Browsing by Subject "CLUSTERS"

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  • Yao, Lei; Garmash, Olga; Bianchi, Federico; Zheng, Jun; Yan, Chao; Kontkanen, Jenni; Junninen, Heikki; Mazon, Stephany Buenrostro; Ehn, Mikael; Paasonen, Pauli; Sipilä, Mikko; Wang, Mingyi; Wang, Xinke; Xiao, Shan; Chen, Hangfei; Lu, Yiqun; Zhang, Bowen; Wang, Dongfang; Fu, Qingyan; Geng, Fuhai; Li, Li; Wang, Hongli; Qiao, Liping; Yang, Xin; Chen, Jianmin; Kerminen, Veli-Matti; Petäjä, Tuukka; Worsnop, Douglas R.; Kulmala, Markku; Wang, Lin (2018)
    Atmospheric new particle formation (NPF) is an important global phenomenon that is nevertheless sensitive to ambient conditions. According to both observation and theoretical arguments, NPF usually requires a relatively high sulfuric acid (H2SO4) concentration to promote the formation of new particles and a low preexisting aerosol loading to minimize the sink of new particles. We investigated NPF in Shanghai and were able to observe both precursor vapors (H2SO4) and initial clusters at a molecular level in a megacity. High NPF rates were observed to coincide with several familiar markers suggestive of H2SO4-dimethylamine (DMA)water (H2O) nucleation, including sulfuric acid dimers and H2SO4-DMA clusters. In a cluster kinetics simulation, the observed concentration of sulfuric acid was high enough to explain the particle growth to similar to 3 nanometers under the very high condensation sink, whereas the subsequent higher growth rate beyond this size is believed to result fromthe added contribution of condensing organic species. These findings will help in understanding urban NPF and its air quality and climate effects, as well as in formulating policies to mitigate secondary particle formation in China.
  • Mason, D. R.; Sand, A. E.; Dudarev, S. L. (2019)
    We describe the development of a new object kinetic Monte Carlo (kMC) code where the elementary defect objects are off-lattice atomistic configurations. Atomic-level transitions are used to transform and translate objects, to split objects and to merge them together. This gradually constructs a database of atomic configurations-a set of relevant defect objects and their possible events generated on-the-fly. Elastic interactions are handled within objects with empirical potentials at short distances, and between spatially distinct objects using the dipole tensor formalism. The model is shown to evolve mobile interstitial clusters in tungsten faster than an equivalent molecular dynamics (MD) simulation, even at elevated temperatures. We apply the model to the evolution of complex defects generated using MD simulations of primary radiation damage in tungsten. We show that we can evolve defect structures formed in cascade simulations to experimentally observable timescales of seconds while retaining atomistic detail. We conclude that the first few nanoseconds of simulation following cascade initiation would be better performed using MD, as this will capture some of the near-temperature-independent evolution of small highly-mobile interstitial clusters. For the 20keV cascade annealing simulations considered here, we observe internal relaxations of sessile objects. These relaxations would be difficult to capture using conventional object kMC, yet are important as they establish the conditions for long timescale evolution.
  • Kangasluoma, Juha; Hering, Susanne; Picard, David; Lewis, Gregory; Enroth, Joonas; Korhonen, Frans; Kulmala, Markku; Sellegri, Karine; Attoui, Michel; Petäjä, Tuukka (2017)
    In this study we characterized the performance of three new particle counters able to detect particles smaller than 3 nm during the Helsinki condensation particle counter (CPC) workshop in summer 2016: the Aerosol Dynamics Inc. (ADI; Berkeley, USA) versatile water condensation particle counter (vWCPC), TSI 3777 nano enhancer (TSI Inc., Shoreview, USA) and modified and boosted TSI 3010-type CPC from Universite Blaise Pascal called a B3010. The performance of all CPCs was first measured with charged tungsten oxide test particles at temperature settings which resulted in supersaturation low enough to not detect any ions produced by a radioactive source. Due to similar measured detection efficiencies, additional comparison between the 3777 and vWCPC were conducted using electrically neutral tungsten oxide test particles and with positively charged tetradodecylammonium bromide. Furthermore, the detection efficiencies of the 3777 and vWCPC were measured with boosted temperature settings yielding supersaturation which was at the onset of homogeneous nucleation for the 3777 or confined within the range of liquid water for the ADI vWCPC. Finally, CPC-specific tests were conducted to probe the response of the 3777 to various inlet flow relative humidities, of the B3010 to various inlet flow rates and of the vWCPC to various particle concentrations. For the 3777 and vWCPC the measured 50% detection diameters (d50s) were in the range of 1.3-2.4 nm for the tungsten oxide particles, depending on the particle charging state and CPC temperature settings, between 2.5 and 3.3 nm for the organic test aerosol, and in the range of 3.2-3.4 nm for tungsten oxide for the B3010.
