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1.
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   

2.
Tropospheric distributions of ozone (O3) and water vapor (H2O) have been presented based on the Measurements of OZone and water vapor by Airbus In-Service AirCraft (MOZAIC) data over the metro and capital city of Delhi, India during 1996–2001. The vertical mixing ratios of both O3 and H2O show strong seasonal variations. The mixing ratios of O3 were often below 40 ppbv near the surface and higher values were observed in the free troposphere during the seasons of winter and spring. In the free troposphere, the high mixing ratio of O3 during the seasons of winter and spring are mainly due to the long-range transport of O3 and its precursors associated with the westerly-northwesterly circulation. In the lower and middle troposphere, the low mixing ratios of ∼20–30 ppbv observed during the months of July–September are mainly due to prevailing summer monsoon circulation over Indian subcontinent. The summer monsoon circulation, southwest (SW) wind flow, transports the O3-poor marine air from the Arabian Sea and Indian Ocean. The monthly averages of rainfall and mixing ratio of H2O show opposite seasonal cycles to that of O3 mixing ratio in the lower and middle troposphere. The change in the transport pattern also causes substantial seasonal variation in the mixing ratio of H2O of 3–27 g/kg in the lower troposphere over Delhi. Except for some small-scale anomalies, the similar annual patterns in the mixing ratios of O3 and H2O are repeated during the different years of 1996–2001. The case studies based on the profiles of O3, relative humidity (RH) and temperature show distinct features of vertical distribution over Delhi. The impacts of long range transport of air mass from Africa, the Middle East, Indian Ocean and intrusions of stratospheric O3 have also been demonstrated using the back trajectory model and remote sensing data for biomass burning and forest fire activities.  相似文献   

3.
A global three-dimensional chemical transport model has been used to identify and evaluate possible candidates for the `missing' surface source required to balance the atmospheric budget of methyl bromide. Both natural and anthropogenic emissions of methyl bromide are `coloured' in the model, thus allowing the global CH3Br distribution to be broken-down into its source components. These coloured CH3Br tracers are then combined in various ways to create one base-line emission scenario and five further plausible scenarios. The additional emission scenarios are specifically designed to test whether the geographical distribution and seasonal cycles of additional vegetation and/or increased biomass burning emissions are consistent with atmospheric observations of methyl bromide mixing ratios. Due to an imbalance in our current understanding of the methyl bromide budget, simulated CH3Br mixing ratios from the base-line emission scenario are significantly lower than atmospheric measurements. Both the inclusion of a vegetation source in the tropics and a double strength biomass burning source substantially improve the agreement between model simulations and atmospheric measurements compared with the base-line emission scenario. While measurement data provides useful information on global fluxes and regional CH3Br seasonal cycles, small differences between the simulated seasonal cycles of different emission scenarios makes it difficult to distinguish between the relative likelihoods of model scenarios containing a tropical vegetation source or an increased biomass burning source. Further measurements performed in continental mid-to-high northern latitudes, central-southern Africa and South America would be of particular benefit in future attempts to constrain the location and magnitude of the natural terrestrial sources of methyl bromide.  相似文献   

4.
利用星载微波临边遥感探测结果,对2006年6月28～29日江淮地区的一次强对流天气过程中对流层上部一氧化碳 (CO) 、臭氧 (O3) 、水汽 (H2O) 和冰水含量 (IWC) 的分布特点进行了研究.强对流天气过程前后的对比分析表明,CO混合比增大,在200 hPa处增加了0.12 ppm (1 ppm=10-6);O3混合比减小,在70 hPa处减少了0.30 ppm;H2O混合比在250 hPa处增加了400 ppm;IWC在强降水发生之前有大幅增长,在200 hPa处最大含量可达0.03 g/m3.CO和O3含量与垂直运动速度两者的相关变化表明,对流垂直输送作用可能是造成对流层上层和平流层低层大气成分变化的机制之一.而H2O和IWC含量的增加主要局限于对流层顶以下,这表明对流层上部水物质的质量和形态是由垂直输送作用和对流系统内部的微物理过程共同决定的.  相似文献   

