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Sökning: WFRF:(Markku Kulmala)

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1.
  • Hari, Pertti, et al. (författare)
  • Prediction of photosynthesis in Scots pine ecosystems across Europe by a needle-level theory
  • 2018
  • Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 18:18, s. 13321-13328
  • Tidskriftsartikel (refereegranskat)abstract
    • Photosynthesis provides carbon for the synthesis of macromolecules to construct cells during growth. This is the basis for the key role of photosynthesis in the carbon dynamics of ecosystems and in the biogenic CO2 assimilation. The development of eddy-covariance (EC) measurements for ecosystem CO2 fluxes started a new era in the field studies of photosynthesis. However, the interpretation of the very variable CO2 fluxes in evergreen forests has been problematic especially in transition times such as the spring and autumn. We apply two theoretical needle-level equations that connect the variation in the light intensity, stomatal action and the annual metabolic cycle of photosynthesis. We then use these equations to predict the photosynthetic CO2 flux in five Scots pine stands located from the northern timberline to Central Europe. Our result has strong implications for our conceptual understanding of the effects of the global change on the processes in boreal forests, especially of the changes in the metabolic annual cycle of photosynthesis.
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2.
  • Nieminen, T., et al. (författare)
  • Parameterization of ion-induced nucleation rates based on ambient = servations
  • 2011
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:7, s. 3393-3402
  • Tidskriftsartikel (refereegranskat)abstract
    • Atmospheric ions participate in the formation of new atmospheric aerosol particles, yet their exact role in this process has remained unclear. Here we derive a new simple parameterization for ion-induced nucleation or, more precisely, for the formation rate of charged 2-nm particles. The parameterization is semi-empirical in the sense that it is based on comprehensive results of one-year-long atmospheric cluster and particle measurements in the size range similar to 1-42 nm within the EUCAARI (European Integrated project on Aerosol Cloud Climate and Air Quality interactions) project. Data from 12 field sites across Europe measured with different types of air ion and cluster mobility spectrometers were used in our analysis, with more in-depth analysis made using data from four stations with concomitant sulphuric acid measurements. The parameterization is given in two slightly different forms: a more accurate one that requires information on sulfuric acid and nucleating organic vapor concentrations, and a simpler one in which this information is replaced with the global radiation intensity. These new parameterizations are applicable to all large-scale atmospheric models containing size-resolved aerosol microphysics, and a scheme to calculate concentrations of sulphuric acid, condensing organic vapours and cluster ions.
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3.
  • Almeida, Joao, et al. (författare)
  • Molecular understanding of sulphuric acid-amine particle nucleation in the atmosphere
  • 2013
  • Ingår i: Nature. - : Springer Science and Business Media LLC. - 0028-0836 .- 1476-4687. ; 502:7471, s. 359-
  • Tidskriftsartikel (refereegranskat)abstract
    • Nucleation of aerosol particles from trace atmospheric vapours is thought to provide up to half of global cloud condensation nuclei(1). Aerosols can cause a net cooling of climate by scattering sunlight and by leading to smaller but more numerous cloud droplets, which makes clouds brighter and extends their lifetimes(2). Atmospheric aerosols derived from human activities are thought to have compensated for a large fraction of the warming caused by greenhouse gases(2). However, despite its importance for climate, atmospheric nucleation is poorly understood. Recently, it has been shown that sulphuric acid and ammonia cannot explain particle formation rates observed in the lower atmosphere(3). It is thought that amines may enhance nucleation(4-16), but until now there has been no direct evidence for amine ternary nucleation under atmospheric conditions. Here we use the CLOUD (Cosmics Leaving OUtdoor Droplets) chamber at CERN and find that dimethylamine above three parts per trillion by volume can enhance particle formation rates more than 1,000-fold compared with ammonia, sufficient to account for the particle formation rates observed in the atmosphere. Molecular analysis of the clusters reveals that the faster nucleation is explained by a base-stabilization mechanism involving acid-amine pairs, which strongly decrease evaporation. The ion-induced contribution is generally small, reflecting the high stability of sulphuric acid-dimethylamine clusters and indicating that galactic cosmic rays exert only a small influence on their formation, except at low overall formation rates. Our experimental measurements are well reproduced by a dynamical model based on quantum chemical calculations of binding energies of molecular clusters, without any fitted parameters. These results show that, in regions of the atmosphere near amine sources, both amines and sulphur dioxide should be considered when assessing the impact of anthropogenic activities on particle formation.
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4.
  • Arneth, Almut, et al. (författare)
  • Clean the Air, Heat the Planet?
  • 2009
  • Ingår i: Science. - : American Association for the Advancement of Science (AAAS). - 1095-9203 .- 0036-8075. ; 326:5953, s. 672-673
  • Tidskriftsartikel (övrigt vetenskapligt/konstnärligt)abstract
    • Measures to control emissions of air pollutants may have unintended climatic consequences.
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5.