  • Vaikkinen, Anu; Kauppila, Tiina J.; Kostiainen, Risto (2016)
    The efficiencies of charge exchange reaction in dopant-assisted atmospheric pressure chemical ionization (DA-APCI) and dopant-assisted atmospheric pressure photoionization (DA-APPI) mass spectrometry (MS) were compared by flow injection analysis. Fourteen individual compounds and a commercial mixture of 16 polycyclic aromatic hydrocarbons were chosen as model analytes to cover a wide range of polarities, gas-phase ionization energies, and proton affinities. Chlorobenzene was used as the dopant, and methanol/water (80/20) as the solvent. In both techniques, analytes formed the same ions (radical cations, protonated molecules, and/or fragments). However, in DA-APCI, the relative efficiency of charge exchange versus proton transfer was lower than in DA-APPI. This is suggested to be because in DA-APCI both dopant and solvent clusters can be ionized, and the formed reagent ions can react with the analytes via competing charge exchange and proton transfer reactions. In DA-APPI, on the other hand, the main reagents are dopant-derived radical cations, which favor ionization of analytes via charge exchange. The efficiency of charge exchange in both DA-APPI and DA-APCI was shown to depend heavily on the solvent flow rate, with best efficiency seen at lowest flow rates studied (0.05 and 0.1 mL/min). Both DA-APCI and DA-APPI showed the radical cation of chlorobenzene at 0.05-0.1 mL/min flow rate, but at increasing flow rate, the abundance of chlorobenzene M+. decreased and reagent ion populations deriving from different gas-phase chemistry were recorded. The formation of these reagent ions explains the decreasing ionization efficiency and the differences in charge exchange between the techniques.
  • Liu, Yun; Liao, Shihong; Liu, Xiangkun; Zhang, Jiajun; An, Rui; Fan, Zuhui (2022)
    The interacting dark energy (IDE) model, which considers the interaction between dark energy and dark matter, provides a natural mechanism to alleviate the coincidence problem and can also relieve the observational tensions under the ?CDM model. Previous studies have put constraints on IDE models by observations of cosmic expansion history, cosmic microwave background, and large-scale structures. However, these data are not yet enough to distinguish IDE models from ?CDM effectively. Because the non-linear structure formation contains rich cosmological information, it can provide additional means to differentiate alternative models. In this paper, based on a set of N-body simulations for IDE models, we investigate the formation histories and properties of dark matter haloes and compare with their ?CDM counterparts. For the model with dark matter decaying into dark energy and the parameters being the best-fitting values from previous constraints, the structure formation is markedly slowed down, and the haloes have systematically lower mass, looser internal structure, higher spin, and anisotropy. This is inconsistent with the observed structure formation, and thus this model can be safely ruled out from the perspective of non-linear structure formation. Moreover, we find that the ratio of halo concentrations between IDE and ?CDM counterparts depends sensitively on the interaction parameter and is independent of halo mass. This can act as a powerful probe to constrain IDE models. Our results concretely demonstrate that the interaction of the two dark components can affect the halo formation considerably, and therefore the constraints from non-linear structures are indispensable.
