Author
Tuukka Petäjä
Other affiliations: Helsinki Institute of Physics, National Center for Atmospheric Research, University of Tyumen ...read more
Bio: Tuukka Petäjä is an academic researcher from University of Helsinki. The author has contributed to research in topics: Aerosol & Particle. The author has an hindex of 82, co-authored 526 publications receiving 30572 citations. Previous affiliations of Tuukka Petäjä include Helsinki Institute of Physics & National Center for Atmospheric Research.
Topics: Aerosol, Particle, Nucleation, Cloud condensation nuclei, Particle size
Papers published on a yearly basis
Papers
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TL;DR: In this paper, the growth rates of new particles during coastal and marine secondary aerosol particle formation events were studied in western Ireland, both at the Mace Head atmospheric research station and onboard the R/V Celtic Explorer as part of the Marine Aerosol Production project.
Abstract: [1] Growth rates of new particles during coastal and marine secondary aerosol particle formation events were studied in western Ireland, both at the Mace Head atmospheric research station and onboard the R/V Celtic Explorer as part of the Marine Aerosol Production project. Strong new particle formation events are frequently detected at Mace Head caused by the emission of precursor gases from exposed seaweed during low tide. Although these events were usually only detected as a mode of particles at a certain size, we were able to link the size of the mode to the growth time of these particles after the initial formation by combining data from several events measured between January 2006 and November 2007 with an air ion spectrometer. Typically, the early growth rates were extremely high, reaching values of several hundred nanometers per hour during the first seconds. The growth rates rapidly decreased and reached values below 1 nm h−1 within 1 h after nucleation. Our results were reproduced with box model calculations. All the obtained growth rates could be explained by the model either by varying the precursor formation time (typically a few seconds) or allowing multiple precursor vapor additions. From the ship-borne measurements, we report the first observations of purely open ocean new particle formation detected in this region. In total, four events were detected during this period, with three having a variable continental influence. An estimated average growth rate in marine conditions was 3 nm h−1 for these events.
41 citations
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TL;DR: In this paper, the gaseous sulfuric acid (H2SO4 ) is known as one of the key precursors for atmospheric new particle formation (NPF) processes, but its measurement remains challenging.
Abstract: . Gaseous sulfuric acid ( H2SO4 ) is known as one of
the key precursors for atmospheric new particle formation (NPF) processes,
but its measurement remains challenging. Therefore, a proxy method that is
able to derive gaseous sulfuric acid concentrations from parameters that can
be measured relatively easily and accurately is highly desirable for the
atmospheric chemistry community. Although such methods are available for
clean atmospheric environments, a proxy that works well in a polluted
atmosphere, such as that found in Chinese megacities, is yet to be developed.
In this study, the gaseous sulfuric acid concentration was measured in
February–March 2018, in urban Beijing using a nitrate based – long
time-of-flight chemical ionization mass spectrometer (LToF-CIMS). A number of
atmospheric parameters were recorded concurrently including the ultraviolet
radiation B (UVB) intensity, the concentrations of O3 ,
NOx (sum of NO and NO2 ), SO2 , and HONO,
and aerosol particle number size distributions. A proxy for atmospheric
daytime gaseous sulfuric acid concentration was derived via a statistical
analysis method using the UVB intensity, [ SO2 ], the condensation
sink (CS), [ O3 ], and [HONO] (or [ NOx ]) as the
predictor variables, where square brackets denote the concentrations of the corresponding species.
In this proxy method, we considered the formation of gaseous sulfuric acid from reactions
of SO2 and OH radicals during the daytime, and the loss of gaseous
sulfuric acid due to its condensation onto the preexisting particles. In
addition, we explored the formation of OH radicals from the conventional
gas-phase photochemistry using O3 as a proxy and from the
photolysis of HONO using HONO (and subsequently NOx ) as a
proxy. Our results showed that the UVB intensity and [ SO2 ] are
dominant factors in the production of gaseous sulfuric acid, and that the
simplest proxy could be constructed with the UVB intensity and
[ SO2 ] alone. When the OH radical production from both homogenously
and heterogeneously formed precursors were considered, the relative errors
were reduced by up to 20 %.
