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1.
Long-term measurements of light hydrocarbons(C2–C5 HCs) were performed in the courseof the EUROTRAC sub-project TOR (Tropospheric Ozone Research) in thesouthern part of the Black Forest in southwest Germany. The measurementscover a time period of five years (January 1989–January 1994) and theair samples were analyzed onsite by an automated GC-system. Pronouncedannual cycles with maxima in late winter and minima in late summer wereobserved in the case of the slowly reacting hydrocarbons ethane, propane andacetylene, reflecting the fact that the seasonal variation of these speciesis photochemically driven. For the shorter lived compounds the seasonalvariations are considerably weaker, connected with a stronger scatter of theindividual measurements, which is caused by different distances to theirmain sources for different wind vectors as well as by varying sourcestrengths. From a detailed characterization of the hydrocarbon patterns theinfluence of two different sources could be distinguished. An extrapolationto photochemical age of zero and completion of our data with those from aspeciated VOC inventory yields an estimated [VOC]/NOx sourceratio for Schauinsland of 5 [ppbC/ppb]. Comparable[VOC]/NOx ratios are observed in automobile exhaust gasesunder low speed conditions, which points to the important role of trafficunder conditions, when freshly polluted air masses from a near-by city areadvected to the site. From an investigation of the photochemical age of theadvected air masses it becomes clear that there must exist biogenic sourcesof light olefins in the vicinity of the observatory during the vegetationperiod. For propene and the butenes we are able to estimate a lower limit oftheir contributions in terms of reactivity to the total reactivity( [HC](i) k_OH(i),i=C2-C5) of the measured hydrocarbons. Forlowest pollution levels in summer (acetylene <300 ppt, about 40%of the summer values) this source is found to be responsible for15–20% of the total C2–C5reactivity observed at Schauinsland. On the average, this source accountsfor 5–10% of the total C2–C5reactivity.  相似文献   

2.
A technique has been developed which can measure low-molecular-weight (C2–C5) oxygenated hydrocarbons down to concentrations of less than 10 parts per trillion (10-12) in the atmosphere. The method uses cryogenic trapping of trace gases from the air, and two-dimensional gas chromatography (2DGC) with flame ionization and photo-ionization detectors to analyze the samples. The method has been used to make extensive measurements in the field, and it is capable of measuring all of the C2–C5 carbonyl compounds in clean tropospheric air. The 2DGC analytical system also makes it possible to prepare accurate, reproducible standards of the low-molecular-weight oxygenated hydrocarbons at trace levels.  相似文献   

3.
The second Arctic Gas and Aerosol Sampling Program (AGASP-II) was conducted across the Alaskan and Canadian Arctic in April 1986, to study the in situ aerosol, and the chemical and optical properties of Arctic haze. The NOAA WP-3D aircraft, with special instrumentation added, made six flights during AGASP-II. Measurements of wind, pressure, temperature, ozone, water vapor, condensation nuclei (CN) concentration, and aerosol scattering extinction (bsp) were used to determine the location of significant haze layers. The measurements made on the first three flights, over the Arctic Ocean north of Barrow and over the Beaufort Sea north of Barter Island, Alaska are discussed in detail in this report of the first phase of AGASP II. In the Alaskan Arctic the WP-3D detected a large and persistent region of haze between 960 and 750 mb, in a thermally stable layer, on 2, 8, and 9 April 1986. At its most dense, the haze contained CN concentrations >10,000 cm–3 and bsp of 80×10–6 m–1 suggesting active SO2 to H2SO4 gas-to-particle conversion. Calculations based upon observed SO2 concentrations and ambient relative humidities suggest that 104–105 small H2SO4 droplets could have been produced in the haze layers. High concentrations of sub-micron H2SO4 droplets were collected in haze. Ozone concentrations were 5–10 ppb higher in the haze layers than in the surrounding troposphere. Outside the regions of haze, CN concentrations ranged from 100 to 400 cm–3 and bsp values were about (20–40)×10–6 m–1. Air mass trajectories were computed to depict the air flow upwind of regions in which haze was observed. In two cases the back trajectories and ground measurements suggested the source to be in central Europe.  相似文献   

