Browsing by Subject "SIZE DISTRIBUTIONS"

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  • Laj, Paolo; Bigi, Alessandro; Rose, Clemence; Andrews, Elisabeth; Myhre, Cathrine Lund; Coen, Martine Collaud; Lin, Yong; Wiedensohler, Alfred; Schulz, Michael; Ogren, John A.; Fiebig, Markus; Gliss, Jonas; Mortier, Augustin; Pandolfi, Marco; Petäjä, Tuukka; Kim, Sang-Woo; Aas, Wenche; Putaud, Jean-Philippe; Mayol-Bracero, Olga; Keywood, Melita; Labrador, Lorenzo; Aalto, Pasi; Ahlberg, Erik; Alados Arboledas, Lucas; Alastuey, Andres; Andrade, Marcos; Artinano, Begona; Ausmeel, Stina; Arsov, Todor; Asmi, Eija; Backman, John; Baltensperger, Urs; Bastian, Susanne; Bath, Olaf; Beukes, Johan Paul; Brem, Benjamin T.; Bukowiecki, Nicolas; Conil, Sebastien; Couret, Cedric; Day, Derek; Dayantolis, Wan; Degorska, Anna; Eleftheriadis, Konstantinos; Fetfatzis, Prodromos; Favez, Olivier; Flentje, Harald; Gini, Maria I.; Gregoric, Asta; Gysel-Beer, Martin; Hallar, A. Gannet; Hand, Jenny; Hoffer, Andras; Hueglin, Christoph; Hooda, Rakesh K.; Hyvärinen, Antti; Kalapov, Ivo; Kalivitis, Nikos; Kasper-Giebl, Anne; Kim, Jeong Eun; Kouvarakis, Giorgos; Kranjc, Irena; Krejci, Radovan; Kulmala, Markku; Labuschagne, Casper; Lee, Hae-Jung; Lihavainen, Heikki; Lin, Neng-Huei; Loeschau, Gunter; Luoma, Krista; Marinoni, Angela; Dos Santos, Sebastiao Martins; Meinhardt, Frank; Merkel, Maik; Metzger, Jean-Marc; Mihalopoulos, Nikolaos; Nhat Anh Nguyen,; Ondracek, Jakub; Perez, Noemi; Perrone, Maria Rita; Petit, Jean-Eudes; Picard, David; Pichon, Jean-Marc; Pont, Veronique; Prats, Natalia; Prenni, Anthony; Reisen, Fabienne; Romano, Salvatore; Sellegri, Karine; Sharma, Sangeeta; Schauer, Gerhard; Sheridan, Patrick; Sherman, James Patrick; Schuetze, Maik; Schwerin, Andreas; Sohmer, Ralf; Sorribas, Mar; Steinbacher, Martin; Sun, Junying; Titos, Gloria; Toczko, Barbara; Tuch, Thomas; Tulet, Pierre; Tunved, Peter; Vakkari, Ville; Velarde, Fernando; Velasquez, Patricio; Villani, Paolo; Vratolis, Sterios; Wang, Sheng-Hsiang; Weinhold, Kay; Weller, Rolf; Yela, Margarita; Yus-Diez, Jesus; Zdimal, Vladimir; Zieger, Paul; Zikova, Nadezda (2020)
    Aerosol particles are essential constituents of the Earth's atmosphere, impacting the earth radiation balance directly by scattering and absorbing solar radiation, and indirectly by acting as cloud condensation nuclei. In contrast to most greenhouse gases, aerosol particles have short atmospheric residence times, resulting in a highly heterogeneous distribution in space and time. There is a clear need to document this variability at regional scale through observations involving, in particular, the in situ near-surface segment of the atmospheric observation system. This paper will provide the widest effort so far to document variability of climate-relevant in situ aerosol properties (namely wavelength dependent particle light scattering and absorption coefficients, particle number concentration and particle number size distribution) from all sites connected to the Global Atmosphere Watch network. High-quality data from almost 90 stations worldwide have been collected and controlled for quality and are reported for a reference year in 2017, providing a very extended and robust view of the variability of these variables worldwide. The range of variability observed worldwide for light scattering and absorption coefficients, single-scattering albedo, and particle number concentration are presented together with preliminary information on their long-term trends and comparison with model simulation for the different stations. The scope of the present paper is also to provide the necessary suite of information, including data provision procedures, quality control and analysis, data policy, and usage of the ground-based aerosol measurement network. It delivers to users of the World Data Centre on Aerosol, the required confidence in data products in the form of a fully characterized value chain, including uncertainty estimation and requirements for contributing to the global climate monitoring system.
