An empirical model for estimating stratospheric ozone vertical distributions over China

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 ...     

Photochemistry in the Arctic Free Troposphere: Ozone Budget and Its Dependence on Nitrogen Oxides and the Production Rate of Free Radicals

Local ozone production and loss rates for the arctic free troposphere (58–85° N, 1–6 km, February–May) during the TroposphericOzone Production about the Spring Equinox (TOPSE) campaign were calculated using a constrained photochemical box model. Estimates were made to assess the importance of local photochemical ozone production relative to transport in accounting for the springtime maximum in arctic free tropospheric ozone. Ozone production and loss rates from our diel steady-state box model constrained by median observations were first compared to two point box models, one run to instantaneous steady-state and the other run to diel steady-state. A consistent picture of local ozone photochemistry was derived by all three box models suggesting that differences between the approaches were not critical. Our model-derived ozone production rates increased by a factor of 28 in the 1–3 km layer and a factor of 7 in the 3–6 kmlayer between February and May. The arctic ozone budget required net import of ozone into the arctic free troposphere throughout the campaign; however, the transport term exceeded the photochemical production only in the lower free troposphere (1–3 km) between February and March. Gross ozone production rates were calculated to increase linearly with NO_x mixing ratiosup to 300 pptv in February and for NO_x mixing ratios up to 500 pptv in May. These NO_x limits are an order of magnitude higher thanmedian NO_x levels observed, illustrating the strong dependence ofgross ozone production rates on NO_x mixing ratios for the majority of theobservations. The threshold NO_x mixing ratio needed for netpositive ozone production was also calculated to increase from NO_x 10pptv in February to 25 pptv in May, suggesting that the NO_x levels needed to sustain net ozone production are lower in winter than spring. This lower NO_x threshold explains how wintertime photochemical ozone production can impact the build-up of ozone over winter and early spring. There is also an altitude dependence as the threshold NO_x neededto produce net ozone shifts to higher values at lower altitudes. This partly explains the calculation of net ozone destruction for the 1–3 km layerand net ozone production for the 3–6 km layer throughout the campaign.     

Simultaneous observations of SAO and QBO in winds, temperature and ozone in the tropical middle atmosphere over Thumba (8.5��N, 77��E)

Owing to the importance of middle atmosphere, recently, a Middle Atmospheric Dynamics (MIDAS) program was carried out during the period 2002?C2007 at Thumba (8.5°N, 77°E). The measurements under this program, involving regular radiosonde/rocket flights as well as atmospheric radars, provided long period observations of winds and temperature in the middle atmospheric region from which waves and oscillations as well as their forcing mechanisms particularly in the low-latitude middle atmosphere could be analyzed. However, a detailed analysis of the forcing mechanisms remains incomplete due to the lack of important measurements like ozone which is a significant contributor to atmospheric dynamics. Presently, profiles of ozone are available from TIMED/SABER (Thermosphere, Ionosphere, Mesosphere Energetics and Dynamics/Sounding of the Atmosphere using Broad Emission Radiometry) satellite globally from about 15 to 100?km, over multiple years since 2002. In this regard, a comprehensive study has been carried out on ozone and its variability at Quasi Biennial Oscillation (QBO) and Semiannual Oscillation (SAO) scales using TIMED/SABER ozone observations during the MIDAS campaign period. Before using the TIMED/SABER ozone measurements, an inter-comparison has been carried out with in situ measurements of ozone obtained under the Southern Hemisphere Additional Ozonesondes (SHADOZ) campaign for the year 2007 at few stations. The inter-comparison showed very good agreement between SABER and ozonesonde derived ozone profiles. After validating the SABER observations, ozone profiles are used extensively to study the QBO and SAO along with temperature and winds in the 20?C100?km height region. It is known that the SAO in mesosphere and stratosphere are in opposite phases, but the present study for the first time reports the aspect of opposite phases in the mesosphere itself. Thus, the present work attempts to study the long-period oscillations in stratosphere and mesosphere in ozone, temperature and winds simultaneously for the first time over this latitude. These observations provided a unique opportunity to explore long-period oscillations in chemistry, dynamics and thermal structure of the middle atmosphere simultaneously.     