5.
The vertical distribution of the CH3Cl mixing ratio in the stratosphere has been measured from samples collected during two balloon flights on the 21 October 1982 and 10 September 1983. Measurements were made with two analytical techniques that were also employed for previous analyses of stratospheric samples: gas chromatography (GC) and a gas chromatograph/mass spectrometer (GC/MS) combination. The results from all balloon flights performed to date are combined to derive an average experimental profile of CH3Cl at midlatitudes. The profile shows that the CH3Cl mixing ratio decreases by about one order of magnitude between 20 and 30 km altitude. A comparison of the new observations with model profiles reveals discrepancies in the lower stratosphere that amount to a factor of about 3. Possible causes for these discrepancies are discussed.  相似文献   

6.
Atmospheric mixing ratios of methyl iodide (CH3I) and other methyl halides have been measured at Cape Grim, Tasmania (41°S, 145°E), since early 1998 as part of the Advanced Global Atmospheric Gases Experiment (AGAGE). This paper analyses about 1700 ambient air CH3I measurements from the 14-month period (March 1998–April 1999). Mixing ratios peaked during the summer, despite faster photolytic loss, suggesting local oceanic emissions were about 2.2–3.6 times stronger in summer than in winter. Back trajectories show that CH3I levels are strongly dependent on air mass origin, with highest mixing ratios in air from the Tasman Sea/Bass Strait region and lowest levels in air originating from the Southern Ocean at higher latitudes. CH3I mixing ratios were not well correlated with other methyl halides in unpolluted marine air. The large variations with season and air mass origin suggest that high frequency, continuous data from key locations will make a significant contribution to the understanding of sources and sinks of this important short-lived atmospheric species.  相似文献   

7.
Formic and acetic acids were measured in a scrub-grass savanna and in a nearby semideciduous forest. Gaseous HCOOH and CH3COOH were collected using the mist-scrubber technique, and were determined using ion chromatography. A strong diurnal cycle was observed at both sites, with higher mixing ratios during daytime. Concentrations in the savanna were always higher than in the forest. Most of the time HCOOH/CH3COOH ratios greater than one were recorded at the savanna site, and ratios less than one at the forest site. Boundary-layer mixing ratios in the savanna region, derived from measurements during midday, are 1.3±0.4 ppbv and 0.7±0.3 ppbv for HCOOH and CH3COOH. Dry depositions velocities between 0.5 and 1 cm s-1 were estimated for the savanna region. Atmospheric residence times of <3 days and >5 days were estimated for the rainy and dry season, respectively.  相似文献   

8.
In 1978–1980 nine aircraft flights to an altitude of up to 15 km were made over western Europe. Sulfur dioxide was measured with a sensitive chemiluminescence method consisting of separate sampling and analysis stages and application of a wet chemical filter procedure (detection limit: 8 pptv SO2).The measurements performed in the upper troposphere and lower stratosphere lead to some unexpected results: (a) the meteorological conditions at the tropopause level have an important influence on the observed SO2 mixing ratio; (b) between the 500 mb and the actual tropopause level the SO2 mixing ratio is found to be <100 pptv, and weak vertical gradients of SO2 suggest only a small flux of tropospheric SO2 into the stratosphere; (c) increasing SO2 mixing ratios within the first kilometers of the stratosphere give strong support to a stratospheric source of SO2.In the light of improved one-dimensional models considering the vertical distribution of stratospheric sulfur compounds (Crutzen, 1981; Turco et al. 1981) it can be shown that the oxidation of organic sulfur compounds (e.g., OCS, CS2) seems to be a stratospheric source of SO2. Furthermore, the flux calculations based on the SO2 mixing ratios measured at the tropopause level indicate that the contribution of tropospheric (man-made) SO2 to the stratospheric aerosol layer is of only minor importance.  相似文献   