  • Granberg, F.; Byggmästar, J.; Nordlund, K. (2020)
    The understanding of materials' behaviour during continuous irradiation is of great interest for utilizing materials in environments where harsh radiation is present, like nuclear power plants. Most power plants, both current and future ones, are based, at least partially, on Fe or FeCr alloys. In this study, we investigate the response of BCC Fe and several FeCr alloys to massively overlapping cascades. The effect of the added chromium on the defect accumulation and defect evolution was studied. Both a bulk setup, for observing the evolution deep inside the material far from grain boundaries and surfaces, and a setup with a nearby open surface, to investigate the effect of a permanent defect sink, were studied. We found that the primary defect production is similar in all materials, and also the build-up before serious overlap is comparable. When cascade overlap starts, we found that different sized clusters are formed in the different materials, depending on the setup. The defect cluster evolution was followed and could be related to the dislocation reactions in the materials. We found that the irradiation mixing was specific to the different chromium concentrations, the low chromium-containing alloy showed ordering, whereas the highest chromium-containing sample showed segregation. (C) 2019 The Authors. Published by Elsevier B.V.
  • Simon, Mario; Heinritzi, Martin; Herzog, Stephan; Leiminger, Markus; Bianchi, Federico; Praplan, Arnaud; Dommen, Josef; Curtius, Joachim; Kuerten, Andreas (2016)
    Amines are potentially important for atmospheric new particle formation, but their concentrations are usually low with typical mixing ratios in the pptv range or even smaller. Therefore, the demand for highly sensitive gas-phase amine measurements has emerged in the last several years. Nitrate chemical ionization mass spectrometry (CIMS) is routinely used for the measurement of gas-phase sulfuric acid in the sub-pptv range. Furthermore, extremely low volatile organic compounds (ELVOCs) can be detected with a nitrate CIMS. In this study we demonstrate that a nitrate CIMS can also be used for the sensitive measurement of dimethylamine (DMA, (CH3)(2)NH) using the NO3-center dot(HNO3)(1-2)center dot(DMA) cluster ion signal. Calibration measurements were made at the CLOUD chamber during two different measurement campaigns. Good linearity between 0 and similar to 120 pptv of DMA as well as a sub-pptv detection limit of 0.7 pptv for a 10 min integration time are demonstrated at 278 K and 38% RH.
  • Rondo, L.; Ehrhart, S.; Kuerten, A.; Adamov, A.; Bianchi, F.; Breitenlechner, M.; Duplissy, J.; Franchin, A.; Dommen, J.; Donahue, N. M.; Dunne, E. M.; Flagan, R. C.; Hakala, J.; Hansel, A.; Keskinen, H.; Kim, J.; Jokinen, T.; Lehtipalo, K.; Leiminger, M.; Praplan, A.; Riccobono, F.; Rissanen, M. P.; Sarnela, N.; Schobesberger, S.; Simon, M.; Sipilä, M.; Smith, J. N.; Tome, A.; Trostl, J.; Tsagkogeorgas, G.; Vaattovaara, P.; Winkler, P. M.; Williamson, C.; Wimmer, D.; Baltensperger, U.; Kirkby, J.; Kulmala, M.; Petäjä, T.; Worsnop, D. R.; Curtius, J. (2016)
    Sulfuric acid is widely recognized as a very important substance driving atmospheric aerosol nucleation. Based on quantum chemical calculations it has been suggested that the quantitative detection of gas phase sulfuric acid (H2SO4) by use of Chemical Ionization Mass Spectrometry (CIMS) could be biased in the presence of gas phase amines such as dimethylamine (DMA). An experiment (CLOUD7 campaign) was set up at the CLOUD (Cosmics Leaving OUtdoor Droplets) chamber to investigate the quantitative detection of H2SO4 in the presence of dimethylamine by CIMS at atmospherically relevant concentrations. For the first time in the CLOUD experiment, the monomer sulfuric acid concentration was measured by a CIMS and by two CI-APi-TOF (Chemical Ionization-Atmospheric Pressure interface-Time Of Flight) mass spectrometers. In addition, neutral sulfuric acid clusters were measured with the CI-APi-TOFs. The CLOUD7 measurements show that in the presence of dimethylamine (
  • Bonny, G.; Castin, N.; Bakaev, A.; Sand, A. E.; Terentyev, D. (2020)
    In recent years, a number of systematic investigations of high-energy collision cascades in tungsten employing advanced defect analysis tools have shown that interstitial clusters can form complex non-planar dislocation structures. These structures are sessile in nature and may potentially have a strong impact on the long-term evolution of the radiation microstructure. To clarify this aspect, we selected several representative primary damage states of cascades debris and performed annealing simulations using molecular dynamics (MD). We found that immobile complexes of non-planar dislocation structures (CDS) evolve into glissile and planar shaped 1/2 <1 1 1 > loops with an activation energy of similar to 1.5 eV. The CDS objects were implemented in an object kinetic Monte Carlo (OKMC) model accounting for the event of transformation into 1-D migrating loops, following the MD data. OKMC was then used to investigate the impact of the transformation event (and the associated activation energy) on the evolution of the microstructure.
