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  • Articles  (19)
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  • Articles  (19)
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  • Springer  (19)
  • American Meteorological Society
  • American Physical Society (APS)
  • International Union of Crystallography
  • Springer Nature
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  • 1
    ISSN: 1573-0662
    Keywords: global model ; three-dimensional ; Lagrangian tropospheric chemistry ; ozone ; NOX ; emission controls
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Geosciences
    Notes: Abstract A three-dimensional Lagrangian tropospheric chemistry modelis used toinvestigate the impact of human activities on the tropospheric distributionofozone and hydroxyl radicals. The model describes the behaviour of 50 speciesincluding methane, carbon monoxide, oxides of nitrogen, sulphur dioxide andnineorganic compounds emitted from human activities and a range of other sources.Thechemical mechanism involves about 100 chemical reactions of which 16 arephotochemical reactions whose diurnal dependence is treated in full. The modelutilises a five minute chemistry time step and a three hour advection timestepfor the 50,000 air parcels. Meteorological data for the winds, temperatures,clouds and so on are taken from the UK Meteorological Office global model for1994 onwards. The impacts of a 50% reduction in European NOXemissions onglobal ozone concentrations are assessed. Surface ozoneconcentrations decrease in summertime and rise in wintertime, but to differentextents.
    Type of Medium: Electronic Resource
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  • 2
    Electronic Resource
    Electronic Resource
    Springer
    Journal of atmospheric chemistry 28 (1997), S. 263-282 
    ISSN: 1573-0662
    Keywords: ozone ; hydrocarbons ; NOx ; photochemistry ; OH-radicals ; budget
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Geosciences
    Notes: Abstract Simultaneous measurements of ozone and ozoneprecursors were made during a field campaign atSchauinsland in the Black Forest and in the valleynorth of Schauinsland that channels the flow ofpolluted air from the city of Freiburg to the site.From the decay of hydrocarbons and NOx between the twomeasuring sites and the known rate coefficients, theconcentration of OH radicals was calculated. From abudget analysis of OH and HOx it is concluded that therelatively high OH concentrations (5–8 ×106cm-3) in the presence of high NO2concentrations cannot be explained by the knownprimary sources. The budget can be closed if efficientrecycling of OH via HO2 is assumed to occur andthat, based on the measured hydrocarbons, 2 HO2molecules are formed for each OH radical that reactswith a hydrocarbon molecule. This assumption is inaccordance with the budget of Ox obtained from ourmeasurements and with results from earliermeasurements of alkylnitrates and peroxy radicals atSchauinsland. A possible conclusion is that the decayof precursors and production of photooxidants in urbanplumes proceeds at a faster rate than is currentlyassumed. The potential role of biogenichydrocarbons for the radical budget is alsodiscussed.
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  • 3
    Electronic Resource
    Electronic Resource
    Springer
    Journal of atmospheric chemistry 28 (1997), S. 61-76 
    ISSN: 1573-0662
    Keywords: ozone ; beryllium-7 ; annual cycle ; spring maximum ; stratosphere-troposphere exchange
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Geosciences
    Notes: Abstract Ozone measurements, performed since 1987, at the Swedish TOR/EUROTRACstation Åreskutan (lat. 63.4° N, long. 13.1° E, 1250 m abovesea level) are analyzed. The annual average ozone concentration at the sitehas increased by about 0.4 ppbv (∼1%) per year during the period1987–1994. The corresponding trends for individual months show adecrease during April–September and an increase during the rest of theyear. The ozone budget at Åreskutan has been investigated using backtrajectories of the air parcels, and the cosmogenic radionuclide7Be as a tracer of stratospheric air. From a simple diagnosticmodel, it is estimated that the contribution of stratospheric ozone to theconcentrations measured at Åreskutan is 5 ppbv (or 14% of themeasured values) on average, reaching a maximum of 23 ppbv (50%),during the episodes of direct stratospheric influence. In spring, thestratospheric contribution to ozone budget at Åreskutan is at itsmaximum, and approximately equal to the net photochemical ozone productionin the air mass affecting the site, whereas in winter, it is compensated byozone chemical sink during the transport of air masses from pollutedEuropean regions, to Scandinavia.
