基于EEMD-SARIMA的对流层延迟预测模型研究

在无气象数据的条件下,提出一种基于集合经验模态分解（EEMD）和季节性自回归移动平均模型（SARIMA）的对流层延迟（ZTD）预报新方法,并分别选取长春、上海、乌鲁木齐3个地区4个季节的ZTD数据进行预测分析。结果表明,基于EEMD-SARIMA的ZTD改正预报模型能够满足不同地区、不同季节下的ZTD估计需求,是一种高精度的ZTD预报方法。     

对流层延迟与可降水量直接转换模型研究

采用线性回归和最小二乘法拟合建立无线电探空可降水量（RS-PWV）与GPS对流层延迟（GPS-ZTD）、地面温度及大气压之间的直接转换模型,并将直接转换模型得到的PWV分别与RS-PWV及GPS反演得到的可降水量（GPS-PWV）进行比较。结果表明,RS-PWV与GPS-ZTD之间存在良好的线性关系,相关系数达0.927 6;RS-PWV与4阶拟合温度和大气压呈现较好的相关性,相关系数分别为0.640 1和－0.626 3;基于ZTD的单阶单因子模型PWV与GPS-PWV的相关系数达到0.969 9;基于ZTD、温度及大气压的单阶多因子模型PWV比基于ZTD的单阶单因子模型PWV精度明显提高,RMS从4.3 mm提高到3.3 mm。     

Characterization of diurnal cycles in ZTD from a decade of global GPS observations

The diurnal cycle of the tropospheric zenith total delay (ZTD) is one of the most obvious signals for the various physical processes relating to climate change on a short time scale. However, the observation of such ZTD oscillations on a global scale with traditional techniques (e.g. radiosondes) is restricted due to limitations in spatial and temporal resolution. Nowadays, the International GNSS Service (IGS) provides an important data source for investigating the diurnal and semidiurnal cycles of ZTD and related climatic signals. In this paper, 10 years of ZTD data from 1997 to 2007 with a 2-hour temporal resolution are derived from global positioning system (GPS) observations taken at 151 globally distributed IGS reference stations. These time series are used to investigate diurnal and semidiurnal oscillations. Significant diurnal and semidiurnal oscillations of ZTD are found for all GPS stations used in this study. The diurnal cycles (24 hours period) have amplitudes between 0.2 and 10.9 mm with an uncertainty of about 0.5 mm and the semidiurnal cycles (12 h period) have amplitudes between 0.1 and 4.3 mm with an uncertainty of about 0.2 mm. The larger amplitudes of the diurnal and semidiurnal ZTD cycles are observed in the low-latitude equatorial areas. The peak times of the diurnal cycles spread over the whole day, while the peak value of the semidiurnal cycles occurs typically about local noon. These GPS-derived diurnal and semidiurnal ZTD signals are similar with the surface pressure tides derived from surface synoptic pressure observations, indicating that atmospheric tides are the main driver of the diurnal and semidiurnal ZTD variations.     

Responses of the tropospheric ozone and odd hydrogen radicals to column ozone change

The response of tropospheric ozone to a change in solar UV penetration due to perturbation on column ozone depends critically on the tropospheric NO _x (NO+NO₂) concentration. At high NO _x or a polluted area where there is net ozone production, a decrease in column ozone will increase the solar UV penetration to the troposphere and thus increase the tropospheric ozone concentration. However, the opposite will occur, for example, at a remote oceanic area where NO _x is so low that there is net ozone destruction. This finding may have important implication on the interpretation of the long term trend of tropospheric ozone. A change in column ozone will also induce change in tropospheric OH, HO₂, and H₂O₂ concentrations which are major oxidants in the troposphere. Thus, the oxidation capacity and, in turn, the abundances of many reduced gases will be perturbed. Our model calculations show that the change in OH, HO₂, and H₂O₂ concentrations are essentially independent of the NO _x concentration.     

Prediction of the abiotic degradability of organic compounds in the troposphere

A statistically relevant correlation between the reaction rate coefficient, k _OH, for the OH radical reaction with 161 organic compounds in the gas phase at 300 K, and the corresponding vertical ionisation energies E _i,v, reveals two classes of compounds: aromatics where –log(k _OH/cm³s^-1)3/2E _i,v(eV)–2 and aliphatics where –log(k _OH/cm³s^-1)4/5E _i,v(eV)+3. The prediction of the rate coefficient, k _OH, for the reaction of OH with organic molecules from the above equations has a probability of about 90%. Assuming a global diurnal mean of the OH radical concentration of 5×10⁵ cm³, the upper limit of the tropospheric half-life of organic compounds and their persistence can be estimated.     