  • Myllys, Nanna; Ponkkonen, Tuomo; Chee, Sabrina; Smith, James (2020)
    The role of an oxidation product of trimethylamine, trimethylamine oxide, in atmospheric particle formation is studied using quantum chemical methods and cluster formation simulations. Molecular-level cluster formation mechanisms are resolved, and theoretical results on particle formation are confirmed with mass spectrometer measurements. Trimethylamine oxide is capable of forming only one hydrogen bond with sulfuric acid, but unlike amines, trimethylamine oxide can form stable clusters via ion-dipole interactions. That is because of its zwitterionic structure, which causes a high dipole moment. Cluster growth occurs close to the acid:base ratio of 1:1, which is the same as for other monoprotic bases. Enhancement potential of trimethylamine oxide in particle formation is much higher than that of dimethylamine, but lower compared to guanidine. Therefore, at relatively low concentrations and high temperatures, guanidine and trimethylamine oxide may dominate particle formation events over amines.
  • Cseh, András; Poczai, Péter; Kiss, Tibor; Balla, Kirsztina; Berki, Zita; Horváth, Ádám; Kúti, Csaba; Karsai, Ildikó (2021)
    Historical wheat landraces are rich sources of genetic diversity offering untapped reservoirs for broadening the genetic base of modern varieties. Using a 20K SNP array, we investigated the accessible genetic diversity in a Central European bread wheat landrace collection with great drought, heat stress tolerance and higher tillering capacity. We discovered distinct differences in the number of average polymorphisms between landraces and modern wheat cultivars, and identified a set of novel rare alleles present at low frequencies in the landrace collection. The detected polymorphisms were unevenly distributed along the wheat genome, and polymorphic markers co-localized with genes of great agronomic importance. The geographical distribution of the inferred Bayesian clustering revealed six genetically homogenous ancestral groups among the collection, where the Central European core bared an admixed background originating from four ancestral groups. We evaluated the effective population sizes (Ne) of the Central European collection and assessed changes in diversity overtime, which revealed a dramatic similar to 97% genetic erosion between 1955 and 2015.
  • Herrero, Annika; Klutsch, Cornelya F. C.; Holmala, Katja; Maduna, Simo N.; Kopatz, Alexander; Eiken, Hans Geir; Hagen, Snorre B. (2021)
    Conservation and management of large carnivores requires knowledge of female and male dispersal. Such information is crucial to evaluate the population's status and thus management actions. This knowledge is challenging to obtain, often incomplete and contradictory at times. The size of the target population and the methods applied can bias the results. Also, population history and biological or environmental influences can affect dispersal on different scales within a study area. We have genotyped Eurasian lynx (180 males and 102 females, collected 2003-2017) continuously distributed in southern Finland (similar to 23,000 km(2)) using 21 short tandem repeats (STR) loci and compared statistical genetic tests to infer local and sex-specific dispersal patterns within and across genetic clusters as well as geographic regions. We tested for sex-specific substructure with individual-based Bayesian assignment tests and spatial autocorrelation analyses. Differences between the sexes in genetic differentiation, relatedness, inbreeding, and diversity were analysed using population-based AMOVA, F-statistics, and assignment indices. Our results showed two different genetic clusters that were spatially structured for females but admixed for males. Similarly, spatial autocorrelation and relatedness was significantly higher in females than males. However, we found weaker sex-specific patterns for the Eurasian lynx when the data were separated in three geographical regions than when divided in the two genetic clusters. Overall, our results suggest male-biased dispersal and female philopatry for the Eurasian lynx in Southern Finland. The female genetic structuring increased from west to east within our study area. In addition, detection of male-biased dispersal was dependent on analytical methods utilized, on whether subtle underlying genetic structuring was considered or not, and the choice of population delineation. Conclusively, we suggest using multiple genetic approaches to study sex-biased dispersal in a continuously distributed species in which population delineation is difficult.
