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1.
  • Roldin, Pontus, et al. (författare)
  • The role of highly oxygenated organic molecules in the Boreal aerosol-cloud-climate system
  • 2019
  • Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 10, s. 1-15
  • Tidskriftsartikel (refereegranskat)abstract
    • Over Boreal regions, monoterpenes emitted from the forest are the main precursors for secondary organic aerosol (SOA) formation and the primary driver of the growth of new aerosol particles to climatically important cloud condensation nuclei (CCN). Autoxidation of monoterpenes leads to rapid formation of Highly Oxygenated organic Molecules (HOM). We have developed the first model with near-explicit representation of atmospheric new particle formation (NPF) and HOM formation. The model can reproduce the observed NPF, HOM gas-phase composition and SOA formation over the Boreal forest. During the spring, HOM SOA formation increases the CCN concentration by ~10 % and causes a direct aerosol radiative forcing of −0.10 W/m2. In contrast, NPF reduces the number of CCN at updraft velocities < 0.2 m/s, and causes a direct aerosol radiative forcing of +0.15 W/m2. Hence, while HOM SOA contributes to climate cooling, NPF can result in climate warming over the Boreal forest.
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2.
  • Mohr, Claudia, et al. (författare)
  • Molecular identification of organic vapors driving atmospheric nanoparticle growth
  • 2019
  • Ingår i: Nature communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 10
  • Tidskriftsartikel (refereegranskat)abstract
    • Particles formed in the atmosphere via nucleation provide about half the number of atmospheric cloud condensation nuclei, but in many locations, this process is limited by the growth of the newly formed particles. That growth is often via condensation of organic vapors. Identification of these vapors and their sources is thus fundamental for simulating changes to aerosol-cloud interactions, which are one of the most uncertain aspects of anthropogenic climate forcing. Here we present direct molecular-level observations of a distribution of organic vapors in a forested environment that can explain simultaneously observed atmospheric nanoparticle growth from 3 to 50 nm. Furthermore, the volatility distribution of these vapors is sufficient to explain nanoparticle growth without invoking particle-phase processes. The agreement between observed mass growth, and the growth predicted from the observed mass of condensing vapors in a forested environment thus represents an important step forward in the characterization of atmospheric particle growth.
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3.
  • 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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4.
  • Kourtchev, Ivan, et al. (författare)
  • Enhanced Volatile Organic Compounds emissions and organic aerosol mass increase the oligomer content of atmospheric aerosols
  • 2016
  • Ingår i: Scientific Reports. - : Springer Science and Business Media LLC. - 2045-2322. ; 6
  • Tidskriftsartikel (refereegranskat)abstract
    • Secondary organic aerosol (SOA) accounts for a dominant fraction of the submicron atmospheric particle mass, but knowledge of the formation, composition and climate effects of SOA is incomplete and limits our understanding of overall aerosol effects in the atmosphere. Organic oligomers were discovered as dominant components in SOA over a decade ago in laboratory experiments and have since been proposed to play a dominant role in many aerosol processes. However, it remains unclear whether oligomers are relevant under ambient atmospheric conditions because they are often not clearly observed in field samples. Here we resolve this long-standing discrepancy by showing that elevated SOA mass is one of the key drivers of oligomer formation in the ambient atmosphere and laboratory experiments. We show for the first time that a specific organic compound class in aerosols, oligomers, is strongly correlated with cloud condensation nuclei (CCN) activities of SOA particles. These findings might have important implications for future climate scenarios where increased temperatures cause higher biogenic volatile organic compound (VOC) emissions, which in turn lead to higher SOA mass formation and significant changes in SOA composition. Such processes would need to be considered in climate models for a realistic representation of future aerosol-climate-biosphere feedbacks.
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5.
