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  • 1
    In: Nature Communications, Springer Science and Business Media LLC, Vol. 10, No. 1 ( 2019-09-25)
    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/m 2 . 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/m 2 . Hence, while HOM SOA contributes to climate cooling, NPF can result in climate warming over the Boreal forest.
    Type of Medium: Online Resource
    ISSN: 2041-1723
    Language: English
    Publisher: Springer Science and Business Media LLC
    Publication Date: 2019
    detail.hit.zdb_id: 2553671-0
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  • 2
    In: Environmental Science & Technology, American Chemical Society (ACS), Vol. 56, No. 19 ( 2022-10-04), p. 13931-13944
    Type of Medium: Online Resource
    ISSN: 0013-936X , 1520-5851
    RVK:
    Language: English
    Publisher: American Chemical Society (ACS)
    Publication Date: 2022
    detail.hit.zdb_id: 280653-8
    detail.hit.zdb_id: 1465132-4
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  • 3
    In: Reviews of Geophysics, American Geophysical Union (AGU), Vol. 55, No. 2 ( 2017-06), p. 509-559
    Abstract: We review some important developments in secondary organic aerosol (SOA) that could impact aerosol radiative forcing and response of climate to greenhouse gases We highlight some of the important processes that involve interactions between natural biogenic emissions and anthropogenic emissions We discuss fundamental SOA properties volatility and viscosity and their relation to evolution of aerosol mass and number concentrations in the atmosphere
    Type of Medium: Online Resource
    ISSN: 8755-1209 , 1944-9208
    URL: Issue
    Language: English
    Publisher: American Geophysical Union (AGU)
    Publication Date: 2017
    detail.hit.zdb_id: 2035391-1
    detail.hit.zdb_id: 209852-0
    detail.hit.zdb_id: 209853-2
    SSG: 16,13
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  • 4
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 22, No. 15 ( 2022-08-04), p. 10023-10043
    Abstract: Abstract. In this study, we modeled the aerosol particle formation along air mass trajectories arriving at the remote Arctic research stations Gruvebadet (67 m a.s.l.) and Zeppelin (474 m a.s.l.), Ny-Ålesund, during May 2018. The aim of this study was to improve our understanding of processes governing secondary aerosol formation in remote Arctic marine environments. We run the Lagrangian chemistry transport model ADCHEM, along air mass trajectories generated with FLEXPART v10.4. The air masses arriving at Ny-Ålesund spent most of their time over the open ice-free ocean. In order to capture the secondary aerosol formation from the DMS emitted by phytoplankton from the ocean surface, we implemented a recently developed comprehensive DMS and halogen multi-phase oxidation chemistry scheme, coupled with the widely used Master Chemical Mechanism (MCM). The modeled median particle number size distributions are in close agreement with the observations in the marine-influenced boundary layer near-sea-surface Gruvebadet site. However, while the model reproduces the accumulation mode particle number concentrations at Zeppelin, it overestimates the Aitken mode particle number concentrations by a factor of ∼5.5. We attribute this to the deficiency of the model to capture the complex orographic effects on the boundary layer dynamics at Ny-Ålesund. However, the model reproduces the average vertical particle number concentration profiles within the boundary layer (0–600 m a.s.l.) above Gruvebadet, as measured with condensation particle counters (CPCs) on board an unmanned aircraft system (UAS). The model successfully reproduces the observed Hoppel minima, often seen in particle number size distributions at Ny-Ålesund. The model also supports the previous experimental findings that ion-mediated H2SO4–NH3 nucleation can explain the observed new particle formation in the marine Arctic boundary layer in the vicinity of Ny-Ålesund. Precursors resulting from gas- and aqueous-phase DMS chemistry contribute to the subsequent growth of the secondary aerosols. The growth of particles is primarily driven via H2SO4 condensation and formation of methane sulfonic acid (MSA) through the aqueous-phase ozonolysis of methane sulfinic acid (MSIA) in cloud and deliquescent droplets.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2022
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 5
    In: Nature Communications, Springer Science and Business Media LLC, Vol. 14, No. 1 ( 2023-08-17)
    Abstract: The oxidation of aromatics contributes significantly to the formation of atmospheric aerosol. Using toluene as an example, we demonstrate the existence of a molecular rearrangement channel in the oxidation mechanism. Based on both flow reactor experiments and quantum chemical calculations, we show that the bicyclic peroxy radicals (BPRs) formed in OH-initiated aromatic oxidation are much less stable than previously thought, and in the case of the toluene derived ipso-BPRs, lead to aerosol-forming low-volatility products with up to 9 oxygen atoms on sub-second timescales. Similar results are predicted for ipso-BPRs formed from many other aromatic compounds. This reaction class is likely a key route for atmospheric aerosol formation, and including the molecular rearrangement of BPRs may be vital for accurate chemical modeling of the atmosphere.
