利用SAGEⅡ遥感分析我国上空平流层臭氧的分布和变化特征

根据1984～1992年的SAGEⅡ观测资料，对平流层臭氧(O3)进行了反演，分析了我国三个纬度区域(20°～50°N)的平流层O3分布和变化特征，得到了可作为参考模式的多年平均的平流层O3总量季节变化曲线和4个月份的垂直分布廓线。     

大气NO2柱浓度多轴差分吸收光谱测量技术及应用

介绍了以太阳散射光为光源的多轴差分吸收光谱技术（Multi-Axis Differential Optical Absorption Spectroscopy,简称MAX-DOAS）,以及MAX-DOAS仪器试验应用.试验中选取中午仪器测量的天顶散射光光谱为参考光谱即Fraunhofer参考光谱,并将测量光谱进行消噪、波长校准以及去除Fraunhofer结构处理.利用分子吸收光学厚度和Ring效应光学厚度对处理后的测量光谱进行最小二乘法拟合,反演出了大气NO2差分斜柱浓度（Differential Slant Column Densities,简称DSCD）.分析了天津武清NO2的差分斜柱浓度反演结果,用简单快捷的几何法将NO2差分斜柱浓度转化成对流层垂直柱浓度（Vertical Column Densities,简称VCD）.研究表明,MAX-DOAS可以有效地监测污染地区对流层NO2的垂直柱浓度.     

1990～2002年北京地区大气臭氧垂直分布Umkehr观测反演研究

基于标准Umkehr反演算法, 利用北京地区Dobson仪器逆转观测资料, 反演计算出臭氧垂直分布.在反演过程中加入气溶胶订正因子, 使反演结果更加合理.利用臭氧垂直分布反演结果, 研究1990～2002年北京地区臭氧垂直分布特征和变化情况.结果表明在1992年秋季和1993年春季期间, 在10.3～23.5 km范围内臭氧浓度有较大幅度降低, 造成了这个期间月平均臭氧总量的明显偏低; 1990年到2002年期间, 臭氧总量的变化呈现出缓慢下降趋势, 但不同高度臭氧含量的变化趋势有所不同.     

Towards a combined SAGE Ⅱ and SCIAMACHY aerosol dataset and implications for stratospheric aerosol trend analysis over East Asia

利用SCIAMACHY临边探测资料反演出平流层气溶胶消光系数廓线。将2003–2004年SCIAMACHY气溶胶反演结果同SAGE Ⅱ探测结果进行对比,结果表明在15–35 km高度范围,反演结果在20–30°N和30–40°N范围平均相对偏差小于20%,在40–50°N范围小于25%。计算出的平流层气溶胶光学厚度与SAGE Ⅱ探测结果的相对偏差在3个纬度范围均小于6%。将SCIAMACHY反演结果与SAGE Ⅱ探测资料相结合,构建平流层气溶胶长期探测资料。根据这些资料,分析东亚(20–50°N,70–150°E)平流层气溶胶变化趋势。结果表明东亚平流层气溶胶在2000–2010年期间呈现显著增加趋势。平流层气溶胶光学厚度在这11年期间平均每年增加5%。中等强度火山爆发对平流层气溶胶增加有显著影响。     

