Formation and fate of secondary organic aerosol components in the atmosphere: explicit modeling at global scale / vorgelegt von Felix Wieser. Wuppertal, [2025]
Inhalt
- Introduction
- Atmospheric aerosols
- Organic aerosol sources and sinks
- Phase partitioning
- Organic aerosols in models
- Thesis objective
- Model introduction
- Box model: CAABA/MECCA
- Global model: the Modular Earth Submodel System
- Chemistry submodels
- Aerosol and partitioning submodels
- Chemical kinetics
- Oxidation of gaseous secondary organic aerosol precursors
- Development of a chemical mechanism to improve secondary organic aerosol formation
- Applied gas and aqueous-phase structure-activity relationships
- Volatile organic compounds from biogenic origin
- Volatile organic compounds from anthropogenic origin
- Model-Model comparison and IEPOX concentrations against observations
- Simulation setup model-model comparison
- Low-volatile organic compound mixing ratio
- Low-volatile organic compound O/C ratio
- Measured and modeled IEPOX secondary organic aerosol tracers
- Model-chamber comparison
- Phase partitioning between gas and aqueous phase
- General
- Henry's law
- Estimation of Henry's law constants
- Estimation of the temperature dependence of Henry's law constants
- Henry's law constants for non-water solvents
- Estimation of Henry's law constants
- Henry's law constants for non-ideal solutions
- Calculation of Henry's law constants based on saturation vapor pressure and infinity dilution activity coefficients
- Estimation of saturation vapor pressures
- Estimation of activity coefficient at infinite dilution
- Estimation of the temperature dependency of Henry's law constants
- Dependence of model results on partitioning coefficients
- Aqueous-phase oxidation
- Development of an aqueous-phase oxidation mechanism routine
- The aqueous-phase oxidation mechanism generator
- Initial setup
- Input handling
- Reaction generation process
- Data post-processing
- Reaction types
- Comparison to literature mechanism generators
- Comparison between generated mechanisms and literature mechanisms proposed based on measurements
- Application of the extended mechanisms to MESSy
- Model configuration
- Secondary organic aerosol burden
- Secondary organic aerosol mass concentrations
- Organic aerosol mass versus station data of the EPA/IMPROVE, EMEP and EANET networks
- Vertical distribution of secondary organic aerosol
- Secondary organic aerosol O/C ratio
- Organics in cloud and rain droplets
- Oxidant concentrations
- Summary and outlook
- Secondary organic aerosols from gaseous precursors
- Phase partitioning between gas and aqueous phase
- Aqueous-phase oxidation
- Outlook
- Appendix
- Additional simulation results
- Estimated Henry's law solubility constants and temperature dependencies
- Subset of the estimated saturation vapor pressures and infinity dilution activity coefficients
- Bibliography