  • GBD 2016 Occupational Risk; Driscoll, Tim; Meretoja, Tuomo J.; Shiri, Rahman (2020)
    Objectives This study provides an overview of the influence of occupational risk factors on the global burden of disease as estimated by the occupational component of the Global Burden of Disease (GBD) 2016 study. Methods The GBD 2016 study estimated the burden in terms of deaths and disability-adjusted life years (DALYs) arising from the effects of occupational risk factors (carcinogens; asthmagens; particulate matter, gases and fumes (PMGF); secondhand smoke (SHS); noise; ergonomic risk factors for low back pain; risk factors for injury). A population attributable fraction (PAF) approach was used for most risk factors. Results In 2016, globally, an estimated 1.53 (95% uncertainty interval 1.39-1.68) million deaths and 76.1 (66.3-86.3) million DALYs were attributable to the included occupational risk factors, accounting for 2.8% of deaths and 3.2% of DALYs from all causes. Most deaths were attributable to PMGF, carcinogens (particularly asbestos), injury risk factors and SHS. Most DALYs were attributable to injury risk factors and ergonomic exposures. Men and persons 55 years or older were most affected. PAFs ranged from 26.8% for low back pain from ergonomic risk factors and 19.6% for hearing loss from noise to 3.4% for carcinogens. DALYs per capita were highest in Oceania, Southeast Asia and Central sub-Saharan Africa. On a per capita basis, between 1990 and 2016 there was an overall decrease of about 31% in deaths and 25% in DALYs. Conclusions Occupational exposures continue to cause an important health burden worldwide, justifying the need for ongoing prevention and control initiatives.
  • GBD 2019 Risk Factors (2020)
    Background Rigorous analysis of levels and trends in exposure to leading risk factors and quantification of their effect on human health are important to identify where public health is making progress and in which cases current efforts are inadequate. The Global Burden of Diseases, Injuries, and Risk Factors Study (GBD) 2019 provides a standardised and comprehensive assessment of the magnitude of risk factor exposure, relative risk, and attributable burden of disease. Methods GBD 2019 estimated attributable mortality, years of life lost (YLLs), years of life lived with disability (YLDs), and disability-adjusted life-years (DALYs) for 87 risk factors and combinations of risk factors, at the global level, regionally, and for 204 countries and territories. GBD uses a hierarchical list of risk factors so that specific risk factors (eg, sodium intake), and related aggregates (eg, diet quality), are both evaluated. This method has six analytical steps. (1) We included 560 risk-outcome pairs that met criteria for convincing or probable evidence on the basis of research studies. 12 risk-outcome pairs included in GBD 2017 no longer met inclusion criteria and 47 risk-outcome pairs for risks already included in GBD 2017 were added based on new evidence. (2) Relative risks were estimated as a function of exposure based on published systematic reviews, 81 systematic reviews done for GBD 2019, and meta-regression. (3) Levels of exposure in each age-sex-location-year included in the study were estimated based on all available data sources using spatiotemporal Gaussian process regression, DisMod-MR 2.1, a Bayesian meta-regression method, or alternative methods. (4) We determined, from published trials or cohort studies, the level of exposure associated with minimum risk, called the theoretical minimum risk exposure level. (5) Attributable deaths, YLLs, YLDs, and DALYs were computed by multiplying population attributable fractions (PAFs) by the relevant outcome quantity for each age-sex-location-year. (6) PAFs and attributable burden for combinations of risk factors were estimated taking into account mediation of different risk factors through other risk factors. Across all six analytical steps, 30 652 distinct data sources were used in the analysis. Uncertainty in each step of the analysis was propagated into the final estimates of attributable burden. Exposure levels for dichotomous, polytomous, and continuous risk factors were summarised with use of the summary exposure value to facilitate comparisons over time, across location, and across risks. Because the entire time series from 1990 to 2019 has been re-estimated with use of consistent data and methods, these