  • Karl, Matthias; Gross, Allan; Pirjola, Liisa; Leck, Caroline (2011)
  • Crenn, V.; Sciare, J.; Croteau, P. L.; Verlhac, S.; Froehlich, R.; Belis, C. A.; Aas, W.; Äijälä, M.; Alastuey, A.; Artinano, B.; Baisnee, D.; Bonnaire, N.; Bressi, M.; Canagaratna, M.; Canonaco, F.; Carbone, C.; Cavalli, F.; Coz, E.; Cubison, M. J.; Esser-Gietl, J. K.; Green, D. C.; Gros, V.; Heikkinen, L.; Herrmann, H.; Lunder, C.; Minguillon, M. C.; Mocnik, G.; O'Dowd, C. D.; Ovadnevaite, J.; Petit, J. -E.; Petralia, E.; Poulain, L.; Priestman, M.; Riffault, V.; Ripoll, A.; Sarda-Esteve, R.; Slowik, J. G.; Setyan, A.; Wiedensohler, A.; Baltensperger, U.; Prevot, A. S. H.; Jayne, J. T.; Favez, O. (2015)
    As part of the European ACTRIS project, the first large Quadrupole Aerosol Chemical Speciation Monitor (Q-ACSM) intercomparison study was conducted in the region of Paris for 3 weeks during the late-fall-early-winter period (November-December 2013). The first week was dedicated to the tuning and calibration of each instrument, whereas the second and third were dedicated to side-by-side comparison in ambient conditions with co-located instruments providing independent information on submicron aerosol optical, physical, and chemical properties. Near real-time measurements of the major chemical species (organic matter, sulfate, nitrate, ammonium, and chloride) in the non-refractory submicron aerosols (NR-PM1) were obtained here from 13 Q-ACSM. The results show that these instruments can produce highly comparable and robust measurements of the NR-PM1 total mass and its major components. Taking the median of the 13 Q-ACSM as a reference for this study, strong correlations (r(2) > 0.9) were observed systematically for each individual Q-ACSM across all chemical families except for chloride for which three Q-ACSMs showing weak correlations partly due to the very low concentrations during the study. Reproducibility expanded uncertainties of Q-ACSM concentration measurements were determined using appropriate methodologies defined by the International Standard Organization (ISO 17025, 1999) and were found to be 9, 15, 19, 28, and 36% for NR-PM1, nitrate, organic matter, sulfate, and ammonium, respectively. However, discrepancies were observed in the relative concentrations of the constituent mass fragments for each chemical component. In particular, significant differences were observed for the organic fragment at mass-to-charge ratio 44, which is a key parameter describing the oxidation state of organic aerosol. Following this first major intercomparison exercise of a large number of Q-ACSMs, detailed intercomparison results are presented, along with a discussion of some recommendations about best calibration practices, standardized data processing, and data treatment.
  • Kalivitis, N.; Kerminen, Veli-Matti; Kouvarakis, G.; Stavroulas, I.; Bougiatioti, A.; Nenes, A.; Manninen, Hanna; Petäjä, Tuukka; Kulmala, Markku; Mihalopoulos, N. (2015)
    While cloud condensation nuclei (CCN) production associated with atmospheric new particle formation (NPF) is thought to be frequent throughout the continental boundary layers, few studies on this phenomenon in marine air exist. Here, based on simultaneous measurement of particle number size distributions, CCN properties and aerosol chemical composition, we present the first direct evidence on CCN production resulting from NPF in the eastern Mediterranean atmosphere. We show that condensation of both gaseous sulfuric acid and organic compounds from multiple sources leads to the rapid growth of nucleated particles to CCN sizes in this environment during the summertime. Sub-100 nm particles were found to be substantially less hygroscopic than larger particles during the period with active NPF and growth (the value of kappa was lower by 0.2-0.4 for 60 nm particles compared with 120 nm particles), probably due to enrichment of organic material in the sub-100 nm size range. The aerosol hygroscopicity tended to be at minimum just before the noon and at maximum in the afternoon, which was very likely due to the higher sulfate-to-organic ratios and higher degree of oxidation of the organic material during the afternoon. Simultaneous with the formation of new particles during daytime, particles formed during the previous day or even earlier were growing into the size range relevant to cloud droplet activation, and the particles formed in the atmosphere were possibly mixed with long-range-transported particles.
