全球对流层天顶延迟特征研究

基于IGS提供的对流层天顶延迟数据,分析单站对流层天顶延迟特征,据此构建单站对流层天顶延迟模型,并对其进行拟合得到相关模型参数;比较模型参数与地理位置的关系,得出对流层天顶延迟与测量时间及测站地理位置的相关性,并分析其在全球范围内的连续分布情况:全球对流层天顶延迟变化具有周年性,且与测站位置和高程密切相关;其较高值多集中在赤道附近,并以赤道为中心向两侧递减。该研究为利用全球IGS站的对流层天顶延迟数据建立无需气象参数的全球对流层天顶延迟模型提供了可靠依据。     

Intercomparison campaign of vertical ozone profiles including electrochemical sondes of ECC and Brewer-Mast type and a ground based UV-differential absorption lidar

An intercomparison campaign was conducted at the Observatoire de Haute Provence (OHP) in Southern France in September 1989 in order to compare the three instruments used for vertical tropospheric ozone profiling in the European TOR (Tropospheric Ozone Research Project) network: balloon borne ECC and Brewer-Mast sondes and a ground based UV-DIAL (DifferentialAbsorptionLidar). Additionally, a stratospheric lidar system and the Dobson spectrophotometer of the OHP were operated. Seven simultaneously measured vertical ozone profiles gave evidence for systematic differences of 15% between both types of electrochemical sondes in the troposphere, the Brewer-Mast sondes reading the smaller ozone values. These differences might be explained on the one hand by a possible contamination of the ozone sensor with reducing substances, causing a negative bias mainly for Brewer-Mast sondes and, on the other hand, by the evolution of the sonde background current during the flight, causing a positive bias for ECC sondes and a negative bias for Brewer-Mast sondes. The tropospheric lidar system, measuring the vertical ozone distribution between 6 and 12–15 km, showed ozone concentrations intermediate between the sonde results. This is in good agreement with its estimated systematic error of better than 7% in the upper troposphere. In the stratosphere, the differences between electrochemical sondes and the lidar are between 5 and 10% before the normalisation with the total ozone values measured by the Dobson spectrophotometer, and always below 5% after. While the Dobson normalisation thus corrects rather well the stratospheric part of the sonde profile, it only partially reduces errors occurring in the troposphere.     

The annual cycle of peroxides and ozone in marine air at Cape Grim, Tasmania

The concentration of gas-phase peroxides has been measured almost continuously at the Cape Grim baseline station (41° S) over a period of 393 days (7702 h of on-line measurements) between February 1991 and March 1992. In unpolluted marine air a distinct seasonal cycle in concentration was evident, from a monthly mean value of>1.4 ppbv in summer (December) to <0.2 ppbv in winter (July). In the summer months a distinct diurnal cycle in peroxides was also observed in clean marine air, with a daytime build-up in concentration and decay overnight. Both the seasonal and diurnal cycles of peroxides concentration were anticorrelated with ozone concentration, and were largely explicable using a simple photochemical box model of the marine boundary layer in which the central processes were daytime photolytic destruction of ozone, transfer of reactive oxygen into the peroxides under the low-NO_x ambient conditions that favour self-reaction between peroxy radicals, and continuous heterogeneous removal of peroxides at the ocean surface. Additional factors affecting peroxides concentrations at intermediate timescales (days to a week) were a dependence on air mass origin, with air masses arriving at Cape Grim from higher latitudes having lower peroxides concentrations, a dependence on local wind speed, with higher peroxides concentrations at lower wind speeds, and a systematic decrease in peroxides concentration during periods of rainfall. Possible physical mechanisms for these synoptic scale dependencies are discussed.     

On the Budget of OH Radicals and Ozone in an Urban Plume from the Decay of C5–C8 Hydrocarbons and NOx

Simultaneous measurements of ozone and ozoneprecursors were made during a field campaign atSchauinsland in the Black Forest and in the valleynorth of Schauinsland that channels the flow ofpolluted air from the city of Freiburg to the site.From the decay of hydrocarbons and NO_x between the twomeasuring sites and the known rate coefficients, theconcentration of OH radicals was calculated. From abudget analysis of OH and HO_x it is concluded that therelatively high OH concentrations (5–8 ×10⁶cm^-3) in the presence of high NO₂concentrations cannot be explained by the knownprimary sources. The budget can be closed if efficientrecycling of OH via HO₂ is assumed to occur andthat, based on the measured hydrocarbons, 2 HO₂molecules are formed for each OH radical that reactswith a hydrocarbon molecule. This assumption is inaccordance with the budget of O_x obtained from ourmeasurements and with results from earliermeasurements of alkylnitrates and peroxy radicals atSchauinsland. A possible conclusion is that the decayof precursors and production of photooxidants in urbanplumes proceeds at a faster rate than is currentlyassumed. The potential role of biogenichydrocarbons for the radical budget is alsodiscussed.     

