Browsing by Subject "OZONE"

Sort by: Order: Results:

Now showing items 1-15 of 15
  • Lappalainen, Hanna K.; Sevanto, Sanna; Dal Maso, Miikka; Taipale, Risto; Kajos, Maija; Kolari, Pasi; Back, Jaana (2013)
  • Raivonen, Maarit; Joensuu, Johanna; Keronen, Petri; Altimir, Nuria; Kolari, Pasi (2014)
  • Berndt, Torsten; Herrmann, Hartmut; Kurten, Theo (2017)
    Criegee intermediates (CIs), mainly formed from gas-phase ozonolysis of alkenes, are considered as atmospheric oxidants besides OH and NO3 radicals as well as ozone. Direct CI measurement techniques are inevitably needed for reliable assessment of CIs' role in atmospheric processes. We found that CIs from ozonolysis reactions can be directly probed by means of chemical ionization mass spectrometry with a detection limit of about 10(4)-10(5) molecules cm(-3). Results from quantum chemical calculations support the experimental findings. The simplest CI, CH2OO, is detectable as an adduct with protonated ethers, preferably with protonated tetrahydrofuran. Kinetic measurements yielded k(CH2OO + SO2) = (3.3 +/- 0.9) X 10(-11) and k(CH2OO + acetic acid) = (1.25 +/- 0.30) x 10(-10) cm(3) molecule(-1) s(-1) at 295 +/- 2 K, in very good agreement with recent measurements using diiodomethane photolysis for CH2OO generation. CIs from the ozonolysis of cydohexene, acting as surrogate for cyclic terpenes, are followed as protonated species (CI)H+ using protonated amines as reagent ions. Kinetic investigations indicate a different reactivity of cydohexene-derived CIs compared with that of simple CIs, such as CH2OO. It is supposed that the aldehyde group significantly influences the CI reactivity of the cydohexene-derived CIs. The direct CI detection method presented here should allow study of the formation and reactivity of a wide range of different CIs formed from atmospheric ozonolysis reactions.
  • Johansson, Karin S. L.; El-Soda, Mohamed; Pagel, Ellen; Meyer, Rhonda C.; Toldsepp, Kadri; Nilsson, Anders K.; Brosche, Mikael; Kollist, Hannes; Uddling, Johan; Andersson, Mats X. (2020)
    Background and Aims The stomatal conductance (g(s)) of most plant species decreases in response to elevated atmospheric CO2 concentration. This response could have a significant impact on plant water use in a future climate. However, the regulation of the CO2 induced stomatal closure response is not fully understood. Moreover, the potential genetic links between short-term (within minutes to hours) and long-term (within weeks to months) responses of g(s) to increased atmospheric CO2 have not been explored. Methods We used Arabidopsis thaliana recombinant inbred lines originating from accessions Col-0 (strong CO2 response) and C24 (weak CO2 response) to study short- and long-term controls of g(s) Quantitative trait locus (QTL) mapping was used to identify loci controlling short- and long-term g(s) responses to elevated CO2 as well as other stomata-related traits. Key Results Short- and long-term stomatal responses to elevated CO2 were significantly correlated. Both short-and long-term responses were associated with a QTL, at the end of chromosome 2. The location of this QTL was confirmed using near-isogonic lines and it was fine-mapped to a 410-kb region. The QTL did not correspond to any known gene involved in stomatal closure and had no effect on the responsiveness to abscisic acid. Additionally, we identified numerous other loci associated with stomatal regulation. Conclusions We identified and confirmed the effect of a strong QTL corresponding to a yet unknown regulator of stomatal closure in response to elevated CO2 concentration. The correlation between short- and long-term stomatal CO2 responses and the genetic link between these traits highlight the importance of understanding guard cell CO2 signalling to predict and manipulate plant water use in a world with increasing atmospheric CO2 concentration. This study demonstrates the power of using natural variation to unravel the genetic regulation of complex traits.