  • Hussein, Tareq; Saleh, Shatha Suleiman Ali; dos Santos, Vanessa N.; Abdullah, Huthaifah; Boor, Brandon E. (2019)
    There is a paucity of comprehensive air quality data from urban areas in the Middle East. In this study, portable instrumentation was used to measure size-fractioned aerosol number, mass, and black carbon concentrations in Amman and Zarqa, Jordan. Submicron particle number concentrations at stationary urban background sites in Amman and Zarqa exhibited a characteristic diurnal pattern, with the highest concentrations during traffic rush hours (2-5 x 10(4) cm(-3) in Amman and 2-7 x 10(4) cm(-3) in Zarqa). Super-micron particle number concentrations varied considerably in Amman (1-10 cm(-3)). Mobile measurements identified spatial variations and local hotspots in aerosol levels within both cities. Walking paths around the University of Jordan campus showed increasing concentrations with proximity to main roads with mean values of 8 x 10(4) cm(-3), 87 mu g/m(3), 62 mu g/m(3), and 7.7 mu g/m(3) for submicron, PM10, PM2.5, and black carbon (BC), respectively. Walking paths in the Amman city center showed moderately high concentrations (mean 10(5) cm(-3), 120 mu g/m(3), 85 mu g/m(3), and 8.1 mu g/m(3) for submicron aerosols, PM10, PM2.5, and black carbon, respectively). Similar levels were found along walking paths in the Zarqa city center. On-road measurements showed high submicron concentrations (>10(5) cm(-3)). The lowest submicron concentration (
  • Zanatta, Marco; Laj, Paolo; Gysel, Martin; Baltensperger, Urs; Vratolis, Stergios; Eleftheriadis, Konstantinos; Kondo, Yutaka; Dubuisson, Philippe; Winiarek, Victor; Kazadzis, Stelios; Tunved, Peter; Jacobi, Hans-Werner (2018)
    Atmospheric aging promotes internal mixing of black carbon (BC), leading to an enhancement of light absorption and radiative forcing. The relationship between BC mixing state and consequent absorption enhancement was never estimated for BC found in the Arctic region. In the present work, we aim to quantify the absorption enhancement and its impact on radiative forcing as a function of microphysical properties and mixing state of BC observed in situ at the Zeppelin Arctic station (78 degrees N) in the spring of 2012 during the CLIMSLIP (Climate impacts of short-lived pollutants in the polar region) project. Single-particle soot photometer (SP2) measurements showed a mean mass concentration of refractory black carbon (rBC) of 39 ngm(-3), while the rBC mass size distribution was of lognormal shape, peaking at an rBC mass-equivalent diameter (D-rBC) of around 240 nm. On average, the number fraction of particles containing a BC core with D-rBC > 80 nm was less than 5% in the size range (overall optical particle diameter) from 150 to 500 nm. The BC cores were internally mixed with other particulate matter. The median coating thickness of BC cores with 220 nm <D-rBC <260 nm was 52 nm, resulting in a core-shell diameter ratio of 1.4, assuming a coated sphere morphology. Combining the aerosol absorption coefficient observed with an Aethalometer and the rBC mass concentration from the SP2, a mass absorption cross section (MAC) of 9.8 m(2) g(-1) was inferred at a wavelength of 550 nm. Consistent with direct observation, a similar MAC value (8.4m(2) g(-1) at 550 nm) was obtained indirectly by using Mie theory and assuming a coated-sphere morphology with the BC mixing state constrained from the SP2 measurements. According to these calculations, the lensing effect is estimated to cause a 54% enhancement of the MAC compared to that of bare BC particles with equal BC core size distribution. Finally, the ARTDECO radiative transfer model was used to estimate the sensitivity of the radiative balance to changes in light absorption by BC as a result of a varying degree of internal mixing at constant total BC mass. The clear-sky noontime aerosol radiative forcing over a surface with an assumed wavelength-dependent albedo of 0.76-0.89 decreased, when ignoring the absorption enhancement, by -0.12 Wm(-2) compared to the base case scenario, which was constrained with mean observed aerosol properties for the Zeppelin site in Arctic spring. The exact magnitude of this forcing difference scales with environmental conditions such as the aerosol optical depth, solar zenith angle and surface albedo. Nevertheless, our investigation suggests that the absorption enhancement due to internal mixing of BC, which is a systematic effect, should be considered for quantifying the aerosol radiative forcing in the Arctic region.
  • Baranizadeh, Elham; Nieminen, Tuomo; Yli-Juuti, Taina; Kulmala, Markku; Petäjä, Tuukka; Leskinen, Ari; Komppula, Mika; Laaksonen, Ari; Lehtinen, Kari E. J. (2017)
    The formation rates of 3 nm particles were estimated at SMEAR IV, Puijo (Finland), where the continuous measurements extend only down to 7 nm in diameter. We extrapolated the formation rates at 7 nm (J(7)) down to 3 nm (J(3)) based on an approximate solution to the aerosol general dynamic equation, assuming a constant condensational growth rate, a power-law size-dependent scavenging rate, and negligible self-coagulation rate for the nucleation mode particles. To evaluate our method, we first applied it to new particle formation (NPF) events in Hyytiala (Finland), which extend down to 3 nm, and, therefore, J(3) and J(7) can be determined directly from the measured size distribution evolution. The Hyytiala results show that the estimated daily mean J(3) values slightly overestimate the observed mean J(3), but a promising 91% of the estimated J(3) values are within a factor of 2 from the measured ones. However, when considering detailed daily time evolution, the agreement is not as good due to fluctuations in data as well as uncertainties in estimated growth rates, which are required in order to calculate the time lag between formation of 3 and 7 nm particles. At Puijo, the mean J(7) for clear NPF days during April 2007-December 2015 was 0.44 cm(-3) s(-1), while the extrapolated mean J(3) was 0.61 cm(-3) s(-1).
