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1.
During the field campaign POPCORN (Photo oxidant formation by plant emitted compounds and OH radicals in North-eastern Germany) in Pennewitt (Mecklenburg-Vorpommern, Germany) in August 1994, carbon monoxide and nonmethane hydrocarbons were measured over a large maize field by in-situ gas chromatography. Throughout the campaign CO and NMHC showed, even for a remote rural area, unexpectedly low mixing ratios. Except a few episodes, CO mixing ratios were around 120 ppb. Ethane was the only hydrocarbon showing mixing ratios exceeding 1 ppb. The mixing ratios of all other NMHC ranged between several hundred ppt and the lower limit of detection which was between 20 and 5 ppt depending on the compound. During three frontal passages CO and NMHC mixing ratios increased significantly, while between August 13 and 16, 1994, polar air masses were encountered with CO and NMHC mixing ratios dropping to values which are typical for North Atlantic background air. During this period average CO mixing ratios were 85 ppb and ethane as the most abundant hydrocarbon decreased to 650 ppt. The large-scale meteorological situation is reflected in an unusual frequency distribution of CO. The distribution shows three maxima which can be assigned to the periods of the frontal passages, to the observation of polar air masses and the rest of the campaign. Two-day backward trajectories were calculated in order to obtain information about the origin of the air masses transported to the site. The observed NMHC and CO data can be attributed to the origin of the air masses and the air mass trajectories. NMHC and CO mixing ratios were well correlated indicating that these compounds originated from similar mostly anthropogenic sources. An exception was isoprene which showed no correlation with CO. With values below 100 ppt the mixing ratio of isoprene, which is emitted by terrestrial vegetation, was also unexpectedly low during the first half of the campaign although the maximum temperatures were around 35°C.  相似文献   

2.
The atmospheric concentration of peroxyacetylnitrate (PAN) was measured during a cruise of the R.S. Polarstern from Bremerhaven (Germany) to Rio Grande do Sul (Brazil) in September/ October 1988. The measurements were made in-situ by a combination of electron capture gaschromatography with a cryogenic preconcentration step. The theoretical lower limit of detection (3) was 0.4 ppt. The mixing ratios of PAN varied by more than three orders of magnitude from 2000 ppt in the English Channel to less than 0.4 ppt south of the Azores (38° N). South of 35° N, PAN levels were below the detection limit, except at 30–31° S off the eastern coast of South America. Here, PAN mixing ratios of 10 to 100 ppt were detected in continentally influenced air masses. Detectable levels of PAN were mostly observed in air masses of continental or high northern origin. Changes in the wind directions were usually associated with substantial changes in the PAN mixing ratios.  相似文献   

3.
During three of the flights with the NOAA P3 Orion over the Arctic icecap in April 1986, the atmospheric concentration of PAN (peroxyacetyl nitrate) was measured. Due to major experimental problems, the uncertainty in the data is large (+/–50%), but, nevertheless, some important trends can be resolved. More than 600 (+/–300) ppt(v) of PAN was present in a moderately dense arctic haze layer, confirming conclusions reached from surface observations at Alert, N.W.T., Canada, that PAN is a major odd nitrogen species in Arctic polluted air masses. In relatively clean air off Barrow, Alaska, PAN levels were well below 100 (+/–50) ppt(v), increasing with altitude, in agreement with theoretical predictions concerning the occurrence of PAN in clean air. PAN mixing ratios in the upper troposphere or lower stratosphere were variable (from ca. 30 (+/–15) ppt(v) on April 13 up to 140 (+/–70) ppt(v) on April 8), suggesting involvement in the tropospheric-stratospheric exchange of odd nitrogen. To place the PAN data in a broader context, measurements of other NOy compounds as well as integrated SOx data are also reported.  相似文献   

