Atmospheric Nucleation: Quantum Calculations, Kinetic Modeling, and Regional Scale Investigations

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This project seeks to improve knowledge of atmospheric nucleation through: (1) quantum mechanical studies of the thermodynamics of molecular clusters; (2) improvement of existing theories and development of new nucleation models; (3) comparison of kinetic modeling results with new data on atmospheric nucleation events; (4) a comprehensive study of particle formation in plumes; and (5) development of nucleation rate look-up tables, incorporation of computationally efficient nucleation modules in existing 3-dimensional air quality models, and an investigation of nucleation processes at regional scales. A novel approach that integrates a quantum mechanics study of cluster thermodynamics with kinetic nucleation modeling will be employed. This model will be used to improve and extend current binary homogeneous, ternary homogeneous, and ion-mediated nucleation theories, and to develop new theories of ternary ion-mediated nucleation and the enhancement of nucleation by organic compounds. The ion sign preference in binary and ternary gaseous mixtures will also be investigated. Recent measurements of pre-nucleation clusters, mobility spectra of cluster ions, and the charged fraction of freshly nucleated nanoparticles will be analyzed in the context of the model.Education and training opportunities will be provided for graduate and postdoctoral students. Nucleation rate look-up tables to be developed under this project will be made available to other investigators. Broader scientific impacts of this work include contributions to quantification of the effects of aerosol indirect radiative forcing on Earth's climate.