A model for studies of tropospheric photochemistry: Description, global distributions, and evaluation

A model for studies of tropospheric photochemistry: Description, global distributions, and evaluation
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DOI:
10.1029/1999jd900425
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发表时间:
1999-11
影响因子:
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通讯作者:
M. Lawrence;P. Crutzen;P. Rasch;B. Eaton;N. Mahowald
M. Lawrence;P. Crutzen;P. Rasch;B. Eaton;N. Mahowald
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文献类型:
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作者:
M. Lawrence;P. Crutzen;P. Rasch;B. Eaton;N. Mahowald

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一个大气光化学和传输模式已经发展并应用于全球对流层化学的研究。大气传输和化学模型-马克斯-普朗克-化学研究所版本(MATCH-MPIC)进行了说明,其全球模拟的主要特点,并与现有的观测结果进行了比较。MATCH-MPIC是一个“离线”模型,它读取最基本气象参数的网格化时间相关值(例如,气象观测站利用这些数据计算大气化学模拟(对流输送、云微物理等)所需的进一步气象参数。MATCH-MPIC的气象学部分模拟平流、对流和干湍流混合的输送,以及整个对流层水文循环(水汽输送、凝结、蒸发和降水)。MATCH-MPIC的光化学成分代表主要的已知来源(例如,工业、生物质燃烧)、转化(化学反应和光解)和汇(例如,湿沉降和干沉降),影响对流层“背景”的O3 hyphen;HOx-NOy-CH 4-CO光化学结构。两个版本的模型的结果被认为是,集中在最近的版本。O3是在相对较好的协议与观察到的探测,虽然它通常被低估在低水平和高估在高水平,特别是对于较新版本的模型。我们的结论是,模拟平流层对流层的O3通量太大,尽管事实上,总通量为1100 Tg(O3)/年,而在最近的文献中估计的上限是超过1400 Tg(O3)/年。OH分布产生对流层CH 4的寿命为10.1年,而早期模型版本的寿命为7.8年,几乎跨越了文献中目前估计的范围(7.5-10.2年)。地面CO混合比与观测结果吻合较好。NO通常被低估,这一问题与最近其他几项模型研究中发现的问题类似。HNO 3也被大大低估了。另一方面,H2 O2和CH 3 OOH与现有的观测结果比较吻合,尽管两者在高浓度时往往被低估,在低浓度时往往被高估。这些差异的可能原因被认为是。
A model of atmospheric photochemistry and transport has been developed and applied toward investigating global tropospheric chemistry. The Model of Atmospheric Transport and Chemistry - Max-Planck-Institute for Chemistry version (MATCH-MPIC) is described and key characteristics of its global simulation are presented and compared to available observations. MATCH-MPIC is an “offline” model which reads in gridded time-dependent values for the most basic meteorological parameters (e.g., temperature, surface pressure, horizontal winds), then uses these to compute further meteorological parameters required for atmospheric chemistry simulations (convective transport, cloud microphysics, etc.). The meteorology component of MATCH-MPIC simulates transport by advection, convection, and dry turbulent mixing, as well as the full tropospheric hydrological cycle (water vapor transport, condensation, evaporation, and precipitation). The photochemistry component of MATCH-MPIC represents the major known sources (e.g., industry, biomass burning), transformations (chemical reactions and photolysis), and sinks (e.g., wet and dry deposition) which affect the O3hyphen;HOx-NOy-CH4-CO photochemical framework of the “background” troposphere. The results of two versions of the model are considered, focusing on the more recent version. O3 is in relatively good agreement with observed soundings, although it is generally underestimated at low levels and overestimated at high levels, particularly for the more recent version of the model. We conclude that the simulated stratosphere-troposphere flux of O3 is too large, despite the fact that the total flux is 1100 Tg(O3)/yr, whereas the upper limit estimated in recent literature is over 1400 Tg(O3)/yr. The OH distribution yields a tropospheric CH4 lifetime of 10.1 years, in contrast to the lifetime of 7.8 years in the earlier model version, which nearly spans the range of current estimates in the literature (7.5–10.2 years). Surface CO mixing ratios are in good agreement with observations. NO is generally underestimated, a problem similar to what has also been found in several other recent model studies. HNO3 is also considerably underestimated. H2O2 and CH3OOH, on the other hand, are in relatively good agreement with available observations, though both tend to be underestimated at high concentrations and overestimated at low concentrations. Possible reasons for these differences are considered.