  • Salminen-Paatero, Susanna; Thölix, Laura E; Kivi, Rigel; Paatero, Jussi (2019)
    Radionuclides 137Cs and 90Sr and total beta activity were determined from air filters collected in Rovaniemi (Finnish Lapland) in1965–2011. Nuclear contamination sources present in the air filter samples as well as temporal changes in radionuclide concentrations were examined. Ozone observations and meteorological modeling were used in combination with radionuclide analyses to study the reasons behind the observed seasonal concentration variation. In general, the magnitude and variation in activity concentrations of 137Cs and 90Sr and total beta activity in the surface air of Rovaniemi in 1965–2011 corresponded well with values from other countries. However, the obtained results prove in practice that hardly any refractory or intermediate radionuclides from the destroyed Chernobyl reactor fuel were introduced to Finnish Lapland. The main source of 137Cs and 90Sr and total beta activity in the surface air of Rovaniemi in 1965–2011 has been intense atmospheric nuclear weapon testing in 1950s–1960s and later tests performed in 1965–1980, as well as leakages from underground nuclear tests in Semipalatinsk, 1966, and Novaya Zemlya, 1987. For 137Cs and total beta activity, the influence of Chernobyl and Fukushima accidents was detected.
  • Li, Yuanyuan; Nie, Wei; Liu, Yuliang; Huang, Dandan; Xu, Zheng; Peng, Xiang; George, Christian; Yan, Chao; Tham, Yee Jun; Yu, Chuan; Xia, Men; Fu, Xiao; Wang, Xinfeng; Xue, Likun; Wang, Zhe; Xu, Zhengning; Chi, Xuguang; Wang, Tao; Ding, Aijun (2020)
    Titanium dioxide (TiO2) is extensively used with the process of urbanization and potentially influences atmospheric chemistry, which is yet unclear. In this work, we demonstrated strong production of Cl-2 from illuminated KCl-coated TiO2 membranes and suggested an important daytime source of chlorine radicals. We found that water and oxygen were required for the reactions to proceed, and Cl-2 production increased linearly with the amount of coated KCl, humidity of the carrier gas, and light intensity. These results suggested that water promotes the reactivity of coated KCl via interaction with the crystal lattice to release free chloride ions (Cl-). The free Cl- transfer charges to O-2 via photoactivated TiO2 to form Cl-2 and probably the O-2(-) radical. In addition to Cl-2, ClO and HOCl were also observed via the complex reactions between Cl/Cl-2 and HOx. An intensive campaign was conducted in Shanghai, during which evident daytime peaks of Cl-2 were observed. Estimated Cl-2 production from TiO2 photocatalysis can be up to 0.2 ppb/h when the TiO2-containing surface reaches 20% of the urban surface, and highly correlated to the observed Cl-2. Our results suggest a non-negligible role of TiO2 in atmospheric photochemistry via altering the radical budget.
  • Hakola, H; Tarvainen, V; Bäck, Jaana; Ranta, H; Bonn, Boris; Rinne, Janne; Kulmala, Markku (2006)
  • Jokinen, Tuija; Kontkanen, Jenni; Lehtipalo, Katrianne; Manninen, Hanna E.; Aalto, Juho; Porcar-Castell, Albert; Garmash, Olga; Nieminen, Tuomo; Ehn, Mikael; Kangasluoma, Juha; Junninen, Heikki; Levula, Janne; Duplissy, Jonathan; Ahonen, Lauri R.; Rantala, Pekka; Heikkinen, Liine; Yan, Chao; Sipila, Mikko; Worsnop, Douglas R.; Back, Jaana; Petäjä, Tuukka; Kerminen, Veli-Matti; Kulmala, Markku (2017)
    Solar eclipses provide unique possibilities to investigate atmospheric processes, such as new particle formation (NPF), important to the global aerosol load and radiative balance. The temporary absence of solar radiation gives particular insight into different oxidation and clustering processes leading to NPF. This is crucial because our mechanistic understanding on how NPF is related to photochemistry is still rather limited. During a partial solar eclipse over Finland in 2015, we found that this phenomenon had prominent effects on atmospheric on-going NPF. During the eclipse, the sources of aerosol precursor gases, such as sulphuric acid and nitrogen-containing highly oxidised organic compounds, decreased considerably, which was followed by a reduced formation of small clusters and nanoparticles and thus termination of NPF. After the eclipse, aerosol precursor molecule concentrations recovered and reinitiated NPF. Our results provide direct evidence on the key role of the photochemical production of sulphuric acid and highly oxidized organic compounds in maintaining atmospheric NPF. Our results also explain the rare occurrence of this phenomenon under dark conditions, as well as its seemingly weak connection with atmospheric ions.