  • Chen, Xuemeng; Kerminen, Veli-Matti; Paatero, Jussi; Paasonen, Pauli; Manninen, Hanna E.; Nieminen, Tuomo; Petäjä, Tuukka; Kulmala, Markku (2016)
    Most of the ion production in the atmosphere is attributed to ionising radiation. In the lower atmosphere, ionising radiation consists mainly of the decay emissions of radon and its progeny, gamma radiation of the terrestrial origin as well as photons and elementary particles of cosmic radiation. These types of radiation produce ion pairs via the ionisation of nitrogen and oxygen as well as trace species in the atmosphere, the rate of which is defined as the ionising capacity. Larger air ions are produced out of the initial charge carriers by processes such as clustering or attachment to preexisting aerosol particles. This study aimed (1) to identify the key factors responsible for the variability in ionising radiation and in the observed air ion concentrations, (2) to reveal the linkage between them and (3) to provide an in-depth analysis into the effects of ionising radiation on air ion formation, based on measurement data collected during 2003-2006 from a boreal forest site in southern Finland. In general, gamma radiation dominated the ion production in the lower atmosphere. Variations in the ionising capacity came from mixing layer dynamics, soil type and moisture content, meteorological conditions, long-distance transportation, snow cover attenuation and precipitation. Slightly similar diurnal patterns to variations in the ionising capacity were observed in air ion concentrations of the cluster size (0.8-1.7 nm in mobility diameters). However, features observed in the 0.81 nm ion concentration were in good connection to variations of the ionising capacity. Further, by carefully constraining perturbing variables, a strong dependency of the cluster ion concentration on the ionising capacity was identified, proving the functionality of ionising radiation in air ion production in the lower atmosphere. This relationship, however, was only clearly observed on new particle formation (NPF) days, possibly indicating that charges after being born underwent different processes on NPF days and non-event days and also that the transformation of newly formed charges to cluster ions occurred in a shorter timescale on NPF days than on non-event days.
  • Gordevičius, Juozas; Narmontė, Milda; Gibas, Povilas; Kvederavičiūtė, Kotryna; Tomkutė, Vita; Paluoja, Priit; Krjutškov, Kaarel; Salumets, Andres; Kriukienė, Edita (2020)
    BackgroundMassively parallel sequencing of maternal cell-free DNA (cfDNA) is widely used to test fetal genetic abnormalities in non-invasive prenatal testing (NIPT). However, sequencing-based approaches are still of high cost. Building upon previous knowledge that placenta, the main source of fetal circulating DNA, is hypomethylated in comparison to maternal tissue counterparts of cfDNA, we propose that targeting either unmodified or 5-hydroxymethylated CG sites specifically enriches fetal genetic material and reduces numbers of required analytical sequencing reads thereby decreasing cost of a test.MethodsWe employed uTOPseq and hmTOP-seq approaches which combine covalent derivatization of unmodified or hydroxymethylated CG sites, respectively, with next generation sequencing, or quantitative real-time PCR.ResultsWe detected increased 5-hydroxymethylcytosine (5hmC) levels in fetal chorionic villi (CV) tissue samples as compared with peripheral blood. Using our previously developed uTOP-seq and hmTOP-seq approaches we obtained whole-genome uCG and 5hmCG maps of 10 CV tissue and 38 cfDNA samples in total. Our results indicated that, in contrast to conventional whole genome sequencing, such epigenomic analysis highly specifically enriches fetal DNA fragments from maternal cfDNA. While both our approaches yielded 100% accuracy in detecting Down syndrome in fetuses, hmTOP-seq maintained such accuracy at ultra-low sequencing depths using only one million reads. We identified 2164 and 1589 placenta-specific differentially modified and 5-hydroxymethylated regions, respectively, in chromosome 21, as well as 3490 and 2002 Down syndrome-specific differentially modified and 5-hydroxymethylated regions, respectively, that can be used as biomarkers for identification of Down syndrome or other epigenetic diseases of a fetus.ConclusionsuTOP-seq and hmTOP-seq approaches provide a cost-efficient and sensitive epigenetic analysis of fetal abnormalities in maternal cfDNA. The results demonstrated that T21 fetuses contain a perturbed epigenome and also indicated that fetal cfDNA might originate from fetal tissues other than placental chorionic villi. Robust covalent derivatization followed by targeted analysis of fetal DNA by sequencing or qPCR presents an attractive strategy that could help achieve superior sensitivity and specificity in prenatal diagnostics.