9.
Methane and carbon dioxide seasonal cycles during years 1998 and 1999 at two Brazilian urban and inland sites are presented. The mixing ratio averages over the studied period of time were 1.80 ppm CH4 and 384.7 ppm CO2. A comparison is made between continental averages and theaverages of the three nearest global network background sites of NOAA-CMDL comprising Ascension Island, Namibia and Easter Island. Inland sites had 0.08 ppm or 4.9% more CH4 and 19.0 ppm or 4.9% moreCO2 than background over the same time span. The CH4 summer minimum observed in remote sites was also detected inland. During the month of October 98 and 99 inland mixing ratios were frequently similar to background.  相似文献   

10.
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   

11.
Formaldehyde (HCHO), acetaldehyde (CH3CHO) and acetone (CH3COCH3) were measured at Wanqingsha (WQS) in south China during November-December 2008–2010. Carbonyl compound pollution characteristics under the influence of the financial crisis (FC) were studied. Atmospheric carbonyl compound concentrations in the 2008 and 2009 sampling periods were affected by the 2008 FC. The industrial downturn plus the high closing down number of the small enterprises with limited emission treatment during the FC played an important role in the reduction of the industry-related CH3CHO and CH3COCH3. In 2010, the recovery of industrial activities occurred, but affected by traffic restriction enforcement in Guangzhou over the Asian Games period, HCHO concentration (daytime 7.59?±?2.59 μg m?3) was lower than expectation. Carbonyl compounds in WQS site were highly influenced by regional pollution transport from different upwind urban cities and industrial districts in the north-northwest to northeast wind sector in winter. Also, the interaction of the winter monsoon with the warm ocean along the coastline as well as day and night boundary layer mixing height variation affected carbonyl compound concentrations in WQS. The daytime mean dry deposition losses of HCHO and CH3CHO were first time model-estimated for 2009 and 2010. For loss of HCHO in the early afternoon, photolysis was the dominant sink, followed by dry deposition and removal by OH radical (?OH), while for CH3CHO, dry deposition was dominant. For the gain of HCHO and CH3CHO, the production rates during early afternoon in 2009 and 2010 were estimated by an indirect approach.  相似文献   

12.
A network of remote and in-situ sensors was deployed in a Paris suburb in order to evaluate the mesoscale evolution of the daily cycle of CO2 and related tracers in the atmospheric boundary layer (ABL) and its relation to ABL dynamics and nearby natural and anthropogenic sources and sinks. A 2-μm heterodyne Doppler differential absorption lidar, which combines measurements of, (1) structure of the atmosphere, (2) radial velocity, and (3) CO2 differential absorption was a particularly unique element of the observational array. We analyse the differences in the diurnal cycle of CO, CO2, lidar reflectivity (a proxy for aerosol content) and H2O using the lidar, airborne measurements in the free troposphere and ground-based measurements made at two sites located few kilometres apart. We demonstrate that vertical mixing dominates the early morning drawdown of CO and aerosol content trapped in the former nocturnal layer but not the H2O and CO2 mixing ratio variations. Surface fluxes, vertical mixing and advection all contribute to the ABL CO2 mixing ratio decrease during the morning transition, with the relative importance depending on the rate and timing of ABL rise. We also show evidence that when the ABL is stable, small-scale (0.1-km vertical and 1-km horizontal) gradients of CO2 and CO are large. The results illustrate the complexity of inferring surface fluxes of CO2 from atmospheric budgets in the stable boundary layer.  相似文献   