4.
Ambient mixing ratios of NO, NO2, and O3 were determined together with the photolysis frequency of NO2, JNO2, at a rural, agricultural site in Germany. The data were collected during the POPCORN-campaign from August 1 to August 24, 1994, in a maize field 6 m above ground. The medians of the NO, NO2, and O3 mixing ratios between 10:00 and 14:00 UT were 0.25, 1.09, and 45 ppbv, respectively. The corresponding median of JNO2 was 6.0 · 10–3 s–1. NOx = NO + NO2 showed a strong diurnal variation with maximum mixing ratios at night, suggestive of a strong local surface source of NO, probably by microbial activity in the soil. The estimated average emission rate was 40 ng(N) m–2 s–1 of NOx, the major part of it probably in the form of NO. The available measurements allowed the estimation of the local NOx budget. At night the budget is almost closed and the measured NOx mixing ratios can be explained by the local source, local dry deposition of NO2, formation of NO3 and N2O5, and vertical exchange of air across the nocturnal inversion. During day-time, the local surface source of NO is not sufficient to explain the measured mixing ratios, and horizontal advection of NOx to the site must be included. The NO2/NO ratio during the morning und late afternoon is lower than predicted from the photostationary state owing to the local NO surface source, but is regulary higher during the hours around noon. For noon, August 10, 1994, the NO2/NO ratio was used to derive the momentary lower limit for the concentration of the peroxy-radicals of 2.2 · 109 cm–3 (86 pptv).  相似文献   

5.
Continuous in-situ measurements of surface ozone (O3), carbon monoxide (CO) and oxides of nitrogen (NOx) were conducted at Udaipur city in India during April 2010 to March 2011. We have analyzed the data to investigate both diurnal and seasonal variations in the mixing ratios of trace gases. The diurnal distribution of O3 showed highest values in the afternoon hours and lower values from evening till early morning. The mixing ratios of CO and NOx showed a sharp peak in the morning hours but lowest in the afternoon hours. The daily mean data of O3, CO and NOx varied in the ranges of 5–51 ppbv, 145–795 ppbv and 3–25 ppbv, respectively. The mixing ratios of O3 were highest of 28 ppbv and lowest 19 ppbv during the pre-monsoon and monsoon seasons, respectively. While the mixing ratios of both CO and NOx showed highest and lowest values during the winter and monsoon seasons, respectively. The diurnal pattern of O3 is mainly controlled by the variations in photochemistry and planetary boundary layer (PBL) depth. On the other hand, the seasonality of O3, CO and NOx were governed by the long-range transport associated mainly with the summer and winter monsoon circulations over the Indian subcontinent. The back trajectory data indicate that the seasonal variations in trace gases were caused mainly by the shift in long-range transport pattern. In monsoon season, flow of marine air and negligible presence of biomass burning in India resulted in lowest O3, CO and NOx values. The mixing ratios of CO and NOx show tight correlations during winter and pre-monsoon seasons, while poor correlation in the monsoon season. The emission ratio of ?CO/?NOx showed large seasonal variability but values were lower than those measured over the Indo Gangetic Plains (IGP). The mixing ratios of CO and NOx decreased with the increase in wind speed, while O3 tended to increase with the wind speed. Effects of other meteorological parameters in the distributions of trace gases were also noticed.  相似文献   

6.
Results of field measurements carried out from June 15 to December 31, 1995, in Córdoba city (Argentina) are presented. During this field campaign, surface ozone mixing ratios were generally around 30–35 ppb (afternoon peak). However, during the first week of September, days with excessive ozone values close to 100 ppb were found. These elevated ozone concentrations appeared together with high values of NOx, CO, PM10, and an unusual meteorological situation for this time of the year. These results made this episode an interesting one to be studied in more detail. In this work, we used chemical and meteorological data to trace the region from where the assumed precursors were emitted and we identified possible source characteristics.  相似文献   

