Systems modelling of stratospheric ozone transport and photochemistry

A scheme of a system of physical and chemical processes controlling the production, transport and destruction of ozone and its gaseous catalysts, as well as other related gases in the low and high stratosphere is presented. An account is made of temperature variations of the stratospheric layer resulting from changes in ozone content; also included is the effect of temperature variations on photochemical reaction rates and ozone and other gases transport between atmospheric layers. Parameters describing major relations of the system are inferred from the analysis of ozone and trace gas data and from the results of model calculations of interdependence between variations in temperature and ozone content of the layer.An analysis of minor fluctuations of the linearized system shows that photochemical processes are responsible for its aperiodic stability and that gas transport between atmospheric layers destabilizes the system.     

Instantaneous global ozone balance including observed nitrogen dioxide

The catalytic destruction of stratospheric ozone by the oxides of nitrogen is believed to be an important part of the global ozone balance. The lack of sufficient measurements of NO _x concentrations has impeded efforts to quantify this process. Recent measurements of stratospheric nitrogen dioxide from ground-based stations as well as aircraft and balloons have provided a first approximation to a global distribution of NO₂ vertical columns at sunset. These observed vertical columns have been translated into time-dependent vertical NO₂ profiles by means of a one-dimensional atmospheric photochemical model. Using recent observations of air temperature and ozone along with this information, the independent instantaneous (one second) rates of ozone production from oxygen photolysis P(O₃), of ozone destruction from pure oxygen species (Chapman reactions) L(O _x ), and of ozone destruction by nitrogen oxides L(NO _x ) were estimated over the three-dimensional atmosphere. These quantities are displayed as zonal average contour maps, summed over various latitude zones, summed over various altitude bands, and integrated globally between 15 and 45 km. Although the global summation between 15 and 45 km by no means tells the complete story, these numbers are of some interest, and the relative values are: P(O₃), 100; L(O _x ), 15; L(NO _x ), 45±15. It is to be emphasized that this relative NO _x contribution to the integrated ozone balance is not a measure of the sensitivity of ozone to possible perturbations of stratospheric NO _x ; recent model results must be examined for current estimates of this sensitivity.     

Mismatch between variations of solar indices, stratospheric ozone and UV-B observed at ground

In solar cycles 22–23, all solar indices showed maxima near 1990 and 2000 and minima in 1996. The maximum to minimum variation was only 1–2% in the UV range 240–350 nm. Dobson ozone intensities did not show any clear relationship with solar cycle and ozone variations were less than 10%. The UV-B (295–325 nm) observed at ground by Brewer spectrophotometers at some locations had variations of 50–100% for 295–300 nm, and 20–50% for 305–325 nm. The maxima were in different years at different locations (even with separations of only 300 km), did not match with the solar cycle, and were far too large to be explained on the basis of ozone changes (1% decrease of ozone is expected to cause 2% increase of UV-B). Thus, if the data are not bad, the UV-B changes do not match with solar activity or ozone changes and must be mostly due to other local effects (clouds, etc.?). When data are averaged over wide geographical regions, UV-B variation ranges are smaller (10–20%, probably because localised, highly varying cloud effects get filtered out), and are roughly as expected from ozone variations.     

一次对流层异常臭氧次峰的观测研究及其动力输送过程的分析

文中分析了 1996年 8月 1日发生在西宁 (36 .4 3°N ,10 1.4 5°E ,海拔 :2 2 96m)地区对流层异常臭氧次峰现象。观测资料揭示了高空低压槽东移是臭氧次峰的主要天气特征。三维后向轨迹计算表明 ,尽管代表臭氧次峰的气团可以追溯到中亚地区 ,但是明显的气团向下输送则发生在新疆、青海间的高空低压槽内。中尺度模拟进一步确认了对流层顶折叠和平流层向下输送是臭氧次峰出现的动力机制。臭氧次峰在对流层高度位置与准无辐散层有关     

First application of MC2-AQ to multiscale air quality modelling over Europe

A three-dimensional air quality model (MC2-AQ) developed for studying oxidant chemistry on regional to urban scales over North America was adapted and implemented for European conditions. The modelling system is based on the Canadian Mesoscale Compressible Community (MC2) Model, a non-hydrostatic meteorological model, to which modules permitting on-line calculations of chemical transformations, anthropogenic and biogenic emissions, and deposition were added. The transport of chemical species is done on the same grid and with the same advection, convection, and diffusion schemes as are used for the meteorological fields. The developed model is highly flexible and was adapted to different scales by allowing for self-nesting. In this paper we present model results for a high-ozone episode, June 18–26, 2000, over Europe. The modelling system was able to reproduce general characteristics (growth, extent, and dissipation) of the pollution episode. Accumulation of ozone precursors during weak wind and high-temperature synoptic conditions was essential for episode formation. Subsequent episode development and advancement across Europe was driven by frontal systems. A stationary front associated with a low-pressure system over Ukraine prevented the further eastward transport of the polluted air mass. The episode was terminated after the passage of a cold front advecting relatively clean Atlantic air mass.     

