Source terms and source strengths of the carbonaceous aerosol in the tropics

Atmospheric aerosol samples were collected in the Ivory Coast, primarily at Lamto (6°N, 5°W) between 1979 and 1981. The samples were analysed for total particulate carbon concentration and isotopic composition (¹³C/¹²C) by mass spectrometry. Observed concentrations were found high compared to values reported for temperate regions. Fine particulate carbon in the submicrometersize range accounted for 50 to 80% of the reported concentrations. At Lamto, both particulate carbon concentrations and isotopic ratios exhibit a large temporal variability which is shown to reflect the diversity of sources and their seasonal evolution. Natural emissions from the equatorial forest during the wet season, and biomass burning during the dry season, appear to be the major sources. The latter, though active during only a third of the year, is, on an annual basis, the most important source. Based on the data obtained at Lamto, an attempt has been made to estimate the flux of fine particulate carbon emitted from the tropical regions into the global troposphere. This flux, which is of the order of 20×10¹² g C/yr, appears to be equivalent to the flux of fine particulate carbon emitted from industrial sources. These results suggest that the tropospheric burden of fine particulate carbon in lowlatitude regions is dominated by the long-range transport of carbonaceous aerosols originating from the Tropics.     

Measurements of stratospheric HO2 and NO2 by matrix isolation and ESR spectroscopy

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.     

Organic matter of the troposphere — V: Application of molecular marker analysis to biogenic emissions into the troposphere for source reconciliations

Organic matter in tropospheric aerosols is derived from two major sources and is admixed depending on the geographic area. These sources are biogenic detritus and anthropogenic emissions. The biogenic materials in the solvent-extractable organic matter are comprised predominantly of higher plant waxes, with lesser amounts of resin and microbial detritus and the anthropogenic components are primarily vehicular emissions (e.g. oils, soot, etc.) and input from combustion (e.g. charcoal, thermally-altered biogenic matter, etc.). Both biogenic detritus and anthropogenic emissions contain organic compounds (C₁₂–C₄₀₊), which can be identified with unique and distinguishable distribution patterns. Molecular composition analysis has been applied to such extracts after suitable chemical separation into subfractions (i.e. hydrocarbons, ketones, aldehydes, carboxylic acids, alcohols, and wax esters). Both homologous compound series and specific natural products (e.g. phytosterols, terpenes, etc.) are identified as molecular markers.Aerosols from rural and remote areas in the western United States, South America, Nigeria and Australia have been analyzed and all contained predominantly plant waxes. The loadings of hydrocarbons ranged approximately from 10–1400 ng/m³ of air, of fatty acids from 10–450 ng/m³ and of fatty alcohols from 10–1650 ng/m³. These higher molecular weight lipids primarily from flora comprise a major component of the organic carbon in rural and remote aerosols. They are thus important indicators for regional biogenic sources in the global cycling of organic carbon.Presented in part at the International Symposium on Biosphere-Atmosphere Exchange, Mainz, E.R. Germany, March 16–22, 1986, for Part IV see Simoneit et al. (1988) Atmos. Environ. 22, 983–1004.     

Sulfate-coated dust particles in the free troposphere over Japan

Airborne aerosol collections were performed over Wakasa bay (36°00′N, 135°30′E) in March and Kumano open sea (34°00′N, 136°50′E) and Seto (35°10′N, 137°10′E) in July 2001 at altitudes between 1.0 and 5.8 km. The particles were individually analyzed using transmission electron microscopy (TEM). Relatively large mineral-dust (mostly clay) particles were abundant in the March samples. They also dominated in July in the mid-troposphere higher than 4 km altitude, whereas sea salt and ammonium sulfate were more abundant at lower altitudes. Ca-coated grid samples show many traces of aqueous sulfate droplets. The proportions of former sulfate droplets to the total collected particles apparently increased with increasing relative humidity at the time of sampling. TEM analysis revealed that a significant fraction of these former droplets enclose mineral-dust particles as well as sea salt, soot, and fly ash. Some enclose mixtures of mineral-dust, sea-salt, soot, and fly ash particles. The results provide evidence that mineral dust from the Asian continent could acquire coatings of sulfate while being transported in the free troposphere. The mineral-dust particles probably acquired the sulfate coatings either through heterogeneous uptake of gaseous SO₂ and subsequent oxidation or through coagulation with cloud or fog droplets. The presence of the mixed particles in sulfate droplets also indicates that aggregation of particles of different origins occurred through cloud processing. Such sulfate-coated dust particles would affect cloud formation, precipitation, and chemistry of the free troposphere.     