7.
This study examines the processes controlling the diurnal variability of ozone (O3) in the marine boundary layer of the Kwajalein Atoll, Republic of the Marshall Islands (latitude 8° 43′ N, longitude 167° 44′ E), during July to September 1999. At the study site, situated in the equatorial Pacific Ocean, O3 mixing ratios remained low, with an overall average of 9–10 parts per billion on a volume basis (ppbv) and a standard deviation of 2.5 ppbv. In the absence of convective storms, daily O3 mixing ratios decreased after sunrise and reached minimum during the afternoon in response to photochemical reactions. The peak-to-peak amplitude of O3 diurnal variation was approximately 1–3 ppbv. During the daytime, O3 photolysis, hydroperoxyl radicals, hydroxyl radicals, and bromine atoms contributed to the destruction of O3, which explained the observed minimum O3 levels observed in the afternoon. The entrainment of O3-richer air from the free troposphere to the local marine boundary layer provided a recovery mechanism of surface O3 mixing ratio with a transport rate of 0.04 to 0.2 ppbv per hour during nighttime. In the presence of convection, downward transport of O3-richer tropospheric air increased surface O3 mixing ratios by 3–12 ppbv. The magnitude of O3 increase due to moist convection was lower than that observed over the continent (as high as 20–30 ppbv). Differences were ascribed to the higher O3 levels in the continental troposphere and weaker convection over the ocean. Present results suggest that moist convection plays a role in surface-level O3 dynamics in the tropical marine boundary layer.  相似文献   

8.
During spring the atmospheric concentration of Peroxyacetyl Nitrate, PAN, in the UK varies over three orders of magnitude due to long range transport and local photochemical production. An experiment at Great Dun Fell was used to determine which of these sources of PAN controlled spring time concentrations and to quantify the contribution of PAN to oxidised nitrogen in cloud water. The gas phase mixing ratio of a wide range of trace gas pollutants, including PAN, along with cloud water chemical composition and aerosol/cloud droplet distributions were measured. A chemical model was developed to determine the contribution of PAN hydrolysis to cloud water nitrification and to quantify the sink strengths of PAN. Chemical reaction following thermal decomposition was found to be the dominant sink mechanism in the model but transport was the most important factor controlling PAN concentration. During cloud episodes PAN concentrations varied from 100 ppt to over 1 ppb but the calculated inorganic oxidised nitrogen loading in the cloud due to PAN dissolution and hydrolysis was an insignificant fraction of the observed total oxidised nitrogen loading of the cloud. Extrapolation of the model to persistent cloud in marine conditions showed that PAN has a negligible effect on cloud nitrification. It was concluded that PAN concentrations were heavily influenced by regional concentrations and that the hydrolysis of PAN in cloud water was an insignificant source of oxidised nitrogen in cloud water.  相似文献   

9.
Mountaintop trace-gas mixing ratios are often assumed to represent free atmospheric values, but are affected by valley planetary boundary-layer (PBL) air at certain times. We hypothesize that the afternoon valley–PBL height relative to the ridgetop is important in the diurnal cycle of mountaintop trace-gas mixing ratios. To investigate this, we use, (1) 4-years (1 January 2009–31 December 2012) of CO and \(\hbox {CO}_{2}\) mixing-ratio measurements and supporting meteorological observations from Pinnacles (\(38.61^{\circ }\hbox {N}\), \(78.35^{\circ }\hbox {W}\), 1017 m a.s.l.), which is a monitoring site in the Appalachian Mountains, (2) regional \(\hbox {O}_{3}\) mixing-ratio measurements, and (3) PBL heights determined from a nearby sounding station. Results reveal that the amplitudes of the diurnal cycles of CO and \(\hbox {CO}_{2}\) mixing ratios vary as a function of the daytime maximum valley–PBL height relative to the ridgetop. The mean diurnal cycle for the subset of days when the afternoon valley–PBL height is at least 400 m below the ridgetop shows a daytime CO mixing-ratio increase, implying the transport of PBL air from the valley to the mountaintop. During the daytime, on days when the PBL heights exceed the mountaintop, PBL dilution and entrainment cause CO mixing ratios to decrease. This decrease in CO mixing ratio, especially on days when PBL heights are at least 400 m above the ridgetop, suggests that measurements from these days can be used as with afternoon measurements from flat terrain in applications requiring regionally-representative measurements.  相似文献   