4.
Observations and model calculations of the concentration of hydrocarbonsat five Scandinavian rural sites during March–June 1993are reported.Decreasing concentrations from March to June are observedat all sites. The highest concentrations of hydrocarbons were found in air massescoming in from the southwest to southeast, indicating that long rangetransport fromcontinental Europe and the U.K. is important in pollution episodes. An episode of elevated concentrations of hydrocarbons observed at three of the sites in the middle of Marchis described and discussed in relation to the synoptic situation and thepresenceof other chemical compounds (NO2, PAN, total nitrate andozone).A Lagrangian numerical model is used to calculate the concentrations of theindividual hydrocarbons at the fivesites and comparison with observations is made.The calculated concentrations for nonmethane hydrocarbons with quite longchemicallifetimes agree well with the observations.For the sum of observed and calculated hydrocarbons the correlationcoefficientsare in the range of 0.65–0.88 for the five sitesand the ratio between calculated and measured concentrations was0.72–0.97, indicating thatthe European VOC emission inventory is quite well estimated.  相似文献   

5.
Samples of interstitial air from within the snow pack on an ice floe on the Arctic Ocean were collected during the April 1994 Polar Sunrise Experiment. The concentrations of C2-C7 hydrocarbons are reported for the first time in the snow pack interstitial air. Alkane concentrations tended to be higher than concentrations in free air samples above the snow but very similar to winter measurements at various locations in the Arctic archipelago. However, ethyne concentrations in both interstitial and free air were highly correlated with ozone mixing ratios, consistent with previous demonstrations of the effects of Br atom chemistry. The analysis of total bromine within the snow pack indicate an enrichment in total Br at the interface layer between snow and free troposphere. The mixing ratios of some brominated compounds, such as CHBr3 and CHBr2Cl, are found to be higher in this top layer of snow relative to the boundary layer. Results were inconclusive due to the limited number of samples, but suggest the possible presence of active bromine in the snow pack and also that some differences exist between chemical reactions occurring in interstitial air compared to air in the boundary layer.  相似文献   

6.
Simultaneousindependent measurements of NOy and NOx(NOx= NO + NO2) by high-sensitivitychemiluminescence systems and of PAN (peroxyacetylnitrate) and PPN (peroxypropionyl nitrate) by GC-ECDwere made at Spitsbergen in the Norwegian Arcticduring the first half year of 1994. The average mixingratio of the sum of PAN and PPN (denoted PANs)increased from around 150 pptv in early winter to amaximum of around 500 pptv in late March, whereasepisodic peak values reached 800 pptv. This occurredsimultaneously with a maximum in ozone which increasedto 45–50 ppbv in March–April. The average NOxmixing ratio was 27 pptv and did not show any cyclethrough the period. The NOy mixing ratio showeda maximum in late March, while the difference betweenNOy and PAN decreased during spring. This is anindication of the dominance of PAN in the NOybudget in the Arctic, but possible changes in theefficiency of the NOy converter could alsocontribute to this. Although most PAN in theArctic is believed to be due to long range transport,the observations indicate local loss and formationrates of up to 1–2 pptv h-1 in April–May.Measurements of carbonyl compounds suggest thatacetaldehyde was the dominant, local precursor ofPAN.Now at 1.  相似文献   

7.
Airborne observations during August 1985 over Greenland and the North American Arctic revealed that dense, discrete haze layers were common above 850 mb. No such hazes were found near the surface in areas remote from local sources of particles. The haze layers aloft were characterized by large light-scattering coefficients due to dry particles (maximum value 1.24 × 10–4m–1) and relatively high total particle concentrations (maximum value 3100 cm–3). Sulfate was the dominant ionic component of the aerosol (0.06 – 1.9 g m–3); carbon soot was also present. Evidence for relatively fresh aerosols, accompanied by NO2 and O3 depletion, was found near, but not within, the haze layers. The hazes probably derived from anthropogenic sources and/or biomass burning at midlatitudes.It is hypothesized that the scavenging of particles by stratus clouds plays an important role in reducing the frequency and intensity of hazes at the surface in the Arctic in summer. Since the detection of haze layers aloft through measurements of column-integrated parameters from the surface (e.g., by lidar) cannot be carried out reliably when clouds are present, such measurements have likely underestimated the occurrence of haze layers in the Arctic, particularly in summer.  相似文献   

