Interactions between tropospheric chemistry and aerosols in a unified general circulation model
Interactions between tropospheric chemistry and aerosols in a unified general circulation model
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DOI：
10.1029/2001jd001260
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发表时间：
2003-01-02
影响因子：
4.4
通讯作者：
Jacob, DJ
中科院分区：
文献类型：
--
作者：
Liao, H;Adams, PJ;Jacob, DJ
在戈达德空间研究所的大气环流模式（GCM）中，建立了一个统一的对流层化学-气溶胶模式。该模型包括对流层臭氧-氮氧化物-碳氢化合物化学以及气溶胶和气溶胶前体的详细模拟。预测的气溶胶种类包括硫酸盐、硝酸盐、铵、黑碳、原生有机碳和次生有机碳。氨和硝酸盐在气相和气溶胶相之间的分配由在线热力学平衡确定，并且二次有机气溶胶的形成基于平衡分配和实验确定的参数。气溶胶和化学之间的双向耦合为气溶胶动力学和气溶胶质量的异质过程和气相光解速率的计算提供了一致的化学场。虽然目前版本的统一模型不包括矿物粉尘的预后治疗，我们包括它的影响，通过使用三维离线领域的光解和异质过程。我们还模拟了硫酸盐和硝酸盐气溶胶与矿物粉尘的基础上，目前可用的化学理解。考虑矿物粉尘吸收的HNO 3和湿清除冰上的HNO 3导致预测的气相HNO 3浓度和测量值之间的协议比以前的全球化学传输模型模拟，特别是在对流层中上部。作为化学和气溶胶之间的耦合的结果，气相和气溶胶物种的全球负担的预测响应非线性变化的NOx，NH3，和硫的排放量。
A unified tropospheric chemistry-aerosol model has been developed within the Goddard Institute for Space Studies general circulation model (GCM). The model includes a detailed simulation of tropospheric ozone-NOx-hydrocarbon chemistry as well as aerosols and aerosol precursors. Predicted aerosol species include sulfate, nitrate, ammonium, black carbon, primary organic carbon, and secondary organic carbon. The partitioning of ammonia and nitrate between gas and aerosol phases is determined by online thermodynamic equilibrium, and the formation of secondary organic aerosols is based on equilibrium partitioning and experimentally determined parameters. Two-way coupling between aerosols and chemistry provides consistent chemical fields for aerosol dynamics and aerosol mass for heterogeneous processes and calculations of gas-phase photolysis rates. Although the current version of the unified model does not include a prognostic treatment of mineral dust, we include its effects on photolysis and heterogeneous processes by using three-dimensional off-line fields. We also simulate sulfate and nitrate aerosols that are associated with mineral dust based on currently available chemical understanding. Considering both mineral dust uptake of HNO3 and wet scavenging of HNO3 on ice leads to closer agreement between predicted gas-phase HNO3 concentrations and measurements than in previous global chemical transport model simulations, especially in the middle to upper troposphere. As a result of the coupling between chemistry and aerosols, global burdens of both gas-phase and aerosol species are predicted to respond nonlinearly to changing emissions of NOx, NH3, and sulfur.