  • Jokinen, T.; Sipilä, M.; Kontkanen, J.; Vakkari, V.; Tisler, P.; Duplissy, E.-M.; Junninen, H.; Kangasluoma, J.; Manninen, H. E.; Petäjä, T.; Kulmala, M.; Worsnop, D. R.; Kirkby, J.; Virkkula, A.; Kerminen, V.-M. (2018)
    Formation of new aerosol particles from trace gases is a major source of cloud condensation nuclei (CCN) in the global atmosphere, with potentially large effects on cloud optical properties and Earth's radiative balance. Controlled laboratory experiments have resolved, in detail, the different nucleation pathways likely responsible for atmospheric new particle formation, yet very little is known from field studies about the molecular steps and compounds involved in different regions of the atmosphere. The scarcity of primary particle sources makes secondary aerosol formation particularly important in the Antarctic atmosphere. Here, we report on the observation of ion-induced nucleation of sulfuric acid and ammonia-a process experimentally investigated by the CERN CLOUD experiment-as a major source of secondary aerosol particles over coastal Antarctica. We further show that measured high sulfuric acid concentrations, exceeding 10(7) molecules cm(-3), are sufficient to explain the observed new particle growth rates. Our findings show that ion-induced nucleation is the dominant particle formation mechanism, implying that galactic cosmic radiation plays a key role in new particle formation in the pristine Antarctic atmosphere.
  • Mamali, D.; Mikkilä, J.; Henzing, B.; Spoor, R.; Ehn, M.; Petäjä, T.; Russchenberg, H.; Biskos, G. (2018)
    Long-term measurements of PM2.5 mass concentrations and aerosol particle size distributions from 2008 to 2015, as well as hygroscopicity measurements conducted over one year (2008-2009) at Cabauw, The Netherlands, are compiled here in order to provide a comprehensive dataset for understanding the trends and annual variabilities of the atmospheric aerosol in the region. PM2.5 concentrations have a mean value of 14.4 mu g m(-3) with standard deviation 2.1 mu g m(-3), and exhibit an overall decreasing trend of -0.74 mu g m(-3) year(-1). The highest values are observed in winter and spring and are associated with a shallower boundary layer and lower precipitation, respectively, compared to the rest of the seasons. Number concentrations of particles smaller than 500 nm have a mean of 9.2 x 10(3) particles cm(-3) and standard deviation 4.9x10(3) particles cm(-3), exhibiting an increasing trend between 2008 and 2011 and a decreasing trend from 2013 to 2015. The particle number concentrations exhibit highest values in spring and summer (despite the increased precipitation) due to the high occurrence of nucleation-mode particles, which most likely are formed elsewhere and are transported to the observation station. Particle hygroscopicity measurements show that, independently of the air mass origin, the particles are mostly externally mixed with the more hydrophobic mode having a mean hygroscopic parameter kappa of 0.1 while for the more hydrophilic mode kappa is 0.35. The hygroscopicity of the smaller particles investigated in this work (i.e., particles having diameters of 35 nm) appears to increase during the course of the nucleation events, reflecting a change in the chemical composition of the particles. (C) 2017 Elsevier B.V. All rights reserved.
  • de Jesus, Alma Lorelei; Thompson, Helen; Knibbs, Luke D.; Kowalski, Michal; Cyrys, Josef; Niemi, Jarkko V.; Kousa, Anu; Timonen, Hilkka; Luoma, Krista; Petäjä, Tuukka; Beddows, David; Harrison, Roy M.; Hopke, Philip; Morawska, Lidia (2020)
    Urbanisation and industrialisation led to the increase of ambient particulate matter (PM) concentration. While subsequent regulations may have resulted in the decrease of some PM matrices, the simultaneous changes in climate affecting local meteorological conditions could also have played a role. To gain an insight into this complex matter, this study investigated the long-term trends of two important matrices, the particle mass (PM2.5) and particle number concentrations (PNC), and the factors that influenced the trends. Mann-Kendall test, Sen's slope estimator, the generalised additive model, seasonal decomposition of time series by LOESS (locally estimated scatterplot smoothing) and the Buishand range test were applied. Both PM2.5 and PNC showed significant negative monotonic trends (0.03-0.6 mg m(-3).yr(-1) and 0.40-3.8 x 10(3) particles. cm(-3). yr(-1), respectively) except Brisbane (+0.1 mg m(-3). yr(-1) and +53 particles. cm(-3). yr(-1), respectively). For the period covered in this study, temperature increased (0.03-0.07 degrees C.yr(-1)) in all cities except London; precipitation decreased (0.02-1.4 mm.yr(-1)) except in Helsinki; and wind speed was reduced in Brisbane and Rochester but increased in Helsinki, London and Augsburg. At the change-points, temperature increase in cold cities influenced PNC while shifts in precipitation and wind speed affected PM2.5. Based on the LOESS trend, extreme events such as dust storms and wildfires resulting from changing climates caused a positive step-change in concentrations, particularly for PM2.5. In contrast, among the mitigation measures, controlling sulphur in fuels caused a negative step-change, especially for PNC. Policies regarding traffic and fleet management (e.g. low emission zones) that were implemented only in certain areas or in a progressive uptake (e.g. Euro emission standards), resulted to gradual reductions in concentrations. Therefore, as this study has clearly shown that PM2.5 and PNC were influenced differently by the impacts of the changing climate and by the mitigation measures, both metrics must be considered in urban air quality management. (C) 2020 Elsevier Ltd. All rights reserved.
