大气气溶胶与痕量气体廓线MAX-DOAS遥测方法研究
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摘要
我国区域性大气污染问题日趋明显,及时准确获取区域污染信息是研究、控制区域污染的前提。尽管我国已建立了以城市为中心的空气质量自动监测站,但不能完全反映大气污染状况,造成空气质量评价指标与公众直观感受不一致。近地面有限指标的监测,不能满足空气污染形成机制、演变和输送过程的研究需求。多轴差分吸收光谱(MAX-DOAS)技术能够对对流层、平流层污染物进行观测,提供气溶胶、痕量气体垂直分布数据,不仅能够更及时、迅速地获取更大区域的污染分布特征,还能够实现在相同观测模式下对卫星数据的校验。本文基于MAX-DOAS技术开展了大气气溶胶、痕量气体廓线监测方法的研究工作。
本文采用自行研制的MAX-DOAS系统观测太阳散射光谱,并对该系统的关键指标,包括视场角、指向精度、杂散光水平、光谱定标等,进行了测试。结果说明系统性能满足观测需求。同时针对MAX-DOAS方法的关键问题进行了深入研究：利用多项式拟合去除散射影响,消除了夫琅禾费结构和Ring效应影响,在痕量气体截面处理中进行了I0效应修正,确定了NO2、O4的拟合波段,最终准确的反演出斜柱浓度。并通过长达16天的国内外同类仪器联合观测对比试验,验证了仪器性能和斜柱浓度反演精度。痕量气体斜柱浓度的成功获取是进一步研究的基础,本文着重于对大气气溶胶和痕量气体廓线的解析方法进行了研究。
利用O4气体斜柱浓度和强度指数中包含着气溶胶信息的特点,研究了基于MAX-DOAS技术的气溶胶反演方法。本文首先利用辐射传输模型SCIATRAN进行模拟计算消除了O4气体吸收截面不准确造成的斜柱浓度误差,提高气溶胶的反演精度。然后分析了O4气体斜柱浓度、强度指数和气溶胶、观测仰角的相关性,通过权重函数量化了二者对气溶胶变化的敏感性。最后基于最优估算法构建了气溶胶消光廓线反演算法,采用了SCIATRAN模拟数据进行了反演算法的性能验证,结果表明算法能够实现对流层低层气溶胶的准确计算,并利用平均核矩阵确定了测量噪声、先验约束对反演解不确定度的影响,分析了反演误差。
利用多个仰角的痕量气体斜柱浓度中包含着其垂直分布信息的特点,研究了基于MAX-DOAS技术的痕量气体廓线反演方法。本文首先分析了NO2气体斜柱浓度对NO2廓线变化的敏感性。针对NO2气体的弱吸收特性,确定采用线性最优估算法进行NO2廓线解析。随后采用SCIATRAN模拟数据进行了反演算法的性能验证,结果表明算法能够实现1km以下的NO2垂直分布的准确计算,并利用平均核矩阵确定了测量噪声、先验约束对反演解不确定度的影响,进行了误差分析。进一步,本文还提出了利用能见度资料快速计算近地面N02体积比浓度的方法。
最后开展了MAX-DOAS的外场观测试验。大气气溶胶消光廓线的观测结果表明,上海地区的颗粒物分布在1km以下,边界层基本稳定。通过和激光雷达的观测数据对比,验证了算法的可行性。同时,试验中获取了N02气体垂直廓线,并将近地面层反演浓度和点式仪器进行了对比,验证反演结果。另外,利用能见度资料准确获取了地表N02的体积比浓度信息。
With severe regional air pollution problem in china, fast and accurate monitoring of regional air pollution is needed effective research and prevention of air pollution. Even air quality monitoring stations have been built centering on the cities, actual situation of air pollution can't been reported completely, causing the disagreement of air quality index and public intuitive feelings. Existing traditional point monitoring techniques can't fulfill the requirement of research in the production, evolution and transfer of air pollution. Multi-axis differential absorption spectroscopy (MAX-DOAS) technology can measure the pollutant in the troposphere and stratosphere, and provide the information of aerosol and trace gas distribution, not just derive the pollutant distribution in large region, but also being used in the validation of satellite data in same observation mode. In this thesis research on the remote sensing of aerosol and trace gas vertical distribution by MAX-DO AS technique has been carried out.