8.
C2–C6 Nonmethane hydrocarbons (NMHC) and radioactive continental tracers were measured during two oceanographic cruises, in June 1982 in the Mediterranean and Red Sea, and in November 1982 across the North Atlantic and South Pacific oceans. Typical concentrations in marine atmosphere are between 0.05 and 0.2 ppbv. Owing to their similar lifetimes, propane and radon-222 are found to be well correlated. This relationship establishes that propane is mainly produced over lands and enables us to estimate its continental source strength at about 60×106 tons of carbon per year.Also at Université de Picardie  相似文献   

9.
Surface observations of several nitrogen oxides in the Canadian high Arctic during the period March-April 1988 are reported. These include data on NO2, the inorganic nitrates HNO3 and particulate nitrate, and the organic nitrates PAN and C3–C7 alkyl-nitrates. It is found that the organic nitrates make up 70–80% of the sum of the measured nitrogen oxides. Based on concurrently measured sulphur oxides, the period of observation was divided into two halves with the first half representing less polluted, more aged air than the second. The preponderance of the organic nitrates was less in the first period than the second. In contrast, there was little difference in the inorganic nitrates and NO2 concentrations. The dominant inorganic nitrate shifted from particulate nitrate in the first period towards gaseous HNO3 in the second. No correlation between the nitrates (inorganic or organic) and O3 was observed; although some indication of a positive correlation between NO2 and O3 has been reported earlier (Bottenheimet al., 1990). Possible explanations for these observations are proposed. A survey of other potential nitrogen oxides that may be present in the Arctic air but not measured in these experiments suggests that the nitrogen oxides not measured here constitute a minor fraction of the total reactive nitrogen (NO y ).Paper submitted to the 7th International Symposium of the Commission for Atmospheric Chemistry and Global Pollution on the Chemistry of the Global Atmosphere held in Chamrousse, France, from 5 to 11 September 1990.  相似文献   

10.
Ground-based FTIR measurements have been performed in the Arctic summer in July 1993 and June 1994 at 79° N to study the zenith column densities of several trace gases in the undisturbed Arctic summer atmosphere. Zenith column densities of H2O, N2O, HNO3, NO2, NO, ClONO2, ClO, HCl, HF, COF2, OCS, SF6, HCN, CH4, C2H6, C2H2, CO, O3, CFC-12, CFC-22, and CO2 were retrieved by line-by-line calculations. The results are compared with winter and springtime observations measured at the same site, with column densities obtained in the Antarctic summer atmosphere, and with measurements at midlatitudes. For HCl the spectra give lower total zenith columns than expected, but the ratio HF/HCl agrees well with midlatitude literature data. Measurements of ClONO2 give low total columns in agreement with observations at midlatitudes. In the undisturbed atmosphere HCl was found to be in excess of ClONO2. The total columns of HNO3, N2O and the sum of NO and NO2 agree with summer observations in Antarctica. Results for the tropospheric trace gas C2H6 are higher by 250% when compared with Antarctic observations. Contrary to N2O and CH4 the seasonal cycle of C2H6 and C2H2 give much higher total columns in winter/spring compared to the summer observations. This is assigned to transport of polluted airmasses from mid-latitudes into the Arctic.  相似文献   

11.
Balloon-borne aerosol measurements were performed with an optical particle counter between 1994 and 2000 at Ny-Ålesund (79°N), Svarbard. Throughout the observation period, continuous decay was found in the concentrations of particles with 0.4–0.6 μm in radius in the Arctic stratosphere, suggesting that Pinatubo aerosols remained even at the end of the 1990s. The decay rate was clearly higher for larger particle sizes, and higher at higher altitude (e-folding time of 970–526 days), suggesting a gravitational sedimentation effect. For smaller particles with R<0.4 μm, slight increases in concentration with time were found, which agreed with the measurements at mid-latitude. The sulfate mass mixing ratio in the Arctic stratosphere before 1998 showed values higher than those at middle latitude, while values were almost the same in both regions after 1998. A possible explanation of the latitudinal difference is a time lag (of 0.5–1 year) in the arrival of Pinatubo aerosols in the Arctic.  相似文献   