基于SCIATRAN模型的二氧化氮DOAS 反演敏感性试验

气溶胶和地表反照率是影响星载SCIAMACHY仪器观测数据定量遥感NO2大气柱总量的2个主要因子.文中利用高光谱分辨率大气辐射传输模型SCIATRAN,在考虑分子吸收和气溶胶多次散射影响基础上,精确模拟了气溶胶、地表反照率和NO2气体浓度变化对差分处理前后卫星反射光谱的影响,并定义影响因子f,对3个模拟参数进行综合评价.结果表明:(1)通过剔除卫星反射光谱中慢变光谱变化成分,DOAS方法明显降低了气溶胶和地表反照率对卫星反射光谱的影响;(2)差分处理前,3个模拟参数的影响强弱依次为地表反照率、气溶胶和NO2浓度;而差分处理后,3个模拟参数的影响强弱依次为NO2浓度、地表反照率和气溶胶.在影响趋势上,气溶胶和地表反照率很相似,均体现为宽带效应,在440-450 nm内有水汽强吸收和多次散射复杂相互作用导致的较大峰值;NO2浓度变化对差分处理前后的光谱都呈现气体吸收结构的影响特性;(3)由于吸收和散射相互作用等因素的影响,在基于卫星观测的差分光谱中仍然残留有气溶胶和地表反照率的误差,地表反照率约占18.6%,气溶胶约占6.2%.因此,当前SCIAMACHY遥感的NO2产品在中国区域浓度偏高,需要对气溶胶和地表反照率进行二次精细化的订正.     

地基遥感大气水汽总量和云液态水总量的研究

介绍了地基微波辐射计遥感反演大气柱中的水汽总量和云液态水总量的辐射传输原理和反演方法。给出了实用的有气候代表性的北京地区4个季节的反演公式，并对反演公式进行了数值检验，分析了反演精度：春、夏、秋、冬4季水汽总量反演的相对标准偏差分别为3．1％、1．6％、2．2％和2．4％。用反演公式反演在香河探测的NASA微波辐射计资料发现：微波辐射计反演的水汽总量平均比探空测量值偏大O．21cm，二者的线性相关系数为0．988．均方根误差为0．16cm：云液态水总量除降水云天外．值均在0．1mm以下。     

不同大气污染物监测密度对CMAQ源同化修正效果影响的模拟

采用(美国环保部的MODEL-3系统的)CMAQ源同化模型及4种不同空间分辨率的SO2、NO2实测资料,反演得到中国不同尺度的同化修正排放源,利用新一代中尺度气象模式WRF与多尺度空气质量模式CMAQ,模拟分析了中国不同观测信息密度对SO2、NO2源同化反演及其浓度预报的影响,重点分析了华北地区SO2、NO2浓度加密观测对改善SO2、NO2排放源和空气质量预报的重要影响。结果表明,采用不同分辨率的实测资料时,SO2、NO2的趋势预报效果改善程度有一定差异;采用较高分辨率的实测资料进行SO2、NO2源同化修正时,可明显减小SO2、NO2浓度的预报误差。华北地区较高分辨率的观测信息对于改进源同化修正效果及SO2、NO2浓度的趋势预报十分重要,尤其是对SO2浓度的预报尤为重要;采用经高分辨率的实测资料同化修正的排放源时,WRF-CMAQ模式对北京城市尺度SO2、NO2浓度的变化趋势、浓度水平和空间分布特征具有较好的预报效果。高分辨率的观测资料和区域源同化反演方法对于区域污染物浓度预报及排放源清单具有显著的改进作用。     

北京晴天紫外波段气溶胶光学厚度反演与分析

利用太阳一大气紫外光谱辐射计(SAUVS)，测量到达北京地表的太阳直接和散射紫外光谱辐射，给出反演大气气溶胶光学厚度的一种方法。结果表明：在紫外波段，大气气溶胶的光学厚度随波长的增加而单调减小，用指数函数可以很好地拟合反演结果。统计得到了3个水平能见度状况下拟合函数的系数值，与全球气溶胶监测网络(AERONET)北京站的资料对比，表明反演结果基本合理。     

北京秋季地面O3的一维模式模拟研究

用一维光化学模式,基本模拟出静稳天气条件下2001年9月9日北京几个主要大气污染物种:O3、NO、NO2、CO以及SO2的日变化特点,并解释了影响O3及NO、NO2、CO和SO2日变化的控制因子作用。初步分析认为,地面O3对非甲烷碳氢化合物(NMHC)的变化很敏感。NMHC的增加或减少,将会造成O3的明显改变。造成9月9日夜间20:00~23:00一次污染物NO、CO和SO2浓度急剧升高的原因是由于夜间大气层结稳定情况下,大气的垂直扩散减弱,污染物在底层积累造成的。由于实际大气中,影响O3生成和损耗的机制很复杂,同时大气的平流输送是影响O3及其他污染物分布的重要因素,用一维模式虽然能够揭示出影响O3变化的几个因子的作用,但要深入分析O3产生和消耗机制,还需要用三维模式。     

