Chen Dean, Xavier Carlton, Clusius Petri, Nieminen Tuomo, Roldin Pontus, Qi Ximeng, Pichelstorfer Lukas, Kulmala Markku, Rantala Pekka, Aalto Juho, Sarnela Nina, Kolari Pasi, Keronen Petri, Rissanen Matti P, Taipale Ditte, Foreback Benjamin, Baykara Metin, Zhou Putian, Boy Michael
Institute for Atmospheric and Earth System Research/Physics, University of Helsinki P.O. Box 64 00014 Helsinki Finland
Institute for Atmospheric and Earth System Research/Forest Sciences, University of Helsinki P.O. Box 64 00014 Helsinki Finland.
Environ Sci Atmos. 2021 Aug 4;1(6):449-472. doi: 10.1039/d1ea00020a. eCollection 2021 Sep 23.
Major atmospheric oxidants (OH, O and NO) dominate the atmospheric oxidation capacity, while HSO is considered as a main driver for new particle formation. Although numerous studies have investigated the long-term trend of ozone in Europe, the trends of OH, NO and HSO at specific sites are to a large extent unknown. The one-dimensional model SOSAA has been applied in several studies at the SMEAR II station and has been validated by measurements in several projects. Here, we applied the SOSAA model for the years 2007-2018 to simulate the atmospheric chemical components, especially the atmospheric oxidants OH and NO, as well as HSO at SMEAR II. The simulations were evaluated with observations from several shorter and longer campaigns at SMEAR II. Our results show that daily OH increased by 2.39% per year and NO decreased by 3.41% per year, with different trends of these oxidants during day and night. On the contrary, daytime sulfuric acid concentrations decreased by 2.78% per year, which correlated with the observed decreasing concentration of newly formed particles in the size range of 3-25 nm with 1.4% per year at SMEAR II during the years 1997-2012. Additionally, we compared our simulated OH, NO and HSO concentrations with proxies, which are commonly applied in case a limited number of parameters are measured and no detailed model simulations are available.
主要的大气氧化剂(羟基自由基、原子氧和一氧化氮)主导着大气氧化能力,而硫酸氢根被认为是新粒子形成的主要驱动因素。尽管众多研究调查了欧洲臭氧的长期趋势,但特定地点的羟基自由基、一氧化氮和硫酸氢根的趋势在很大程度上仍不为人知。一维模型SOSAA已在几项针对 SMEAR II 站的研究中得到应用,并在多个项目的测量中得到验证。在此,我们应用SOSAA模型对2007 - 2018年进行模拟,以模拟大气化学成分,特别是大气氧化剂羟基自由基和一氧化氮,以及SMEAR II 处的硫酸氢根。利用SMEAR II 站几次长短不一的观测活动所获得的观测数据对模拟结果进行了评估。我们的结果表明,每日羟基自由基浓度每年增加2.39%,一氧化氮浓度每年下降3.41%,且这些氧化剂在白天和夜晚呈现出不同的趋势。相反,白天硫酸浓度每年下降2.78%,这与1997 - 2012年期间SMEAR II 站观测到的3 - 25纳米粒径范围内新形成粒子浓度每年下降1.4%相关。此外,我们将模拟得到的羟基自由基、一氧化氮和硫酸氢根浓度与替代指标进行了比较,这些替代指标通常在测量参数数量有限且没有详细模型模拟可用的情况下应用。