NOx的准两年周期变化及其与臭氧准两年周期振荡的关系Ⅰ.资料分析

利用1992～2000年HALOE的观测资料,分析了平流层NPx(这里是指NO和NO2)混合比的垂直经向分布结构、季节变化和年际变化,并与O3混合比的年际变化进行比较.结果表明:(1)在各纬度平流层NOx混合比的垂直结构基本相似,从平流层下层向上随高度增加,分别在1～2hPa(NO)和5～10 hPa(NO2)达到极大值,再向上NOx混合比随高度减小.另外,NO混合比在1.0×l0-5hPa高度附近还有一个极值区.在平流层下层,它们的极值区下方,NOx混合比基本从热带向两极增大.NO混合比在平流层位于1～2 hPa之间有一个高值区,在1.0×10-5hPa附近还有一个更大的极值.而NO2只有一个浓度高值区,位置在5～10 hPa.(2)NOx混合比在中低纬的高度分布和经向分布上都存在准两年周期振荡(简称QBO).NO2的QBO较NO更明显,赤道上空的NOx的QBO最明显,北半球NOx的QBO较南半球更明显,而20～5hPa的NOx的QBO又较其他气层更明显.(3)在热带30 km以上,NOx的QBO与O3混合比的QBO位相相反;而中纬地区及30 km以下的热带,它们有一个位相差,但不完全相反.     

NO_x的准两年周期变化及其与臭氧准两年周期振荡的关系 I.资料分析

利用 1 992～ 2 0 0 0年HALOE的观测资料 ,分析了平流层NOx (这里是指NO和NO2 )混合比的垂直经向分布结构、季节变化和年际变化 ,并与O3混合比的年际变化进行比较。结果表明 :( 1 )在各纬度平流层NOx混合比的垂直结构基本相似 ,从平流层下层向上随高度增加 ,分别在 1～ 2hPa (NO)和 5～ 1 0hPa (NO2 )达到极大值 ,再向上NOx混合比随高度减小。另外 ,NO混合比在 1 0× 1 0 - 5hPa高度附近还有一个极值区。在平流层下层 ,它们的极值区下方 ,NOx混合比基本从热带向两极增大。NO混合比在平流层位于 1～ 2hPa之间有一个高值区 ,在 1 0× 1 0 - 5hPa附近还有一个更大的极值。而NO2 只有一个浓度高值区 ,位置在 5～ 1 0hPa。 ( 2 )NOx混合比在中低纬的高度分布和经向分布上都存在准两年周期振荡(简称QBO)。NO2 的QBO较NO更明显 ,赤道上空的NOx的QBO最明显 ,北半球NOx 的QBO较南半球更明显 ,而 2 0～ 5hPa的NOx的QBO又较其他气层更明显。 ( 3)在热带 30km以上 ,NOx的QBO与O3混合比的QBO位相相反 ;而中纬地区及 30km以下的热带 ,它们有一个位相差 ,但不完全相反     

准定常行星波对大气中臭氧输运的动力作用

本文从拉格朗日平均环流观点讨论了行星波对大气中O3的输运作用。理论分析表明，当行星波是定常保守时，行星波对大气中O3没有输运作用；而非定常的行星波对大气中O3有明显的输运作用，它可以强迫出一个正的输运环流，即从热带上升，而从高纬下沉的环流；此外，只有当耗散的行星波传播到平流层才会在平流层强迫出输运环流。为了说明行星波对大气中O3输运的动力作用，本文还利用一组34层波—流相互耦合球坐标原始方程谱模式计算了地球大气中行星波对O3变化的作用，其计算的O3变化与实际观测到的O3分布变化很相似。     

大气臭氧与气溶胶垂直分布的高空气球探测

本文给出了1993年9月12日利用高空科学气球在河北省香河地区探测到的大气臭氧和气溶胶的垂直分布。结果发现:(1) 大气臭氧的数密度在整个对流层较低(～10[12]mol/cm3)，并从地面到对流层顶略有下降；对流层顶以上开始快速增加，极值层高度在～24 km，其值为4.78×10[12]mol/cm3；臭氧分压有类似的分布特征，极值146×10[-4]Pa，位于同一高度；(2) 在平流层低层，臭氧分压有一个次极值62×10[-4]Pa，位于15～16 km；(3) 0～30 km大气气溶胶数密度呈现出三个峰值:143，8和1.1 个/cm[3]，分别位于近地面、5 km和21 km；（4）气溶胶的数密度谱在对流层为双模态；在平流层，次峰消失。同时，我们还与其他观测结果作了比较分析。     