  • Artaxo, Paulo, et al. (författare)
  • Tropical and Boreal Forest – Atmosphere Interactions : A Review
  • 2022
  • Ingår i: Tellus. Series B, Chemical and physical meteorology. - : Stockholm University Press. - 0280-6509 .- 1600-0889. ; 74:1, s. 24-163
  • Forskningsöversikt (refereegranskat)abstract
    • This review presents how the boreal and the tropical forests affect the atmosphere, its chemical composition, its function, and further how that affects the climate and, in return, the ecosystems through feedback processes. Observations from key tower sites standing out due to their long-term comprehensive observations: The Amazon Tall Tower Observatory in Central Amazonia, the Zotino Tall Tower Observatory in Siberia, and the Station to Measure Ecosystem-Atmosphere Relations at Hyytiäla in Finland. The review is complemented by short-term observations from networks and large experiments.The review discusses atmospheric chemistry observations, aerosol formation and processing, physiochemical aerosol, and cloud condensation nuclei properties and finds surprising similarities and important differences in the two ecosystems. The aerosol concentrations and chemistry are similar, particularly concerning the main chemical components, both dominated by an organic fraction, while the boreal ecosystem has generally higher concentrations of inorganics, due to higher influence of long-range transported air pollution. The emissions of biogenic volatile organic compounds are dominated by isoprene and monoterpene in the tropical and boreal regions, respectively, being the main precursors of the organic aerosol fraction.Observations and modeling studies show that climate change and deforestation affect the ecosystems such that the carbon and hydrological cycles in Amazonia are changing to carbon neutrality and affect precipitation downwind. In Africa, the tropical forests are so far maintaining their carbon sink.It is urgent to better understand the interaction between these major ecosystems, the atmosphere, and climate, which calls for more observation sites, providing long-term data on water, carbon, and other biogeochemical cycles. This is essential in finding a sustainable balance between forest preservation and reforestation versus a potential increase in food production and biofuels, which are critical in maintaining ecosystem services and global climate stability. Reducing global warming and deforestation is vital for tropical forests.
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6.
  • Beck, Lisa J., et al. (författare)
  • Differing Mechanisms of New Particle Formation at Two Arctic Sites
  • 2021
  • Ingår i: Geophysical Research Letters. - 0094-8276 .- 1944-8007. ; 48:4
  • Tidskriftsartikel (refereegranskat)abstract
    • New particle formation in the Arctic atmosphere is an important source of aerosol particles. Understanding the processes of Arctic secondary aerosol formation is crucial due to their significant impact on cloud properties and therefore Arctic amplification. We observed the molecular formation of new particles from low-volatility vapors at two Arctic sites with differing surroundings. In Svalbard, sulfuric acid (SA) and methane sulfonic acid (MSA) contribute to the formation of secondary aerosol and to some extent to cloud condensation nuclei (CCN). This occurs via ion-induced nucleation of SA and NH3 and subsequent growth by mainly SA and MSA condensation during springtime and highly oxygenated organic molecules during summertime. By contrast, in an ice-covered region around Villum, we observed new particle formation driven by iodic acid but its concentration was insufficient to grow nucleated particles to CCN sizes. Our results provide new insight about sources and precursors of Arctic secondary aerosol particles.
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7.
  • Bianchi, Federico, et al. (författare)
  • Highly Oxygenated Organic Molecules (HOM) from Gas-Phase Autoxidation Involving Peroxy Radicals : A Key Contributor to Atmospheric Aerosol
  • 2019
  • Ingår i: Chemical Reviews. - : American Chemical Society (ACS). - 0009-2665 .- 1520-6890. ; 119:6, s. 3472-3509
  • Forskningsöversikt (refereegranskat)abstract
    • Highly oxygenated organic molecules (HOM) are formed in the atmosphere via autoxidation involving peroxy radicals arising from volatile organic compounds (VOC). HOM condense on pre-existing particles and can be involved in new particle formation. HOM thus contribute to the formation of secondary organic aerosol (SOA), a significant and ubiquitous component of atmospheric aerosol known to affect the Earths radiation balance. HOM were discovered only very recently, but the interest in these compounds has grown rapidly. In this Review, we define HOM and describe the currently available techniques for their identification/quantification, followed by a summary of the current knowledge on their formation mechanisms and physicochemical properties. A main aim is to provide a common frame for the currently quite fragmented literature on HOM studies. Finally, we highlight the existing gaps in our understanding and suggest directions for future HOM research.
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8.
  • Blichner, Sara M., 1989-, et al. (författare)
  • Process-evaluation of forest aerosol-cloud-climate feedback shows clear evidence from observations and large uncertainty in models
  • 2024
  • Ingår i: Nature Communications. - 2041-1723. ; 15
  • Tidskriftsartikel (refereegranskat)abstract
    • Natural aerosol feedbacks are expected to become more important in the future, as anthropogenic aerosol emissions decrease due to air quality policy. One such feedback is initiated by the increase in biogenic volatile organic compound (BVOC) emissions with higher temperatures, leading to higher secondary organic aerosol (SOA) production and a cooling of the surface via impacts on cloud radiative properties. Motivated by the considerable spread in feedback strength in Earth System Models (ESMs), we here use two long-term observational datasets from boreal and tropical forests, together with satellite data, for a process-based evaluation of the BVOC-aerosol-cloud feedback in four ESMs. The model evaluation shows that the weakest modelled feedback estimates can likely be excluded, but highlights compensating errors making it difficult to draw conclusions of the strongest estimates. Overall, the method of evaluating along process chains shows promise in pin-pointing sources of uncertainty and constraining modelled aerosol feedbacks.