空气质量数值模式预报中资料同化的初步研究

利用嵌套网格空气质量预报模式,在对上海市环境监测中心提供的观测数据进行必要的质量控制后,采用最优插值方法对可吸入颗粒物(PM10)、二氧化氮(NO2)和二氧化硫(SO2)进行资料同化。选取2004年8月1～20日做作逐日同化试验的结果表明,无论是PM10、NO2还是SO2,其同化偏差平均值均在20μg.m-3以下,比同化前减少了至少50%;3种污染物的同化偏差小于其未同化偏差的天数均在16天以上。在大气清洁和污染两种情况下,对PM10分别作10天的同化试验表明,同化后的均方根误差均小于同化之前。此同化方法能利用观测数据较好地修正空气质量模式预报场,从而为模式提供与实际更加接近的初始场。     

Intercomparison of NO<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript>, SO<Subscript>2</Subscript>, O<Subscript>3</Subscript>, and aromatic hydrocarbons measured by a commercial DOAS system and traditional point monitoring techniques

A field-based intercomparison study of a(DOAS) instrument (OPSIS AB, Sweden) andcommercial Differential Optical Absorption Spectroscopydifferent point-sample monitoring techniques (PM, basedon an air monitoring station, an air monitoring vehicle, and various chemical methods) was conducted inBeijing from October 1999 to January 2000. The mixing ratios of six trace gases including NO, NO2, SO2,03, benzene, and toluene were monitored continuously during the four months. A good agreement betweenthe DOAS and PM data was found for NO2 and SO2. However, the concentrations of benzene, toluene,and NO obtained by DOAS were significantly lower than those measured by the point monitors. Theozone levels monitored by the DOAS were generally higher than those measured by point monitors. Theseresults may be attributed to a strong vertical gradient of the NO-O3-NO2 system and of the aromatics atthe measurement site. Since the exact data evaluation algorithm is not revealed by the manufacturer ofthe DOAS system, the error in the DOAS analysis can also not be excluded.     

Intercomparison of NO_x, SO_2, O_3, and Aromatic Hydrocarbons Measured by a Commercial DOAS System and Traditional Point Monitoring Techniques

A field-based Intercomparison study of a commercial Differential Optical Absorption Spectroscopy (DOAS) instrument (OPSIS AB, Sweden) and different point-sample monitoring techniques (PM, based on an air monitoring station, an air monitoring vehicle, and various chemical methods) was conducted in Beijing from October 1999 to January 2000. The mixing ratios of six trace gases including NO, NO2, SO2, O3, benzene, and toluene were monitored continuously during the four months. A good agreement between the DOAS and PM data was found for NO2 and SO2. However, the concentrations of benzene, toluene, and NO obtained by DOAS were significantly lower than those measured by the point monitors. The ozone levels monitored by the DOAS were generally higher than those measured by point monitors. These results may be attributed to a strong vertical gradient of the NO-O3-NO2 system and of the aromatics at the measurement site. Since the exact data evaluation algorithm is not revealed by the manufacturer of the DOAS sys     