results supersede previously published GBD estimates of attributable burden. Findings The largest declines in risk exposure from 2010 to 2019 were among a set of risks that are strongly linked to social and economic development, including household air pollution; unsafe water, sanitation, and handwashing; and child growth failure. Global declines also occurred for tobacco smoking and lead exposure. The largest increases in risk exposure were for ambient particulate matter pollution, drug use, high fasting plasma glucose, and high body-mass index. In 2019, the leading Level 2 risk factor globally for attributable deaths was high systolic blood pressure, which accounted for 10.8 million (95% uncertainty interval [UI] 9.51-12.1) deaths (19.2% [16.9-21.3] of all deaths in 2019), followed by tobacco (smoked, second-hand, and chewing), which accounted for 8.71 million (8.12-9.31) deaths (15.4% [14.6-16.2] of all deaths in 2019). The leading Level 2 risk factor for attributable DALYs globally in 2019 was child and maternal malnutrition, which largely affects health in the youngest age groups and accounted for 295 million (253-350) DALYs (11.6% [10.3-13.1] of all global DALYs that year). The risk factor burden varied considerably in 2019 between age groups and locations. Among children aged 0-9 years, the three leading detailed risk factors for attributable DALYs were all related to malnutrition. Iron deficiency was the leading risk factor for those aged 10-24 years, alcohol use for those aged 25-49 years, and high systolic blood pressure for those aged 50-74 years and 75 years and older. Interpretation Overall, the record for reducing exposure to harmful risks over the past three decades is poor. Success with reducing smoking and lead exposure through regulatory policy might point the way for a stronger role for public policy on other risks in addition to continued efforts to provide information on risk factor harm to the general public. Copyright (C) 2020 The Author(s). Published by Elsevier Ltd.
  • Venäläinen, A.; Jalkanen, P.; Tuboltsev, V.; Savin, A.; Räisänen, J. (2018)
    Cluster deposited Pd films exhibit ferromagnetism in the temperature range from 1.8 to 400K. The magnetization properties are found to be dependent on the film thickness. The varying morphology of the resulting Pd film with respect to thickness suggests that cluster size, deposition energy, and substrate type are crucial for the resulting film magnetization. This is demonstrated by the characteristic ferromagnetic hysteresis with the temperature dependent saturation magnetization, remanence. and coercivity of palladium nanocluster aggregates. The temperature dependence of the saturation magnetization, remanence, and coercivity of Pd nanoclusters were measured using an ultra-high-sensitive magnetometer based on a superconducting quantum interference device, and the morphology of the samples was analyzed by tunneling electron microscopy. Published by AIP Publishing.
  • Myllys, Nanna; Ponkkonen, Tuomo; Passananti, Monica; Elm, Jonas; Vehkamäki, Hanna; Olenius, Tinja (2018)
    The role of a strong organobase, guanidine, in sulfuric acid-driven new-particle formation is studied using state-of-the-art quantum chemical methods and molecular cluster formation simulations. Cluster formation mechanisms at the molecular level are resolved, and theoretical results on cluster stability are confirmed with mass spectrometer measurements. New-particle formation from guanidine and sulfuric acid molecules occurs without thermodynamic barriers under studied conditions, and clusters are growing close to a 1:1 composition of acid and base. Evaporation rates of the most stable clusters are extremely low, which can be explained by the proton transfers and symmetrical cluster structures. We compare the ability of guanidine and dimethylamine to enhance sulfuric acid-driven particle formation and show that more than 2000-fold concentration of dimethylamine is needed to yield as efficient particle formation as in the case of guanidine. At similar conditions, guanidine yields 8 orders of magnitude higher particle formation rates compared to dimethylamine. Highly basic compounds such as guanidine may explain experimentally observed particle formation events at low precursor vapor concentrations, whereas less basic and more abundant bases such as ammonia and amines are likely to explain measurements at high concentrations.
