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  • 1
    In: Environmental Science: Atmospheres, Royal Society of Chemistry (RSC), Vol. 1, No. 6 ( 2021), p. 449-472
    Abstract: Major atmospheric oxidants (OH, O 3 and NO 3 ) dominate the atmospheric oxidation capacity, while H 2 SO 4 is considered as a main driver for new particle formation. Although numerous studies have investigated the long-term trend of ozone in Europe, the trends of OH, NO 3 and H 2 SO 4 at specific sites are to a large extent unknown. The one-dimensional model SOSAA has been applied in several studies at the SMEAR II station and has been validated by measurements in several projects. Here, we applied the SOSAA model for the years 2007–2018 to simulate the atmospheric chemical components, especially the atmospheric oxidants OH and NO 3 , as well as H 2 SO 4 at SMEAR II. The simulations were evaluated with observations from several shorter and longer campaigns at SMEAR II. Our results show that daily OH increased by 2.39% per year and NO 3 decreased by 3.41% per year, with different trends of these oxidants during day and night. On the contrary, daytime sulfuric acid concentrations decreased by 2.78% per year, which correlated with the observed decreasing concentration of newly formed particles in the size range of 3–25 nm with 1.4% per year at SMEAR II during the years 1997–2012. Additionally, we compared our simulated OH, NO 3 and H 2 SO 4 concentrations with proxies, which are commonly applied in case a limited number of parameters are measured and no detailed model simulations are available.
    Type of Medium: Online Resource
    ISSN: 2634-3606
    Language: English
    Publisher: Royal Society of Chemistry (RSC)
    Publication Date: 2021
    detail.hit.zdb_id: 3057711-1
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  • 2
    In: Frontiers in Forests and Global Change, Frontiers Media SA, Vol. 3 ( 2020-10-6)
    Type of Medium: Online Resource
    ISSN: 2624-893X
    Language: Unknown
    Publisher: Frontiers Media SA
    Publication Date: 2020
    detail.hit.zdb_id: 2968523-0
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  • 3
    Online Resource
    Online Resource
    Copernicus GmbH ; 2021
    In:  Atmospheric Chemistry and Physics Vol. 21, No. 23 ( 2021-12-01), p. 17389-17431
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 21, No. 23 ( 2021-12-01), p. 17389-17431
    Abstract: Abstract. Most trees emit volatile organic compounds (VOCs) continuously throughout their life, but the rate of emission and spectrum of emitted VOCs become substantially altered when the trees experience stress. Despite this, models to predict the emissions of VOCs do not account for perturbations caused by biotic plant stress. Considering that such stresses have generally been forecast to increase in both frequency and severity in the future climate, the neglect of stress-induced plant emissions in models might be one of the key obstacles for realistic climate change predictions, since changes in VOC concentrations are known to greatly influence atmospheric aerosol processes. Thus, we constructed a model to study the impact of biotic plant stresses on new particle formation and growth throughout a full growing season. We simulated the influence on aerosol processes caused by herbivory by the European gypsy moth (Lymantria dispar) and autumnal moth (Epirrita autumnata) feeding on pedunculate oak (Quercus robur) and mountain birch (Betula pubescens var. pumila), respectively, and also fungal infections of pedunculate oak and balsam poplar (Populus balsamifera var. suaveolens) by oak powdery mildew (Erysiphe alphitoides) and poplar rust (Melampsora larici-populina), respectively. Our modelling results indicate that all the investigated plant stresses are capable of substantially perturbing both the number and size of aerosol particles in atmospherically relevant conditions, with increases in the amount of newly formed particles by up to about an order of magnitude and additional daily growth of up to almost 50 nm. We also showed that it can be more important to account for biotic plant stresses in models for local and regional predictions of new particle formation and growth during the time of infestation or infection than significant variations in, e.g. leaf area index and temperature and light conditions, which are currently the main parameters controlling predictions of VOC emissions. Our study thus demonstrates that biotic plant stress can be highly atmospherically relevant. To validate our findings, field measurements are urgently needed to quantify the role of stress emissions in atmospheric aerosol processes and for making integration of biotic plant stress emission responses into numerical models for prediction of atmospheric chemistry and physics, including climate change projection models, possible.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 4
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 16, No. 11 ( 2016-06-10), p. 7171-7194