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  • 4
    Electronic Resource
    Electronic Resource
    Springer
    Journal of atmospheric chemistry 28 (1997), S. 245-262 
    ISSN: 1573-0662
    Keywords: free troposphere ; ozone ; non methane hydrocarbons ; peroxyacetylnitrate ; carbon monoxide ; photo chemistry ; North Atlantic ; seasonal cycle ; long range transport ; back-trajectories ; photochemical age
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Geosciences
    Notes: Abstract Free tropospheric measurements of ozone, peroxyacetylnitrate andprecursors (CO, NMHC) that were made within the framework of the EUROTRACsub-project TOR (Tropospheric Ozone Research) between 1990 and 1995 at theGAW station Izana, Tenerife (28°18′N, 16°30′W) arediscussed. The average annual cycles reveal the importance of transport fromnorthern mid-latitudes and the role of photo-chemistry. According toair-mass trajectories, which were supplied to us from AEROCE(Atmosphere/Ocean Chemistry Experiment), transport from northernmid-latitudes is associated with high precursor concentrations in winter,whereas ozone concentrations in winter are not much influenced by transportpatterns, suggesting a rather uniform distribution over the northern part ofthe Northern Hemisphere around mean value of 43 ± 5 ppb. In summer,high ozone concentrations of up to 90 ppb are often encountered duringtransport from north, while the levels of precursors are much lower than inwinter, because of photochemical destruction. Trajectories from southerlylatitudes and the Sahara usually have the lowest ozone concentrationsassociated with them.
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  • 5
    Electronic Resource
    Electronic Resource
    Springer
    Journal of atmospheric chemistry 26 (1997), S. 77-91 
    ISSN: 1573-0662
    Keywords: ozone ; soot ; solar radiation
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Geosciences
    Notes: Abstract The soot-ozone reaction at low concentrations (ppm O3) hasbeen examined todetermine any influence of solar radiation on its products and kinetics. Theeffect of simulatedsolar radiation is to change the product distribution towardsCO2(g), CO (g) and H2O(g) at theexpense of soot surface functional groups formation. Little effect on theextent or rate ofdiminution of O3 through this rapid reaction is observed. Theinitial rate laws for formation ofall products remain the same under simulated solar radiation, with changes inthe rate constants(and thus in the relative importance of mechanistic pathways) responsible forthe differingproduct distributions. Decarboxylation of soot surface functionalities hasbeen shown to be onepossible mechanism underlying these effects. Atmospheric soot, particularlythat emitted nearthe tropopause by increasing numbers of subsonic and supersonic aircraft, mayplay a role inozone depletion; the rapid diminution of ozone in soot's presence isunaffected by solarradiation.
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  • 6
    ISSN: 1573-0662
    Keywords: biogenic hydrocarbons ; ozone ; nitrate radicals ; aerosol formation ; gas/particle partitioning
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Geosciences
    Notes: Abstract Measurements of aerosol formation during thephotooxidation of α-pinene, β-pinene,d-3-carene, d-limonene, ocimene, linalool, terpinene-4-ol, andtrans-caryophyllene were conducted in anoutdoor smog chamber. Daylight experiments in thepresence of $${\text{NO}}_x $$ and dark experiments withelevated ozone concentrations were performed. Theevolution of the aerosol was simulated by theapplication of a gas/particle absorption model inconnection with a chemical reaction mechanism. Thefractional aerosol yield is shown to be a function ofthe organic aerosol mass concentration andtemperature. Ozone and, for selected hydrocarbons, theNO3 reaction of the compounds were found torepresent efficient routes to the formation ofcondensable products. For initial hydrocarbon mixingratios of about 100 ppb, the fractional aerosol yieldsfrom daylight runs have been estimated to be ∼5%for open-chain hydrocarbons, such as ocimene andlinalool, 5–25% for monounsaturated cyclicmonoterpenes, such as α-pinene, d-3-carene, orterpinene-4-ol, and ∼40% for a cyclic monoterpenewith two double bonds like d-limonene. For the onlysesquiterpene investigated, trans-caryophyllene, afractional aerosol yield of close to 100% wasobserved. The majority of the compounds studied showedan even higher aerosol yield during dark experimentsin the presence of ozone.