10.
Chemical amplification, CA, a method commonly used for the detection of peroxy radicals, HO2 and RO2, was found to be sensitive towards ClOx (Cl+ClO+OClO) as well. ClOx is reduced by NO to Cl atoms which react with carbon monoxide in the presence of O2. The reaction sequence thus initiated oxidizes CO to CO2 and NO to NO2, with a chain length of 300 ± 60. This allows the atmospheric ClOx content to be measured under ambient conditions with a detection limit of better than 1 ppt. In parallel peroxy radicals are indicated with a chain length of 160 ± 15. Chemical amplification is not specific and does not indicate which radical chain it is seeing. Identification relies solely on plausibility. During the ARCtic Tropospheric Ozone Chemistry (ARCTOC) campaign in spring 1995 and 1996 the CA technique was used at Ny-Ålesund. ClOx at mixing ratios of up to 2 ppt were found in the boundary layer under certain conditions. The low concentrations of ClOx indicate that the arctic boundary ozone depletion is mainly driven by bromine.  相似文献   

11.
Concentrations of peroxy radicals were measured by a chemical amplification technique at a remote forested site as part of the Program for Research on Oxidants in a Forested Region in Nikko (PROFRN). During the measurement period of 22–27 July 2002, the mixing ratios of peroxy radicals averaged for 3 min at midday ranged from 109 to 134 pptv at a height approximately 5 m above the forest canopy. Significant diurnal variation in concentrations of peroxy radicals was observed, with the maximum usually occurring around noon. Most of the variation was driven by changes in the intensity of solar radiation. However, it was found that the peroxy radical concentration reached its peak about 3-h later than that of solar radiation on 24 and 26 July. The origins of this delay are discussed based on an analysis of the total radical budget in that period. A transport of polluted air masses to the site was one of possible causes for the inconsistency. In addition, the measured peroxy radical concentrations were compared with those derived from the deviations of NO-NO2-O3 photo-stationary state (PSSD) for clear days. The estimated half-hour-average concentrations of peroxy radical were in agreement with the PERCA measured in the morning and late afternoon. However the two techniques differed by as much as a factor of two during the time of near midday.  相似文献   

12.
Atmospheric hydroxyl (OH), hydroperoxy (HO2), total peroxy (HO2 and organic peroxy radicals, RO2) mixing ratios and OH reactivity (first order OH loss rate) were measured at a rural site in central Pennsylvania during May and June 2002. OH and HO2 mixing ratios were measured with laser induced fluorescence (LIF); HO2 + RO2 mixing ratios were measured with chemical ionization mass spectrometry (CIMS). The daytime maximum mixing ratios were up to 0.6 parts per trillion by volume (pptv) for OH, 30 pptv for HO2, and 45 pptv for HO2 + RO2. A parameterized RACM (Regional Atmospheric Chemistry Mechanism) box model was used to predict steady state OH, HO2 and HO2 + RO2 concentrations by constraining the model to the measured OH reactivity and previously measured volatile organic compound (VOC) distributions. The averaged model calculations are generally in good agreement with the observations. For OH, the model matched the observations for day and night, with an average observed-to-modeled ratio of 0.80. In previous studies such as PROPHET98, nighttime NO was near 0 pptv and observed nighttime OH was significantly larger than modeled OH. In this study, nighttime observed and modeled OH agree to within measurement and model uncertainties because the main source of the nighttime OH was the reaction HO2 + NO → OH + NO2, with the NO being continually emitted from the surrounding fertilized corn field. The observed-to-modeled ratio for HO2 is 1.0 on average, although daytime HO2 is underpredicted by a factor of 1.2 and nighttime HO2 is over-predicted by a factor of ∼2. The average measured and modeled HO2 + RO2 agree well during daytime, but the modeled value is about twice the measured value during nighttime. While measured HO2 + RO2 values agree with modeled values for NO mixing ratios less than a few parts per billion by volume (ppbv), it increases substantially above the expected value for NO greater than a few ppbv. This observation of the higher-than-expected HO2 + RO2 with the CIMS technique confirms the observed increase of HO2 above expected values at higher NO mixing ratios in HO2 measurements with the LIF technique. The maximum instantaneous O3 production rate calculated from HO2 and RO2 reactions with NO was as high as 10–15 ppb h−1 at midday; the total daily O3 production varied from 13 to 113 ppbv d−1 and was 48 ppbv d−1 on average during this campaign.  相似文献   