12.
Measurements of NOx (NO +NO2) and the sum of reactive nitrogenconstituents, NOy, were made near the surface atAlert (82.5°N), Canada during March and April1998. In early March when solar insolation was absentor very low, NOx mixing ratios were frequentlynear zero. After polar sunrise when the sun was abovethe horizon for much or all of the day a diurnalvariation in NOx and NOy was observed withamplitudes as large as 30–40 pptv. The source ofactive nitrogen is attributed to release from the snowsurface by a process that is apparently sensitized bysunlight. If the source from the snowpack is a largescale feature of the Arctic then the diurnal trendsalso require a competing process for removal to thesurface. From the diurnal change in the NO/NO2ratio, mid-April mixing ratios for the sum of peroxyand halogen oxide radicals of 10 pptv werederived for periods when ozone mixing ratios were inthe normal range of 30–50 ppbv. Mid-day ozoneproduction and loss rates with the active nitrogensource were estimated to be 1–2 ppbv/day and in nearbalance. NOy mixing ratios which averaged only295±66 pptv do not support a large accumulation inthe high Arctic surface layer in the winter and springof 1998. The small abundance of NOy relative tothe elevated mixing ratios of other long-livedanthropogenic constituents requires that reactivenitrogen be removed to the surface during transport toor during residence within the high Arctic.  相似文献   

13.
As a component of the Canadian Arctic Haze Study, held coincident with the second Arctic Gas and Aerosol Sampling Program (AGASP II), vertical profiles of aerosol size distribution (0.17 m), light scattering parameters and cloud particle concentrations were obtained with an instrumented aircraft and ground-based lidar system during April 1986 at Alert. Northwest Territories. Average aerosol number concentrations range from about 200 cm–3 over the Arctic ice cap to about 100 cm–3 at 6 km. The aerosol size spectrum is virtually free of giant or coarse aerosol particles, and does not vary significantly with altitude. Most of the aerosol volume is concentrated in the 0.17–0.50 m size range, and the aerosol number concentration is found to be a good surrogate for the SO4 = concentration of the Arctic haze aerosol. Comparison of the aircraft and lidar data show that, when iced crystal scattering is excluded, the aerosol light scattering coefficient and the lidar backscattering coefficient are proportional to the Arctic haze aerosol concentration. Ratios of scattering to backscattering, scattering to aerosol number concentration, and backscattering to aerosol number concentration are 15.3 steradians, 1.1×10–13 m2, and 4.8×10–15 m2 sr–1, respectively. Aerosol scattering coefficients calculated from the measured size distributions using Mie scattering agree well with measured values. The calculations indicate the aerosol absorption optical depth over 6 km to range between 0.011 and 0.018. The presence of small numbers of ice crystals (10–20 crystals 1–1 measured) increased light scattering by over a factor of ten.  相似文献   

14.
In part two of this series of papers on the IMS model, we present the chemistry reaction mechanism usedand compare modelled CH4, CO, and O3 witha dataset of annual surface measurements. The modelled monthly and 24-hour mean tropospheric OH concentrationsrange between 5–22 × 105 moleculescm–3, indicating an annualaveraged OH concentration of about 10 × 105 moleculescm–3. This valueis close to the estimated 9.7 ± 0.6 × 105 moleculescm–3 calculated fromthe reaction of CH3CCl3 with OH radicals.Comparison with CH4 generally shows good agreementbetween model and measurements, except for the site at Barrow where modelledwetland emission in the summer could be a factor 3 too high.For CO, the pronounced seasonality shown in the measurements is generally reproduced by the model; however, the modelled concentrations are lower thanthe measurements. This discrepancy may due to lower the CO emission,especially from biomass burning,used in the model compared with other studies.For O3, good agreement between the model and measurements is seenat locations which are away from industrial regions. The maximum discrepancies between modelled results and measurementsat tropical and remote marine sites is about 5–10 ppbv,while the discrepancies canexceed 30 ppbv in the industrial regions.Comparisons in rural areas at European and American continental sites arehighly influenced by the local photochemicalproduction, which is difficult to model with a coarse global CTM.The very large variations of O3 at these locations vary from about15–25 ppbv in Januaryto 55–65 ppbv in July–August. The observed annual O3amplitude isabout 40 ppbv compared with about 20 ppbv in the model. An overall comparison of modelled O3 with measurements shows thatthe O3seasonal surface cycle is generally governed bythe relative importance of two key mechanisms that drivea springtime ozone maximum and asummertime ozone maximum.  相似文献   