    Abstract: Abstract. Recently, the number and amount of biogenically emitted volatile organic compounds (VOCs) has been discussed in great detail. Depending on the ecosystem, the published number varies between a dozen and several hundred compounds. We present ecosystem exchange fluxes from a mixed oak–hornbeam forest in the Po Valley, Italy. The fluxes were measured by a proton transfer reaction-time-of-flight (PTR-ToF) mass spectrometer and calculated using the eddy covariance (EC) method. Detectable fluxes were observed for up to 29 compounds, dominated by isoprene, which comprised over 60 % of the total upward flux (on a molar basis). The daily average of the total VOC upward flux was 10.4 nmol m−2 s−1. Methanol had the highest concentration and accounted for the largest downward flux. Methanol seemed to be deposited to dew, as the downward flux happened in the early morning, right after the calculated surface temperature came closest to the calculated dew point temperature.We estimated that up to 30 % of the upward flux of methyl vinyl ketone (MVK) and methacrolein (MACR) originated from atmospheric oxidation of isoprene. A comparison between two methods for the flux detection (manual and automated) was made. Their respective advantages and disadvantages were discussed and the differences in their results shown. Both provide comparable results.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2016
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 5
    Online Resource
    Online Resource
    Copernicus GmbH ; 2017
    In:  Atmospheric Chemistry and Physics Vol. 17, No. 23 ( 2017-12-04), p. 14309-14332
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 17, No. 23 ( 2017-12-04), p. 14309-14332
    Abstract: Abstract. A multilayer gas dry deposition model has been developed and implemented into a one-dimensional chemical transport model SOSAA (model to Simulate the concentrations of Organic vapours, Sulphuric Acid and Aerosols) to calculate the dry deposition velocities for all the gas species included in the chemistry scheme. The new model was used to analyse in-canopy sources and sinks, including gas emissions, chemical production and loss, dry deposition, and turbulent transport of 12 featured biogenic volatile organic compounds (BVOCs) or groups of BVOCs (e.g. monoterpenes, isoprene+2-methyl-3-buten-2-ol (MBO), sesquiterpenes, and oxidation products of mono- and sesquiterpenes) in July 2010 at the boreal forest site SMEAR II (Station for Measuring Ecosystem–Atmosphere Relations). According to the significance of modelled monthly-averaged individual source and sink terms inside the canopy, the selected BVOCs were classified into five categories: 1. Most of emitted gases are transported out of the canopy (monoterpenes, isoprene + MBO). 2. Chemical reactions remove a significant portion of emitted gases (sesquiterpenes). 3. Bidirectional fluxes occur since both emission and dry deposition are crucial for the in-canopy concentration tendency (acetaldehyde, methanol, acetone, formaldehyde). 4. Gases removed by deposition inside the canopy are compensated for by the gases transported from above the canopy (acetol, pinic acid, β-caryophyllene's oxidation product BCSOZOH). 5. The chemical production is comparable to the sink by deposition (isoprene's oxidation products ISOP34OOH and ISOP34NO3). Most of the simulated sources and sinks were located above about 0.2 hc (canopy height) for oxidation products and above about 0.4 hc for emitted species except formaldehyde. In addition, soil deposition (including deposition onto understorey vegetation) contributed 11–61 % to the overall in-canopy deposition. The emission sources peaked at about 0.8–0.9 hc, which was higher than 0.6 hc where the maximum of dry deposition onto overstorey vegetation was located. This study provided a method to enable the quantification of the exchange between atmosphere and biosphere for numerous BVOCs, which could be applied in large-scale models in future. With this more explicit canopy exchange modelling system, this study analysed both the temporal and spatial variations in individual in-canopy sources and sinks, as well as their combined effects on driving BVOC exchange. In this study 12 featured BVOCs or BVOC groups were analysed. Other compounds could also be investigated similarly by being classified into these five categories.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2017
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 6
    Online Resource
    Online Resource
    Copernicus GmbH ; 2019
    In:  Atmospheric Chemistry and Physics Vol. 19, No. 23 ( 2019-11-29), p. 14431-14453
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 19, No. 23 ( 2019-11-29), p. 14431-14453