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  • 7
    Electronic Resource
    Electronic Resource
    Springer
    Journal of atmospheric chemistry 28 (1997), S. 77-95 
    ISSN: 1573-0662
    Keywords: ozone ; tropopause folding ; stratospheric ozone intrusion
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Geosciences
    Notes: Abstract The analysis of surface ozone variability requires besides chemicalstudies the consideration of meteorological conditions and dynamicprocesses. Our research focuses on the mechanisms in connection with coldfront passages. A statistical study and case studies of cold front passageswere carried out at six German ground-based sites during the year 1990.After the passage of cold fronts three typical developments of thenear-ground ozone concentrations could be identified. Usually the ozoneconcentrations decrease due to advection of clean air masses or due toenhanced cloudiness preventing the photochemical production of ozone,chemical destruction by nitrogenoxides, and heterogeneous chemistry. In somecases the concentrations increased by reason of downward mixing of ozoneenriched air intruded from the stratosphere into the troposphere bytropopause foldings. For a few cases no modification set in. The decreasewas mostly twice as strong as the increase. The latter was between 4 and 8ppb on the average. Special emphasis is given to the transport ofstratospheric ozone down to the ground. There is no direct evidence forstratospheric ozone at ground level, because it can‘t be distinguished fromthe tropospheric one, but from case studies circumstantial evidence is foundin favour of it. As an example of increasing ozone behind the passage ofcold fronts one case study typical of all other case studies is presented.It shows the characteristic properties of the corresponding fronts, whichare fast movement, a vertical split structure and strong convection.
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  • 8
    ISSN: 1573-0662
    Keywords: Chine vehicles ; ozone ; aerosols ; carbon dioxide ; alternative fuels
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Geosciences
    Notes: Abstract Local surface travel needs in the People‘s Republic of China (mainlandChina) have traditionally been met largely by nonpolluting bicycles. A majorautomobile manufacturing/importing effort has begun in the country over thelast decade, and planning documents indicate that the Chinese may strive toacquire more than 100 million vehicles early in the next century. By analogywith large automotive fleets already existing in the western world, bothregional and global scale pollution effects are to be expected from theincrease. The present work adopts the latest projections of Chinese automobilemanufacture and performs some quantitative assessments of the extent ofpollution generation.Focus for the investigation is placed upon the oxidant ozone. Emissions of theprecursor species nitrogen oxides and volatile organics are constructed basedon data for the current automotive sector in the eastern portion of the UnitedStates. Ozone production is first estimated from measured values forcontinental/oceanic scale yields relative to precursor oxidation. Theestimates are then corroborated through idealized two dimensional modeling ofthe photochemistry taking place in springtime air flow off the Asian land massand toward the Pacific Ocean. The projected fleet sizes could increase coastaland remote oceanic ozone concentrations by tens of parts per billion (ppb)in the lower troposphere. Influences on the tropospheric aerosol system andon the major greenhouse gas carbon dioxide are treated peripherally. Nitrogenoxides created during the vehicular internal combustion process willcontribute to nitrate pollution levels measured in the open Pacific. Thepotential for soot and fugitive dust increases should be considered as theautomotive infrastructure develops. Since the emerging Chinese automotivetransportation system will represent a substantial addition to the globalfleet and all the carbon in gasoline is eventually oxidized completely, asignificant rise in global carbon dioxide inputs will ensue as well.Some policy issues are treated preliminary. The assumption is made thatalterations to regional oxidant/aerosol systems and to terrestrial climate areconceivable. The likelihood that the Chinese can achieve the latest vehiclefleet goals is discussed, from the points of view of new production, positivepollution feedbacks from a growing automobile industry, and known petroleumreserves. Vehicular fuel and maintenance options lying before the Chinese areoutlines and compared. To provide some perspective on the magnitude of theenvironmental changes associated with an Asian automotive buildup, recentestimates of the effects of future air traffic over the Pacific Rim aredescribed.