  • Bingen, Christine; Robert, Charles E.; Stebel, Kerstin; Bruehl, Christoph; Schallock, Jennifer; Vanhellemont, Filip; Mateshvili, Nina; Hoepfner, Michael; Trickl, Thomas; Barnes, John E.; Jumelet, Julien; Vernier, Jean-Paul; Popp, Thomas; de Leeuw, Gerrit; Pinnock, Simon (2017)
    This paper presents stratospheric aerosol climate records developed in the framework of the Aerosol_cci project, one of the 14 parallel projects from the ESA Climate Change Initiative. These data records were processed from a stratospheric aerosol dataset derived from the GOMOS experiment, using an inversion algorithm optimized for aerosol retrieval, called AerGOM. They provide a suite of aerosol parameters, such as the aerosol extinction coefficient at different wavelengths in the UV-visible range.The extinction record includes the total extinction as well as separate fields for liquid sulfate aerosols and polar stratospheric clouds (PSCs). Several additional fields (PSC flag, etc.) are also provided. The resulting stratospheric aerosol dataset, which spans the whole duration of the GOMOS mission (2002-2012), was validated using different reference datasets (lidar and balloon profiles). In the present paper, the emphasis is put on the extinction records. After a thorough analysis of the original AerGOM dataset, we describe the methodology used to construct the gridded CCI-GOMOS dataset and the resulting improvements on both the AerGOM algorithm and the binning procedure, in terms of spatio-temporal resolution, coverage and data quality. The extinction datasets were validated using lidar profiles from three ground-based stations (Mauna Loa, Garmisch-Partenkirchen, Dumont d'Urville). The median difference of the CCI-GOMOS (Level 3) extinction and ground-based lidar profiles is between similar to 15% and similar to 45% in the 16-21 km altitude range, depending on the considered site and aerosol type. The CCI-GOMOS dataset was subsequently used, together with a MIPAS SO2 time series, to update a volcanic eruption inventory published previously, thus providing a more comprehensive list of eruptions for the ENVISAT period (2002-2012). The number of quantified eruptions increases from 102 to 230 in the updated inventory. This new inventory was used to simulate the evolution of the global radiative forcing by application of the EMAC chemistry-climate model. Results of this simulation improve the agreement between modelled global radiative forcing of stratospheric aerosols at about 100 hPa compared to values estimated from observations. Medium eruptions like the ones of Soufriere Hills/Rabaul (2006), Sarychev (2009) and Nabro (2011) cause a forcing change from about -0.1 W/m(2) to -0.2 W/m(2). (C) 2017 The Authors. Published by Elsevier Inc.
  • Hellén, Heidi; Leck, Caroline; Paatero, Jussi; Virkkula, Aki; Hakola, Hannele (2012)
  • Karppinen, Toni; Ala-Houhala, Meri; Ylianttila, Lasse; Kautiainen, Hannu; Lakkala, Kaisa; Hannula, Henna-Reetta; Turunen, Esa; Viljakainen, Heli; Reunala, Timo; Snellman, Erna (2017)
    Humans obtain vitamin D from conversion of 7-dehydrocholesterol in the skin by ultraviolet B (UVB) radiation or from dietary sources. As the radiation level is insufficient in winter, vitamin D deficiency is common at higher latitudes. We assessed whether vernal solar UVB radiation at latitudes 61 degrees N and 67 degrees N in Finland has an impact on serum 25-hydroxyvitamin D [S-25(OH) D] concentrations. Twenty-seven healthy volunteers participated in outdoor activities in snow-covered terrain for 4-10 days in March or April, with their face and hands sun-exposed. The personal UVB doses and S-25(OH) D levels were monitored. A mean UVB dose of 11.8 standard erythema doses (SED) was received during an average of 12.3 outdoor hours. The mean S-25(OH) D concentration in subjects with a baseline concentration below 90.0 nmol/L (n=13) increased significantly, by 6.0 nmol/L from an initial mean of 62.4 nmol/L (p
  • Yli-Pelkonen, Vesa Johannes; Scott, Anna A.; Viippola, Juho Viljami; Setälä, Heikki Martti (2017)
    Trees and other vegetation absorb and capture air pollutants, leading to the common perception that they, and trees in particular, can improve air quality in cities and provide an important ecosystem service for urban inhabitants. Yet, there has been a lack of empirical evidence showing this at the local scale with different plant configurations and climatic regions. We studied the impact of urban park and forest vegetation on the levels of nitrogen dioxide (NO2) and ground-level ozone (O3) while controlling for temperature during early summer (May) using passive samplers in Baltimore, USA. Concentrations of O3 were significantly lower in tree-covered habitats than in adjacent open habitats, but concentrations of NO2 did not differ significantly between tree-covered and open habitats. Higher temperatures resulted in higher pollutant concentrations and NO2 and O3 concentration were negatively correlated with each other. Our results suggest that the role of trees in reducing NO2 concentrations in urban parks and forests in the Mid-Atlantic USA is minor, but that the presence of tree-cover can result in lower O3 levels compared to similar open areas. Our results further suggest that actions aiming at local air pollution mitigation should consider local variability in vegetation, climate, micro-climate, and traffic conditions.