  • Zhou, Putian, et al. (författare)
  • Simulating dust emissions and secondary organic aerosol formation over northern Africa during the mid-Holocene Green Sahara period
  • 2023
  • Ingår i: Climate of the Past. - 1814-9324 .- 1814-9332. ; 19:12, s. 2445-2462
  • Tidskriftsartikel (refereegranskat)abstract
    • Paleo-proxy data indicate that a “Green Sahara” thrived in northern Africa during the early- to mid-Holocene (MH; 11 000 to 5000 years before present), characterized by more vegetation cover and reduced dust emissions. Utilizing a state-of-the-art atmospheric chemical transport model, TM5-MP, we assessed the changes in biogenic volatile organic compound (BVOC) emissions, dust emissions and secondary organic aerosol (SOA) concentrations in northern Africa during this period relative to the pre-industrial (PI) period. Our simulations show that dust emissions reduced from 280.6 Tg a−1 in the PI to 26.8 Tg a−1 in the MH, agreeing with indications from eight marine sediment records in the Atlantic Ocean. The northward expansion in northern Africa resulted in an increase in annual emissions of isoprene and monoterpenes during the MH, around 4.3 and 3.5 times higher than that in the PI period, respectively, causing a 1.9-times increase in the SOA surface concentration. Concurrently, enhanced BVOC emissions consumed more hydroxyl radical (OH), resulting in less sulfate formation. This effect counteracted the enhanced SOA surface concentration, altogether leading to a 17 % increase in the cloud condensation nuclei at 0.2 % super saturation over northern Africa. Our simulations provide consistent emission datasets of BVOCs, dust and the SOA formation aligned with the northward shift of vegetation during the “Green Sahara” period, which could serve as a benchmark for MH aerosol input in future Earth system model simulation experiments.
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6.
  • 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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7.
  • Foreback, Benjamin, et al. (författare)
  • A new implementation of FLEXPART with Enviro-HIRLAM meteorological input, and a case study during a heavy air pollution event
  • 2024
  • Ingår i: big earth data. - 2096-4471.
  • Tidskriftsartikel (refereegranskat)abstract
    • We integrated Enviro-HIRLAM (Environment-High Resolution Limited Area Model) meteorological output into FLEXPART (FLEXible PARTicle dispersion model). A FLEXPART simulation requires meteorological input from a numerical weather prediction (NWP) model. The publicly available version of FLEXPART can utilize either ECMWF (European Centre for Medium-range Weather Forecasts) Integrated Forecast System (IFS) forecast or reanalysis NWP data, or NCEP (U.S. National Center for Environmental Prediction) Global Forecast System (GFS) forecast or reanalysis NWP data. The primary benefits of using Enviro-HIRLAM are that it runs at a higher resolution and accounts for aerosol effects in meteorological fields. We compared backward trajectories generated with FLEXPART using Enviro-HIRLAM (both with and without aerosol effects) to trajectories generated using NCEP GFS and ECMWF IFS meteorological inputs, for a case study of a heavy haze event which occurred in Beijing, China in November 2018. We found that results from FLEXPART were considerably different when using different meteorological inputs. When aerosol effects were included in the NWP, there was a small but noticeable difference in calculated trajectories. Moreover, when looking at potential emission sensitivity instead of simply expressing trajectories as lines, additional information, which may have been missed when looking only at trajectories as lines, can be inferred.
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8.
  • Leinonen, Ville, et al. (författare)
  • Comparison of particle number size distribution trends in ground measurements and climate models
  • 2022
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 22:19, s. 12873-12905
  • Tidskriftsartikel (refereegranskat)abstract
    • Despite a large number of studies, out of all drivers of radiative forcing, the effect of aerosols has the largest uncertainty in global climate model radiative forcing estimates. There have been studies of aerosol optical properties in climate models, but the effects of particle number size distribution need a more thorough inspection. We investigated the trends and seasonality of particle number concentrations in nucleation, Aitken, and accumulation modes at 21 measurement sites in Europe and the Arctic. For 13 of those sites, with longer measurement time series, we compared the field observations with the results from five climate models, namely EC-Earth3, ECHAM-M7, ECHAM-SALSA, NorESM1.2, and UKESM1. This is the first extensive comparison of detailed aerosol size distribution trends between in situ observations from Europe and five earth system models (ESMs). We found that the trends of particle number concentrations were mostly consistent and decreasing in both measurements and models. However, for many sites, climate models showed weaker decreasing trends than the measurements. Seasonal variability in measured number concentrations, quantified by the ratio between maximum and minimum monthly number concentration, was typically stronger at northern measurement sites compared to other locations. Models had large differences in their seasonal representation, and they can be roughly divided into two categories: for EC-Earth and NorESM, the seasonal cycle was relatively similar for all sites, and for other models the pattern of seasonality varied between northern and southern sites. In addition, the variability in concentrations across sites varied between models, some having relatively similar concentrations for all sites, whereas others showed clear differences in concentrations between remote and urban sites. To conclude, although all of the model simulations had identical input data to describe anthropogenic mass emissions, trends in differently sized particles vary among the models due to assumptions in emission sizes and differences in how models treat size-dependent aerosol processes. The inter-model variability was largest in the accumulation mode, i.e. sizes which have implications for aerosol–cloud interactions. Our analysis also indicates that between models there is a large variation in efficiency of long-range transportation of aerosols to remote locations. The differences in model results are most likely due to the more complex effect of different processes instead of one specific feature (e.g. the representation of aerosol or emission size distributions). Hence, a more detailed characterization of microphysical processes and deposition processes affecting the long-range transport is needed to understand the model variability.