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9.
  • Boy, Michael, et al. (författare)
  • Positive feedback mechanism between biogenic volatile organic compounds and the methane lifetime in future climates
  • 2022
  • Ingår i: npj Climate and Atmospheric Science. - : Springer Science and Business Media LLC. - 2397-3722. ; 5:1
  • Tidskriftsartikel (refereegranskat)abstract
    • A multitude of biogeochemical feedback mechanisms govern the climate sensitivity of Earth in response to radiation balance perturbations. One feedback mechanism, which remained missing from most current Earth System Models applied to predict future climate change in IPCC AR6, is the impact of higher temperatures on the emissions of biogenic volatile organic compounds (BVOCs), and their subsequent effects on the hydroxyl radical (OH) concentrations. OH, in turn, is the main sink term for many gaseous compounds including methane, which is the second most important human-influenced greenhouse gas in terms of climate forcing. In this study, we investigate the impact of this feedback mechanism by applying two models, a one-dimensional chemistry-transport model, and a global chemistry-transport model. The results indicate that in a 6 K temperature increase scenario, the BVOC-OH-CH4 feedback increases the lifetime of methane by 11.4% locally over the boreal region when the temperature rise only affects chemical reaction rates, and not both, chemistry and BVOC emissions. This would lead to a local increase in radiative forcing through methane (ΔRFCH4) of approximately 0.013 Wm−2 per year, which is 2.1% of the current ΔRFCH4. In the whole Northern hemisphere, we predict an increase in the concentration of methane by 0.024% per year comparing simulations with temperature increase only in the chemistry or temperature increase in chemistry and BVOC emissions. This equals approximately 7% of the annual growth rate of methane during the years 2008–2017 (6.6 ± 0.3 ppb yr−1) and leads to an ΔRFCH4 of 1.9 mWm−2 per year.
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10.
  • Boyer, Matthew, et al. (författare)
  • A full year of aerosol size distribution data from the central Arctic under an extreme positive Arctic Oscillation : insights from the Multidisciplinarydrifting Observatory for the Study of Arctic Climate (MOSAiC) expedition
  • 2023
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 23:1, s. 389-415
  • Tidskriftsartikel (refereegranskat)abstract
    • The Arctic environment is rapidly changing due to accelerated warming in the region. The warming trend is driving a decline in sea ice extent, which thereby enhances feedback loops in the surface energy budget in the Arctic. Arctic aerosols play an important role in the radiative balance and hence the climate response in the region, yet direct observations of aerosols over the Arctic Ocean are limited. In this study, we investigate the annual cycle in the aerosol particle number size distribution (PNSD), particle number concentration (PNC), and black carbon (BC) mass concentration in the central Arctic during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition. This is the first continuous, year-long data set of aerosol PNSD ever collected over the sea ice in the central Arctic Ocean. We use a k-means cluster analysis, FLEXPART simulations, and inverse modeling to evaluate seasonal patterns and the influence of different source regions on the Arctic aerosol population. Furthermore, we compare the aerosol observations to land-based sites across the Arctic, using both long-term measurements and observations during the year of the MOSAiC expedition (2019–2020), to investigate interannual variability and to give context to the aerosol characteristics from within the central Arctic. Our analysis identifies that, overall, the central Arctic exhibits typical seasonal patterns of aerosols, including anthropogenic influence from Arctic haze in winter and secondary aerosol processes in summer. The seasonal pattern corresponds to the global radiation, surface air temperature, and timing of sea ice melting/freezing, which drive changes in transport patterns and secondary aerosol processes. In winter, the Norilsk region in Russia/Siberia was the dominant source of Arctic haze signals in the PNSD and BC observations, which contributed to higher accumulation-mode PNC and BC mass concentrations in the central Arctic than at land-based observatories. We also show that the wintertime Arctic Oscillation (AO) phenomenon, which was reported to achieve a record-breaking positive phase during January–March 2020, explains the unusual timing and magnitude of Arctic haze across the Arctic region compared to longer-term observations. In summer, the aerosol PNCs of the nucleation and Aitken modes are enhanced; however, concentrations were notably lower in the central Arctic over the ice pack than at land-based sites further south. The analysis presented herein provides a current snapshot of Arctic aerosol processes in an environment that is characterized by rapid changes, which will be crucial for improving climate model predictions, understanding linkages between different environmental processes, and investigating the impacts of climate change in future Arctic aerosol studies.
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