13.
The intensive field study POPCORN (Photo-Oxidant Formation by Plant Emitted Compounds and OH Radicals in North-Eastern Germany) was carried out in a rural area of North-Eastern Germany during August 1994. An overview of the objectives, measurements and major results of this campaign is presented. Measurements of a set of relevant atmospheric trace compounds, including the hydroxyl radical, along with meteorological data were performed to increase the understanding of OH radical chemistry and photo-oxidant formation. Additionally, plant emissions and the exchange of trace gases between a maize field and the atmosphere were investigated. Budgets of selected trace gases were calculated to assess the relative importance of local sources, chemistry or transport. Intercomparisons between measurement techniques were a central issue of POPCORN and included measurements of OH, hydrocarbons, formaldehyde, photolysis frequencies and vertical fluxes. OH radical concentrations were measured simultaneously by LIF (Laser Induced Fluorescence) and DOAS (Differential Optical Absorption Spectroscopy). Both methods showed good agreement. Maximum OH concentrations were around 107 cm–3 and the diurnal cycles closely followed the rate of primary production via ozone photolysis. Generally, the trace gas composition during POPCORN was characterized by relatively low concentrations of most compounds, e.g. CO: 85–200 ppb, ethane: 0.6–2 ppb, and moderate NOx levels: 0.5–5 ppb (at noontime). Concentrations of individual biogenic volatile organic compounds (VOC) were mostly well below 100 ppt. However, formaldehyde and acetaldehyde which partly originate from biological sources were observed at mixing ratios of some ppb.  相似文献   

14.
Gas-phase H2O2, organic peroxides and carbonyl compoundswere determined at various sites from Mid-July to early August 1998 during the BERLIOZ campaign in Germany. The sites were located northwest of Berlin and were chosen to determine pollutants downwind of the city emissions during a summer smog episode. Hydrogen peroxide (H2O2),methyl hydroperoxide (MHP, CH3OOH) and occasionally hydroxymethyl hydroperoxide (HMHP, HOCH2OOH) were quantified in air samples by commercial fluorimetric methods and classical HPLC with post-column derivatisation by horseradish peroxidase/p-hydroxyphenyl acetic acid and fluorimetric detection. Carbonyl compounds were determined in ambient air by a novel method based onO-pentafluorobenzyl hydroxylamine as derivatisation agent.Mixing ratio profiles of the hydroperoxides and the carbonyl compounds are reported for the intensive phase of the campaign, 20–21 July, 1998. Peroxides showed pronounced diurnal variations with peak mixing ratios in the early afternoon. At times, a second maximum was observed in the late afternoon. The major part of the H2O2 was formed throughrecombination reactions of HO2 radicals, but there is some evidencethat H2O2 is also formed from ozonolysis ofanthropogenic and/or biogenic alkenes. Diurnal variations of mixing ratios of various carbonyl compounds are reported: alkanals (C2 to C10,isobutanal), unsaturated carbonyl compounds (methacrolein, methylvinylketone, acrolein), hydroxycarbonyl (glycolaldehyde, hydroxyacetone) and dicarbonyl compounds (glyoxal, methylglyoxal, biacetyl), aromatic compounds (benzaldehyde, o- and m-tolylaldehyde) and pinonaldehyde.  相似文献   