High-Latitude Springtime Photochemistry. Part Ii: Sensitivity Studies of Ozone Production

A seven-year record of surface ozone measurements from Denali NationalPark, Alaska shows a persistent spring maximum. These data, combined withmeasurements of NO_x, hydrocarbons, O₃, and PANfrom a continental site in Alaska during the spring of 1995 are used as thebasis for a sensitivity study to explore tropospheric photochemistry in thisregion. Because of the relatively high concentrations of NO_x(mean of 116, median of 91 pptv), the net tendency was for photochemicalozone production. The range of net O₃ production for averageconditions measured at this site during spring is between 0.96–3.9ppbv/day depending on the assumptions used; in any case, this productionmust contribute to the observed springtime maximum in O₃.Model calculations showed that of the anthropogenic ozone precursors, onlyNO_x had a strong effect on the rate of ozone production; themeasured concentrations of anthropogenic hydrocarbons did not significantlyaffect the ozone budget. Naturally produced biogenic hydrocarbons, such asisoprene, may also have a significant effect on ozone production, even atconcentrations of a few 10's of pptv. An observed temperature-isoprenerelationship from a boreal site in Canada indicates that isoprene may bepresent during the Alaskan spring. Measurements of isoprene taken duringthe spring of 1996 suggest that reactive biogenic hydrocarbon emissionsbegin before the emergence of leaves on deciduous trees and that theconcentrations were sufficient to accelerate ozone production.     

High atmospheric NO x levels and multiple photochemical steady states

Previous zero-dimensional photochemical calculations indicate that multiple tropospheric steady states may exist, in which different NO _x (NO+NO₂) levels could be supported by the same source of NO _x . To investigate this possibility more closely, a one-dimensional photochemical model has been used to estimate the rate of removal of atmospheric NO _x compounds at different NO _x levels. At low NO _x levels NO _x is photochemically converted to HNO₃, which is removed by either wet or dry deposition. At high NO _x levels formation of HNO₃ is inhibited, and NO _x is removed by a variety of other processes, including rainout of N₂O₄ and N₂O₅, surface deposition of NO and NO₂, and direct dissolution of NO and NO₂ in rainwater. Multiple steady states are possible if surface deposition of NO _x is relatively inefficient. The NO _x source required to trigger high atmospheric NO _x levels is approximately 10 to 15 times the present global emission rate-less than half the source strength predicted by the zero-dimensional model. NO _x mixing ratios in excess of 10^-7 would cause severe damage to the ozone layer and could result in either a climatic warming or cooling, depending upon the amount of NO₂ present.     

A model investigation of the impact of increases in anthropogenic NO x emissions between 1967 and 1980 on tropospheric ozone

Recent observations suggest that the abundance of ozone between 2 and 8 km in the Northern Hemisphere mid-latitudes has increased by about 12% during the period from 1970 to 1981. Earlier estimates were somewhat more conservative suggesting increases at the rate of 7% per decade since the start of regular observations in 1967. Previous photochemical model studies have indicated that tropospheric ozone concentrations would increase with increases in emissions of CO, CH₄ and NO _x . This paper presents an analysis of tropospheric ozone which suggests that a significant portion of its increase may be attributed to the increase in global anthropogenic NO _x emissions during this period while the contribution of CH₄ to the increase is quite small. Two statistical models are presented for estimating annual global anthropogenic emissions of NO _x and are used to derive the trend in the emissions for the years 1966–1980. These show steady increase in the emissions during this interval except for brief periods of leveling off after 1973 and 1978. The impact of this increase in emissions on ozone is estimated by calculations with a onedimensional (latitudinal) model which includes coupled tropospheric photochemistry and diffusive meridional transport. Steady-state photochemical calculations with prescribed NO _x emissions appropriate for 1966 and 1980 indicate an ozone increase of 8–11% in the Northern Hemisphere, a result which is compatible with the rise in ozone suggested by the observations.     