  • Rose, C.; Sellegri, K.; Asmi, E.; Hervo, M.; Freney, E.; Colomb, A.; Junninen, H.; Duplissy, J.; Sipilä, Mikko; Kontkanen, J.; Lehtipalo, K.; Kulmala, Markku (2015)
    The formation of new aerosol particles in the atmosphere is a key process influencing the aerosol number concentration as well as the climate, in particular at high altitude, where the newly formed particles directly influence cloud formation. However, free tropospheric new particle formation (NPF) is poorly documented due to logistic limitations and complex atmospheric dynamics around high-altitude stations that make the observation of this day-time process challenging. Recent improvements in measurement techniques make now possible the detection of neutral clusters down to similar to 1 nm sizes, which opens new horizons in our understanding of the nucleation process. Indeed, only the charged fraction of clusters has been reported in the upper troposphere up to now. Here we report day-time concentrations of charged and neutral clusters (1 to 2.5 nm mobility diameter) recorded at the interface between the boundary layer (BL) and the FT as well as in the FT at the altitude site of Puy de Dome (1465 m a.s.l.), central France, between 10 and 29 February 2012. Our findings demonstrate that in the FT, and especially at the interface between the BL and the FT, the formation of 1.5 nm neutral clusters significantly exceeds the one of ionic clusters during NPF events, clearly indicating that they dominate in the nucleation process. We also observe that the total cluster concentration significantly increases during NPF events compared to the other days, which was not clearly observed for the charged cluster population in the past. During the studied period, the nucleation process does not seem to be sulfuric acid-limited and could be promoted by the transport of pollutants to the upper troposphere, coupled with low temperatures.
  • Karl, Matthias; Kukkonen, Jaakko; Keuken, Menno P.; Lutzenkirchen, Susanne; Pirjola, Liisa; Hussein, Tareq (2016)
    This study evaluates the influence of aerosol processes on the particle number (PN) concentrations in three major European cities on the temporal scale of 1aEuro-h, i.e., on the neighborhood and city scales. We have used selected measured data of particle size distributions from previous campaigns in the cities of Helsinki, Oslo and Rotterdam. The aerosol transformation processes were evaluated using the aerosol dynamics model MAFOR, combined with a simplified treatment of roadside and urban atmospheric dispersion. We have compared the model predictions of particle number size distributions with the measured data, and conducted sensitivity analyses regarding the influence of various model input variables. We also present a simplified parameterization for aerosol processes, which is based on the more complex aerosol process computations; this simple model can easily be implemented to both Gaussian and Eulerian urban dispersion models. Aerosol processes considered in this study were (i) the coagulation of particles, (ii) the condensation and evaporation of two organic vapors, and (iii) dry deposition. The chemical transformation of gas-phase compounds was not taken into account. By choosing concentrations and particle size distributions at roadside as starting point of the computations, nucleation of gas-phase vapors from the exhaust has been regarded as post tail-pipe emission, avoiding the need to include nucleation in the process analysis. Dry deposition and coagulation of particles were identified to be the most important aerosol dynamic processes that control the evolution and removal of particles. The error of the contribution from dry deposition to PN losses due to the uncertainty of measured deposition velocities ranges from -76 to +64aEuro-%. The removal of nanoparticles by coagulation enhanced considerably when considering the fractal nature of soot aggregates and the combined effect of van der Waals and viscous interactions. The effect of condensation and evaporation of organic vapors emitted by vehicles on particle numbers and on particle size distributions was examined. Under inefficient dispersion conditions, the model predicts that condensational growth contributes to the evolution of PN from roadside to the neighborhood scale. The simplified parameterization of aerosol processes predicts the change in particle number concentrations between roadside and urban background within 10aEuro-% of that predicted by the fully size-resolved MAFOR model.