41 citations
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University of Helsinki1, Paul Scherrer Institute2, Helsinki Institute of Physics3, University of Eastern Finland4, Stockholm University5, CERN6, University of Beira Interior7, University of Lisbon8, University of Vienna9, Goethe University Frankfurt10, University of Innsbruck11, University of California, Irvine12, University of Leeds13, Carnegie Mellon University14, Russian Academy of Sciences15, California Institute of Technology16, Moscow Institute of Physics and Technology17, University of Manchester18, Boston College19, Nanjing University20, Finnish Meteorological Institute21
TL;DR: In this paper, the influence of ions on the nucleation rates under precisely controlled and atmospherically relevant conditions is quantified using a novel instrument setup consisting of two nanoparticle counters, one of them equipped with an ion filter.
Abstract: . The formation of secondary particles in the atmosphere accounts for more than half of global cloud condensation nuclei. Experiments at the CERN CLOUD (Cosmics Leaving OUtdoor Droplets) chamber have underlined the importance of ions for new particle formation, but quantifying their effect in the atmosphere remains challenging. By using a novel instrument setup consisting of two nanoparticle counters, one of them equipped with an ion filter, we were able to further investigate the ion-related mechanisms of new particle formation. In autumn 2015, we carried out experiments at CLOUD on four systems of different chemical compositions involving monoterpenes, sulfuric acid, nitrogen oxides, and ammonia. We measured the influence of ions on the nucleation rates under precisely controlled and atmospherically relevant conditions. Our results indicate that ions enhance the nucleation process when the charge is necessary to stabilize newly formed clusters, i.e., in conditions in which neutral clusters are unstable. For charged clusters that were formed by ion-induced nucleation, we were able to measure, for the first time, their progressive neutralization due to recombination with oppositely charged ions. A large fraction of the clusters carried a charge at 1.5 nm diameter. However, depending on particle growth rates and ion concentrations, charged clusters were largely neutralized by ion–ion recombination before they grew to 2.5 nm. At this size, more than 90 % of particles were neutral. In other words, particles may originate from ion-induced nucleation, although they are neutral upon detection at diameters larger than 2.5 nm. Observations at Hyytiala, Finland, showed lower ion concentrations and a lower contribution of ion-induced nucleation than measured at CLOUD under similar conditions. Although this can be partly explained by the observation that ion-induced fractions decrease towards lower ion concentrations, further investigations are needed to resolve the origin of the discrepancy.
40 citations
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University of Helsinki1, Goethe University Frankfurt2, CERN3, Finnish Meteorological Institute4, California Institute of Technology5, Helsinki Institute of Physics6, Environment Canada7, Dalhousie University8, Paul Scherrer Institute9, ETH Zurich10, University of Vienna11, Leibniz Association12, Centra13, University of Innsbruck14, Carnegie Mellon University15, Lebedev Physical Institute16, University of Leeds17
TL;DR: In this article, the results of laboratory measurements of the ion-ion recombination coefficient at different temperatures, relative humidities and concentrations of ozone and sulfur dioxide were presented, and the best agreement of the retrieved ion−ion recombinations coefficient with the commonly used literature value of 1.6 × 10−6 cm3 s−1 was found at a temperature of 5 °C and a relative humidity of 40 % (1.5 ± 0.6) × 10 −6 cm 3 s− 1.
