Pospisilova V, Lopez-Hilfiker F D, Bell D M, El Haddad I, Mohr C, Huang W, Heikkinen L, Xiao M, Dommen J, Prevot A S H, Baltensperger U, Slowik J G
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland.
Tofwerk AG, 3600 Thun, Switzerland.
Sci Adv. 2020 Mar 13;6(11):eaax8922. doi: 10.1126/sciadv.aax8922. eCollection 2020 Mar.
Highly oxygenated organic molecules (HOMs) are formed from the oxidation of biogenic and anthropogenic gases and affect Earth's climate and air quality by their key role in particle formation and growth. While the formation of these molecules in the gas phase has been extensively studied, the complexity of organic aerosol (OA) and lack of suitable measurement techniques have hindered the investigation of their fate post-condensation, although further reactions have been proposed. We report here novel real-time measurements of these species in the particle phase, achieved using our recently developed extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF). Our results reveal that condensed-phase reactions rapidly alter OA composition and the contribution of HOMs to the particle mass. In consequence, the atmospheric fate of HOMs cannot be described solely in terms of volatility, but particle-phase reactions must be considered to describe HOM effects on the overall particle life cycle and global carbon budget.
高氧化态有机分子(HOMs)由生物源和人为源气体氧化形成,通过在颗粒物形成和生长中的关键作用影响地球气候和空气质量。虽然气相中这些分子的形成已得到广泛研究,但有机气溶胶(OA)的复杂性以及缺乏合适的测量技术阻碍了对其凝结后归宿的研究,尽管已有进一步反应的相关提议。我们在此报告利用最近开发的萃取电喷雾电离飞行时间质谱仪(EESI - TOF)实现的对这些颗粒相物种的新型实时测量。我们的结果表明,凝聚相反应迅速改变OA组成以及HOMs对颗粒质量的贡献。因此,HOMs在大气中的归宿不能仅用挥发性来描述,还必须考虑颗粒相反应以描述HOMs对整个颗粒生命周期和全球碳收支的影响。