中间层顶区域大气平均风场年和半年振荡的全球结构

利用2003~2011年TIDI(TIMED Doppler Interferometer)风场观测数据研究了中间层顶区域80~105 km纬向平均风场年振荡和半年振荡振幅和相位的全球分布结构,并给出了它们的年际变化。在热带地区,纬向风半年振荡最显著。振幅峰值中心位于南半球10°S~20°S范围,出现与平流层半年振荡类似的相对于赤道不对称的分布,并且振幅峰值与以前在该区域的研究结果存在较大差别。在中高纬度地区,纬向风和经向风被年振荡所控制。纬向风在高度100 km以下中高纬度都存在振幅大值中心;经向风年振荡只出现在两半球中纬度高度95 km以下,并且南北半球振幅峰值中心分布不一致。分析结果还显示年振荡和半年振荡振幅存在显著地年际变化,相位的年际变化则较小,但北半球热带地区经向风年振荡振幅和相位表现出2年周期的变化。     

Extremely low temperatures in the stratosphore and very low total ozone amount above northern and central Europe during winter 1989

On 1 February 1989, -83.5°C was recorded in 27.8 hPa over Hohenpeißenberg, the lowest temperature in the 22-year series. This was measured together with a very low total ozone amount of 266 DU. This may be compared with nearly twice this amount on 27 February 1989. The situation was very unusual: following an extremely cold winter in the Arctic stratosphere, the stratospheric cold pole was located over southern Scandinavia on 1 February in a very southerly position. The analyzed temperatures of -92 °C in 30 hPa were also unusual. Even though the low ozone amounts over Hohenpeißenberg were probably dynamically caused, an additional very small ozone decrease due to heterogeneous reactions in altitudes from 23–28 km, where the temperatures lie below -80 °C, cannot be ruled out. Extinction measurements by the orbitting SAGE II instrument indeed show polar stratospheric clouds over Europe near 50° N during the period 31 January–2 February. Also, polar stratospheric clouds were previously observed over Kiruna at similarly low temperatures and signs of a corresponding small ozone decrease were noted there.     

平流层臭氧季节变化的动力和光化学作用之比较

1992年到2005年的HALOE资料显示, 在臭氧光化损耗中, ClOx 和NOx 的贡献大小和作用位置有所差异。SOCRATES3模式模拟表明, 两半球夏季高纬极区的臭氧减少, 主要是NOx的化学贡献; 北极春季和南极冬季副极地臭氧的变化, 主要是动力输送引起。南、北极春季臭氧减少的化学机制也有所不同, 南极春季的臭氧耗损包括极区内ClOx 的异相化学作用和副极区NOx的化学作用; 北极春季的臭氧耗损主要以NOx 和ClOx 的气相化学作用为主, 其中NOx 的作用更大。动力和光化学在臭氧变化中的贡献表明, 整个中低平流层及低纬平流层高层的动力输送贡献可达到45%, 而高纬平流层中上层, 化学作用贡献在65%以上。     

The Upper Stratospheric Ozone Budget: An Update of Calculations Based on HALOE Data

On the basis of data obtained by the Halogen Occultation Experiment (HALOE) on the Upper Atmosphere Research Satellite (UARS) box model calculations are performed to investigate the ozone budget in the upper stratosphere. The HALOE data comprise measurements of major source gases and key chemical species involved in the ozone destruction cycles. In comparison to earlier calculations using version 17 of the HALOE data, the calculated ozone destruction rate increases when the updated data version 18 is used. However, as with the previous study using version 17 of the HALOE data, no evidence for a significant model ozone deficit is found.     

Impact of Air Transport on Seasonal Variations and Trends of Surface Ozone at Kislovodsk High Mountain Station

The impact of air transport on the surface ozone variations is analyzed at Kislovodsk High Mountain Station for the period 1989–1996 on the basis of 2D back trajectories. It was shown that the contribution of photochemical and dynamical processes is different for the different seasons. In summer months the surface ozone concentration is governed by photochemical ozone production in semi polluted air from the regions of Northern Caspian, Southern Ural and Volga region. Time of the seasonal ozone maximum appearance is defined by joint influence of the processes of photochemical production and destruction in the eastern sectors and advection from Ukraine and Central Europe. The value of the seasonal minimum is determined by the processes of ozone destruction in the air coming from northeastern direction in the stable frontal zone. Distribution of sectors of the air transport changes from year to year and it can partly explain strong negative trend of the surface ozone concentration at the site.     