  • Toropainen, Antti Elia; Kangasluoma, Juha; Kurten, Theo; Vehkamäki, Hanna; Keshavarz, Fatemeh; Kubecka, Jakub (2021)
    Using a combination of quantum chemistry and cluster size distribution dynamics, we study the heterogeneous nucleation of n-butanol and water onto sodium chloride (NaCl)(10) seeds at different butanol saturation ratios and relative humidities. We also investigate how the heterogeneous nucleation of butanol is affected by the seed size through comparing (NaCl)(5), (NaCl)(10), and ( NaCl)(25) seeds and by seed electrical charge through comparing (Na10Cl9)(+), (NaCl)(10), and (Na9Cl10)(-) seeds. Butanol is a common working fluid for condensation particle counters used in atmospheric aerosol studies, and NaCl seeds are frequently used for calibration purposes and as model systems, for example, sea spray aerosol. In general, our simulations reproduce the experimentally observed trends for the NaCl-BuOH-H2O system, such as the increase of nucleation rate with relative humidity and with temperature (at constant supersaturation of butanol). Our results also provide molecular-level insights into the vapor-seed interactions driving the first steps of the heterogeneous nucleation process. The main purpose of this work is to show that theoretical studies can provide molecular understanding of initial steps of heterogeneous nucleation and that it is possible to find cost-effective yet accurate-enough combinations of methods for configurational sampling and energy evaluation to successfully model heterogeneous nucleation of multicomponent systems. In the future, we anticipate that such simulations can also be extended to chemically more complex seeds.
  • Cassidy, Cathal; Singh, Vidyadhar; Grammatikopoulos, Panagiotis; Djurabekova, Flyura; Nordlund, Kai; Sowwan, Mukhles (2013)
  • Leino, Katri; Nieminen, Tuomo; Manninen, Hanna E.; Petäjä, Tuukka; Kerminen, Veli-Matti; Kulmala, Markku (2016)
    Secondary aerosol formation from gas-phase precursors is a frequent phenomenon occurring in a boreal environment. Traditionally, this process is identified visually from observational data on total and ion number size distributions. Here, we introduce a new, objective classification method for the new particle formation events based on measured intermediate-ion concentrations. The intermediate-ion concentration is a suitable indicator of new particle formation, because it is linked to the atmospheric new particle formation. The concentration of intermediate ions is typically very low (below 5 cm(-3)) when there is no new particle formation or precipitation events occurring. In this study, we analysed concentrations of negative intermediate ions at the Station for Measuring Ecosystem Atmosphere Relations (SMEAR II) in Hyytiala, Finland, during the years 2003-2013. We found that the half-hour median concentration of negative intermediate ions in sizes 2-4 nm was > 20 cm(-3) during 77.5% of event days classified by traditional method. The corresponding value was 92.3% in the case of 2-7 nm negative ions. In addition, the intermediate-ion concentration varied seasonally in a similar manner as the number of event days, peaking in the spring. A typical diurnal variation of the intermediate-ion concentration resembled that of the particle concentration during the event days. We developed here a new method for classifying new particle formation events based on intermediate-ion concentrations. The new method is complementary to the traditional event analysis and it can also be used as an automatic way of determining new particle formation events from large data sets.
  • Kangasluoma, Juha; Ahonen, Lauri R.; Laurila, Tiia M.; Cai, Runlong; Enroth, Joonas; Mazon, Stephany Buenrostro; Korhonen, Frans; Aalto, Pasi P.; Kulmala, Markku; Attoui, Michel; Petäjä, Tuukka (2018)
    Measurement of atmospheric sub-10 nm nanoparticle number concentrations has been of substantial interest recently, which, however, is subject to considerable uncertainty. We report a laboratory characterization of a high flow differential mobility particle sizer (HFDMPS), which is based on the Half-mini type differential mobility analyzer (DMA) and nano condensation nuclei counter (A11), and show the first results from atmospheric observations. The HFDMPS utilizes the state-of-the-art aerosol technology, and is optimized for sub-10 nm particle size distribution measurements by a moderate resolution DMA, optimized and characterized low-loss particle sampling line and minimal dilution in the detector. We present an exhaustive laboratory calibration to the HFDMPS and compare the measured size data to the Hyytiala long-term DMPS and Neutral cluster and ion spectrometer. The HFDMPS detects about two times higher 3-10 nm particle concentrations than the long-term DMPS, and the counting uncertainties are halved as compared to the long-term DMPS. The HFDMPS did not observe any sub-2.5 nm particles in Hyytiala, and the reason for that was shown to be the inability of diethylene glycol to condense on such small biogenic particles. Last, we discuss the general implications of our results to the sub-10 nm DMPS based measurements.