Time-dependent 3D simulations of tropospheric ozone depletion events in the Arctic spring using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem)
Time-dependent 3D simulations of tropospheric ozone depletion events in the Arctic spring using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem)
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DOI：
10.5194/acp-21-7611-2021
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发表时间：
2021-05
影响因子：
6.3
通讯作者：
M. Herrmann;H. Sihler;U. Friess;T. Wagner;U. Platt;E. Gutheil
中科院分区：
文献类型：
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作者：
M. Herrmann;H. Sihler;U. Friess;T. Wagner;U. Platt;E. Gutheil
抽象。对流层溴释放和臭氧消耗事件（ODEs），因为它们通常发生在北极春季使用的区域模型的基础上的开放源代码软件包天气研究和预报模型加上化学（WRF-Chem）。为此，MOZART（臭氧和相关化学示踪剂模型）-MOSAIC（模拟气溶胶相互作用和化学模型）化学反应机制通过溴和氯反应以及通过雪表面上的非均相反应的活性溴排放机制进行了扩展。模拟区域面积为5040 km×4960 km，以阿拉斯加州的Utqiagivik（以前的巴罗）北部为中心，时间间隔为2009年2月至5月。对不同强度的溴排放进行了几次模拟，并通过与臭氧混合比的现场测量和臭氧探测仪测量进行比较，以及与全球臭氧监测实验-2号卫星仪器的对流层BrO垂直柱密度进行比较来进行评价。基础溴排放方案包括由于臭氧氧化溴化物而直接排放溴。基本排放率的模拟结果与观测结果吻合良好;然而，排放速度加快50%的模拟表现得更好。溴排放由于溴氧化臭氧被发现是重要的溴爆炸提供了一个初始的种子。溴释放由于N2 O 5被认为是重要的，从2月到3月中旬，但无关紧要。模拟BrO与原位和多轴差分光学吸收光谱（MAX-DOAS）数据的比较提示，在陆地或海岸附近的溴释放和再循环机制缺失。卤素化学的考虑大大提高了臭氧混合比的预测相对于观察。气象轻推是一个很好的预测ODE在3个月的时间是必不可少的。
Abstract. Tropospheric bromine release and ozone depletion events (ODEs) as they commonly occur in the Arctic spring are studied using a regional model based on the open-source software package Weather Research and Forecasting model coupled with Chemistry (WRF-Chem). For this purpose, the MOZART (Model for Ozone and Related chemical Tracers)–MOSAIC (Model for Simulating Aerosol Interactions and Chemistry) chemical reaction mechanism is extended by bromine and chlorine reactions as well as an emission mechanism for reactive bromine via heterogeneous reactions on snow surfaces. The simulation domain covers an area of 5040 km×4960 km , centered north of Utqiaġvik (formerly Barrow), Alaska, and the time interval from February through May 2009. Several simulations for different strengths of the bromine emission are conducted and evaluated by comparison with in situ and ozone sonde measurements of ozone mixing ratios as well as by comparison with tropospheric BrO vertical column densities (VCDs) from the Global Ozone Monitoring Experiment-2 (GOME-2) satellite instrument. The base bromine emission scheme includes the direct emission of bromine due to bromide oxidation by ozone. Results of simulations with the base emission rate agree well with the observations; however, a simulation with 50 % faster emissions performs somewhat better. The bromine emission due to bromide oxidation by ozone is found to be important to provide an initial seed for the bromine explosion. Bromine release due to N2O5 was found to be important from February to mid March but irrelevant thereafter. A comparison of modeled BrO with in situ and multi-axis differential optical absorption spectroscopy (MAX-DOAS) data hints at missing bromine release and recycling mechanisms on land or near coasts. A consideration of halogen chemistry substantially improves the prediction of the ozone mixing ratio with respect to the observations. Meteorological nudging is essential for a good prediction of ODEs over the 3-month period.