北半球春季大气臭氧变化特征及其对大气温度和环流场的影响

该文利用美国1978～1993年TOMS臭氧资料以及NCEP提供的全球再分析资料,研究北半球大气臭氧变化特征及其对大气温度和环流的影响.研究表明1987年前后北半球40°N以北的中高纬地区春季大气臭氧柱总量的趋势变化存在明显的突变,大部分地区突然减少,与其相对应的对流层(平流层)平均温度突然升高(降低),300 hPa(30 hPa)层位势高度也突然增高(下降).但是在北大西洋北部和哈德逊湾地区大气臭氧柱总量却突然增加,与其相对应的对流层(平流层)平均温度突然降低(升高),300 hPa(30 hPa)位势高度突然下降(增高),平均温度突然升高(降低 )1～2°C.研究还表明,大气温度和环流的趋势变化主要是由于大气臭氧的趋势变化所引起.另一方面,在同一地区1979～1992年春季大气臭氧柱总量强弱异常年的大气温度场和环流场的差异也存在相同的分布特征,这一事实进一步说明大气臭氧柱总量的多少是决定大气温度场和环流场差异的重要原因.     

南极昭和站平流层臭氧变化与NAT凝结温度的关系

根据南极昭和站的臭氧和气象探空资料，分析了昭和站上空平流层内几个等压面（20，30，50，70，100和150 hPa）上臭氧变化与硝酸·三水合物（分子式HNO3·3H2O，记为NAT）凝结温度的关系，给出了臭氧变化的一个基本特征。     

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。     

利用卫星大气成分资料分析夏季亚洲季风区平流层-对流层输送特征

首先利用臭氧探空资料验证了Aura-MLS卫星反演臭氧产品在青藏高原地区的可信度, 然后基于2005年和2006年夏季的数据产品确定了亚洲季风区夏季对流层向平流层的输送通道。结果表明, 青藏高原及其周边区域上对流层－下平流层（UT/LS）中, 一氧化碳(CO)和臭氧（O3）浓度散点分布大体上呈现出典型的“L”型分布, 夏季季节内变化反相关特征表现最明显的高度位于150 hPa附近。从时间变化上看, 7月份相关系数最大, 说明该月份对流层－平流层物质交换最为强烈。100 hPa高度位于对流层顶高度以上, 具有对流层特性的大气主要分布在青藏高原东南侧、 孟加拉湾、 印度半岛、 阿拉伯海以及阿拉伯半岛等区域上空, 说明该区域可能是亚洲季风区夏季对流层向平流层物质输送的一个主要通道。     

HALOE资料揭示的热带平流层CH4时空变化特征

中层大气微量成分的分布和变化是中层大气研究的重要问题之一,但是长期以来中层大气的资料非常少。卤素掩星试验（HALOE）对中层大气多种微量气体进行观测,形成中层大气多种微量元素的空间分布和时间演变资料组,这是对中层大气微量气体含量资料的极大补充。作者利用1992～2003年HALOE资料分析热带地区（20°S～20°N）平均的CH4的垂直分布和时间演变特征。结果表明:热带平流层CH4混合比在平流层下层有较充分的混合;热带平流层CH4混合比的季节变化明显,在平流层中上层以年循环为主,而在平流层下部以半年变化为主;热带平流层CH4混合比的年际变化主要有准2年和准5年振荡。       

平流层臭氧对地表有机氯排放的多耦合响应

采用一个包含平流层化学、辐射、动力相互作用的二维模式,对地表有机氯排放变化影响平流层的具体过程作出评估,从而确定平流层臭氧对于地表有机氯排放的多耦合响应,也检验了“蒙特利尔议定书”的减排效果。结果表明,以议定书框架协议达成的20世纪90年代地表有机氯排放减少按30％计算,通过输送、扩散和一系列化学反应,导致平流层中上层的各活性化学族的浓度发生变化,稳定后平流层40km到48km经向平均的相对变化率,ClOx减少20％,HOx和NOx增加2％左右,O3恢复5％左右。此外,这些成分变化导致平流层中上层辐射加热率增加,平流层变冷趋势减缓0．6K。     

Column Observations of Stratospheric Gases at Søndre Strømfjord, Greenland During Winter 1994-1995

As part of the Second European Stratospheric Arctic and Mid-latitude Experiment (SESAME) field campaign, observations were made during the period from October 1994 to April 1995 at Søndre Strømfjord, Greenland (67°N, 53°W). Using a Fourier transform spectrometer, high resolution (0.06 cm-1) infrared spectra were recorded with the sun as a radiation source. Column amounts of trace gases including HCl, HF, HNO3, N2O and O3 are shown for five time periods during the course of the 1994-95 Arctic winter. Results are compared with lower stratospheric potential vorticity fields to describe variations in trace gas column amounts.     