  • Karl, Matthias; Pirjola, Liisa; Karppinen, Ari; Jalkanen, Jukka-Pekka; Ramacher, Martin Otto Paul; Kukkonen, Jaakko (2020)
    Marine traffic in harbors can be responsible for significant atmospheric concentrations of ultrafine particles (UFPs), which have widely recognized negative effects on human health. It is therefore essential to model and measure the time evolution of the number size distributions and chemical composition of UFPs in ship exhaust to assess the resulting exposure in the vicinity of shipping routes. In this study, a sequential modelling chain was developed and applied, in combination with the data measured and collected in major harbor areas in the cities of Helsinki and Turku in Finland, during winter and summer in 2010-2011. The models described ship emissions, atmospheric dispersion, and aerosol dynamics, complemented with a time-microenvironment-activity model to estimate the short-term UFP exposure. We estimated the dilution ratio during the initial fast expansion of the exhaust plume to be approximately equal to eight. This dispersion regime resulted in a fully formed nucleation mode (denoted as Nuc(2)). Different selected modelling assumptions about the chemical composition of Nuc(2) did not have an effect on the formation of nucleation mode particles. Aerosol model simulations of the dispersing ship plume also revealed a partially formed nucleation mode (Nuc(1); peaking at 1.5 nm), consisting of freshly nucleated sulfate particles and condensed organics that were produced within the first few seconds. However, subsequent growth of the new particles was limited, due to efficient scavenging by the larger particles originating from the ship exhaust. The transport of UFPs downwind of the ship track increased the hourly mean UFP concentrations in the neighboring residential areas by a factor of two or more up to a distance of 3600 m, compared with the corresponding UFP concentrations in the urban background. The substantially increased UFP concentrations due to ship traffic significantly affected the daily mean exposures in residential areas located in the vicinity of the harbors.
  • Kukkonen, J.; Karl, M.; Keuken, M. P.; van der Gon, H. A. C. Denier; Denby, B. R.; Singh, V.; Douros, J.; Manders, A.; Samaras, Z.; Moussiopoulos, N.; Jonkers, S.; Aarnio, M.; Karppinen, A.; Kangas, L.; Lutzenkirchen, S.; Petäjä, T.; Vouitsis, I.; Sokhi, R. S. (2016)
    We present an overview of the modelling of particle number concentrations (PNCs) in five major European cities, namely Helsinki, Oslo, London, Rotterdam, and Athens, in 2008. Novel emission inventories of particle numbers have been compiled both on urban and European scales. We used atmospheric dispersion modelling for PNCs in the five target cities and on a European scale, and evaluated the predicted results against available measured concentrations. In all the target cities, the concentrations of particle numbers (PNs) were mostly influenced by the emissions originating from local vehicular traffic. The influence of shipping and harbours was also significant for Helsinki, Oslo, Rotterdam, and Athens, but not for London. The influence of the aviation emissions in Athens was also notable. The regional background concentrations were clearly lower than the contributions originating from urban sources in Helsinki, Oslo, and Athens. The regional background was also lower than urban contributions in traffic environments in London, but higher or approximately equal to urban contributions in Rotterdam. It was numerically evaluated that the influence of coagulation and dry deposition on the predicted PNCs was substantial for the urban background in Oslo. The predicted and measured annual average PNCs in four cities agreed within approximately
  • Dall'Osto, M.; Beddows, D. C. S.; Asmi, A.; Poulain, L.; Hao, L.; Freney, E.; Allan, J. D.; Canagaratna, M.; Crippa, M.; Bianchi, F.; de Leeuw, G.; Eriksson, A.; Swietlicki, E.; Hansson, H. C.; Henzing, J. S.; Granier, C.; Zemankova, K.; Laj, P.; Onasch, T.; Prevot, A.; Putaud, J. P.; Sellegri, K.; Vidal, M.; Virtanen, A.; Simo, R.; Worsnop, D.; O'Dowd, C.; Kulmala, M.; Harrison, Roy M. (2018)
    The formation of new atmospheric particles involves an initial step forming stable clusters less than a nanometre in size (similar to 10 nm). Although at times, the same species can be responsible for both processes, it is thought that more generally each step comprises differing chemical contributors. Here, we present a novel analysis of measurements from a unique multi-station ground-based observing system which reveals new insights into continental-scale patterns associated with new particle formation. Statistical cluster analysis of this unique 2-year multi-station dataset comprising size distribution and chemical composition reveals that across Europe, there are different major seasonal trends depending on geographical location, concomitant with diversity in nucleating species while it seems that the growth phase is dominated by organic aerosol formation. The diversity and seasonality of these events requires an advanced observing system to elucidate the key processes and species driving particle formation, along with detecting continental scale changes in aerosol formation into the future.