Solar scatter spectrum is collected with MAX-DOAS instrument developed in our laboratory. Key parameters of MAX-DOAS was tested, include the field of view, pointing precision, stray light, spectral calibration and so on, showing good performance for monitoring requirement. Also, intensive study on unique problems of MAX-DOAS technique was conducted. The interference of scatter was removed with polynomial fitting, the effect of Fraunhofer structures and Ring effect were eliminated, I0effect correction was performed during the cross section processing, and the fitting windows of NO2, O4was determined. Finally the slant column density (SCD) has been retrieved precisely. A MAX-DOAS intercomparison campaign was attended, which included the instrument from home and abroad, and lasted for16days, and result evaluated the performance and SCD retrieval precision of MAX-DOAS further. Precisely retrieval of SCD is the guarantee of the following profile calculation, and in this thesis the work paid particular emphasis on the retrieval of aerosol and trace gas distribution.
Based on the character that O4SCD and intensity index contain the information of aerosol, research on the aerosol retrieval with MAX-DOAS was carried out. At first, as O4absorption cross section inaccuracy cause the error of SCD, and this problem is solved with simulation of radiative transfer model. Then, the sensitivity of aerosol retrieval was analysed. The relationship between O4SCD, intensity index and aerosol, elevation angle was summarized, and the sensitivity was quantized with the weighting function. An aerosol extinction profile retrieval algorithm has been developed based on the optimal estimation method (OEM). The algorithm was validated with SCIATRAN simulated data, and result showed that the aerosol in the low troposphere can be derived precisely with this algorithm. The averaging kernel matrix was introduced for analyzing the effect of measurement noise and a priori information on the uncertainty of retrieval solution, and error analysis of the retrieval algorithm were carried out too.
On account of that trace gas vertical distribution information can be derived from several SCD of different elevation angles, research on the trace gas profile retrieval wilh MAX-DOAS was carried out At first, the sensitivity of NO2SCD on the variation of profile is analysed in this thesis. For the speciality of weak absorption of NQ2, NO2vertical profile retrieval was fulfilled with linear optimal estimation method. Then the retrieval algorithm was validated with SCIATRAN simulated data, showing that this algorithm can be used for the the NO2profile retrieval below1km. The averaging kernel matrix was also introduced for analyzing the effect of measurement noise and a priori information on the uncertainty of retrieval solution, and used for error analysis. Moreover, a fast convert method from SCD to NO2concentration was developed.
Field campaigns with developed MAX-DOAS instrument were held. Measurement result of aerosol extinction profiles showed that the particulate matter in Shanghai concentrated below1km, and the height of boundary layer was steady. Through the validation with Lidar, good agreement proved the feasibility of aerosol retrieval. The result of NO2vertical profile was also derived, and the concentrations of the lowest layer were validated with point measurement data. Furthermore, surface NO2mixing ratio information was derived based on the visibility data.
本文采用自行研制的MAX-DOAS系统观测太阳散射光谱,并对该系统的关键指标,包括视场角、指向精度、杂散光水平、光谱定标等,进行了测试。结果说明系统性能满足观测需求。同时针对MAX-DOAS方法的关键问题进行了深入研究：利用多项式拟合去除散射影响,消除了夫琅禾费结构和Ring效应影响,在痕量气体截面处理中进行了I0效应修正,确定了NO2、O4的拟合波段,最终准确的反演出斜柱浓度。并通过长达16天的国内外同类仪器联合观测对比试验,验证了仪器性能和斜柱浓度反演精度。痕量气体斜柱浓度的成功获取是进一步研究的基础,本文着重于对大气气溶胶和痕量气体廓线的解析方法进行了研究。
利用O4气体斜柱浓度和强度指数中包含着气溶胶信息的特点,研究了基于MAX-DOAS技术的气溶胶反演方法。本文首先利用辐射传输模型SCIATRAN进行模拟计算消除了O4气体吸收截面不准确造成的斜柱浓度误差,提高气溶胶的反演精度。然后分析了O4气体斜柱浓度、强度指数和气溶胶、观测仰角的相关性,通过权重函数量化了二者对气溶胶变化的敏感性。最后基于最优估算法构建了气溶胶消光廓线反演算法,采用了SCIATRAN模拟数据进行了反演算法的性能验证,结果表明算法能够实现对流层低层气溶胶的准确计算,并利用平均核矩阵确定了测量噪声、先验约束对反演解不确定度的影响,分析了反演误差。
利用多个仰角的痕量气体斜柱浓度中包含着其垂直分布信息的特点,研究了基于MAX-DOAS技术的痕量气体廓线反演方法。本文首先分析了NO2气体斜柱浓度对NO2廓线变化的敏感性。针对NO2气体的弱吸收特性,确定采用线性最优估算法进行NO2廓线解析。随后采用SCIATRAN模拟数据进行了反演算法的性能验证,结果表明算法能够实现1km以下的NO2垂直分布的准确计算,并利用平均核矩阵确定了测量噪声、先验约束对反演解不确定度的影响,进行了误差分析。进一步,本文还提出了利用能见度资料快速计算近地面N02体积比浓度的方法。
最后开展了MAX-DOAS的外场观测试验。大气气溶胶消光廓线的观测结果表明,上海地区的颗粒物分布在1km以下,边界层基本稳定。通过和激光雷达的观测数据对比,验证了算法的可行性。同时,试验中获取了N02气体垂直廓线,并将近地面层反演浓度和点式仪器进行了对比,验证反演结果。另外,利用能见度资料准确获取了地表N02的体积比浓度信息。
