当前位置: X-MOL 学术Atmos. Chem. Phys. › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
Secondary aerosol formation in marine Arctic environments: a model measurement comparison at Ny-Ålesund
Atmospheric Chemistry and Physics ( IF 5.2 ) Pub Date : 2022-08-04 , DOI: 10.5194/acp-22-10023-2022
Carlton Xavier , Metin Baykara , Robin Wollesen de Jonge , Barbara Altstädter , Petri Clusius , Ville Vakkari , Roseline Thakur , Lisa Beck , Silvia Becagli , Mirko Severi , Rita Traversi , Radovan Krejci , Peter Tunved , Mauro Mazzola , Birgit Wehner , Mikko Sipilä , Markku Kulmala , Michael Boy , Pontus Roldin

In this study, we modeled the aerosol particle formation along air mass trajectories arriving at the remote Arctic research stations Gruvebadet (67 m a.s.l.) and Zeppelin (474 m a.s.l.), Ny-Ålesund, during May 2018. The aim of this study was to improve our understanding of processes governing secondary aerosol formation in remote Arctic marine environments. We run the Lagrangian chemistry transport model ADCHEM, along air mass trajectories generated with FLEXPART v10.4. The air masses arriving at Ny-Ålesund spent most of their time over the open ice-free ocean. In order to capture the secondary aerosol formation from the DMS emitted by phytoplankton from the ocean surface, we implemented a recently developed comprehensive DMS and halogen multi-phase oxidation chemistry scheme, coupled with the widely used Master Chemical Mechanism (MCM).The modeled median particle number size distributions are in close agreement with the observations in the marine-influenced boundary layer near-sea-surface Gruvebadet site. However, while the model reproduces the accumulation mode particle number concentrations at Zeppelin, it overestimates the Aitken mode particle number concentrations by a factor of ∼5.5. We attribute this to the deficiency of the model to capture the complex orographic effects on the boundary layer dynamics at Ny-Ålesund. However, the model reproduces the average vertical particle number concentration profiles within the boundary layer (0–600 m a.s.l.) above Gruvebadet, as measured with condensation particle counters (CPCs) on board an unmanned aircraft system (UAS).The model successfully reproduces the observed Hoppel minima, often seen in particle number size distributions at Ny-Ålesund. The model also supports the previous experimental findings that ion-mediated H2SO4–NH3 nucleation can explain the observed new particle formation in the marine Arctic boundary layer in the vicinity of Ny-Ålesund. Precursors resulting from gas- and aqueous-phase DMS chemistry contribute to the subsequent growth of the secondary aerosols. The growth of particles is primarily driven via H2SO4 condensation and formation of methane sulfonic acid (MSA) through the aqueous-phase ozonolysis of methane sulfinic acid (MSIA) in cloud and deliquescent droplets.

中文翻译:

北极海洋环境中的二次气溶胶形成:新奥勒松的模型测量比较

在这项研究中,我们模拟了 2018 年 5 月期间到达位于新奥勒松的偏远北极研究站 Gruvebadet(67 m asl)和 Zeppelin(474 m asl)的气溶胶颗粒形成。本研究的目的是提高我们对偏远北极海洋环境中控制二次气溶胶形成过程的理解。我们沿着使用 FLEXPART v10.4 生成的气团轨迹运行拉格朗日化学传输模型 ADCHEM。到达新奥勒松的气团大部分时间都在开阔的无冰海洋上空度过。为了从海洋表面的浮游植物释放的 DMS 中捕获二次气溶胶形成,我们实施了最近开发的综合 DMS 和卤素多相氧化化学方案,以及广泛使用的主化学机制 (MCM)。模拟的中值粒径分布与近海面 Gruvebadet 站点受海洋影响的边界层的观测结果非常一致。然而,虽然该模型再现了 Zeppelin 的累积模式粒子数浓度,但它高估了 Aitken 模式粒子数浓度一个因子 ~5.5 . 我们将此归因于模型在捕捉复杂地形对 Ny-Ålesund 边界层动力学的影响方面的缺陷。然而,该模型再现了 Gruvebadet 上方边界层(0-600 m asl)内的平均垂直粒子数浓度分布,这是用无人驾驶飞机系统(UAS)上的冷凝粒子计数器(CPC)测量的。该模型成功地再现了观察到 Hoppel 极小值,通常出现在 Ny-Ålesund 的粒径分布中。该模型还支持了之前的实验结果,即离子介导的 H 2 SO 4 –NH 3成核作用可以解释在 Ny-Ålesund 附近的北极海洋边界层中观察到的新粒子形成。由气相和水相 DMS 化学产生的前体有助于后续气溶胶的生长。颗粒的生长主要通过 H 2 SO 4冷凝和通过甲烷亚磺酸 (MSIA) 在云和潮解液滴中的水相臭氧分解形成甲烷磺酸 (MSA) 来驱动。
更新日期:2022-08-05
down
wechat
bug