A global simulation of tropospheric ozone and related tracers: Description and evaluation of MOZART, version 2
A global simulation of tropospheric ozone and related tracers: Description and evaluation of MOZART, version 2
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DOI：
10.1029/2002jd002853
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发表时间：
2003-12-24
影响因子：
4.4
通讯作者：
Brasseur, GP
中科院分区：
文献类型：
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作者：
Horowitz, LW;Walters, S;Brasseur, GP
[1] 我们开发了一个全球三维化学迁移模型，称为臭氧和相关化学示踪剂模型 (MOZART)，版本 2。该模型将向社区提供，该模型建立在国家大气研究中心 (NCAR) 大气迁移和化学模型 (MATCH) 的框架之上，可以轻松地通过各种气象输入和模型分辨率来驱动。在这项工作中，我们描述了模型的标准配置，其中模型由 NCAR 社区气候模型 (MACCM3) 中层大气版本 (MACCM3) 每 3 小时的气象输入驱动，并使用 20 分钟的时间步长和 2.8 度纬度 x 2.8 度经度的水平分辨率，34 个垂直层延伸至约 40 公里。该模型包括对流层臭氧、氮氧化物和碳氢化合物化学的详细化学方案，包括 63 种化学物质。示踪剂平流是使用带有压力固定器的通量形式半拉格朗日方案来执行的。模型中包含亚网格尺度的对流和边界层参数化。地表排放包括化石燃料燃烧、生物燃料和生物质燃烧、生物和土壤排放以及海洋排放。包括干沉积和湿沉积的参数化。几种长寿物种（包括臭氧）的平流层浓度受到气候值放宽的限制。模型很好地模拟了对流层臭氧的分布，包括季节性以及水平和垂直梯度。然而，该模型往往高估了北高纬度对流层顶附近的臭氧。氮氧化物 (NOx) 和硝酸 (HNO3) 的浓度与观测值非常吻合，但模型高估了对流层上层几个地点的过氧乙酰硝酸盐 (PAN)。大多数地点的一氧化碳 (CO) 模拟效果良好，但北半球某些地点的季节性周期被低估。我们发现，原位光化学的产生和损失在对流层臭氧预算中占主导地位，超过了平流层和干沉降的输入。大约 75% 的对流层臭氧产生和损失发生在热带地区，其中热带对流层上层的净产生量较大。北温带地区对流层臭氧的产生和损失是南温带地区的三到四倍。全球二氧化碳来源包括光化学生产（55%）和直接排放（45%）。热带地区主导着 CO 的化学过程，约占对流层产生和损失的 75%。对流层臭氧和二氧化碳的全球预算总体上与最近研究发现的范围一致。甲烷（9.5 年）和甲基氯仿（5.7 年）的寿命与对流层羟基自由基 ( OH) 氧化的关系（衡量全球 OH 丰度的两个有用指标）与最近的估计非常吻合。非甲烷碳氢化合物和含氧中间体（羰基化合物和过氧化物）的浓度通常与观察结果非常吻合。
[1] We have developed a global three-dimensional chemical transport model called Model of Ozone and Related Chemical Tracers (MOZART), version 2. This model, which will be made available to the community, is built on the framework of the National Center for Atmospheric Research (NCAR) Model of Atmospheric Transport and Chemistry ( MATCH) and can easily be driven with various meteorological inputs and model resolutions. In this work, we describe the standard configuration of the model, in which the model is driven by meteorological inputs every 3 hours from the middle atmosphere version of the NCAR Community Climate Model (MACCM3) and uses a 20-min time step and a horizontal resolution of 2.8degrees latitude x 2.8degrees longitude with 34 vertical levels extending up to approximately 40 km. The model includes a detailed chemistry scheme for tropospheric ozone, nitrogen oxides, and hydrocarbon chemistry, with 63 chemical species. Tracer advection is performed using a flux-form semi-Lagrangian scheme with a pressure fixer. Subgrid-scale convective and boundary layer parameterizations are included in the model. Surface emissions include sources from fossil fuel combustion, biofuel and biomass burning, biogenic and soil emissions, and oceanic emissions. Parameterizations of dry and wet deposition are included. Stratospheric concentrations of several long-lived species ( including ozone) are constrained by relaxation toward climatological values. The distribution of tropospheric ozone is well simulated in the model, including seasonality and horizontal and vertical gradients. However, the model tends to overestimate ozone near the tropopause at high northern latitudes. Concentrations of nitrogen oxides (NOx) and nitric acid (HNO3) agree well with observed values, but peroxyacetylnitrate (PAN) is overestimated by the model in the upper troposphere at several locations. Carbon monoxide ( CO) is simulated well at most locations, but the seasonal cycle is underestimated at some sites in the Northern Hemisphere. We find that in situ photochemical production and loss dominate the tropospheric ozone budget, over input from the stratosphere and dry deposition. Approximately 75% of the tropospheric production and loss of ozone occurs within the tropics, with large net production in the tropical upper troposphere. Tropospheric production and loss of ozone are three to four times greater in the northern extratropics than the southern extratropics. The global sources of CO consist of photochemical production ( 55%) and direct emissions (45%). The tropics dominate the chemistry of CO, accounting for about 75% of the tropospheric production and loss. The global budgets of tropospheric ozone and CO are generally consistent with the range found in recent studies. The lifetime of methane (9.5 years) and methylchloroform (5.7 years) versus oxidation by tropospheric hydroxyl radical ( OH), two useful measures of the global abundance of OH, agree well with recent estimates. Concentrations of nonmethane hydrocarbons and oxygenated intermediates (carbonyls and peroxides) generally agree well with observations.