With severe regional air pollution problem in china, fast and accurate monitoring of regional air pollution is needed effective research and prevention of air pollution. Even air quality monitoring stations have been built centering on the cities, actual situation of air pollution can't been reported completely, causing the disagreement of air quality index and public intuitive feelings. Existing traditional point monitoring techniques can't fulfill the requirement of research in the production, evolution and transfer of air pollution. Multi-axis differential absorption spectroscopy (MAX-DOAS) technology can measure the pollutant in the troposphere and stratosphere, and provide the information of aerosol and trace gas distribution, not just derive the pollutant distribution in large region, but also being used in the validation of satellite data in same observation mode. In this thesis research on the remote sensing of aerosol and trace gas vertical distribution by MAX-DO AS technique has been carried out.
Solar scatter spectrum is collected with MAX-DOAS instrument developed in our laboratory. Key parameters of MAX-DOAS was tested, include the field of view, pointing precision, stray light, spectral calibration and so on, showing good performance for monitoring requirement. Also, intensive study on unique problems of MAX-DOAS technique was conducted. The interference of scatter was removed with polynomial fitting, the effect of Fraunhofer structures and Ring effect were eliminated, I0effect correction was performed during the cross section processing, and the fitting windows of NO2, O4was determined. Finally the slant column density (SCD) has been retrieved precisely. A MAX-DOAS intercomparison campaign was attended, which included the instrument from home and abroad, and lasted for16days, and result evaluated the performance and SCD retrieval precision of MAX-DOAS further. Precisely retrieval of SCD is the guarantee of the following profile calculation, and in this thesis the work paid particular emphasis on the retrieval of aerosol and trace gas distribution.
Based on the character that O4SCD and intensity index contain the information of aerosol, research on the aerosol retrieval with MAX-DOAS was carried out. At first, as O4absorption cross section inaccuracy cause the error of SCD, and this problem is solved with simulation of radiative transfer model. Then, the sensitivity of aerosol retrieval was analysed. The relationship between O4SCD, intensity index and aerosol, elevation angle was summarized, and the sensitivity was quantized with the weighting function. An aerosol extinction profile retrieval algorithm has been developed based on the optimal estimation method (OEM). The algorithm was validated with SCIATRAN simulated data, and result showed that the aerosol in the low troposphere can be derived precisely with this algorithm. The averaging kernel matrix was introduced for analyzing the effect of measurement noise and a priori information on the uncertainty of retrieval solution, and error analysis of the retrieval algorithm were carried out too.
On account of that trace gas vertical distribution information can be derived from several SCD of different elevation angles, research on the trace gas profile retrieval wilh MAX-DOAS was carried out At first, the sensitivity of NO2SCD on the variation of profile is analysed in this thesis. For the speciality of weak absorption of NQ2, NO2vertical profile retrieval was fulfilled with linear optimal estimation method. Then the retrieval algorithm was validated with SCIATRAN simulated data, showing that this algorithm can be used for the the NO2profile retrieval below1km. The averaging kernel matrix was also introduced for analyzing the effect of measurement noise and a priori information on the uncertainty of retrieval solution, and used for error analysis. Moreover, a fast convert method from SCD to NO2concentration was developed.
Field campaigns with developed MAX-DOAS instrument were held. Measurement result of aerosol extinction profiles showed that the particulate matter in Shanghai concentrated below1km, and the height of boundary layer was steady. Through the validation with Lidar, good agreement proved the feasibility of aerosol retrieval. The result of NO2vertical profile was also derived, and the concentrations of the lowest layer were validated with point measurement data. Furthermore, surface NO2mixing ratio information was derived based on the visibility data.
引文
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