    Abstract: Abstract. Total hydroxyl radical (OH) reactivity measurements were conducted at the second Station for Measuring Ecosystem–Atmosphere Relations (SMEAR II), a boreal forest site located in Hyytiälä, Finland, from April to July 2016. The measured values were compared with OH reactivity calculated from a combination of data from the routine trace gas measurements (station mast) as well as online and offline analysis with a gas chromatographer coupled to a mass spectrometer (GC–MS) and offline liquid chromatography. Up to 104 compounds, mostly volatile organic compounds (VOCs) and oxidized VOCs, but also inorganic compounds, were included in the analysis, even though the data availability for each compound varied with time. The monthly averaged experimental total OH reactivity was found to be higher in April and May (ca. 20 s−1) than in June and July (7.6 and 15.4 s−1, respectively). The measured values varied much more in spring with high reactivity peaks in late afternoon, with values higher than in the summer, in particular when the soil was thawing. Total OH reactivity values generally followed the pattern of mixing ratios due to change of the boundary layer height. The missing reactivity fraction (defined as the difference between measured and calculated OH reactivity) was found to be high. Several reasons that can explain the missing reactivity are discussed in detail such as (1) missing measurements due to technical issues, (2) not measuring oxidation compounds of detected biogenic VOCs, and (3) missing important reactive compounds or classes of compounds with the available measurements. In order to test the second hypothesis, a one-dimensional chemical transport model (SOSAA) has been used to estimate the amount of unmeasured oxidation products and their expected contribution to the reactivity for three different short periods in April, May, and July. However, only a small fraction (〈4.5 %) of the missing reactivity can be explained by modelled secondary compounds (mostly oxidized VOCs). These findings indicate that compounds measured but not included in the model as well as unmeasured primary emissions contribute the missing reactivity. In the future, non-hydrocarbon compounds from sources other than vegetation (e.g. soil) should be included in OH reactivity studies.
    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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  • 7
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 13, No. 10 ( 2020-10-22), p. 5595-5619
    Abstract: Abstract. We developed a simple algorithm to classify clouds based on global radiation and cloud base height measured by pyranometer and ceilometer, respectively. We separated clouds into seven different classes (stratus, stratocumulus, cumulus, nimbostratus, altocumulus + altostratus, cirrus + cirrocumulus + cirrostratus and clear sky + cirrus). We also included classes for cumulus and cirrus clouds causing global radiation enhancement, and we classified multilayered clouds, when captured by the ceilometer, based on their height and characteristics (transmittance, patchiness and uniformity). The overall performance of the algorithm was nearly 70 % when compared with classification by an observer using total-sky images. The performance was best for clouds having well-distinguishable effects on solar radiation: nimbostratus clouds were classified correctly in 100 % of the cases. The worst performance corresponds to cirriform clouds (50 %). Although the overall performance of the algorithm was good, it is likely to miss the occurrences of high and multilayered clouds. This is due to the technical limits of the instrumentation: the vertical detection range of the ceilometer and occultation of the laser pulse by the lowest cloud layer. We examined the use of clearness index, which is defined as a ratio between measured global radiation and modeled radiation at the top of the atmosphere, as an indicator of clear-sky conditions. Our results show that cumulus, altocumulus, altostratus and cirriform clouds can be present when the index indicates clear-sky conditions. Those conditions have previously been associated with enhanced aerosol formation under clear skies. This is an important finding especially in the case of low clouds coupled to the surface, which can influence aerosol population via aerosol–cloud interactions. Overall, caution is required when the clearness index is used in the analysis of processes affected by partitioning of radiation by clouds.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
    detail.hit.zdb_id: 2505596-3
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  • 8
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 21, No. 19 ( 2021-10-06), p. 14761-14787