Analysis of the origins and implications of the18O content of stratospheric water vapor

Factors influencing the¹⁸O content of stratospheric H₂O are reviewed in order to provide a theoretical framework for the interpretation of measurements of this quantity, which are now becoming available. Depletions in¹⁸O of 5–10% in stratospheric H₂O are expected based on the known correlation between that of D and¹⁸O in tropospheric H₂O and observed measurements of large (typically 50%) depletions of D in stratospheric H₂O. H₂O formed in the stratosphere as a result of oxidation of CH₄ can be expected to reflect primarily the¹⁸O content of stratospheric O₂, which is the same as that of tropospheric O₂ (slightly enhanced with respect to standard mean ocean water). Thus, a reduction in the¹⁸O depletion is expected with increasing altitude, but not a large enhancement in¹⁸O in upper stratospheric H₂O as found in recent far infrared measurements. The observed large enhancement of¹⁸O in stratospheric O₃ is not expected to be reflected in stratospheric H₂O. Necessary laboratory data for the improved quantification of these effects are reviewed.     

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.     

Effect of methane emission increases in East Asia on atmospheric circulation and ozone

We used a fully coupled chemistry–climate model(version 3 of the Whole Atmosphere Community Climate Model,WACCM3) to investigate the effect of methane(CH4) emission increases,especially in East Asia and North America,on atmospheric temperature,circulation and ozone(O3). We show that CH4 emission increases strengthen westerly winds in the Northern Hemisphere midlatitudes,accelerate the Brewer–Dobson(BD) circulation,and cause an increase in the mass flux across the tropopause. However,the BD circulation in the tropics between 10?S and 10?N at 100 h Pa weakens as CH4 emissions increase in East Asia and strengthens when CH4 emissions increase in North America. When CH4 emissions are increased by 50% in East Asia and 15% globally,the stratospheric temperature cools by up to 0.15 K,and the stratospheric O3 increases by 45 ppbv and 60 ppbv,respectively. A 50% increase of CH4 emissions in North America(with an amplitude of stratospheric O3 increases by 60 ppbv) has a greater influence on the stratospheric O3 than the same CH4 emissions increase in East Asia. CH4 emission increases in East Asia and North America reduce the concentration of tropospheric hydroxyl radicals(4% and 2%,respectively) and increase the concentration of mid-tropospheric O3(5% and 4%,respectively) in the Northern Hemisphere midlatitudes. When CH4 emissions increase in East Asia,the increase in the tropospheric O3 concentration is largest in August. When CH4 emissions increase in North America,the increase in the O3 concentration is largest in July in the mid-troposphere,and in April in the upper troposphere.     

Effect of increasing CO2 on the stratospheric level of CO and O3

Production and destruction processes of carbon monoxide (CO) and ozone (O3) are examined in the light of increasing amount of atmospheric carbon dioxide (CO2). It is found that doubling of CO2 will increase the stratospheric concentration of CO and will have positive effect on O3 concentration.     

Aircraft measurements and model simulations of stratospheric ozone and N2O: implications for chemistry and transport processes in the models

Airborne measurements of stratospheric ozone and N₂O from the SCIAMACHY (Scanning Imaging Absorption Spectrometer) Validation and Utilization Experiment (SCIA-VALUE) are presented. The campaign was conducted in September 2002 and February–March 2003. The Airborne Submillimeter Radiometer (ASUR) observed stratospheric constituents like O₃ and N₂O, among others, spanning a latitude from 5°S to 80°N during the survey. The tropical ozone source regions show high ozone volume mixing ratios (VMRs) of around 11 ppmv at 33 km altitude, and the altitude of the maximum VMR increases from the tropics to the Arctic. The N₂O VMRs show the largest value of 325 ppbv in the lower stratosphere, indicating their tropospheric origin, and they decrease with increasing altitude and latitude due to photolysis. The sub-tropical and polar mixing barriers are well represented in the N₂O measurements. The most striking seasonal difference found in the measurements is the large polar descent in February–March. The observed features are interpreted with the help of SLIMCAT and Bremen Chemical Transport Model (CTMB) simulations. The SLIMCAT simulations are in good agreement with the measured O₃ and N₂O values, where the differences are within 1 ppmv for O₃ and 15 ppbv for N₂O. However, the CTMB simulations underestimate the tropical middle stratospheric O₃ (1–1.5 ppmv) and the tropical lower stratospheric N₂O (15–30 ppbv) measurements. A detailed analysis with various measurements and model simulations suggests that the biases in the CTMB simulations are related to its parameterised chemistry schemes.     