15.
Simultaneous measurements of peroxy and nitrate radicals at Schauinsland   总被引:3,自引:0,他引:3  
We present simultaneous field measurements of NO3 and peroxy radicals made at night in a forested area (Schauinsland, Black Forest, 48° N, 8° N, 1150 ASL), together with measurements of CO, O3, NO x , NO y , and hydrocarbons, as well as meteorological parameters. NO2, NO3, HO2, and (RO2) radicals are detected with matrix isolation/electron spin resonance (MIESR). NO3 and HO2 were found to be present in the range of 0–10 ppt, whilst organic peroxy radicals reached concentrations of 40 ppt. NO3, RO2, and HO2 exhibited strong variations, in contrast to the almost constant values of the longer lived trace gases. The data suggest anticorrelation between NO3 and RO2 radical concentrations at night.The measured trace gas set allows the calculation of NO3 and peroxy radical concentrations, using a chemical box model. From these simulations, it is concluded that the observed anthropogenic hydrocarbons are not sufficient to explain the observed RO2 concentrations. The chemical budget of both NO3 and RO2 radicals can be understood if emissions of monoterpenes are included. The measured HO2 can only be explained by the model, when NO concentrations at night of around 5 ppt are assumed to be present. The presence of HO2 radicals implies the presence of hydroxyl radicals at night in concentrations of up to 105 cm–3.  相似文献   

16.
A series of 149 measurements of the HCHO mixing ratio were made between 0 and 10 km altitude and 70° N to 60° S latitude during TROPOZ II. The data show a vertical decrease of the HCHO mixing ratio with altitude at all latitudes and a broad latitudinal maximum in the HCHO mixing ratio between 30° N and 30° S at all altitudes. The measured mixing ratios of HCHO are considerably higher than those expected from CH4 oxidation alone, but agree broadly with the average latitude by altitude distribution of HCHO derived by a 2D model including emissions of C1–C7 hydrocarbons. A number of the regional scale deviations of the measured HCHO distribution from the average modelled one can be explained in terms of the local wind field.  相似文献   

17.
Summary Synoptic activity for the Arctic is examined for the period 1952–1989 using the National Meteorological Center sea level pressure data set. Winter cyclone activity is most common near Iceland, between Svalbard and Scandinavia, the Norwegian and Kara seas, Baffin Bay and the eastern Canadian Arctic Archipelago; the strongest systems are found in the Iceland and Norwegian seas. Mean cyclone tracks, prepared for 1975–1989, confirm that winter cyclones most frequently enter the Arctic from the Norwegian and Barents seas. Winter anticyclones are most frequent and strongest over Siberia and Alaska/Yukon, with additional frequency maxima of weaker systems found over the central Arctic Ocean and Greenland.During summer, cyclonic activity remains common in the same regions as observed for winter, but increases over Siberia, the Canadian Arctic Archipelago and the Central Aretic, related to cyclogenesis over northern parts of Eurasia and North America. Eurasian cyclones tend to enter the Aretic Ocean from the Laptev Sea eastward to the Chukchi Sea, augmenting the influx of systems from the Norwegian and Barents seas. The Siberian and Alaska/Yukon anticyclone centers disappear, with anticyclone maxima forming over the Kara, Laptev, East Siberian and Beaufort seas, and southeastward across Canada. Summer cyclones and anticyclones exhibit little regional variability in mean central pressure, and are typically 5–10 mb weaker than their winter counterparts.North of 65°N, cyclone and anticyclone activity peaks curing summer, and is at a minimum during winter. Trends in cyclone and anticyclone activity north of 65°N are examined through least squares regression. Since 1952, significant positive trends are found for cyclone numbers during winter, spring and summer, and for anticyclone numbers during spring, summer and autumn.With 11 Figures  相似文献   