Perturbations in tropical middle atmosphere during winter, 1984–1985

Summary Using high altitude rocketsonde data for Thumba (8.5 N, 76.9E) and Balasore (21.5 N, 86.9E) and the stratalert messages for high latitudes for the winter (December–March) 1984–1985, an examination has been made to study the perturbations in the temperature and winds in the tropical middle atmosphere and their linkage with the dynamical events occurring over the high-latitude middle atmosphere during that winter.The results of analysis indicated occurrence of strong cooling in the mesosphere over a period of seven days (5–12 December 1984) and the depth of the cooling layer was 15 km. This incident was followed by a strong warming over a period of seven days (12–19 December 1984) and the depth of the warming layer was 13 km. The major warming event, which occurred over high latitudes during the later part of December and the first week of January, was followed by the cooling in the mesosphere and warming in the stratosphere at Thumba. Also the zonal winds were strong easterly and the meridional winds were northerly in the upper stratosphere and the lower mesosphere over tropics during the same period. Weaker zonal winds/stronger easterly winds were generally noticed to be associated with coolings/warmings over tropics.With 7 Figures     

Vertical Distribution of Stratospheric Ozone over China

Based on the Stratospheric Aerosol and Gas Experiment (SAGE) II and the Halogen Occultation Ex-periment (HALOE) ozone profiles and the Total Ozone Mapping Spectrometer (TOMS) total ozone data sets,the characteristics and variations of the vertical distribution of stratospheric ozone covering the latitude bands of 50oN±5oN,40oN±5oN,30oN±5oN,and 20oN±5oN and the longitude range of 75-135oE are investigated.The results indicate that the ozone distribution pattern over China not only has general behaviors,but also has particular char-acteristics.In view of the situation that ozone distribu-tions have substantial deviation from zonal symmetry in northern China,the differences of the vertical ozone dis-tribution between the east and the west part of northern China are studied.The results indicate that during winter,spring,and autumn,in the latitude bands of 50oN±5oN,40oN±5oN,ozone concentrations in the eastern part (105 -135oE) are obviously higher than those of the west (75-105oE) at the altitudes of ozone density maximum and below;during summer,in the latitude band of 50oN±5oN,the east-west ozone profile difference is small,but in the latitude band of 40oN±5oN,the east-west total ozone difference becomes as large as 14.0 DU,and the east-west ozone profile difference mainly exists in the lowermost stratosphere and troposphere.     

拉萨地区1998年夏季臭氧总量及垂直廓线的观测研究

该文根据1998年6~10月上旬在拉萨地区进行的臭氧总量及臭氧垂直廓线的观测结果, 并结合同期同纬度其他两个臭氧站数据资料, 证实了以拉萨地区为代表的青藏高原在夏季存在“臭氧低谷”的现象.分析表明, 地基和卫星观测的臭氧总量有一定误差. Umkehr观测反演结果表明夏季拉萨地区平流层臭氧分布和同纬度其他地区相比略有不同; 在对流层, 探空资料显示了该地区对流层臭氧有低值分布的特征.     

Study on the Trace Species in the Stratosphere and Their Impact on Climate

The trace gases （O3, HCl, CH4, H2O, NO, NO2） in the stratosphere play an important role, not only in the photochemical processes in which the ozone layer destroyed, but also in the radiative processes. In this paper, we review the works on the distribution and variation of the trace gases in the stratosphere and their impact on climate, which have been carried out at the University of Science and Technology of China in the recent 20 years. The Halogen Occultation Experiment （HALOE） data were used to analyse the distribution and variation of the mixing ratio of these trace gases and the temperature trends in the stratosphere in the most recent decade. And the reanalyzed National Centers of Environmental Prediction （NCEP）/NCAR data were also used to give the temperature trends and compared with the results from HALOE data. Numerical simulations were also carried out to study the impact of ozone depletion on the global climate. In this review, the distributions of the trace gases, especially those over the Qinghai-Xizang Plateau, are discussed, and the variations and trends for the trace gases in various levels in the stratosphere have been given for the most recent decade. The temperature variation and the cooling trend obtained from HALOE data in the middle and lower stratosphere for the last 13 years are significant, which agree well with the results from NCEP/NCAR data. While the temperature trend in the upper stratosphere in this period do not seem to have much cooling. The numerical simulations show that either the Antarctic ozone hole or the ozone valley over Qinghai-Xizang Plateau affect not only the temperature and circulation in the stratosphere, but also the temperature, pressure and wind fields in the troposphere, then lead to the global climate change.     