Abstract: . We present the results of laboratory measurements of the ion–ion recombination coefficient at different temperatures, relative humidities and concentrations of ozone and sulfur dioxide. The experiments were carried out using the Cosmics Leaving OUtdoor Droplets (CLOUD) chamber at CERN, the walls of which are made of conductive material, making it possible to measure small ions. We produced ions in the chamber using a 3.5 GeV c−1 beam of positively charged pions (π+) generated by the CERN Proton Synchrotron (PS). When the PS was switched off, galactic cosmic rays were the only ionization source in the chamber. The range of the ion production rate varied from 2 to 100 cm−3 s−1, covering the typical range of ionization throughout the troposphere. The temperature ranged from −55 to 20 °C, the relative humidity (RH) from 0 to 70 %, the SO2 concentration from 0 to 40 ppb, and the ozone concentration from 200 to 700 ppb. The best agreement of the retrieved ion–ion recombination coefficient with the commonly used literature value of 1.6 × 10−6 cm3 s−1 was found at a temperature of 5 °C and a RH of 40 % (1.5 ± 0.6) × 10−6 cm3 s−1. At 20 °C and 40 % RH, the retrieved ion–ion recombination coefficient was instead (2.3 ± 0.7) × 10−6 cm3 s−1. We observed no dependency of the ion–ion recombination coefficient on ozone concentration and a weak variation with sulfur dioxide concentration. However, we observed a more than fourfold increase in the ion–ion recombination coefficient with decreasing temperature. We compared our results with three different models and found an overall agreement for temperatures above 0 °C, but a disagreement at lower temperatures. We observed a strong increase in the recombination coefficient for decreasing relative humidities, which has not been reported previously.
40 citations
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TL;DR: Airmodus A11 Particle Size Magnifier (PSM) and a combination of a high resolution differential mobility analyzer (DMA) and an electrometer were used in this article.
40 citations
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TL;DR: Results of older bio-kinetic studies with NSPs and newer epidemiologic and toxicologic studies with airborne ultrafine particles can be viewed as the basis for the expanding field of nanotoxicology, which can be defined as safety evaluation of engineered nanostructures and nanodevices.
Abstract: Although humans have been exposed to airborne nanosized particles (NSPs; < 100 nm) throughout their evolutionary stages, such exposure has increased dramatically over the last century due to anthropogenic sources. The rapidly developing field of nanotechnology is likely to become yet another source through inhalation, ingestion, skin uptake, and injection of engineered nanomaterials. Information about safety and potential hazards is urgently needed. Results of older bio-kinetic studies with NSPs and newer epidemiologic and toxicologic studies with airborne ultrafine particles can be viewed as the basis for the expanding field of nanotoxicology, which can be defined as safety evaluation of engineered nanostructures and nanodevices. Collectively, some emerging concepts of nanotoxicology can be identified from the results of these studies. When inhaled, specific sizes of NSPs are efficiently deposited by diffusional mechanisms in all regions of the respiratory tract. The small size facilitates uptake into cells and transcytosis across epithelial and endothelial cells into the blood and lymph circulation to reach potentially sensitive target sites such as bone marrow, lymph nodes, spleen, and heart. Access to the central nervous system and ganglia via translocation along axons and dendrites of neurons has also been observed. NSPs penetrating the skin distribute via uptake into lymphatic channels. Endocytosis and biokinetics are largely dependent on NSP surface chemistry (coating) and in vivo surface modifications. The greater surface area per mass compared with larger-sized particles of the same chemistry renders NSPs more active biologically. This activity includes a potential for inflammatory and pro-oxidant, but also antioxidant, activity, which can explain early findings showing mixed results in terms of toxicity of NSPs to environmentally relevant species. Evidence of mitochondrial distribution and oxidative stress response after NSP endocytosis points to a need for basic research on their interactions with subcellular structures. Additional considerations for assessing safety of engineered NSPs include careful selections of appropriate and relevant doses/concentrations, the likelihood of increased effects in a compromised organism, and also the benefits of possible desirable effects. An interdisciplinary team approach (e.g., toxicology, materials science, medicine, molecular biology, and bioinformatics, to name a few) is mandatory for nanotoxicology research to arrive at an appropriate risk assessment.