A one-dimensional photochemical model of the troposphere with planetary boundary-layer parameterization

The results from a one-dimensional photochemical model of the troposphere representative of summertime conditions at Northern Hemisphere mid-latitudes are presented. A parameterization of mixing processes within the planetary boundary layer (PBL) has been incorporated into the model for both the daytime convective PBL and the formation of the nocturnal PBL. One result of the parameterized PBL is that the concentrations of some trace species in the free troposphere are 20–30% higher than when mixing processes are described by a vertical eddy diffusion coefficient which is held constant with respect to height and time.The calculations indicate that the lifetime of the oxides of nitrogen (NO _x =NO+NO₂) against photochemical conversion to nitric acid (HNO₃) during summertime conditions is on the order of 6 h. This lifetime is short enough to deplete most of the NO _x in the PBL, resulting in the finding that other reactive nitrogen species (HNO₃ and peroxyacetyl nitrate) are more abundant than NO _x throughout the free troposphere, even though NO _x is the most abundant reactive nitrogen species at the surface. The effects of the inclusion of anthropogenic nonmethane hydrocarbon (NMHC) chemistry are also discussed. The inclusion of NMHC chemistry has a pronounced effect on the photochemistry of tropospheric oxone and increases thein situ column production by more than 30%.     

基于全球气象再分析资料的InSAR对流层延迟改正研究

气压、温度和水汽含量等大气物理参数的时空变化导致的对流层延迟是制约合成孔径雷达干涉测量(Interferometric Synthetic Aperture Radar,InSAR)高精度应用的重要因素之一.最新研究显示气象再分析资料在补偿对流层延迟影响方面具有巨大的应用潜力,这促使我们对其有效性和鲁棒性做进一步的研究和探索.本文首先推导了利用气象再分析资料对InSAR进行对流层延迟校正的算法;然后以美国南加州地区的ENVISAT ASAR数据为例,分析了基于两种气象再分析资料(ERA-Interim和North American Regional Reanalysis,NARR)校正InSAR对流层延迟改正的效果;通过与MERIS水汽延迟改正结果比较,验证了该方法的有效性.实验结果表明:(1)不能简单忽略干延迟,可通过气象再分析资料进行有效估计;(2)通过与MERIS水汽产品获得的对流层延迟比较发现,气象再分析资料能够取得接近于MERIS的改善效果;(3)对ERA-Interim和NARR两种气象再分析资料而言,虽然后者具有更高的时间和空间分辨率,但在改正InSAR对流层延迟方面并没有表现出比前者更明显的优势;(4)气象再分析资料可以很好地估计与地形强相关的垂直分层延迟,但对于小尺度的湍流混合延迟的捕捉能力有限.综合分析认为,气象再分析资料的优势在于其数据可随时获得、免费和全球覆盖,它可以显著减弱大尺度的垂直分层延迟对干涉图相位的影响,从而有助于InSAR获取更真实可靠的地形高程和地表形变信息.     

Ammonium Photoproduction from Aquatic Humic and Colloidal Matter

It has recently been shown thatnitrogen contained in humic substances can be releasedas low molecular weight species through photochemicalprocesses or reactions. Nitrogen released in thismanner may then become available for biological useand chemical reactivity. This report providesadditional kinetic data for nitrogen photochemistry oforganic matter in natural waters from Louisiana andfor Suwannee River humic and fulvic acids. Naturalwater samples were fractionated into colloidal(>0.2 m, <1000 Dalton) and dissolved (>1000Dalton) fractions and the kinetics of these fractionsas well as 0.2 m filtered water samples weremeasured. For irradiations of less than 10 hours ofsimulated noon-time sun, samples showed linearproduction of ammonium and first-order fading at350 nm. Ammonium photoproduction was enhanced asmuch as three-fold by lowering pH, but linear kineticswere maintained. Light-dark cycling showed continuedrelease of ammonium immediately after irradiation,followed by uptake at longer post irradiation times.A two step mechanism was proposed to explain theobserved kinetics. Calculated net daytime release ofammonium from natural surface waters ranged from 0.33to 1.9 M h^-1 in the samples studied,corresponding to a photic zone conversion rate of9–20% of the total organic nitrogen per day intoammonium.