首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到20条相似文献，搜索用时 31 毫秒
1.
Vertical distributions of dimethylsulfide (DMS), sulfur dioxide (SO2), aerosol methane-sulfonate (MSA), non-sea-salt sulfate (nss-SO4 2-), and other aerosol ions were measured in maritime air west of Tasmania (Australia) during December 1986. A few cloudwater and rainwater samples were also collected and analyzed for major anions and cations. DMS concentrations in the mixed layer (ML) were typically between 15–60 ppt (parts per trillion, 10–12; 24 ppt=1 nmol m–3 (20°C, 1013 hPa)) and decreased in the free troposphere (FT) to about <1–2.4 ppt at 3 km. One profile study showed elevated DMS concentrations at cloud level consistent with turbulent transport (cloud pumping) of air below convective cloud cells. In another case, a diel variation of DMS was observed in the ML. Our data suggest that meteorological rather than photochemical processes were responsible for this behavior. Based on model calculations we estimate a DMS lifetime in the ML of 0.9 days and a DMS sea-to-air flux of 2–3 mol m–2 d–1. These estimates pertain to early austral summer conditions and southern mid-ocean latitudes. Typical MSA concentrations were 11 ppt in the ML and 4.7–6.8 ppt in the FT. Sulfur-dioxide values were almost constant in the ML and the lower FT within a range of 4–22 ppt between individual flight days. A strong increase of the SO2 concentration in the middle FT (5.3 km) was observed. We estimate the residence time of SO2 in the ML to be about 1 day. Aqueous-phase oxidation in clouds is probably the major removal process for SO2. The corresponding removal rate is estimated to be a factor of 3 larger than the rate of homogeneous oxidation of SO2 by OH. Model calculations suggest that roughly two-thirds of DMS in the ML are converted to SO2 and one-third to MSA. On the other hand, MSA/nss-SO4 2- mole ratios were significantly higher compared to values previously reported for other ocean areas suggesting a relatively higher production of MSA from DMS oxidation over the Southern Ocean. Nss-SO4 2- profiles were mostly parallel to those of MSA, except when air was advected partially from continental areas (Africa, Australia). In contrast to SO2, nss-SO4 2- values decreased significantly in the middle FT. NH4 +/nss-SO4 2- mole ratios indicate that most non-sea-salt sulfate particles in the ML were neutralized by ammonium.  相似文献   

2.
There are large uncertainties in identifying and quantifying the natural and anthropogenic sources of chloromethanes – methyl chloride (CH3Cl), chloroform (CHCl3) and dichloromethane (CH2Cl2), which are responsible for about 15% of the total chlorine in the stratosphere. We report two years of in situ observations of these species from the AGAGE (Advanced Global Atmospheric Gas Experiment) program at Cape Grim, Tasmania (41° S, 145° E). The average background levels of CH3Cl, CHCl3 and CH2Cl2 during 1998–2000 were 551± 8, 6.3± 0.2 and 8.9± 0.2 ppt (dry air mole fractions expressed in parts per 1012) respectively, with a two-year average amplitude of the seasonal cycles in background air of 25, 1.1 and 1.5 ppt respectively. The CH3Cl and CHCl3 records at Cape Grim show clear episodes of elevated mixing ratios up to 1300 ppt and 55 ppt respectively, which are highly correlated, suggesting common source(s). Trajectory analyses show that the sources of CH3Cl and CHCl3 that are responsible for these elevated observations are located in coastal-terrestrial and/or coastal-seawater regions in Tasmania and the south-eastern Australian mainland. Elevated levels of CH2Cl2 (up to 70 ppt above background) are associated mainly with emissions from the Melbourne/Port Phillip region, a large urban/industrial complex (population 3.5 million) 300 km north of Cape Grim.Now at the Centre for Atmospheric ChemistryNow at School of Environmental Sciences  相似文献   

3.
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   

4.
During the winters of 1981 and 1982, measurements were taken on two Japanese islands of the aerosol and gaseous species which had been carried by northwesterly monsoons over the Pacific Ocean. The aerosols were characterized as sea-salt particles; soil particles, and as particles of sulfate, nitrate, organics and elemental carbon. At Chichi-jima island, which is about 800 km away from the main islands of Japan, it was found that the level of the anthropogenic components of the aerosols was considerably higher than their background level. The mean concentrations of the species on the islands are given in tabular forms. According to a survey made on board a ferry boat, the aerosol and gaseous species were fairly uniformly distributed along the southern coast of the main Japanese islands.  相似文献   