18.
To systematically explain relations between light hydrocarbons, CO, and CO2 concentrations/emissions of biomassburning, we measured concentrations/emissions of carbon gases – CO,CO2, light hydrocarbons (CH4, C2H6,C2H4, C2H2, C3H8, C3H6,n-C4H10, i-C4H10, n-C5H12,i-C5H12), and THC (total hydrocarbon) – in the burning of dead plant material, mainly Imperata grass, byclosed-chamber experiments and by time-series analyses of gas concentrations in combustion plumes in relatively efficient and inefficient combustion situations. Concentrations of hydrocarbons measured were well correlated to [CO] although [C2H2] was exceptionally well correlated to[CO2]. The phase diagrams (relation between [CO]/ [CO2] and [hydrocarbon]/ [CO2]) obtained by the time-seriesexperiments well illustrated the variation in the overall emission rates of the closed-chamber experiments. The higher rates of decrease in hydrocarbon concentration with increasing carbon number in the efficient case compared with the inefficient case probably reflected the rate of oxidation and the amount of radicals. The overall concentrations (or emissions) of C2H4 and C3H6 were higher thanthose of C2H6 and C3H8, suggesting a linkage to mechanisms in whichthe predominant path of hydrocarbon oxidation is through the degradation of alkyl radicals, which can be immediately converted into or formed from alkenes. For C3 and C4 species, normal-chain species hadhigher emissions than iso-chain species under lower combustion efficiency. This may be attributable to the presence of tertiary C–H bonds in iso-species,which show more reactivity in the abstraction of H than secondary C–H bonds unless the carbon number is large.  相似文献   

19.
A rotating laboratory model of the Barents Sea was forced by computed inflows of Atlantic Water and Arctic Surface Water for the period 1979–1984. Ad hoc tidal excursions over the shoals north of Bear Island and deep water production as a result of winter cooling and salt rejection in the eastern part of the basin were calibrated in the model. The high spatial resolution in the basin, which was 5 m in diameter, provided the basis for simulating several physical scales simultaneously. The simulated current features of interest include (1) the spreading of the Norwegian Coastal Current over Tromsøflaket, (2) a warm-core jet along the southeastern slope of the Svalbardbanken, which pushes the ice front far to the NE of Hopen Island, (3) the anticyclonic circulation around Sentralbanken, which drives Arctic Surface Water and ice far south in the eastern basin, (4) Norwegian Coastal Water flowing north across the Bear Island Channel, (5) deep water outflows north through the Franz-Victoria Trough and west through the Bear Island Channel, (6) the dependence of dense water accumulation and flushing on the variable Atlantic inflow, and (7) a robust, tidally driven circulation on the Svalbardbanken and around Bear Island. The Polar Front along the Svalbardbanken is fairly stationary, although its location is highly variable in the Sentralbanken area as a result of underflows (and winds—which were not simulated). The residence time for the Arctic Surface Water on Sentralbanken is about 8 months. Comparisons with available field measurements show a validation that is better than existing numerical model simulations.Entrainment of Arctic Surface Water on Svalbardbanken to the Atlantic inflow holds the Polar Front sharp and modifies the Atlantic Water as it flows to the Arctic Ocean. The simulated warm-core jet along this slope had a core speed up to 85 cm s−1, whereas the best available current measurements near the core show surges up to about 30 cm s−1. The simulated vorticity of the current is −0.33f, where f is the planetary vorticity. This can be provided from the conservation of potential vorticity. Both field data and laboratory simulations show that particles trapped in the Bear Island Current take 5–8 days to circle the island, which is 20 km in diameter. Except for surface confetti, agreement between model and field data was good for the southern flow east of Sentralbanken, but poor for the Murman Current. A model ‘wind’ caused a significant departure in this region and may be responsible for an exaggerated warm-core jet past Svalbardbanken.  相似文献   

20.
Several years of measurements of ozone, hydrocarbons, sulphate and meteorological parameters from Spitsbergen in the Norwegian Arctic are presented. Most of the measurements were taken on the Zeppelin Mountain at an altitude of 474 m a.s.l. The focus is the episodes of ozone depletion in the lower troposphere in spring, which are studied in a climatological way. Episodes of very low ozone concentrations are a common feature on the Zeppelin Mountain in spring. The low ozone episodes were observed from late March to the beginning of June. When the effect of transport direction was subtracted, the frequenty of the low ozone episodes was found to peak in the beginning of May, possibly reflecting the seasonal cycle in the actual depletion process. Analyses based on trajectory calculations show that most of the episodes occurred when the air masses were transported from W-N. Ozone soundings show that the ozone depletion may extend from the surface and up to 3–4 km altitude. The episodes were associated with a cold boundary layer beneath a thermally stable layer, suppressing mixing with the free troposphere. The concentration of several individual hydrocarbons was much lower during episodes of low ozone than for the average conditions. The change in concentration ratio between the hydrocarbons was in qualitative agreement with oxidation of hydrocarbons by Br and Cl atoms rather than by OH radicals.  相似文献   

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