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  • 9
    ISSN: 1573-0662
    Keywords: PAN ; ozone ; troposphere ; photochemistry ; Alaska
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Geosciences
    Notes: Abstract Springtime measurements of NOx, ozone, PAN,J(NO2), and other compounds were made near Ny-Ålesund,Svalbard (78°54′N, 11°53′E), in 1994 and Poker Flat,Alaska (65°08′N, 147°29′W), in 1995. At Svalbard medianmixing ratios for PAN and NOx of 237 and 23.7 pptv,respectively, were observed. The median mixing ratios at Poker Flat for PANand NOx were 79.5 and 85.9 pptv, respectively. These data areused to estimate thermal PAN decomposition using several differentapproaches. At Svalbard PAN decomposition was very small, while at PokerFlat up to 30 pptv/h PAN decomposed. At both sites the NOx/PANratio increased with temperature between –10 and 20°C implyingthat PAN decomposition is an important NOx source. In-situozone production was calculated from the measured NO, NO2,O3, J(NO2), and temperature data, using thesteady state assumption Median ozone production was 605 pptv/h at PokerFlat, and one order of magnitude smaller at Svalbard during the daytime.Only at Poker Flat could a direct influence on the diurnal ozone cycle beobserved from in-situ production. These results imply that PAN decompositionis a major source of NOx in the high latitude troposphere, andthat this contributes to the observed spring maximum in surface ozone.
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  • 10
    Electronic Resource
    Electronic Resource
    Springer
    Journal of atmospheric chemistry 27 (1997), S. 249-269 
    ISSN: 1573-0662
    Keywords: atmospheric surface layer ; constant-flux layer ; ozone ; nitric oxide ; radon ; thoron ; thoron exhalation ; Damköhler ratio ; eddy diffusivity
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Geosciences
    Notes: Abstract We have discussed the behavior of a non-conserved scalar in the stationary, horizontally homogeneous, neutral surface-flux layer and, on the basis of conventional second-order closure, derived analytic expressions for flux and for mean concentration of a gas, subjected to a first-order removal process. The analytic flux solution showed a clear deviation from the constant flux, characterizing a conserved scalar in the surface-flux layer. It decreases with height and is reduced by an order of magnitude of the surface flux at a height equal to about the typical mean distance a molecule can travel before destruction. The predicted mean concentration profile, however, shows only a small deviation from the logarithmic behavior of a conserved scalar. The solution is consistent with assuming a flux-gradient relationship with a turbulent diffusivity corrected by the Damköhler ratio, the ratio of a characteristic turbulent time scale and the scalar mean lifetime. We show that if we use only first-order closure and neglect the effect of the Damköhler ratio on the turbulent diffusivity we obtain another analytic solution for the profiles of the flux and the mean concentration which, from an experimental point of view, is indistinguishable from the first analytic solution. We have discussed two cases where the model should apply, namely NO which, by night, is irreversibly destroyed by interaction with mainly O3 and the radioactive 220Rn. Only in the last case was it possible to find data to shed light on the validity of our predictions. The agreement seemed such that a falsification of our model was impossible. It is shown how the model can be used to predict the surface flux of 220Rn from measured concentration profiles.
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