5.
A new gas chromatographic technique with a modified photoionization detector connected in series with a conventional flame ionization detector was used to determine low concentrations of atmospheric hydrocarbons in remote atmospheres. Average mixing ratios of five aromatic hydrocarbons measured between 42°N and 30°S latitude in the Pacific Ocean in October/November 1983 were highest in the Northern Hemisphere. The average mixing ratios in the northern and southern marine atmospheres were 49±25 ppt (n=35) and 10±2 ppt (n=21) for benzene, 20±12 ppt (n=32) and 5.6±1.6 ppt (n=12) for toluene, 7.6±3.7 ppt (n=35) and 3.7±1.6 ppt (n=21) for ethylbenzene, 25±12 ppt (n=35) and 13±5 ppt (n=20) for the sum of m- and p-xylenes, and 14±6 ppt (n=35) and 6.6±3.0 ppt (n=21) for o-xylene, respectively. The first latitudinal gradients for these five aromatic compounds are reported. Benzene and toluene mixing ratios measured between July 1982 and October 1983 at a rural, mid-latitude continental site in eastern Washington state gave average values of 226±108 ppt and 133±84 ppt, respectively, with higher wintertime than summertime benzene levels. These continental samples gave calculated air mass ages averaging six days based on benzene-to-toluene ratios.  相似文献   

6.
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   

7.
During the cruise ANT VII/1 (September/October 1988) of the German research vessel Polarstern the latitudinal distributions of several nonmethane hydrocarbons were measured over the Atlantic between 45°N and 30°S by in-situ gas chromatography.On the average, the highest mixing ratios of ethane, propane, i- and n-butane, ethene and acetylene were observed in the Northern Hemisphere around 40° N and just north of the intertropical convergence zone, respectively. South of the equator, a bulge in the mixing ratios of ethane and acetylene was observed indicating aged biomass burning emissions. This observation coincided with enhanced tropospheric ozone found in this region at this season. On the average ethane and acetylene mixing ratios were around 500 and 100 ppt, respectively, whereas the levels of the other NMHC were in the range of some ppt up to 100 ppt.compared with the results of the cruise ANT V/5 (March/April, 1987), the ethane mixing ratios in September/October proved to be a factor of 3 lower in the Northern Hemisphere and a factor of 2 higher in the Southern Hemisphere, probably due to seasonal effects. Possible causes are the higher OH radical concentrations in summer, which result in a faster removal of ethane or stronger emission from biomass burning which also peaks in the dry season.The relative pattern of the hydrocarbons just north of the ITCZ was very similar for both measurement series. In this region, the NMHC were advected by long-range transport from the continent, whereas generally the ocean itself acts as a major NMHC source. This is supported by the results of a balance calculation between oceanic emissions and atmospheric removal rates.  相似文献   

8.
During the POPCORN campaign between 3 and 24 August 1994 we measured peroxyacetyl nitrate (PAN) in a rural area of Mecklenburg-Vorpommern (North-Eastern Germany) above a corn field. A total of about 5000 PAN measurements were carried out within the three weeks of the campaign. Measured PAN mixing ratios ranged from below the detection limit of 10 ppt up to an afternoon maximum of 1 ppb. The mean value of all data was 140 ppt. The daily mean PAN mixing ratios were typically in the range of 50 to 250 ppt, but during a clean air episode PAN mixing ratios of well below 40 ppt were observed. The characteristic relative diurnal variation of the PAN mixing ratios with a late night/early morning minimum and an afternoon maximum persisted during these episodes. The daily averages of the PAN mixing ratios showed clear episodic variations which coincided with the duration of typical synoptic episodes of two to six days duration. Based on the measurements of the various parameters determining the PAN formation and destruction rates, the local budget for PAN was calculated. During daytime the calculated net photochemical formation rate of PAN was nearly always significantly higher than the observed change of the PAN concentration. This demonstrates that substantial amounts of PAN (often in the range of several hundred ppt/h) were exported from the corn field. The resulting removal of NOx to some extent effects the budget of nitrogen oxides (NOx), but the export of odd oxygen radicals in the form of PAN during daytime often amounted up to 30–50% of the OH-radical formation by ozone photolysis. Thus the importance of PAN as reservoir and transport medium for odd oxygen radicals can be very substantial and may have a significant impact on the budget and distribution of odd oxygen radicals.  相似文献   