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9.
  • Nieminen, Tuomo, et al. (författare)
  • Global analysis of continental boundary layer new particle formation based on long-term measurements
  • 2018
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 18:19, s. 14737-14756
  • Tidskriftsartikel (refereegranskat)abstract
    • Atmospheric new particle formation (NPF) is an important phenomenon in terms of global particle number concentrations. Here we investigated the frequency of NPF, formation rates of 10 nm particles, and growth rates in the size range of 10-25 nm using at least 1 year of aerosol number size-distribution observations at 36 different locations around the world. The majority of these measurement sites are in the Northern Hemisphere. We found that the NPF frequency has a strong seasonal variability. At the measurement sites analyzed in this study, NPF occurs most frequently in March-May (on about 30 % of the days) and least frequently in December-February (about 10 % of the days). The median formation rate of 10 nm particles varies by about 3 orders of magnitude (0.01-10 cm(-3) s(-1)) and the growth rate by about an order of magnitude (1-10 nm h(-1)). The smallest values of both formation and growth rates were observed at polar sites and the largest ones in urban environments or anthropogenically influenced rural sites. The correlation between the NPF event frequency and the particle formation and growth rate was at best moderate among the different measurement sites, as well as among the sites belonging to a certain environmental regime. For a better understanding of atmospheric NPF and its regional importance, we would need more observational data from different urban areas in practically all parts of the world, from additional remote and rural locations in North America, Asia, and most of the Southern Hemisphere (especially Australia), from polar areas, and from at least a few locations over the oceans.
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10.
  • Pandolfi, Marco, et al. (författare)
  • A European aerosol phenomenology-6 : scattering properties of atmospheric aerosol particles from 28 ACTRIS sites
  • 2018
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 18:11, s. 7877-7911
  • Tidskriftsartikel (refereegranskat)abstract
    • This paper presents the light-scattering properties of atmospheric aerosol particles measured over the past decade at 28 ACTRIS observatories, which are located mainly in Europe. The data include particle light scattering (sigma(sp)) and hemispheric backscattering (sigma(bsp)) coefficients, scattering Angstrom exponent (SAE), backscatter fraction (BF) and asymmetry parameter (g). An increasing gradient of sigma(sp) is observed when moving from remote environments (arctic/mountain) to regional and to urban environments. At a regional level in Europe, sigma(sp) also increases when moving from Nordic and Baltic countries and from western Europe to central/eastern Europe, whereas no clear spatial gradient is observed for other station environments. The SAE does not show a clear gradient as a function of the placement of the station. However, a west-to-east-increasing gradient is observed for both regional and mountain placements, suggesting a lower fraction of fine-mode particle in western/south-western Europe compared to central and eastern Europe, where the fine-mode particles dominate the scattering. The g does not show any clear gradient by station placement or geographical location reflecting the complex relationship of this parameter with the physical properties of the aerosol particles. Both the station placement and the geographical location are important factors affecting the intraannual variability. At mountain sites, higher sigma(sp) and SAE values are measured in the summer due to the enhanced boundary layer influence and/or new particle-formation episodes. Conversely, the lower horizontal and vertical dispersion during winter leads to higher sigma(sp) values at all low-altitude sites in central and eastern Europe compared to summer. These sites also show SAE maxima in the summer (with corresponding g minima). At all sites, both SAE and g show a strong variation with aerosol particle loading. The lowest values of g are always observed together with low sigma(sp) values, indicating a larger contribution from particles in the smaller accumulation mode. During periods of high sigma(sp) values, the variation of g is less pronounced, whereas the SAE increases or decreases, suggesting changes mostly in the coarse aerosol particle mode rather than in the fine mode. Statistically significant decreasing trends of sigma(sp) are observed at 5 out of the 13 stations included in the trend analyses. The total reductions of sigma(sp) are consistent with those reported for PM2.5 and PM10 mass concentrations over similar periods across Europe.
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