Accounting seasonal nonstationarity in time series models for short-term ozone level forecast

Due to the nonlinear feature of a ozone process, regression based models such as the autoregressive models with an exogenous vector process (ARX) suffer from persistent diurnal behaviors in residuals that cause systematic over-predictions and under-predictions and fail to make accurate multi-step forecasts. In this article we present a simple class of the functional coefficient ARX (FARX) model which allows the regression coefficients to vary as a function of another variable. As a special case of the FARX model, we investigate the threshold ARX (TARX) model of Tong [Lecture notes in Statistics, Springer-Verlag, Berlin, 1983; Nonlinear time series: a dynamics system approach, Oxford University Press, Oxford, 1990] which separates the ARX model in terms of a variable called the threshold variable. In this study we use time of day as the threshold variable. The TARX model can be used directly for ozone forecasts; however, investigation of the estimated coefficients over the threshold regimes suggests polynomial coefficient functions in the FARX model. This provides a parsimonious model without deteriorating the forecast performance and successfully captures the diurnal nonstationarity in ozone data. A general linear F-test is used to test varying coefficients and the portmanteau tests, based on the autocorrelation and partial autocorrelation of fitted residuals, are used to test error autocorrelations. The proposed models were applied to a 2 year dataset of hourly ozone concentrations obtained in downtown Cincinnati, OH, USA. For the exogenous processes, outdoor temperature, wind speed, and wind direction were used. The results showed that both TARX and FARX models substantially improve one-day-ahead forecasts and remove the diurnal pattern in residuals for the cases considered.     

我国地面O3、NOX、SO2背景值的观测研究

从1994年8月至1995年8月，在龙凤山、临安大气污染监测站和瓦里关大气本底基准观象台对O3、NOX及SO2首次进行了长期的连续观测。初步分析表明:3站地面O3的平均浓度、月际分布和日变化特征因地理环境、海拔高度和天气条件的不同，表现出明显的差异性。平均地面O3浓度，龙凤山为34.8×10-9,临安为39.1×10-9,瓦里关山为49.3×10-9,龙凤山和临安的月平均地面O3浓度分布较复杂，在6～7月和12月～1月较低，10月底～11月初较高。而在瓦里关山，月平均地面O3浓度变化较平稳，6月份最大，12月最小。龙凤山和临安地面O3平均日变化量较大，下午浓度最高，清晨最小；而瓦里关山地面O3平均日变化较小，上午浓度略低；NOX和SO2的分布具有明显的局地性特征，在龙凤山，临安和瓦里关山，3站的总平均浓度分别为2.7×10-9（NOX）和0.7×10-9(SO2),8.1×10-9(NOX)和16.1×10-9（SO2），0.04×10-9（NOX）和0.15×10-9（SO2）。     

中国地区近地面太阳紫外辐射的分布及其对大气臭氧层破坏的响应

本文在充分考虑太阳紫外辐射在大气中传输的物理过程的基础上,引入局地地面气压、臭氧和地表反照率的时空变化,利用Delta-Eddington近似法计算了中国地区冬季(1月)和夏季(7月)晴天时地面太阳紫外辐射(0.290—0.400μm)和紫外B辐射(0.290—0.325μm)的分布,并进一步计算出臭氧总量减少5％、15％时紫外B的变化.结果指出,由于臭氧总量的减少,中国北部地区紫外B的增加比南部地区显著.平均而言,臭氧总量减少1％时,冬季紫外B将增加1％左右,夏季紫外B将增加0.6％—0.7％.     

Ozone measurements from the Balloon Intercomparison Campaign

Measurements of the Balloon Intercomparison Campaign (BIC), conducted during fall, 1982 (BIC-1) and summer, 1983 (BIC-2), are reported. Results of five remote and two in situ techniques agree (with a few exceptions) within 95% confidence level uncertainties and generally within 15% above 20 km. Weighted mean profiles, which best represent conditions during the capaign, are used as a comparison standard. Accuracies of experiments indicated by BIC generally confirm estimated uncertainites for ECC sondes, UV photometry, and microwave emission experiments, are somewhat better for far IR emission and IR absorption experiments, and are somewhat worse for IR emission and solar UV absorption experiments. The large collection of BIC measurements confirms a problem reported earlier with current theoretical modeling of ozone near 40 km where transport is negligible and the chemistry is believed to be simpler.