    Type of Medium: Online Resource
    ISSN: 2041-1723
    Language: English
    Publisher: Springer Science and Business Media LLC
    Publication Date: 2023
    detail.hit.zdb_id: 2553671-0
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  • 6
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 16, No. 4 ( 2016-03-01), p. 2477-2492
    Abstract: Abstract. New particle formation (NPF) has been investigated intensively during the last 2 decades because of its influence on aerosol population and the possible contribution to cloud condensation nuclei. However, intensive measurements and modelling activities on this topic in urban metropolitan areas in China with frequent high-pollution episodes are still very limited. This study provides results from a comprehensive modelling study on the occurrence of NPF events in the western part of the Yangtze River Delta (YRD) region, China. The comprehensive modelling system, which combines the WRF-Chem (the Weather Research and Forecasting model coupled with Chemistry) regional chemical transport model and the MALTE-BOX sectional box model (the model to predict new aerosol formation in the lower troposphere), was shown to be capable of simulating atmospheric nucleation and subsequent growth. Here we present a detailed discussion of three typical NPF days, during which the measured air masses were notably influenced by either anthropogenic activities, biogenic emissions, or mixed ocean and continental sources. Overall, simulated NPF events were generally in good agreement with the corresponding measurements, enabling us to get further insights into NPF processes in the YRD region. Based on the simulations, we conclude that biogenic organic compounds, particularly monoterpenes, play an essential role in the initial condensational growth of newly formed clusters through their low-volatility oxidation products. Although some uncertainties remain in this modelling system, this method provides a possibility to better understand particle formation and growth processes.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2016
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  • 7
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 18, No. 14 ( 2018-07-19), p. 10255-10274
    Abstract: Abstract. The Amazon Basin is a unique region to study atmospheric aerosols, given their relevance for the regional hydrological cycle and the large uncertainty of their sources. Multi-year datasets are crucial when contrasting periods of natural conditions and periods influenced by anthropogenic emissions. In the wet season, biogenic sources and processes prevail, and the Amazonian atmospheric composition resembles preindustrial conditions. In the dry season, the basin is influenced by widespread biomass burning emissions. This work reports multi-year observations of high time resolution submicrometer (10–600 nm) particle number size distributions at a rain forest site in Amazonia (TT34 tower, 60 km NW from Manaus city), between 2008 and 2010 and 2012 and 2014. The median particle number concentration was 403 cm−3 in the wet season and 1254 cm−3 in the dry season. The Aitken mode (∼ 30–100 nm in diameter) was prominent during the wet season, while the accumulation mode (∼ 100–600 nm in diameter) dominated the particle size spectra during the dry season. Cluster analysis identified groups of aerosol number size distributions influenced by convective downdrafts, nucleation events and fresh biomass burning emissions. New particle formation and subsequent growth was rarely observed during the 749 days of observations, similar to previous observations in the Amazon Basin. A stationary 1-D column model (ADCHEM – Aerosol Dynamics, gas and particle phase CHEMistry and radiative transfer model) was used to assess the importance of the processes behind the observed diurnal particle size distribution trends. Three major particle source types are required in the model to reproduce the observations: (i) a surface source of particles in the evening, possibly related to primary biological emissions; (ii) entrainment of accumulation mode aerosols in the morning; and (iii) convective downdrafts transporting Aitken mode particles into the boundary layer mostly during the afternoon. The latter process has the largest influence on the modeled particle number size distributions. However, convective downdrafts are often associated with rain and, thus, act as both a source of Aitken mode particles and a sink of accumulation mode particles, causing a net reduction in the median total particle number concentrations in the surface layer. Our study shows that the combination of the three mentioned particle sources is essential to sustain particle number concentrations in Amazonia.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2018
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 8
    Online Resource
    Online Resource
    Copernicus GmbH ; 2019
    In:  Atmospheric Chemistry and Physics Vol. 19, No. 4 ( 2019-03-01), p. 2701-2712
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 19, No. 4 ( 2019-03-01), p. 2701-2712