7,092 citations
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University of Illinois at Urbana–Champaign1, Joint Institute for the Study of the Atmosphere and Ocean2, Cooperative Institute for Research in Environmental Sciences3, University of Leeds4, University of Oslo5, United States Environmental Protection Agency6, University of Michigan7, Pacific Northwest National Laboratory8, German Aerospace Center9, United States Department of Energy10, Max Planck Society11, University of Tokyo12, National Oceanic and Atmospheric Administration13, Forschungszentrum Jülich14, Norwegian Meteorological Institute15, Indian Institute of Technology Bombay16, China Meteorological Administration17, Peking University18, Met Office19, Desert Research Institute20, Clarkson University21, Stanford University22, European Centre for Medium-Range Weather Forecasts23, International Institute of Minnesota24, Goddard Institute for Space Studies25, Yale University26, University of Washington27, University of California, Irvine28
TL;DR: In this paper, the authors provided an assessment of black-carbon climate forcing that is comprehensive in its inclusion of all known and relevant processes and that is quantitative in providing best estimates and uncertainties of the main forcing terms: direct solar absorption; influence on liquid, mixed phase, and ice clouds; and deposition on snow and ice.
Abstract: Black carbon aerosol plays a unique and important role in Earth's climate system. Black carbon is a type of carbonaceous material with a unique combination of physical properties. This assessment provides an evaluation of black-carbon climate forcing that is comprehensive in its inclusion of all known and relevant processes and that is quantitative in providing best estimates and uncertainties of the main forcing terms: direct solar absorption; influence on liquid, mixed phase, and ice clouds; and deposition on snow and ice. These effects are calculated with climate models, but when possible, they are evaluated with both microphysical measurements and field observations. Predominant sources are combustion related, namely, fossil fuels for transportation, solid fuels for industrial and residential uses, and open burning of biomass. Total global emissions of black carbon using bottom-up inventory methods are 7500 Gg yr−1 in the year 2000 with an uncertainty range of 2000 to 29000. However, global atmospheric absorption attributable to black carbon is too low in many models and should be increased by a factor of almost 3. After this scaling, the best estimate for the industrial-era (1750 to 2005) direct radiative forcing of atmospheric black carbon is +0.71 W m−2 with 90% uncertainty bounds of (+0.08, +1.27) W m−2. Total direct forcing by all black carbon sources, without subtracting the preindustrial background, is estimated as +0.88 (+0.17, +1.48) W m−2. Direct radiative forcing alone does not capture important rapid adjustment mechanisms. A framework is described and used for quantifying climate forcings, including rapid adjustments. The best estimate of industrial-era climate forcing of black carbon through all forcing mechanisms, including clouds and cryosphere forcing, is +1.1 W m−2 with 90% uncertainty bounds of +0.17 to +2.1 W m−2. Thus, there is a very high probability that black carbon emissions, independent of co-emitted species, have a positive forcing and warm the climate. We estimate that black carbon, with a total climate forcing of +1.1 W m−2, is the second most important human emission in terms of its climate forcing in the present-day atmosphere; only carbon dioxide is estimated to have a greater forcing. Sources that emit black carbon also emit other short-lived species that may either cool or warm climate. Climate forcings from co-emitted species are estimated and used in the framework described herein. When the principal effects of short-lived co-emissions, including cooling agents such as sulfur dioxide, are included in net forcing, energy-related sources (fossil fuel and biofuel) have an industrial-era climate forcing of +0.22 (−0.50 to +1.08) W m−2 during the first year after emission. For a few of these sources, such as diesel engines and possibly residential biofuels, warming is strong enough that eliminating all short-lived emissions from these sources would reduce net climate forcing (i.e., produce cooling). When open burning emissions, which emit high levels of organic matter, are included in the total, the best estimate of net industrial-era climate forcing by all short-lived species from black-carbon-rich sources becomes slightly negative (−0.06 W m−2 with 90% uncertainty bounds of −1.45 to +1.29 W m−2). The uncertainties in net climate forcing from black-carbon-rich sources are substantial, largely due to lack of knowledge about cloud interactions with both black carbon and co-emitted organic carbon. In prioritizing potential black-carbon mitigation actions, non-science factors, such as technical feasibility, costs, policy design, and implementation feasibility play important roles. The major sources of black carbon are presently in different stages with regard to the feasibility for near-term mitigation. This assessment, by evaluating the large number and complexity of the associated physical and radiative processes in black-carbon climate forcing, sets a baseline from which to improve future climate forcing estimates.