9.
Two airborne campaigns were carried out to measure the tropospheric concentrations and variability of CO2, CO and O3 over Siberia. In order to quantify the influence of remote and regional natural and anthropogenic sources, we analysed a total of 52 vertical profiles of these species collected in April and September 2006, every ∼200 km and up to 7 km altitude. CO2 and CO concentrations were high in April 2006 (respectively 385–390 ppm CO2 and 160–200 ppb CO) compared to background values. CO concentrations up to 220 ppb were recorded above 3.5 km over eastern Siberia, with enhancements in 500–1000 m thick layers. The presence of CO enriched air masses resulted from a quick frontal uplift of a polluted air mass exposed to northern China anthropogenic emissions and to fire emissions in northern Mongolia. A dominant Asian origin for CO above 4 km (71.0%) contrasted with a dominant European origin below this altitude (70.9%) was deduced both from a transport model analysis, and from the contrasted ΔCO/ΔCO2 ratio vertical distribution. In September 2006, a significant O3 depletion (∼–30 ppb) was repeatedly observed in the boundary layer, as diagnosed from virtual potential temperature profiles and CO2 gradients, compared to the free troposphere aloft, suggestive of a strong O3 deposition over Siberian forests.  相似文献   

10.
In situ AGAGE GC-MS measurements of methyl bromide (CH3Br) and methyl chloride (CH3Cl) at Mace Head, Ireland and Cape Grim, Tasmania (1998–2001) reveal a complex pattern of sources. At Mace Head both gases have well-defined seasonal cycles with similar average annual decreases of 3.0% yr−1 (CH3Br) and 2.6% yr−1 (CH3Cl), and mean northern hemisphere baseline mole fractions of 10.37 ± 0.05 ppt and 535.7 ± 2.2 ppt, respectively. We have used a Lagrangian dispersion model and local meteorological data to segregate the Mace Head observations into different source regions, and interpret the results in terms of the known sources and sinks of these two key halocarbons. At Cape Grim CH3Br and CH3Cl also show annual decreases in their baseline mixing ratios of 2.5% yr−1 and 1.5% yr−1, respectively. Mean baseline mole fractions were 7.94 ± 0.03 ppt (CH3Br) and 541.3 ± 1.1 ppt (CH3Cl). Although CH3Cl has astrong seasonal cycle there is no well-defined seasonal cycle in the Cape Grim CH3Br record. The fact that both gases are steadily decreasing in the atmosphere at both locations implies that a change has occurred which is affecting a common, major source of both gases (possibly biomass burning) and/or their major sink process (destruction by hydroxyl radical).  相似文献   

11.
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   

12.
The CloudSat satellite data from June 2006 to April 2011 are used to investigate the characteristics of cloud vertical profiles over East Asia(20°-50°N,80°-120°E),with particular emphasis on the profiles of precipitative clouds in comparison with those of nonprecipitative clouds,as well as the seasonal variations of these profiles.There are some obvious differences between the precipitative and nonprecipitative cloud profiles.Generally,precipitative clouds mainly locate below 8 km with radar reflectivity in the range of-20 to 15 dBZ and maximum values appearing within 2-4-km height,and the clouds usually reach the ground;while nonprecipitative clouds locate in the layers of 4-12 km with radar reflectivity between-28 and 0 dBZ and maximum values within 8-10-km height.There are also some differences among the liquid precipitative,solid precipitative,and possible drizzle precipitative cloud profiles.In precipitative clouds,radar reflectivity increases rapidly from 11 to 7 km in vertical,implying that condensation and collision-coalescence processes play a crucial role in the formation of large-size drops.The frequency distribution of temperature at-15℃ is consistent with the highest frequency of radar reflectivity in solid precipitative clouds,which suggests that the temperatures near-15℃ are conductive to deposition and accretion processes.The vertical profiles of liquid precipitative clouds show almost the same distributions in spring,summer,and autumn but with differences in winter at mainly lower levels.In contrast,the vertical profiles of solid precipitative clouds change from spring to winter with an alternate double and single high-frequency core,which is consistent with variations of the frequency distribution of temperature at-15℃.The vertical profiles of nonprecipitative clouds show a little change with season.The observations also show that the precipitation events over East Asia are mostly related to deep convective clouds and nimbostratus clouds.These results are expected to be useful for evaluation of weather and climate models and for improvement of microphysical parameterizations in numerical models.  相似文献   