  • Yli-Pelkonen, Vesa Johannes; Scott, Anna A.; Viippola, Juho Viljami; Setälä, Heikki Martti (2017)
    Trees and other vegetation absorb and capture air pollutants, leading to the common perception that they, and trees in particular, can improve air quality in cities and provide an important ecosystem service for urban inhabitants. Yet, there has been a lack of empirical evidence showing this at the local scale with different plant configurations and climatic regions. We studied the impact of urban park and forest vegetation on the levels of nitrogen dioxide (NO2) and ground-level ozone (O3) while controlling for temperature during early summer (May) using passive samplers in Baltimore, USA. Concentrations of O3 were significantly lower in tree-covered habitats than in adjacent open habitats, but concentrations of NO2 did not differ significantly between tree-covered and open habitats. Higher temperatures resulted in higher pollutant concentrations and NO2 and O3 concentration were negatively correlated with each other. Our results suggest that the role of trees in reducing NO2 concentrations in urban parks and forests in the Mid-Atlantic USA is minor, but that the presence of tree-cover can result in lower O3 levels compared to similar open areas. Our results further suggest that actions aiming at local air pollution mitigation should consider local variability in vegetation, climate, micro-climate, and traffic conditions.
  • Drozd, Greg T.; Kurten, Theo; Donahue, Neil M.; Lester, Marsha I. (2017)
    We used the steady-state master equation to model unimolecular decay of the Criegee intermediate formed from ozonolysis of 2,3-dimethyl-2-butene (tetramethylethylene, TME). Our results show the relative importance and time scales for both the prompt and thermal unimolecular decay of the dimethyl-substituted Criegee intermediate, (CH3)(2)COO. Calculated reactive fluxes show the importance of quantum mechanical tunneling for both prompt and thermal decay to OH radical products. We constrained the initial energy distribution of chemically activated (CH3)(2)COO formed in TME ozonolysis by combining microcanonical rates k(E) measured experimentally under collision-free conditions and modeled using semiclassical transition-state theory (SCTST) with pressure dependent yields of stabilized Criegee intermediates measured with scavengers in flow-tube experiments. Thermal decay rates under atmospheric conditions k(298 K, 1 atm) increase by more than 1 order of magnitude when tunneling is included. Accounting for tunneling has important consequences for interpreting pressure dependent yields of stabilized Criegee intermediates, particularly with regard to the fraction of Criegee intermediates formed in the zero-pressure limit.
  • Hellen, Heidi; Schallhart, Simon; Praplan, Arnaud P.; Petäjä, Tuukka; Hakola, Hannele (2017)
    An in situ method for studying gas-phase C-2-C-7 monocarboxylic volatile organic acids (VOAs) in ambient air was developed and evaluated. Samples were collected directly into the cold trap of the thermal desorption unit (TD) and analysed in situ using a gas chromatograph (GC) coupled to a mass spectrometer (MS). A polyethylene glycol column was used for separating the acids. The method was validated in the laboratory and tested on the ambient air of a boreal forest in June 2015. Recoveries of VOAs from fluorinated ethylene propylene (FEP) and heated stainless steel inlets ranged from 83 to 123 %. Different VOAs were fully desorbed from the cold trap and well separated in the chromatograms. Detection limits varied between 1 and 130 pptv and total uncertainty of the method at mean ambient mixing ratios was between 16 and 76 %. All straight chain VOAs except heptanoic acid in the ambient air measurements were found with mixing ratios above the detection limits. The highest mixing ratios were found for acetic acid and the highest relative variations for hexanoic acid. In addition, mixing ratios of acetic and propanoic acids measured by the novel GC-MS method were compared with proton-mass-transfer time-off-light mass spectrometer (PTR-TOFMS) data. Both instruments showed similar variations, but differences in the mixing ratio levels were significant.