  • Lazaridis, Mihalis; Eleftheriadis, Kostas; Zdimal, Vladia; Schwarz, Jaroslav; Wagner, Zdenek; Ondracek, Jakub; Drossinos, Yannis; Glytsos, Thodoros; Vratolis, Sterios; Torseth, Kjetil; Moravec, Pavel; Hussein, Tareq; Smolik, Jiri (2017)
    Indoor/outdoor aerosol size distribution was measured in four European cities (Oslo-Norway, Prague-Czech Republic, Milan-Italy and Athens-Greece) during 2002 in order to examine the differences in the characteristics of the indoor/outdoor modal structure and to evaluate the effect of indoor sources to the aerosol size distributions. All the measurement sites were naturally ventilated and were occupied during the campaigns by permanent residents or for certain time periods by the technical staff responsible for the instrumentation. Outdoor particle number (PN) concentrations presented the higher values in Milan and Athens (median values 1.4 x 10(4) # cm(-3) and 2.9 x 10(4) # cm(-3) respectively) as a result of elevated outdoor emissions and led to correspondingly higher indoor values compared to Oslo and Prague. In absence of indoor activities, the indoor concentrations followed the fluctuations of the outdoor concentrations in all the measurement sites. Indoor activities (cooking, smoking, etc.) resulted in elevated indoor PN concentrations (maximum values ranging between 1.7 x 10(5) # cm(-3) and 3.2 x 10(5) # cm(-3)) and to I/O ratios higher than one. The I/O ratios were size dependant and for periods without indoor activities, they presented the lowest values for particles <50 nm (0.51 +/- 0.15) and the ratios increased with fine particle size (0.79 +/- 0.12 for particles between 100-200 nm). The analysis of the modal structure showed that the indoor aerosol size distribution characteristics differ from the outdoors under the effect of indoor sources. The percentage of unimodal size distributions increased during indoor emissions, compared to periods without indoor sources, along with the number concentration of Aitken mode particles, indicating emissions in specific size ranges according to the type of the indoor source.
  • Wagner, Robert; Manninen, Hanna E.; Franchin, Alessandro; Lehtipalo, Katrianne; Mirme, Sander; Steiner, Gerhard; Petäjä, Tuukka; Kulmala, Markku (2016)
    Here, we present a calibration of the Neutral cluster and Air Ion Spectrometer (NAIS, Airel Ltd.) for the size and concentration of ions in the mobility-diameter size-range 0.98-29.1 nm. Previous studies raised accuracy issues in size and concentration determination and highlighted the importance of used data inversion algorithm. Therefore, we investigated the performance of the NAIS by using five inversion methods. The presented results illustrate that the size information given by the NAIS is very accurate, regardless of the version of the data inversion. The number concentrations determined by the NAIS were 15%-30% too low especially at the lower end of the measurement size range (<5 nm), whereas concentrations at diameters 19.6 nm and larger were overestimated by up to 8%. With the correction presented in this study, the uncertainty of the ion concentration measurement of the NAIS can be reduced to less than 10%, allowing the NAIS to be used in quantitative ion cluster studies and more accurate determination of formation and growth rates.
  • Schmale, Julia; Baccarini, Andrea; Thurnherr, Iris; Henning, Silvia; Efraim, Avichay; Regayre, Leighton; Bolas, Conor; Hartmann, Markus; Welti, Andre; Lehtipalo, Katrianne; Aemisegger, Franziska; Tatzelt, Christian; Landwehr, Sebastian; Modini, Robin L.; Tummon, Fiona; Johnson, Jill S.; Harris, Neil; Schnaiter, Martin; Toffoli, Alessandro; Derkani, Marzieh; Bukowiecki, Nicolas; Stratmann, Frank; Dommen, Josef; Baltensperger, Urs; Wernli, Heinz; Rosenfeld, Daniel; Gysel-Beer, Martin; Carslaw, Ken S. (2019)
    Uncertainty in radiative forcing caused by aerosol-cloud interactions is about twice as large as for CO2 and remains the least well understood anthropogenic contribution to climate change. A major cause of uncertainty is the poorly quantified state of aerosols in the pristine preindustrial atmosphere, which defines the baseline against which anthropogenic effects are calculated. The Southern Ocean is one of the few remaining near-pristine aerosol environments on Earth, but there are very few measurements to help evaluate models. The Antarctic Circumnavigation Expedition: Study of Preindustrial-like Aerosols and their Climate Effects (ACE-SPACE) took place between December 2016 and March 2017 and covered the entire Southern Ocean region (Indian, Pacific, and Atlantic Oceans; length of ship track >33,000 km) including previously unexplored areas. In situ measurements covered aerosol characteristics [e.g., chemical composition, size distributions, and cloud condensation nuclei (CCN) number concentrations], trace gases, and meteorological variables. Remote sensing observations of cloud properties, the physical and microbial ocean state, and back trajectory analyses are used to interpret the in situ data. The contribution of sea spray to CCN in the westerly wind belt can be larger than 50%. The abundance of methanesulfonic acid indicates local and regional microbial influence on CCN abundance in Antarctic coastal waters and in the open ocean. We use the in situ data to evaluate simulated CCN concentrations from a global aerosol model. The extensive, available ACE-SPACE dataset () provides an unprecedented opportunity to evaluate models and to reduce the uncertainty in radiative forcing associated with the natural processes of aerosol emission, formation, transport, and processing occurring over the pristine Southern Ocean.