13.
The three-dimensional variational data assimilation (3DVAR) technique in the advanced weather research and forecast model is used to study the impact of assimilating Moderate Resolution Spectroradiometer (MODIS) retrieved temperature and humidity profiles on the dynamic and thermodynamic features for three monsoon depressions over the Bay of Bengal, India. For better understanding of the role of various physical processes in the evolution of monsoon depression, a detailed diagnostic study is performed on all the three depression cases. Numerical experiments were conducted in a system of two-way nested domains with a horizontal resolution of 36 and 12 km, respectively. The assimilation of MODIS data did improve the mean sea level pressure patterns and spatial distribution of rainfall patterns in all the three monsoon depression cases studied. Higher values of equitable threat score and lower bias values are seen consistently for the entire rainfall threshold range and for all the three depression cases with 3DVAR assimilation of MODIS temperature and humidity profiles. The current operational regional models in India do not ingest the MODIS temperature and humidity profiles and hence the present study is particularly relevant to the operational forecasting community in India in their ongoing efforts to improve weather forecasting over India.  相似文献   

14.
Based on the Stratospheric Aerosol and Gas Experiment (SAGE) II and the Halogen Occultation Experiment (HALOE) ozone profiles and the Total Ozone Mapping Spectrometer (TOMS) total ozone data sets, an empirical model for estimating the vertical distribution of stratospheric ozone over China is proposed. By using this model, the vertical distribution of stratospheric (16–50 km) ozone can be estimated according to latitude, month and total ozone. Comparisons are made between the modeled ozone profiles and the ...  相似文献   

15.
Field observations of the influence of topography on steady, neutrally-stratified boundary-layer flow were carried out in February 1981 and March 1984 on Kettles Hill near Pincher Creek, Alberta, Canada. The primary measurements were of wind speed at 3,6, and 10 m levels at stations in linear arrays along and across the major axis of this gentle, 1 km long and 100 m high, elliptical hill. Wind profile measurements up to heights of 200 m were made with TALA kites and tethersondes on the hilltop and at a reference site located about 3.7 km west of the hilltop. In addition, AIRsondes were flown and tracked from the reference site to provide additional data. The field observations provided the basic data for a comparison with wind-tunnel and numerical model simulations of the same flow. The wind-tunnel investigation was carried out in the Atmospheric Environment Service Boundary-Layer Wind Tunnel while the numerical model used was MS3DJH. For horizontal profiles of normalized mean wind speed at given heights above the prototype terrain, model results agree reasonably well with the field data. The wind-tunnel predictions are slightly high in most cases. For vertical profiles of wind speed up to 200 m above the hilltop, the numerical and wind-tunnel values are higher than were observed. The sensitivity of the normalized wind speed at the hilltop to deviations from non-logarithmic upwind profiles is demonstrated with data from the March 1984 experiment. A comparison of prototype with numerical-model mean-wind-direction perturbations at the 10 m level shows reasonable agreement except near the summit of the hill.Contractor: 24 Heslop Drive, Toronto.  相似文献   

16.
Vertical profiles of stratospheric HO2 and NO2 concentrations were determined using matrix isolation and ESR. Up to 10 different samples per flight were collected in situ by a balloon borne cryosampler. Free radicals and trace constituents which are condensable at 68 K are trapped in a polycristalline H2O or D2O matrix. After collection, the samples are stored at a temperature below 83 K until they are analysed in the laboratory by X-band ESR spectroscopy at 4 K. The HO2 and NO2 were identified and calibrated by comparison with standard samples collected in the laboratory under typical stratospheric sampling conditions. From several flights over Southern France (44°N) we obtained two profiles of the stratospheric NO2 mixing ratio. One, from 21 October 1982, agrees well with previous measurements. The other, from 8 October 1981, is lower by one order of magnitude. The few HO2 data obtained around 35 km altitude agree with previous measurements. An isolated measurement at 17 km altitude is one order of magnitude higher than the model predicted HO2 concentration.  相似文献   