13.
During 18–23 July 1990, 31 smoke samples were collected from an aircraft flying at low altitudes through the plumes of tropical savanna fires in the Northern Territory, Australia. The excess (above background) mixing ratios of 17 different trace gases including CO2, CO, CH4, several non-methane hydrocarbons (NMHC), CH3CHO, NO x (– NO + NO2), NH3, N2O, HCN and total unspeciated NMHC and sulphur were measured. Emissionratios relative to excess CO2 and CO, and emissionfactors relative to the fuel carbon, nitrogen or sulphur content are determined for each measured species. The emission ratios and factors determined here for carbon-based gases, NO x , and N2O are in good agreement with those reported from other biomass burning studies. The ammonia data represent the first such measurements from savanna fires, and indicate that NH3 emissions are more than half the strength of NO x emissions. The emissions of NO x , NH3, N2O and HCN together represent only 27% of the volatilised fuel N, and are primarily NO x (16%) and NH3 (9%). Similarly, only 56% of the volatilised fuel S is accounted for by our measurements of total unspeciated sulphur.  相似文献   

14.
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   

15.
Results of more than 800 new measurements of methane (CH4) concentrations in the Southern Hemisphere troposphere (34–41° S, 130–150° E) are reported. These were obtained between September 1980 and March 1983 from the surface at Cape Grim, Tasmania, through the middle (3.5–5.5 km) to the upper troposphere (7–10 km). The concentration of CH4 increased throughout the entire troposphere over the measurement period, adding further support to the view that CH4 concentrations are currently increasing on a global scale. For data averaged vertically through the troposphere the rate of increase found was 20 ppbv/yr or 1.3%/yr at December 1981. In the surface CH4 data a seasonal cycle with a peak to peak amplitude of approximately 28 ppbv is seen, with the minimum concentration occurring in March and the maximum in September–October. A cycle with the same phase as that seen at the surface, but with a significantly decreased amplitude, is apparent in the mid troposphere but no cycle is detected in the upper tropospheric data. The phase and amplitude of the cycle are qualitatively in agreement with the concept that the major sink for methane is oxidation by hydroxyl radicals. Also presented is evidence of a positive vertical gradient in methane, with a suggestion that the magnitude of this gradient has changed over the period of measurements.  相似文献   

16.
As part of the TROPOZ II large-scale measurement campaign in January 1991 we deployed a Four Laser Airborne Infra Red (FLAIR) tunable diode laser spectrometer on board a Caravelle 116 research aircraft. We report here in situ CO measurements which were obtained with one of the four channels of the FLAIR instrument at a time resolution of either one or two minutes. The flight route of the TROPOZ II campaign followed the Atlantic coasts of North America, the Pacific and Atlantic coasts of South America and the Atlantic coasts of West Africa and Europe. A total of 48 CO vertical profiles extending from the surface to 10.5 km altitude were obtained. In the meridional direction adjacent profiles were separated by less than 10° latitude. Polewards of 30°S the CO distribution was very homogeneous with a mean mixing ratio of 55 ppbv. Between 30°S and the equator, the CO mixing ratio above 8 km altitude ranged up to 130 ppbv and was 20–60 ppbv higher than in the mid free troposhere. Three day backward trajectories for these CO rich airmasses originated over Amazonia. Earlier trace gas measurements as well as circulation studies suggested that these airmasses were of Northern Hemispheric origin and had been rapidly convected to the upper troposphere over central South America. The influence of biomass burning is clearly apparent from the measurements performed at 10°N on the African side of the Atlantic with CO mixing ratios being 100–300% higher than on the Central American side. CO mixing ratios further north ranged from 80 to 130 ppbv in the free troposphere and increased to 130–150 ppbv at lower altitudes.  相似文献   