4,591 citations
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01 Jan 2014
TL;DR: Myhre et al. as discussed by the authors presented the contribution of Working Group I to the Fifth Assessment Report of the Intergovernmental Panel on Climate Change (IPCC) 2013: Anthropogenic and Natural Radiative forcing.
Abstract: This chapter should be cited as: Myhre, G., D. Shindell, F.-M. Bréon, W. Collins, J. Fuglestvedt, J. Huang, D. Koch, J.-F. Lamarque, D. Lee, B. Mendoza, T. Nakajima, A. Robock, G. Stephens, T. Takemura and H. Zhang, 2013: Anthropogenic and Natural Radiative Forcing. In: Climate Change 2013: The Physical Science Basis. Contribution of Working Group I to the Fifth Assessment Report of the Intergovernmental Panel on Climate Change [Stocker, T.F., D. Qin, G.-K. Plattner, M. Tignor, S.K. Allen, J. Boschung, A. Nauels, Y. Xia, V. Bex and P.M. Midgley (eds.)]. Cambridge University Press, Cambridge, United Kingdom and New York, NY, USA. Coordinating Lead Authors: Gunnar Myhre (Norway), Drew Shindell (USA)
3,684 citations
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University of Gothenburg1, University College Cork2, Paul Scherrer Institute3, Weizmann Institute of Science4, Chalmers University of Technology5, Norwegian Meteorological Institute6, University of Antwerp7, Carnegie Mellon University8, University of Lyon9, Centre national de la recherche scientifique10, University of California, Berkeley11, University of York12, Leibniz Institute for Neurobiology13, University of Mainz14, University of Florida15, University of Colorado Boulder16, Forschungszentrum Jülich17, Ghent University18, University of Manchester19, Aix-Marseille University20, California Institute of Technology21
TL;DR: In this article, an overview of the atmospheric degradation mechanisms for SOA precursors, gas-particle partitioning theory and analytical techniques used to determine the chemical composition of SOA is presented.
Abstract: Secondary organic aerosol (SOA) accounts for a significant fraction of ambient tropospheric aerosol and a detailed knowledge of the formation, properties and transformation of SOA is therefore required to evaluate its impact on atmospheric processes, climate and human health. The chemical and physical processes associated with SOA formation are complex and varied, and, despite considerable progress in recent years, a quantitative and predictive understanding of SOA formation does not exist and therefore represents a major research challenge in atmospheric science. This review begins with an update on the current state of knowledge on the global SOA budget and is followed by an overview of the atmospheric degradation mechanisms for SOA precursors, gas-particle partitioning theory and the analytical techniques used to determine the chemical composition of SOA. A survey of recent laboratory, field and modeling studies is also presented. The following topical and emerging issues are highlighted and discussed in detail: molecular characterization of biogenic SOA constituents, condensed phase reactions and oligomerization, the interaction of atmospheric organic components with sulfuric acid, the chemical and photochemical processing of organics in the atmospheric aqueous phase, aerosol formation from real plant emissions, interaction of atmospheric organic components with water, thermodynamics and mixtures in atmospheric models. Finally, the major challenges ahead in laboratory, field and modeling studies of SOA are discussed and recommendations for future research directions are proposed.
3,324 citations