    Abstract: Abstract. Atmospheric particulate water is ubiquitous, affecting particle transport and uptake of gases. Yet, research on the effect of water on secondary organic aerosol (SOA) mass yields is not consistent. In this study, the SOA mass yields of an α-pinene and m-xylene mixture, at a concentration of 60 µg m−3, were examined using an oxidation flow reactor operated at a relative humidity (RH) of 60 % and a residence time of 160 s. Wet or dried ammonium sulfate and ammonium nitrate seed particles were used. By varying the amount of seed particle surface area, the underestimation of SOA formation induced by the short residence time in flow reactors was confirmed. Starting at a SOA mass concentration of ∼5 µg m−3, the maximum yield increased by a factor of ∼2 with dry seed particles and on average a factor of 3.2 with wet seed particles. Hence, wet particles increased the SOA mass yield by ∼60 % compared to the dry experiment. Maximum yield in the reactor was achieved using a surface area concentration of ∼1600 µm2 cm−3. This corresponded to a condensational lifetime of 20 s for low-volatility organics. The O:C ratio of SOA on wet ammonium sulfate was significantly higher than when using ammonium nitrate or dry ammonium sulfate seed particles, probably due to differences in heterogeneous chemistry.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 9
    In: Geoscientific Model Development, Copernicus GmbH, Vol. 13, No. 11 ( 2020-11-18), p. 5663-5685
    Abstract: Abstract. High-resolution modelling is needed to understand urban air quality and pollutant dispersion in detail. Recently, the PALM model system 6.0, which is based on large-eddy simulation (LES), was extended with the detailed Sectional Aerosol module for Large Scale Applications (SALSA) v2.0 to enable studying the complex interactions between the turbulent flow field and aerosol dynamic processes. This study represents an extensive evaluation of the modelling system against the horizontal and vertical distributions of aerosol particles measured using a mobile laboratory and a drone in an urban neighbourhood in Helsinki, Finland. Specific emphasis is on the model sensitivity of aerosol particle concentrations, size distributions and chemical compositions to boundary conditions of meteorological variables and aerosol background concentrations. The meteorological boundary conditions are taken from both a numerical weather prediction model and observations, which occasionally differ strongly. Yet, the model shows good agreement with measurements (fractional bias 〈0.67, normalised mean squared error 〈6, fraction of the data within a factor of 2 〉0.3, normalised mean bias factor 〈0.25 and normalised mean absolute error factor 〈0.35) with respect to both horizontal and vertical distribution of aerosol particles, their size distribution and chemical composition. The horizontal distribution is most sensitive to the wind speed and atmospheric stratification, and vertical distribution to the wind direction. The aerosol number size distribution is mainly governed by the flow field along the main street with high traffic rates and in its surroundings by the background concentrations. The results emphasise the importance of correct meteorological and aerosol background boundary conditions, in addition to accurate emission estimates and detailed model physics, in quantitative high-resolution air pollution modelling and future urban LES studies.
    Type of Medium: Online Resource
    ISSN: 1991-9603
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
    detail.hit.zdb_id: 2456725-5
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  • 10
    In: Geoscientific Model Development, Copernicus GmbH, Vol. 12, No. 4 ( 2019-04-11), p. 1403-1422
    Abstract: Abstract. Urban pedestrian-level air quality is a result of an interplay between turbulent dispersion conditions, background concentrations, and heterogeneous local emissions of air pollutants and their transformation processes. Still, the complexity of these interactions cannot be resolved by the commonly used air quality models. By embedding the sectional aerosol module SALSA2.0 into the large-eddy simulation model PALM, a novel, high-resolution, urban aerosol modelling framework has been developed. The first model evaluation study on the vertical variation of aerosol number concentration and size distribution in a simple street canyon without vegetation in Cambridge, UK, shows good agreement with measurements, with simulated values mainly within a factor of 2 of observations. Dispersion conditions and local emissions govern the pedestrian-level aerosol number concentrations. Out of different aerosol processes, dry deposition is shown to decrease the total number concentration by over 20 %, while condensation and dissolutional increase the total mass by over 10 %. Following the model development, the application of PALM can be extended to local- and neighbourhood-scale air pollution and aerosol studies that require a detailed solution of the ambient flow field.
    Type of Medium: Online Resource
    ISSN: 1991-9603
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
    detail.hit.zdb_id: 2456725-5
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