热带平流层臭氧准两年周期振荡的特征及数值模拟

利用HALOE的观测资料、对热带地区平流层臭氧垂直分布的年际变化及其准两年周期振荡（QBO）进行研究，并同赤道上空平均的纬向风场的准两年周期振荡进行了模拟研究。资料分析结果表明，平流层臭氧浓度高值区的位置在南北方向上和垂直方向上的有明显的准两年周期，臭氧浓度高值中心的南北移动和上下移动又引起局地臭氧总量的周期性变化和准两年周期振荡南北半球不对称。而臭氧浓度中心位置的准两年周期变化与赤道上空平均纬向风的准两年周期振荡密切相关。资料分析还表明，赤道上空平流层中臭氧浓度QBO的位相随高度变化多次。模拟试验表明，纬向风QBO引起垂直经圈环流的变化，在平流层有三对余差环流圈。它们对O3在不同纬度和高度的输送是引起O3准两年周期振荡的重要动力原因。其中，余差环流在平流层中层（25－35km)的环流圈起着重要的作用。     

瑞利散射激光雷达探测平流层和中间层低层大气温度

介绍了一台瑞利散射激光雷达,它能够探测22～60 km范围内大气温度的垂直分布;比较了两种反演温度的数据处理方法.该激光雷达分别与UARS/HALOE卫星和无线电探空仪观测结果进行了对比,均表现了较好的一致性.同时还模拟分析了平流层低层气溶胶对计算温度的影响.     

The Role of In Situ Photochemistry in the Control of Ozone during Spring at the Jungfraujoch (3,580 m asl) – Comparison of Model Results with Measurements

A photochemical box model has been used to model themeasured diurnal ozone cycle in spring at Jungfraujochin the Swiss Alps. The comparison of the modelleddiurnal ozone cycle with the mean measured diurnalozone cycle in spring, over the period 1988–1996,shows a good agreement both with regard to the shapeand amplitude. Ozone concentrations increase duringthe daytime and reach a maximum at about 16:00–17:00(GMT) in both the modelled and the mean observed ozonecycle, indicative of net ozone production during thedaytime at Jungfraujoch in spring. The agreement isbetter when the modelled ozone cycle is compared withthe mean measured diurnal cycle (1988–1996) filteredfor north-westerly winds >5 m/s (representative ofregional background conditions at Jungfraujoch). Inaddition to ozone, the modelled diurnal cycle of[HO₂] + [CH₃O₂] also shows rather goodagreement with the mean diurnal cycle of the peroxyradicals measured during FREETEX '96, a FREETropopsheric Experiment at Jungfraujoch in April/May1996. Furthermore, this mean diurnal cycle of the sumof the peroxy radicals measured during FREETEX '96 isused to calculate, using steady-state expressions, therespective diurnal cycle of the OH radical. Thecomparison of the OH diurnal cycle, calculated fromthe peroxy radical measurements during FREETEX '96,with the modelled one, reveals also good agreement.The net ozone production rate during the day-time is0.27 ppbv h^-1 from the model, and 0.13 ppbvh^-1 from the observations during FREETEX '96. Theobservations and model results both suggest that thediurnal ozone variation in spring at Jungfraujoch isprimarily of photochemical origin. Furthermore, theobserved and modelled positive net ozone productionrates imply that tropospheric in situphotochemistry contributes significantly to theobserved high spring ozone values in the observedbroad spring-summer ozone maximum at Jungfraujoch.     

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.     

Aerosol black carbon measurements in the Arctic haze during AGASP-II

During the second Arctic Gas and Aerosol Sampling Program conducted in April 1986, we performed measurements of the optically absorbing carbonaceous component of the ambient aerosol from the NOAA WP-3D aircraft operating between sea level and 10 km altitude. We collected the aerosol of filters that were exposed for several hours; we also operated the aethalometer to measure the concentration of aerosol black carbon in real time. The filter analyses represent averages over the altitude range and time span during which the filter was collecting. The real-time results were sorted by altitude to calculate vertical profiles of black carbon concentration. Values typically ranged from 300 to 500 ng m^–3 at lower altitudes, decreasing gradually to 25 to 100 ng m^–3 at 8–10 km. Strong stratification at lower altitudes was frequently observed. The magnitude of these concentrations suggests that the sources are distant regions of considerable fuel consumption. The presence of this material in the tropospheric column and its probable deposition to the high-albedo surface may result in perturbations of the solar radiation balance. The concentrations measured at the highest altitudes may mean that particulate carbon and accompanying emissions for which it is a tracer are mixing into the stratosphere.     