15.
The room-temperature photodecomposition of acetone diluted with synthetic air was studied at nine wavelengths in the spectral region 250–330 nm. The quantum yields for the products CO2 and CO indicated that it was not possible to suppress secondary reactions sufficiently, even with acetone/air mixing ratios as low as 150 ppmv, to derive from these data primary acetone photodissociation quantum yields. The behavior of CO2 and CO formation nevertheless provides some insight into the mechanism of acetone photodecomposition. When small amounts of NO2 are added to acetone/air mixtures, peroxyacetyl nitrate (PAN) is formed. Quantum yields for PAN are reported. They are better suited to represent primary quantum yields for acetone photodissociation, because PAN is a direct indicator for the formation of acetyl radicals. The data were combined with absorption cross-sections for acetone measured at wavelengths up to 360 nm to calculate photodissociation coefficients applicable to the ground-level atmosphere at 40° northern latitude. Comparison with the rates for the reaction of acetone with OH radicals shows that both processes contribute almost equally to the total acetone losses in the lower atmosphere. The resulting atmospheric life time at 40° northern latitude is 32 days, on average. This value must be considered an upper limit, since it does not take into account acetone losses due to the reaction of excited triplet acetone with oxygen.  相似文献   

16.
The 2.4-dinitrophenylhydrazine coated silica cartridge technique (DSC) was used for the measurements of HCHO and CH3CHO during the POPCORN campaign in August 1994. A total number of 505 measurements was carried out using an automatic sampling system. The sampling time for each measurement was 30 minutes. During the first two weeks of the campaign samples were taken every 3 hours and during the last two weeks every 30 minutes. No significant diurnal variation of HCHO and CH3CHO was observed. The average mixing ratios of HCHO and CH3CHO were 1.8 ±1.0 ppb and 1.4 ±1.3 ppb. The results for HCHO are in a good agreement with simultaneous measurements by differential optical absorption spectroscopy (DOAS). The absence of a strong diurnal variation of the HCHO mixing ratio can be explained by production and destruction processes during day and night. The measured mixing ratios of HCHO and CH3CHO, especially the mixing ratios during night, are a strong indication that during the POPCORN campaign the maize was a local source of HCHO and CH3CHO.  相似文献   

17.
Characteristics of carbonyl compounds in ambient air of Shanghai,China   总被引：3，自引：0，他引：3  
The levels of carbonyl compounds in Shanghai ambient air were measured in five periods from January 2007 to October 2007 (covering winter, high-air-pollution days, spring, summer and autumn). A total of 114 samples were collected and eighteen carbonyls were identified. Formaldehyde, acetaldehyde and acetone were the most abundant carbonyls and their mean concentrations of 19.40 ± 12.00, 15.92 ± 12.07 and 11.86 ± 7.04 μg m−3 respectively, in the daytime for five sampling periods. Formaldehyde and acetaldehyde showed similar diurnal profiles with peak mixing ratios in the morning and early afternoon during the daytime. Their mean concentrations were highest in summer and lowest in winter. Acetone showed reversed seasonal variation. The high molecular weight (HMW, ≥C5) carbonyls also showed obvious diurnal variations with higher concentrations in the daytime in summer and autumn, while they were all not detected in winter. Formaldehyde and acetaldehyde played an important role in removing OH radicals in the atmosphere, but the contribution of acetone was below 1%. The carbonyls levels in high-air-pollution days were reported. More carbonyl species with higher concentrations were found in high-air-pollution days than in spring. These carbonyls were transported with other pollutants from north and northwest in March 27 to April 2, 2007 and then mixed with local sources. Comparing with Beijing and Guangzhou, the concentrations of formaldehyde and acetaldehyde in Shanghai were the highest, which indicated that the air pollution in Shanghai was even worse than expected.  相似文献   