CFSv2 ensemble prediction of the wintertime Arctic Oscillation

Lagged ensembles from the operational Climate Forecast System version 2 (CFSv2) seasonal hindcast dataset are used to assess skill in forecasting interannual variability of the December–February Arctic Oscillation (AO). We find that a small but statistically significant portion of the interannual variance (>20 %) of the wintertime AO can be predicted at leads up to 2 months using lagged ensemble averages. As far as we are aware, this is the first study to demonstrate that an operational model has discernible skill in predicting AO variability on seasonal timescales. We find that the CFS forecast skill is slightly higher when a weighted ensemble is used that rewards forecast runs with the most accurate representations of October Eurasian snow cover extent (SCE), hinting that a stratospheric pathway linking October Eurasian SCE with the AO may be responsible for the model skill. However, further analysis reveals that the CFS is unable to capture many important aspects of this stratospheric mechanism. Model deficiencies identified include: (1) the CFS significantly underestimates the observed variance in October Eurasian SCE, (2) the CFS fails to translate surface pressure anomalies associated with SCE anomalies into vertically propagating waves, and (3) stratospheric AO patterns in the CFS fail to propagate downward through the tropopause to the surface. Thus, alternate boundary forcings are likely contributing to model skill. Improving model deficiencies identified in this study may lead to even more skillful predictions of wintertime AO variability in future versions of the CFS.     

HNO3 and PSC Measurements from the Transall: Sequestering of HNO3 in the Winter of 1994/95

In the winter of 1994/95 the TRANSALL research aircraft performed several flights in the region of the Arctic vortex during the period of low stratospheric temperatures. The results of simultaneous measurements of HNO3 column amounts by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) and of aerosol backscatter profiles by the Ozone Lidar EXperiment (OLEX) are presented for two typical flight scenarios across the polar vortex boundary on December 17, 1994 and January 11/12, 1995. On December 17 and January 12, the column amounts of gaseous HNO3 decreased significantly in regions with low stratospheric temperatures. This decrease was correlated with the extent of the polar stratospheric clouds. Depolarisation measurements showed that type Ib PSCs were observed primarily, but equilibrium calculations for H2SO4/HNO3/H2O aerosols seem to underestimate the observed HNO3 sequestering.     

低纬地区平流层准零风层时空分布特征分析

利用ERA-Interim逐日再分析资料,使用EOF（Empirical Orthogonal Function）等统计方法,分析了中国低纬地区平流层准零风层（Quasi-Zero Wind Layer,QZWL）的时空分布特征,旨在为平流层飞艇寻找合适的运行区域及时段。低纬地区QZWL主要受到热带平流层大气环流季节性变化和平流层准两年振荡（Quasi-BiennialOscillation,QBO）的影响。在二者共同作用下,低纬地区QZWL高概率带可分为南北两支:“北支”出现在10月至次年4月间,QBO东风位相时期,“北支”中心纬度基本维持在20°N附近,西风位相时期,“北支”中心纬度随高度降低南移明显;“南支”仅出现在QBO西风位相期间,5~11月在5°N附近,其余时段与“北支”合并,可以认为是“北支”向南延伸。通过对比海口站和南沙站Weibull概率密度函数与风速资料的拟合结果,表明Weibull分布可以很好拟合不同QBO位相下平流层逐月风速频率分布,根据Weibull分布计算特定的累积概率风速值,可以作为选取适宜平流层飞艇运行的低风速风场的判据。海口站30~50 hPa高度11月至次年4月、南沙站50~70 hPa高度QBO西风位相时期全年均较为适合平流层飞艇运行。     

平流层大气臭氧含量变化特征

利用卫星观测臭氧总含量TOMS（第7版）资料，分析了平流层臭氧含量的变化特征，结果表明，全球臭氧总含量呈下降趋势，准两年振荡是臭氧变化中除年周期外的最显著的变化周期。