The latitudinal distribution of carbon monoxide across the pacific from California to Antarctica

The results of a research study of the carbon monoxide concentration from California to 90° S, Antarctica are presented. The data both extend and support other research studies of the latitudinal distribution of carbon monoxide in that higher concentrations are evident over the Northern Hemisphere than over the Southern Hemisphere. Carbon monoxide concentrations range between 50 to 60 ppb with a few peaks into the 60s in the latitudinal area south of the ITCZ and values of 80 ppb or higher at latitudes north of Hawaii. A comparison is also made of carbon monoxide and ozone concentrations along the flight tract between California and Antarctica, over the Ellsworth Mountains of Antarctica, and between 78° S and the South Pole. These ozone-carbon monoxide data show statistically significant negative correlations in the upper troposphere and lower stratosphere over Antarctica. It is believed that this is a good indication of mixing across the tropopause.     

MEASUREMENTS AND MODEL SIMULATIONS OF SURFACE OZONE VARIATIONS AT DIFFERENT BACKGROUND CONCENTRATIONS OF THE PRECURSORS

Ozone photochemical production and loss in very different environments at Waliguan baselinestation and Lin'an background station were simulated by using the measurement data and photo-chemical box model.The results show that net ozone photochemical production rate is negative,about 0.5 ppb/d,at Waliguan baseline sation,because of very low precursor concentrations.Butat Lin'an background station,the net photochemical ozone production is positive,about 2—3 ppb/h.which is very closed with the measurement at Lin'an.That means ozone production was con-trolled by photochemical reactions at Lin'an background station,because of the higher precursorconcentrations.The net destruction rate,at Waliguan Mt.,is not large,so that future increase inanthropogenic emission of reactive nitrogen will lead to larger production rates of steady-state O_3concentration.     

Two-dimensional modelling of some CFC replacement compounds

The Cambridge 2-D Eulerian model has been used to study the potential atmospheric distributions and lifetimes of a number of CFC replacement compounds and their degradation products. The study has focused on HFC 134a and HCFCs 123, 141b and 142b and the major products formed by their atmospheric degradation. The loss of these compounds and their products by hydroxyl radical attack, photolysis and in-cloud hydrolysis have been investigated. The study has shown that HCFCs 141b and 142b have sufficiently long lifetimes to enter the stratosphere in significant quantities, where degradation leads to an increase in the total stratospheric chlorine concentration. The study has also highlighted areas where further experimental work would be valuable, in particular characterisation of the product channels for the degradation reactions and determination of the removal rates of the products in the aqueous phase.     

Boundary-layer ozone depletion as seen in the Norwegian Arctic in spring

Several years of measurements of ozone, hydrocarbons, sulphate and meteorological parameters from Spitsbergen in the Norwegian Arctic are presented. Most of the measurements were taken on the Zeppelin Mountain at an altitude of 474 m a.s.l. The focus is the episodes of ozone depletion in the lower troposphere in spring, which are studied in a climatological way. Episodes of very low ozone concentrations are a common feature on the Zeppelin Mountain in spring. The low ozone episodes were observed from late March to the beginning of June. When the effect of transport direction was subtracted, the frequenty of the low ozone episodes was found to peak in the beginning of May, possibly reflecting the seasonal cycle in the actual depletion process. Analyses based on trajectory calculations show that most of the episodes occurred when the air masses were transported from W-N. Ozone soundings show that the ozone depletion may extend from the surface and up to 3–4 km altitude. The episodes were associated with a cold boundary layer beneath a thermally stable layer, suppressing mixing with the free troposphere. The concentration of several individual hydrocarbons was much lower during episodes of low ozone than for the average conditions. The change in concentration ratio between the hydrocarbons was in qualitative agreement with oxidation of hydrocarbons by Br and Cl atoms rather than by OH radicals.     

Chemical Mechanism Development: Laboratory Studies and Model Applications

Within the German Tropospheric Research Programme (TFS) numerous kinetic and mechanistic studies on the tropospheric reaction/degradation of the following reactants were carried out: oxygenated VOC, aromatic VOC, biogenic VOC, short-lived intermediates, such as alkoxy and alkylperoxy radicals.At the conception of the projects these selected groups were classes of VOC or intermediates for which the atmospheric oxidation mechanisms were either poorly characterised or totally unknown. The motivation for these studies was the attainment of significant improvements in our understanding of the atmospheric chemical oxidation processes of these compounds, particularly with respect to their involvement in photooxidant formation in the troposphere. In the present paper the types of experimental investigations performed and the results obtained within the various projects are briefly summarised. The major achievements are highlighted and discussed in terms of their contribution to improving our understanding of the chemical processes controlling photosmog formation in the troposphere.