in the peak particle number concentration when all settings were done carefully. The consistency of these reference instruments to the total particle number concentration was demonstrated to be less than 5%. Additionally, a new data structure for particle number size distributions was introduced to store and disseminate the data at EMEP (European Monitoring and Evaluation Program). This structure contains three levels: raw data, processed data, and final particle size distributions. Importantly, we recommend reporting raw measurements including all relevant instrument parameters as well as a complete documentation on all data transformation and correction steps. These technical and data structure standards aim to enhance the quality of long-term size distribution measurements, their comparability between different networks and sites, and their transparency and traceability back to raw data.
- ItemNon-volatile residuals of newly formed atmospheric particles in the boreal forest(München : European Geopyhsical Union, 2007) Ehn, M.; Petäjä, T.; Birmili, W.; Junninen, H.; Aalto, P.; Kulmala, M.The volatility of sub-micrometer atmospheric aerosol particles was studied in a rural background environment in Finland using a combination of a heating tube and a scanning mobility particle sizer. The analysis focused on nanoparticles formed through nucleation which were subsequently observed during their growth in the diameter range between 5 and 60 nm. During the 6 days of new particle formation shown in detail, the concentrations of newly formed particles increased up to 10 000 cm−3. The number of nucleation mode particles measured after volatilization in the heating tube at 280°C was up to 90% of the total number under ambient conditions. Taking into account the absolute accuracy of the size distribution measurements, all ambient particles found in the rural atmosphere could have a non-volatile core after volatilization at 280°C. As the regional new particle formation events developed over time as a result of further vapor condensation, the newly formed particles grew at an average growth rate of 2.4±0.3 nm h−1. Importantly, the non-volatile cores of nucleation mode particles were also observed to grow over time, however, at a lower average growth rate of 0.6±0.3 nm h−1. One implication of the volatility analysis is that the newly formed particles, which have reached ambient diameters of 15 nm, are unlikely to consist of sulfuric acid, ammonium sulfate, and water alone. A relatively constant ratio between the growth rate of the ambient particles as well as their non-volatile cores indicates that non-volatile matter is formed only gradually in the growing particles. The non-volatile fraction of the particles showed some correlation with the ambient temperature. The composition and formation mechanism of this non-volatile material in nucleation mode particles are, to date, not known.
- ItemSO2 oxidation products other than H2SO4 as a trigger of new particle formation. Part 2: Comparison of ambient and laboratory measurements, and atmospheric implications(München : European Geopyhsical Union, 2008) Laaksonen, A.; Kulmala, M.; Bernd, T.; Stratmann, F.; Mikkonen, S.; Ruuskanen, A.; Lehtinen, K.E.J.; Dal Maso, M.; Aalto, P.; Petäjä, T.; Riipinen, I.; Sihto, S.-L.; Janson, R.; Arnold, F.; Hanke, M.; Ücker, J.; Umann, B.; Sellegri, K.; O'Dowd, C.D.; Viisanen, Y.Atmospheric new particle formation is generally thought to occur due to homogeneous or ion-induced nucleation of sulphuric acid. We compare ambient nucleation rates with laboratory data from nucleation experiments involving either sulphuric acid or oxidized SO2. Atmospheric nucleation occurs at H2SO4 concentrations 2–4 orders of magnitude lower than binary or ternary nucleation rates of H2SO4 produced from a liquid reservoir, and atmospheric H2SO4 concentrations are very well replicated in the SO2 oxidation experiments. We hypothesize these features to be due to the formation of free HSO5 radicals in pace with H2SO4 during the SO2 oxidation. We suggest that at temperatures above ~250 K these radicals produce nuclei of new aerosols much more efficiently than H2SO4. These nuclei are activated to further growth by H2SO4 and possibly other trace species. However, at lower temperatures the atmospheric relative acidity is high enough for the H2SO4–H2O nucleation to dominate.
- ItemA new feedback mechanism linking forests, aerosols, and climate(München : European Geopyhsical Union, 2004) Kulmala, M.; Suni, T.; Lehtinen, K.E.J.; Dal Maso, M.; Boy, M.; Reissell, A.; Rannik, Ü.; Aalto, P.; Keronen, P.; Hakola, H.; Bäck, J.; Hoffmann, T.; Vesala, T.; Hari, P.The possible connections between the carbon balance of ecosystems and aerosol-cloud-climate interactions play a significant role in climate change studies. Carbon dioxide is a greenhouse gas, whereas the net effect of atmospheric aerosols is to cool the climate. Here, we investigated the connection between forest-atmosphere carbon exchange and aerosol dynamics in the continental boundary layer by means of multiannual data sets of particle formation and growth rates, of CO2 fluxes, and of monoterpene concentrations in a Scots pine forest in southern Finland. We suggest a new, interesting link and a potentially important feedback among forest ecosystem functioning, aerosols, and climate: Considering that globally increasing temperatures and CO2 fertilization are likely to lead to increased photosynthesis and forest growth, an increase in forest biomass would increase emissions of non-methane biogenic volatile organic compounds and thereby enhance organic aerosol production. This feedback mechanism couples the climate effect Of CO2 with that of aerosols in a novel way.