Exploration of the influence of environmental conditions on secondary organic aerosol formation and organic species properties using explicit simulations: development of the VBS-GECKO parameterization

• Published in: Atmospheric chemistry and physics Vol. 18; no. 18; pp. 13411 - 13428
• Main Authors: Lannuque, Victor, Camredon, Marie, Couvidat, Florian, Hodzic, Alma, Valorso, Richard, Madronich, Sasha, Bessagnet, Bertrand, Aumont, Bernard
• Format: Journal Article
• Language: English
• Published: Katlenburg-Lindau Copernicus GmbH 21.09.2018; European Geosciences Union; Copernicus Publications
• Subjects: Aerosol formation; Aerosols; Air pollution; Air quality; Air quality models; Alkanes; Alkenes; Artefacts; Atmosphere; Atmospheric models; Atomic properties; Benzene; Chemical transport; Chemistry; Computer simulation; Enthalpy; Environmental aspects; Environmental conditions; Environmental Sciences; Evolution; Exploration; Geckos; Henrys law; Humidity; Hydrocarbons; Kinetics; Limonene; Mathematical models; Modelling; Nitrogen compounds; Optimization; Organic chemistry; Organic compounds; Organic loading; Oxidation; Oxides; p-Xylene; Parameterization; Precursors; Properties; Properties (attributes); Reaction kinetics; Secondary aerosols; Simulation; Three dimensional models; Toluene; Vaporization; Volatility; Xylene; α-Pinene; OXIDATION; RADICAL-INITIATED REACTIONS; TROPOSPHERIC DEGRADATION; CHEMICAL MECHANISM; VAPOR-PRESSURE; MOLECULAR-STRUCTURE; PURE COMPONENT PROPERTIES; VOLATILITY BASIS-SET; SOA FORMATION; PARTICULATE MATTER
• ISSN: 1680-7324; 1680-7316; 1680-7324
• DOI: 10.5194/acp-18-13411-2018

Atmospheric chambers have been widely used to study secondary organic aerosol (SOA) properties and formation from various precursors under different controlled environmental conditions and to develop parameterization to represent SOA formation in chemical transport models (CTMs). Chamber experiments are however limited in number, performed under conditions that differ from the atmosphere and can be subject to potential artefacts from chamber walls. Here, the Generator for Explicit Chemistry and Kinetics of Organics in the Atmosphere (GECKO-A) modelling tool has been used in a box model under various environmental conditions to (i) explore the sensitivity of SOA formation and properties to changes on physical and chemical conditions and (ii) develop a volatility basis set (VBS)-type parameterization. The set of parent hydrocarbons includes n-alkanes and 1-alkenes with 10, 14, 18, 22 and 26 carbon atoms, α-pinene, β-pinene and limonene, benzene, toluene, o-xylene, m-xylene and p-xylene. Simulated SOA yields and their dependences on the precursor structure, organic aerosol load, temperature and NOx levels are consistent with the literature. GECKO-A was used to explore the distribution of molar mass, vaporization enthalpy, OH reaction rate and Henry's law coefficient of the millions of secondary organic compounds formed during the oxidation of the different precursors and under various conditions. From these explicit simulations, a VBS-GECKO parameterization designed to be implemented in 3-D air quality models has been tuned to represent SOA formation from the 18 precursors using GECKO-A as a reference. In evaluating the ability of VBS-GECKO to capture the temporal evolution of SOA mass, the mean relative error is less than 20 % compared to GECKO-A. The optimization procedure has been automated to facilitate the update of the VBS-GECKO on the basis of the future GECKO-A versions, its extension to other precursors and/or its modification to carry additional information.