18.
The mixing ratios for ozone and NOx (NO+NO2) have been measured at a rural site in the United States. From the seasonal and diurnal trends in the ozone mixing ratio over a wide range of NOx levels, we have drawn certain conclusions concerning the ozone level expected at this site in the absence of local photochemical production of ozone associated with NOx from anthropogenic sources. In the summer (June 1 to September 1), the daily photochemical production of ozone is found to increase in a linear fashion with increasing NOx mixing ratio. For NOx mixing ratios less than 1 part per billion by volume (ppbv), the daily increase is found to be (17±3) [NOx]. In contrast, the winter data (December 1 to March 1) indicate no significant increase in the afternoon ozone level, suggesting that the photochemical production of ozone during the day in winter approximately balances the chemical titration of ozone by NO and other pollutants in the air. The extrapolated intercept corresponding to [NOx]=0 taken from the summer afternoon data is 13% less than that observed from the summer morning data, suggesting a daytime removal mechanism for O3 in summer that is attributed to the effects of both chemistry and surface deposition. No significant difference is observed in the intercepts inferred from the morning and afternoon data taken during the winter.The results contained herein are used to deduce the background ozone level at the measurement site as a function of season. This background is equated with the natural ozone background during winter. However, the summer data suggest that the background ozone level at our site is elevated relative to expected natural ozone levels during the summer even at low NOx levels. Finally, the monthly daytime ozone mixing ratios are reported for 0[NOx]0.2 ppbv, 0.3 ppbv[NOx]0.7 ppbv and 1 ppbv[NOx]. These monthly ozone averages reflect the seasonal ozone dependence on the NOx level.  相似文献   

19.
Ozone Concentrations in Rural Regions of the Yangtze Delta in China   总被引：4，自引：0，他引：4  
Elevated concentrations of ozone have been observed at six non-urban, surface monitoring sites in the Yangtze Delta of China during a 16-month field experiment carried out in 1999 and 2000 as part of the joint Chinese-American China-MAP Project (the Yangtze Delta of china as an Evolving Metro-Agro-Plex). The average daytime (0900–1600 h) ozone levels for the monitoring period at sites ranged from 35 to 47 ppbv (parts per billion by volume) and the mean ozone levels from 26 to 35 ppbv. Observed data show seasonal variation obviously, with highest mixing ratios of ozone in May. Average daytime ozone levels in May at sites were between 60 and 79 ppbv. High ozone concentrations were most prevalent during the late spring. Frequency counts of hourly mean ozone concentration over 60 ppbv and 40 ppbv appeared peak values of 22–39% and 42–74% in May at sites. Even higher daytime ozone levels were observed during two regional episodes, in which average daytime (0900–1600 h) ozone concentrations during 10 May and 23 May 2000 were 68 to 81 ppbv, during Oct. 18 and Oct. 28, 1999 were 59 to 67 ppbv at sites. Peak value of ozone mixing ratio appearing in late spring, instead of in summer, was attributed to summer monsoon. Backward trajectories showed that ozone episodes associated with meteorological conditions. Also many high ozone levels associated with high CO levels and high CO to NO x ratios, which suggests a contribution from sources of emission involving incomplete combustion.  相似文献   

20.
We measured the surface energy budget of an Alpine grassland in highly complex terrain to explore possibilities and limitations for application of the eddy-covariance technique, also for CO2 flux measurements, at such non-ideal locations. This paper focuses on the influence of complex terrain on the turbulent energy measurements of a characteristic high Alpine grassland on Crap Alv (Alp Weissenstein) in the Swiss Alps during the growing season 2006. Measurements were carried out on a topographic terrace with a slope of 25◦ inclination. Flux data quality is assessed via the closure of the energy budget and the quality flag method used within the CarboEurope project. During 93% of the time the wind direction was along the main valley axis (43% upvalley and 50% downvalley directions). During the transition times of the typical twice daily wind direction changes in a mountain valley the fraction of high and good quality flux data reached a minimum of ≈50%, whereas during the early afternoon ≈70% of all records yielded good to highest quality (CarboEurope flags 0 and 1). The overall energy budget closure was 74 ± 2%. An angular correction for the shortwave energy input to the slope improved the energy budget closure slightly to 82 ± 2% for afternoon conditions. In the daily total, the measured turbulent energy fluxes are only underestimated by around 8% of net radiation. In summary, our results suggest that it is possible to yield realistic energy flux measurements under such conditions. We thus argue that the Crap Alv site and similar topographically complex locations with short-statured vegetation should be well suited also for CO2 flux measurements.  相似文献   

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