17.
The applicability of the tungsten oxide denuder tube technique for the measurement of ammonia in the rural troposphere was investigated. The technique is based on selective chemisorption of NH3 from a gas stream, thermal desorption, conversion to NO, and analysis by NO–O3 chemiluminescence. Nitric acid, which is also collected and desorbed as NO, was distinguished from NH3 by differences in desorption temperature. Substituted amines were also collected, but desorbed at a slightly lower temperature than NH3 in dry air. At high relative humidities, alkylamines may be hydrolyzed to NH3 on the denuder surface and hence detected as NH3. Overheating of the denuder tube during the temperature-programmed desorption was found to cause significant irreversible degradation of system performance.The technique was used to measure NH3 mixing ratios at two rural locations in the United States. At a mountain site in Colorado during the winter of 1984, the average NH3 mixing ratio was 0.20 ppbv (=0.08 ppbv). At an isolated coastal site in northern California during the spring of 1985, the average NH3 mixing ratio was 0.36 ppbv (=0.17 ppbv). Correlations of the latter measurements with wind direction and NO x level suggest that the NH3 mixing ratio in Pacific marine air at 40°N is <-0.25 ppbv.  相似文献   

18.
Carbon dioxide (CO2) has been measured at Alert by grab flask sampling since 1975 as part of the World Meteorological Organization's Background Air Pollution Monitoring Program. Deviations of CO2 concentration from the mean annual cycle have previously been attributed to air masses arriving at Alert from the source regions of the industrialized parts of Europe and the Soviet Union. In situ measurements of ambient CO2 and methane (CH4) were made at Alert using an automated gas chromatograph, as part of the Arctic Haze Study during April 1986. The temporal behaviour of CO2 and CH4 during this period was found to be highly correlated with measurements of particulate sulphate and other atmospheric trace species of anthropogenic origin. Examination of calculated air mass back-trajectories provided further evidence that the observed short-term increases in CO2 and CH4 mixing ratios were due to long-range transport from anthropogenic source regions.  相似文献   

19.
The simultaneous measurements of NO, NO2 and HNOA mixing‐ratio profiles carried out on the Stratoprobe balloon flight of 22 July 1974 have been simulated with a time‐dependent model using the measured temperature and ozone profiles. The calculated ratios of NO/NO2, HNO3/NO2 using currently accepted photochemistry are consistent with the measured ratios within the experimental errors of the measurements. The measured NO2/NO ratio is almost a factor of two smaller than predicted, although the discrepancy is still within the experimental errors. A remarkable proportionality in the NO2 and O3 profiles has been noted and is unexplained. A time‐dependent simulation has been employed to convert the measurements into diurnally‐averaged profiles suitable for intercomparison with two‐dimensional stratospheric models and a comparison with constituent profiles from Prinn et al. (1975) is carried out as an example. The NOV mixing ratio, formed from the sum of the NO, NO2 and HNO2 measurements is similar to the NOV mixing ratio from several one‐ and two‐dimensional models used to predict the effects of SST's on the ozone layer. The odd nitrogen mixing ratio is roughly constant from 20 to 35 km at 11 ppbv.  相似文献   

20.
利用瓦里关大气本底站甲烷观测数据对美国Aqua卫星的AIRS观测结果进行对比分析,并分析研究了2003~2012年青藏高原对流层大气甲烷的时空分布特征,结果表明:1)AIRS观测结果与近地面观测资料变化趋势一致,存在显著的正相关关系,突变时间比较一致,可以用于青藏高原区域的甲烷浓度特征分析。2)青藏高原对流层甲烷浓度在空间分布上存在显著的西北—东南走向的低值带及其南北侧存在4个固定的高值中心,分别位于阿里、那曲、山南和玉树。3)青藏高原甲烷浓度呈现显著随高度而降低的趋势,年平均甲烷浓度分别为1.810ppm(1 ppm=10-6)、1.797 ppm和1.781 ppm。在对流层中层和中上层,甲烷浓度基本呈现低值带最低、南北侧均高的山谷型分布特征。在对流层层顶,以低值带为分界线,呈现明显的南高北低特征。4)青藏高原甲烷浓度随时间呈缓慢上升趋势,平均速度为0.0018 ppm/a,夏季上升最快,秋季上升最慢。5)青藏高原甲烷存在明显的单峰型季节变化特征,夏秋季高,冬春季低,与东部地区冬、夏双峰型特征不同,随着高度上升季节变化更为明显。  相似文献   

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