    Abstract: Abstract. The East African lowland and highland areas consist of water-limited and humid ecosystems. The magnitude and seasonality of biogenic volatile organic compounds (BVOCs) emissions and concentrations from these functionally contrasting ecosystems are limited due to a scarcity of direct observations. We measured mixing ratios of BVOCs from two contrasting ecosystems, humid highlands with agroforestry and dry lowlands with bushland, grassland, and agriculture mosaics, during both the rainy and dry seasons of 2019 in southern Kenya. We present the diurnal and seasonal characteristics of BVOC mixing ratios and their reactivity and estimated emission factors (EFs) for certain BVOCs from the African lowland ecosystem based on field measurements. The most abundant BVOCs were isoprene and monoterpenoids (MTs), with isoprene contributing 〉 70 % of the total BVOC mixing ratio during daytime, while MTs accounted for 〉 50 % of the total BVOC mixing ratio during nighttime at both sites. The contributions of BVOCs to the local atmospheric chemistry were estimated by calculating the reactivity towards the hydroxyl radical (OH), ozone (O3), and the nitrate radical (NO3). Isoprene and MTs contributed the most to the reactivity of OH and NO3, while sesquiterpenes dominated the contribution of organic compounds to the reactivity of O3. The mixing ratio of isoprene measured in this study was lower than that measured in the relevant ecosystems in western and southern Africa, while that of monoterpenoids was similar. Isoprene mixing ratios peaked daily between 16:00 and 20:00 (all times are given as East Africa Time, UTC+3),​​​​​​​ with a maximum mixing ratio of 809 pptv (parts per trillion by volume) and 156 pptv in the highlands and 115 and 25 pptv in the lowlands during the rainy and dry seasons, respectively. MT mixing ratios reached their daily maximum between midnight and early morning (usually 04:00 to 08:00), with mixing ratios of 254 and 56 pptv in the highlands and 89 and 7 pptv in the lowlands in the rainy and dry seasons, respectively. The dominant species within the MT group were limonene, α-pinene, and β-pinene. EFs for isoprene, MTs, and 2-Methyl-3-buten-2-ol (MBO) were estimated using an inverse modeling approach. The estimated EFs for isoprene and β-pinene agreed very well with what is currently assumed in the world's most extensively used biogenic emissions model, the Model of Emissions of Gases and Aerosols from Nature (MEGAN), for warm C4 grass, but the estimated EFs for MBO, α-pinene, and especially limonene were significantly higher than that assumed in MEGAN for the relevant plant functional type. Additionally, our results indicate that the EF for limonene might be seasonally dependent in savanna ecosystems.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 9
    In: Frontiers in Forests and Global Change, Frontiers Media SA, Vol. 6 ( 2023-3-23)
    Abstract: Published biogenic volatile organic compound (BVOC) emission rates of Norway spruces vary a lot. In this study we combined published Norway spruce emission rates measured in boreal forests and added our new, unpublished emission data from Southern (SF) and Northern Finland (NF). Standardized summer monthly mean emission potentials of isoprene vary from below the detection limit to 7 μg g –1 (dw) h –1 , and monoterpene (MT) and sesquiterpene (SQT) emission potentials 0.01–3 μg g –1 (dw) h –1 and 0.03–2.7 μg g –1 (dw) h –1 , respectively. In this study, we found much higher SQT emissions from Norway spruces than previously measured, and on average SQTs had higher emission potentials than isoprene or MTs. The highest monthly mean SQT emission potential of 13.6 μg g –1 (dw) h –1 was observed in September in Southern Finland. We found that none of the younger (33–40 years) trees in Hyytiälä, Southern Finland, emitted isoprene, while one 50-year-old tree was a strong isoprene emitter. The difference due to age could not be confirmed, since all measured small trees were growing in Hyytiälä, so this could also be due to the same genetic origin. On average, older trees ( & gt;80 years) emitted about ten times more isoprene and MTs than younger ones ( & lt;80 years), but no clear difference was seen in SQT emissions. SQT emissions can be more related to stress effects. As shown here for Norway spruce, it is possible that the emission factor of SQTs is significantly higher than what is currently used in models, which may have significant effects on the prediction of formation and growth of new particles, since the secondary organic aerosol (SOA) formation potential of SQTs is high, and this may have significant effects on the formation and growth of new particles. Due to the high secondary organic aerosol (SOA) formation potentials of SQTs, the impact on SOA formation and mass could be even higher.
    Type of Medium: Online Resource
    ISSN: 2624-893X
    Language: Unknown
    Publisher: Frontiers Media SA
    Publication Date: 2023
    detail.hit.zdb_id: 2968523-0
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  • 10
    In: Atmospheric Environment: X, Elsevier BV, Vol. 8 ( 2020-12), p. 100097-
    Type of Medium: Online Resource
    ISSN: 2590-1621
    Language: English
    Publisher: Elsevier BV
    Publication Date: 2020
    detail.hit.zdb_id: 2967860-2
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