Tropospheric parameters: combination studies based on homogeneous VLBI and GPS data

The combination of tropospheric parameters derived from different space-geodetic techniques has not been of large interest in geodesy so far. However, due to the high correlation between station coordinates and tropospheric parameters, the latter should not be neglected in combinations. This paper deals with the comparison and combination of tropospheric parameters derived from global positioning system (GPS) and very long baseline interferometry (VLBI) observations stemming from a 15-day campaign of continuous VLBI observations in 2002 (CONT02). The observation data of both techniques were processed homogeneously to avoid systematic differences between the solutions. We compared the tropospheric estimates of GPS and VLBI at eight co-location sites and found a very good agreement in the temporal behavior of the tropospheric zenith path delays (ZPD), reflected by correlation factors up to 0.98. Following this, a combination of the tropospheric parameters was performed. We demonstrate that the combination of tropospheric parameters leads to a stabilization of combined station networks. This becomes visible in the improvement of the repeatabilities of the station height components. Furthermore, the potential use of independent data from water vapor radiometers (WVRs) to validate space-technique-derived tropospheric parameters was investigated. Correlation coefficients of 0.95 or better were estimated between the tropospheric parameters of WVR and GPS or VLBI. Additionally, the utility of the tropospheric parameters for validation of local tie vectors was investigated. Both tropospheric zenith delays and tropospheric gradients were found to be very suitable to validate the height component and the horizontal components of the local tie, respectively.     

Photochemical oxidation of dimethylsulfide in seawater

Dimethylsulfide(DMS) is generally thought to be lost from the surface oceans by evasion into the atmosphere as well as consumption by microbe.However,photochemical process might be important in the removal of DMS in the oceanic photic zone.A kinetic investigation into the photochemical oxidation of DMS in seawater was performed.The photo-oxidation rates of DMS were influenced by various factors including the medium,dissolved oxygen,photosensitizers,and heavy metal ions.The photo-oxidation rates of DMS were higher in seawater than in distilled water,presumably due to the effect of salinity existing in seawater.Three usual photosensitizers(humic acid,fulvic acid and anthroquinone),especially in the presence of oxygen,were able to enhance the photo-oxidation rate of DMS,with the fastest rate observed with anthroquinone.Photo-oxidation of DMS followed first order reaction kinetics with the rate constant ranging from 2.5×10-5 to 34.3×10-5 s-1.Quantitative analysis showed that approximately 32% of the photochemically removed DMS was converted to dimethylsulfoxide.One of the important findings was that the presence of Hg2 could markedly accelerate the photo-oxidation rate of DMS in seawater.The mechanism of mercuric catalysis for DMS photolysis was suggested according to the way of CTTM(charge transfer to metal) of DMS-Hg2 complex.     

中纬低层大气重力波动量通量谱的探空观测

本文利用中纬站点Miramar Nas(32.87°N,117.15°W)的探空数据提取了对流层和低平流层的惯性重力波参数并计算了动量通量-相速度谱.分析表明低层大气重力波动量通量谱很好地满足高斯分布.高斯拟合的参数分析显示:(1)冬季西风急流对向东传播的波的吸收使得对流层向西传播的波的高斯峰值明显强于向东传播的波;(2)重力波在由对流层向平流层的传播过程中谱展会增大,这可能是波与背景相互作用以及波-波相互作用的结果;(3)急流对重力波的吸收与反射以及对流层顶附近波的耗散使得低平流层总动量通量远小于对流层的.受背景风场影响,谱的季节变化呈现出一定规律.多普勒效应对谱产生了两方面的影响,一方面背景风较大时多普勒效应会使谱展宽,另一方面多普勒效应会显著改变谱的中心本征相速度,使得动量通量谱在同一方向上呈现不对称性.     

INTEX-B NO_2排放源在中国地区的应用与检验

将INTEX-B排放源应用到空气质量模型Model3-CMAQ中,对中国地区对流层NO2的浓度分布进行了数值模拟,并与OMI卫星对流层NO2资料进行了对比和验证。结果表明：将INTEX-B排放源应用到Model3-CMAQ模式,模拟的NO2浓度在中国地区的分布、季节变化规律与卫星资料所得结果一致。敏感性试验表明,工业及电厂排放对NO2的浓度贡献最大,而交通排放的贡献相对较小,两种排放均主要集中在京津、长江三角洲等经济发达地区。