17.
  相似文献   

18.
Ozone mixing ratios observed by the Bordeaux microwave radiometer between 1995 and 2002 in an altitude range 25–75 km show diurnal variations in the mesosphere and seasonal variations in terms of annual and semi-annual oscillations (SAO) in the stratosphere and in the mesosphere. The observations with 10–15 km altitude resolution are presented and compared to photochemical and transport model results.Diurnal ozone variations are analyzed by averaging the years 1995–1997 for four representative months and six altitude levels. The photochemical models show a good agreement with the observations for altitudes higher than 50 km. Seasonal ozone variations mainly appear as an annual cycle in the middle and upper stratosphere and a semi-annual cycle in the mesosphere with amplitude and phase depending on altitude. Higher resolution (2 km) HALOE (halogen occultation experiment) ozone observations show a phase reversal of the SAO between 44 and 64 km. In HALOE data, a tendancy for an opposite water vapour cycle can be identified in the altitude range 40–60 km.Generally, the relative variations at all altitudes are well explained by the transport model (up to 54 km) and the photochemical models. Only a newly developed photochemical model (1-D) with improved time-dependent treatment of water vapour profiles and solar flux manages to reproduce fairly well the absolute values.  相似文献   

19.
The profiles of aerosol extinction coefficients are investigated by micro-pulse lidar(MPL)combined with the meteorological data in the lower troposphere at Meteorological ResearchInstitute(MRI).Japan.Larger extinction values of aerosol are demonstrated in the nocturnalstable air layer with larger Richardson number,and light wind velocities are favorable for aerosolconcentrating in the planetary boundary layer(PBL).But aerosol extinction coefficients showlarger values over the altitudes of 2.0 to 5.0km where correspond to higher relative humidity(RH).The tops of PBL identified by the aerosol extinction profiles almost agree with ones byradiosonde data.The diurnal variations of aerosol extinction profiles are clearly displayed,intensive aerosol layers usually are formed over the period of mid-morning to 1400 Loeal Time(LT).then elapse in the cloudless late afternoon and nighttime.Thermal eonvection or turbulenttransport from the surfaee probably dominates these temporal and spatial changes of aerosoldistribution.  相似文献   

20.
Measurements from July 4 to July 8, 2005 by a high resolution visible radiometer, a Raman lidar, a ground particulate matter sampler, and ground meteorological sensors have been combined in synergy to infer the intrusion over south-east Italy, of air masses from north-west Sahara, the Atlantic Ocean, and the continental Europe. It is shown that backscatter coefficient, depolarization-ratio, and lidar ratio vertical profiles represent the best tools to detect the intrusion of long range transported air masses and to monitor their effects on the vertical distribution of aerosol optical and microphysical properties. High resolution radiometers are instead important tools to monitor changes on columnar aerosol properties and size distributions.Backscatter coefficient, depolarization-ratio, and lidar ratio vertical profiles have revealed that aerosol optical and microphysical properties significantly changed with time and space during African dust outbreaks: the intrusion of dust particles that at first occurred above 2 km of altitude extending up to 6 km, affected the all aerosol load down to ground within few hours. Aerosol size distributions showed during dust events a clear bimodality with an accumulation mode maximum at 0.24 µm and a coarse mode maximum at 0.94 μm. Conversely, we have found that during the advection of air masses from the Atlantic and continental Europe, aerosol particles were mainly located below 2 km, their optical and microphysical properties were affected by smaller changes in time and space, and were characterized by depolarization ratios rather close to those due to a pure molecular atmosphere. In this case bimodal size distributions with an accumulation mode showing two sub-modes at 0.16 μm and 0.24 μm, respectively and a coarse mode centred at 0.94 μm have also been observed.  相似文献   

设为首页 | 免责声明 | 关于勤云 | 加入收藏

Copyright©北京勤云科技发展有限公司  京ICP备09084417号