A Method for Retrieving Vertical Ozone Profiles from Limb Scattered Measurements

A two-step method is employed in this study to retrieve vertical ozone profiles using scattered measure- ments from the limb of the atmosphere. The combination of the Differential Optical Absorption Spectroscopy (DOAS) and the Multiplicative Algebraic Reconstruction Technique (MART) is proposed. First, the limb radiance, measured over a range of tangent heights, is processed using the DOAS technique to recover the effective column densities of atmospheric ozone. Second, these effective column densities along the lines of sight (LOSs) are inverted using the MART coupled with a forward model SCIATRAN (radiative transfer model for SCIAMACHY) to derive the ozone profiles. This method is applied to Optical Spectrograph and Infra Red Imager System (OSIRIS) radiance, using the wavelength windows 571-617 nm. Vertical ozone profiles between 10 and 48 km are derived with a vertical resolution of 1 km. The results illustrate a good agreement with the cloud-free coincident SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) ozone measurements, with deviations less than ± 10% ( ± 5% for altitudes from 17 to 47 km). Furthermore, sensitivities of retrieved ozone to aerosol, cloud parameters and NO 2 concentration are also investigated.     

A differential optical absorption spectroscopy method for {X_{CO_2}} retrieval from ground-based Fourier transform spectrometers measurements of the direct solar beam

A differential optical absorption spectroscopy (DOAS)-like algorithm is developed to retrieve the column-averaged dry-air mole fraction of carbon dioxide from ground-based hyper-spectral measurements of the direct solar beam. Different to the spectral fitting method, which minimizes the difference between the observed and simulated spectra, the ratios of multiple channel-pairs——one weak and one strong absorption channel——are used to retrieve X CO2 from measurements of the shortwave infrared (SWIR) band. Based on sensitivity tests, a super channel-pair is carefully selected to reduce the effects of solar lines, water vapor, air temperature, pressure, instrument noise, and frequency shift on retrieval errors. The new algorithm reduces computational cost and the retrievals are less sensitive to temperature and H2O uncertainty than the spectral fitting method. Multi-day Total Carbon Column Observing Network (TCCON) measurements under clear-sky conditions at two sites (Tsukuba and Bremen) are used to derive X CO2 for the algorithm evaluation and validation. The DOAS-like results agree very well with those of the TCCON algorithm after correction of an airmass-dependent bias.     

Observations of the Nitrate Radical in the Marine Boundary Layer

A study of the nitrate radical (NO3) has been conducted through a series of campaigns held at the Weybourne Atmospheric Observatory, located on the coast of north Norfolk, England. The NO3 concentration was measured in the lower boundary layer by the technique of differential optical absorption spectroscopy (DOAS). Although the set of observations is limited, seasonal patterns are apparent. In winter, the NO3 concentration in semi-polluted continental air masses was found to be of the order of 10 ppt, with an average turnover lifetime of 2.4 minutes. During summer in clean northerly air flows, the concentration was about 6 ppt with a lifetime of 7.2 minutes. The major loss mechanisms for the radical were investigated in some detail by employing a chemical box model, constrained by a suite of ancillary measurements. The model indicates that during the semi-polluted conditions experienced in winter, the major loss of NO3 occurred indirectly through reactions of N2O5, either in the gas-phase with H2O, or through uptake on aerosols. The most important direct loss was via reactions of NO3 with a number of unsaturated nonmethane hydrocarbons. The cleaner air masses observed during the summer were of marine origin and contained elevated concentrations of dimethyl sulfide (DMS), which provided the major loss route for NO3. The box model was then used to investigate the conditions in the remote marine boundary layer under which DMS will be oxidised more rapidly at night (by NO3) than during the day (by OH). This should occur if the concentration of NO2 is more than about 60% that of DMS.     

Slant Column Measurements of O3 and NO2 During the NDSC Intercomparison of Zenith-Sky UV-Visible Spectrometers in June 1996