基于WACCM+DART的临近空间SABER和MLS臭氧观测同化试验研究

本研究在WACCM+DART（Whole Atmosphere Community Climate Model,Data Assimilation Research Test-Bed）临近空间资料同化预报系统中加入SABER（Sounding of the Atmosphere using Broadband Emission Radiometry）和MLS（Microwave Limb Sounder）臭氧观测同化接口,并以2016年2月一次平流层爆发性增温（SSW）过程为模拟个例进行了SABER和MLS臭氧观测同化试验,得出以下结论:同化SABER和MLS臭氧体积浓度观测得出的WACCM+DART臭氧分析场能够较真实反映SSW期间北极上空平流层臭氧廓线随时间的演变特征,且与ERA5（Fifth Generation of ECMWF Reanalyses）再分析资料描述的臭氧变化特征具有很好的一致性;基于SABER和MLS臭氧观测的WACCM臭氧6 h预报检验表明同化臭氧观测对臭氧分析和预报误差的改善效果主要体现在南半球高纬平流层和北半球中高纬平流层中上层-中间层底部;基于ERA5再分析资料的WACCM+DART分析场检验表明同化SABER和MLS臭氧体积浓度资料可在提高北半球高纬地区上平流层-中间层底部臭氧场分析质量的同时减小该地区上平流层-中间层底部温度场和中间层底部纬向风场的分析误差;基于MLS臭氧资料的臭氧中期预报检验表明相对控制试验同化SABER和MLS臭氧体积浓度资料能更好改善0~5 d下平流层和中间层底部臭氧的预报效果。     

Fast-J2: Accurate Simulation of Stratospheric Photolysis in Global Chemical Models

Modeling photochemistry in the stratosphere requires solution of the equationof radiative transfer over an extreme range of wavelengths and atmosphericconditions, from transmission through the Schumann–Runge bands ofO₂ in the mesosphere, to multiple scattering from troposphericclouds and aerosols. The complexity and range of conditions makes photolysiscalculations in 3-D chemical transport models computationally expensive. Thisstudy pesents a fast and accurate numerical method, Fast-J2, for calculatingphotolysis rates (J-values) and the deposition of solar flux in stratosphere.Fast-J2 develops an optimized, super-wide 11-bin quadrature for wavelengthsfrom 177 to 291 nm that concatenates with the 7-bin quadrature (291–850nm) already developed for the troposphere as Fast-J. Below 291 nm the effectsof Rayleigh scattering are implemented as a pseudo-absorption, and above 291nm the full multiple-scattering code of Fast-J is used. Fast-J2 calculates themean ultraviolet-visible radiation field for these 18 wavelength binsthroughout the stratosphere, and thus new species and new cross sections canbe readily implemented. In comparison with a standard, high-resolution,multiple-scattering photolysis model, worst-case errors in Fast-J2 do notexceed 5% over a wide range of solar zenith angles, altitudes(0–60 km), latitudes, and seasons where the rates are important inphotochemistry.     

A Comparison of Match Ozonesonde-Derived and 3D Model Ozone Loss Rates in the Arctic Polar Vortex during the Winters of 1994/95 and 1995/96

Ozone loss rates from ozonesonde data reported in the Match experiments of winters 1994/95 and 1995/96 inside the Arctic polar vortex are compared with simulations of the same winters performed using the SLIMCAT 3D chemistry and transport model. For 1994/95 SLIMCAT reproduces the location and timing of the diagnosed ozone destruction, reaching 10 ppbv/sunlit hour in late January as observed. SLIMCAT underestimates the loss rates observed in February and March by 1–3 ppbv/sunlit hour. By the end of March, SLIMCAT ozone exceeds the observations by 25–35%. In January 1995 the ozonesonde-derived loss rates at levels above 525 K are not chemical in origin but due to poor conservation of air parcels. Correcting temperature biases in the model forcing data significantly improved the agreement between the model and observed ozone at the end of winter 1994/95, increasing ozone destruction in SLIMCAT in February and March. The SLIMCAT simulation of winter 1995/96 does not reproduce the maximum ozone loss rates diagnosed by Match of 13 ppbv/sunlit hour. Comparing the data for the two winters reveals that the SLIMCAT photochemistry is least able to reproduce observed losses at low temperatures or when low temperatures coincide with high solar zenith angles (SZA). When cold (T = 192 K), high SZA (90°)matches are excluded from the 1995/96 analysis, agreement between the diagnoses and SLIMCAT is better with ozone loss rates of up to 6 ppbv/sunlit hour. For the rest of the winter SLIMCAT consistently underestimates the Match rates of ozone loss by 1–3 ppbv/sunlit hour. In March 1996 the monthly mean SLIMCAT ozone is 50% greater than observations at 430–540 K. In both winters, ozone destruction rates peaked more rapidly and declined more slowly in the Match observations than in the SLIMCAT simulations. The differences between the observed and modelled cumulative ozone losses demonstrate that the total ozone destruction by the end of the winter is sensitive to errors in the instantaneous ozone loss rates of 1–3 ppbv/sunlit hour.