1. Acidity and the multiphase chemistry of atmospheric aqueous particles and clouds
- Author
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A. Tilgner, T. Schaefer, B. Alexander, M. Barth, J. L. Collett Jr., K. M. Fahey, A. Nenes, H. O. T. Pye, H. Herrmann, and V. F. McNeill
- Subjects
Atmospheric Science ,010504 meteorology & atmospheric sciences ,nonmetal redox kinetics ,QC1-999 ,Chemical reaction ,01 natural sciences ,Troposphere ,QD1-999 ,radical-induced oxidation ,0105 earth and related environmental sciences ,Aqueous solution ,heterogeneous sulfate production ,Chemistry ,Cloud systems ,Physics ,brown carbon formation ,aquated sulfur-dioxide ,Atmospheric research ,Trace gas ,Aerosol ,Deposition (aerosol physics) ,marine boundary-layer ,Environmental chemistry ,low-molecular-weight ,san-joaquin-valley ,catalyzed aldol condensation ,secondary organic aerosol - Abstract
The acidity of aqueous atmospheric solutions is a key parameter driving both the partitioning of semi-volatile acidic and basic trace gases and their aqueous-phase chemistry. In addition, the acidity of atmospheric aqueous phases, e.g., deliquesced aerosol particles, cloud, and fog droplets, is also dictated by aqueous-phase chemistry. These feedbacks between acidity and chemistry have crucial implications for the tropospheric lifetime of air pollutants, atmospheric composition, deposition to terrestrial and oceanic ecosystems, visibility, climate, and human health. Atmospheric research has made substantial progress in understanding feedbacks between acidity and multiphase chemistry during recent decades. This paper reviews the current state of knowledge on these feedbacks with a focus on aerosol and cloud systems, which involve both inorganic and organic aqueousphase chemistry. Here, we describe the impacts of acidity on the phase partitioning of acidic and basic gases and buffering phenomena. Next, we review feedbacks of different acidity regimes on key chemical reaction mechanisms and kinetics, as well as uncertainties and chemical subsystems with incomplete information., Finally, we discuss atmospheric implications and highlight the need for future investigations, particularly with respect to reducing emissions of key acid precursors in a changing world, and the need for advancements in field and laboratory measurements and model tools.