In June 1996, 16 UV-visible sensors from 11 institutes measured spectra of the zenith sky for more than 10 days. Spectra were analysed in real-time to determine slant column amounts of O3 and NO2. Spectra of Hg lamps and lasers were measured, and the amount of NO2 in a cell was determined by each spectrometer. Some spectra were re-analysed after obvious errors were found. Slant columns were compared in two ways: by examining regression analyses against comparison instruments over the whole range of solar zenith angles; and by taking fractional differences from a comparison instrument at solar zenith angles between 85° and 91°. Regression identified which pairs of instruments were most consistent, and so which could be used as universal comparison instruments. For O3, regression slopes for the whole campaign agreed within 5% for most instruments despite the use of different cross-sections and wavelength intervals, whereas similar agreement was only achieved for NO2 when the same cross-sections and wavelength intervals were used and only one half-day's data was analysed. Mean fractional differences in NO2 from a comparison instrument fall within ±7% (1-sigma) for most instruments, with standard deviations of the mean differences averaging 4.5%. Mean differences in O3 fall within ±2.5% (1- sigma) for most instruments, with standard deviations of the mean differences averaging 2%. Measurements of NO2 in the cell had similar agreement to measurements of NO2 in the atmosphere, but for some instruments measurements with cell and atmosphere relative to a comparison instrument disagreed by more than the error bars.     

Multi-species chemical data assimilation with the Danish Eulerian hemispheric model: system description and verification

Satellite retrievals of atmospheric composition provide a wealth of data on a global scale. These complement results from atmospheric chemistry-transport models (CTMs), and can be combined using data assimilation. We present two assimilation schemes coupled to the Danish Eulerian Hemispheric Model (DEHM), a three-dimensional, off-line CTM with full photochemistry: a variant on the ensemble Kalman filter and the three-dimensional variational scheme. The aim of this paper is to describe the two schemes and present an initial assessment of their impacts on model skill. Retrievals of multiple atmospheric trace gases are assimilated, namely: NO₂ tropospheric column densities, CH₄ total column densities, and partial column concentrations of O₃, CO and CH₄; these data are retrieved from four satellite sensors. Data for each species are assimilated independently of one another, and other species are only adjusted indirectly via the model’s chemistry and dynamics. Assimilation results are compared with measurements from surface monitoring stations and other satellite retrievals, and preliminary validation results are presented.Reference simulations (without assimilation) grossly underestimate surface CO concentrations, and both assimilation schemes eliminate this large and systematic model bias. The assimilation improves the spatial correlation of modelled CO with surface observations, and improves the spatial correlation between forecasts and retrievals for CO, NO₂ and O₃. Results for CH₄ show a loss of skill due to a mismatch in model bias between two assimilated CH₄ data-sets. Finally, we discuss differences in methodology and results between this paper and a recent study on multi-species chemical data assimilation. Joint optimisation of initial conditions and emission rates offers a promising direction for improving modelled boundary-layer concentrations.     

COVID-19疫情期间全球空气质量变化:臭氧响应的区域间差异

疫情期间全球各地一次排放大幅削减,而臭氧等二次污染的响应则存在着区域间差异.结合地面和卫星观测发现,同在氮氧化物大幅下降的情况下,臭氧在东亚和欧洲呈现出可达14ppb的上升信号,而北美则下降为主(约2-4ppb).我们结合气象分析和臭氧敏感性进一步讨论了臭氧响应差异性的原因,一方面受臭氧与前体物间关系的影响;另一方面来...     

利用探空资料验证GOME卫星臭氧数据

利用1996年3月-2003年6月部分时段拉萨、西宁、北京3个站的臭氧探空资料验证了GOME（Global Ozone Monitoring Experiment）卫星臭氧廓线及对流层臭氧柱总量。对比结果表明:在对流层中下层,拉萨和西宁两地GOME与探空的平均偏差小于5%,北京地区平均偏差小于10%;在对流层上层/平流层下层,拉萨和西宁平均偏差小于10%,北京小于20%;在平流层中上层3个站的平均偏差均小于5%。在对流层上层/平流层下层区域,GOME与臭氧探空的平均偏差在北京明显高于拉萨和西宁。3个地区对流层柱总量的平均偏差都在10%以内,表明该资料可用于研究我国对流层臭氧总量的变化规律。同时段的GOME最低层（0~2.5km）月平均臭氧浓度对比结果显示,GOME结果同地面臭氧观测值有很好的相关性,GOME臭氧浓度反映了拉萨、瓦里关、临安地面臭氧浓度的主要变化特征。