Vertical Profiles of Tropospheric Ozone From MAX‐DOAS Measurements During the CINDI‐2 Campaign: Part 1—Development of a New Retrieval Algorithm
Vertical Profiles of Tropospheric Ozone From MAX‐DOAS Measurements During the CINDI‐2 Campaign: Part 1—Development of a New Retrieval Algorithm
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DOI：
10.1029/2018jd028647
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发表时间：
2018-09
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通讯作者：
Yang Wang;J. Puķı̄te;T. Wagner;Sebastian Donner;S. Beirle;A. Hilboll;M. Vrekoussis;A. Richter;A. Apituley;A. Piters;M. Allaart;H. Eskes;A. Frumau;M. Van Roozendael;J. Lampel;U. Platt;Stefan Schmitt;D. Swart;J. Vonk
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作者：
Yang Wang;J. Puķı̄te;T. Wagner;Sebastian Donner;S. Beirle;A. Hilboll;M. Vrekoussis;A. Richter;A. Apituley;A. Piters;M. Allaart;H. Eskes;A. Frumau;M. Van Roozendael;J. Lampel;U. Platt;Stefan Schmitt;D. Swart;J. Vonk
对流层臭氧(O_3)的地面测量对于大气化学、空气污染、气候变化的研究和卫星验证都很有价值。多轴差分光学吸收光谱(MAX-DOAS)技术已被广泛用于提取对流层中痕量气体和气溶胶的垂直剖面。然而，由于平流层臭氧吸收的影响，由MAX-DOAS测量得到的对流层臭氧尚未得到令人满意的结果。在这项研究中，我们开发了两种新的从MAX-DOAS测量数据中反演对流层臭氧的方法。在方法1中，在反演时考虑了来自外部数据源的平流层臭氧剖面。在方法2中，根据对流层和平流层臭氧吸收结构在紫外光谱范围内随温度变化的差异来分离平流层和对流层臭氧。首先通过对合成光谱的应用验证了这两种方法的可行性。然后将它们应用于在荷兰卡博(2016年9月)的CINDI-2运动期间记录的真实MAX-DOA测量。将所得结果与独立的臭氧测量结果和全球化学输送模式模拟结果进行了比较。对于这两种方法，近地表臭氧浓度与独立的数据集都有很好的一致性。然而，只有使用方法1才能合理地得到对流层臭氧廓线，而使用方法2在1公里以上高度对其进行了显著高估，这可能是由于在DOA拟合中用于校正旋转拉曼散射结构的环谱的近似。讨论了两种方法的优缺点，并提出了进一步研究的改进方向。
Ground‐based measurements of tropospheric ozone (O3) are valuable for studies of atmospheric chemistry, air pollution, climate change, and for satellite validation. The Multi Axis Differential Optical Absorption Spectroscopy (MAX‐DOAS) technique has been widely used to derive vertical profiles of trace gases and aerosols in the troposphere. However, tropospheric O3 has not yet been satisfactorily derived from MAX‐DOAS measurements due to the influence of stratospheric O3 absorption. In this study, we developed two new retrieval approaches for tropospheric O3 from MAX‐DOAS measurements. In method 1, stratospheric O3 profiles from external data sources are considered in the retrieval. In method 2, stratospheric and tropospheric O3 are separated based on the temperature‐dependent differences between tropospheric and stratospheric O3 absorption structures in the UV spectral range. The feasibility of both methods is first verified by applying them to synthetic spectra. Then they are applied to real MAX‐DOAS measurements recorded during the CINDI‐2 campaign in Cabauw, the Netherlands (September 2016). The obtained results are compared with independent O3 measurements and global chemical transport model simulations. Good agreement of the near‐surface O3 concentrations with the independent data sets is found for both methods. However, tropospheric O3 profiles are only reasonably derived using method 1, while they are significantly overestimated at altitudes above 1 km using method 2, probably due to the approximation of the ring spectra used to correct the rotational Raman scattering structures in the DOAS fit. Advantages and disadvantages of both methods are discussed and improvement directions are suggested for further studies.