Assessment of the GECKO-A Modeling Tool and Simplified 3D Model Parameterizations for SOA Formation

Abstract:

Explicit chemical mechanisms aim to embody the current knowledge of the transformations occurring in the atmosphere during the oxidation of organic matter. These explicit mechanisms are therefore useful tools to explore the fate of organic matter during its tropospheric oxidation and examine how these chemical processes shape the composition and properties of the gaseous and the condensed phases. Furthermore, explicit mechanisms provide powerful benchmarks to design and assess simplified parameterizations to be included 3D model. Nevertheless, the explicit mechanism describing the oxidation of hydrocarbons with backbones larger than few carbon atoms involves millions of secondary organic compounds, far exceeding the size of chemical mechanisms that can be written manually. Data processing tools can however be designed to overcome these difficulties and automatically generate consistent and comprehensive chemical mechanisms on a systematic basis. The Generator for Explicit Chemistry and Kinetics of Organics in the Atmosphere (GECKO-A) has been developed for the automatic writing of explicit chemical schemes of organic species and their partitioning between the gas and condensed phases. GECKO-A can be viewed as an expert system that mimics the steps by which chemists might develop chemical schemes. GECKO-A generates chemical schemes according to a prescribed protocol assigning reaction pathways and kinetics data on the basis of experimental data and structure-activity relationships. In its current version, GECKO-A can generate the full atmospheric oxidation scheme for most linear, branched and cyclic precursors, including alkanes and alkenes up to C25. Assessments of the GECKO-A modeling tool based on chamber SOA observations will be presented. GECKO-A was recently used to design a parameterization for SOA formation based on a Volatility Basis Set (VBS) approach. First results will be presented.