Theoretical Studies of Ion-Molecule and Ion-Surface Collisions
Abstract
This project was concerned with the development of theoretical methods for describing atomic and molecular processes that are important in high performance combustion applications, in plasmas, in the upper atmosphere, and in Low Earth Orbit. The methods involved a combination of electronic structure and molecular dynamics approaches, with emphasis on methods for describing the motions of nuclei where forces are derived directly from electronic structure theory. For gas-phase processes, these so-called direct dynamics methods used density functional theory forces, while for gas-surface processes, mixed quantum/classical methods were developed. A particular focus of the research was on electron-molecule collisions that lead to fragmentation into neutral radical species. Here a theory of electron-impact-excitation-dissociation was developed, and used to study the electron-induced fragmentation of methane as well as its VUV photodissociation. The direct dynamics technology was also used to study a number of bimolecular reactions at hyperthermal energies. The studies of the reactions of atoms and ions with liquids focused on O and F atoms reacting with squalane or ionic liquids. Other studies considered the reaction of atomic oxygen with graphite and graphite oxide surfaces. In all of these studies detailed comparisons with experiment were made, providing a key link between what is observed and the underlying reaction mechanisms.
Document Details
- Document Type
- Technical Report
- Publication Date
- Dec 07, 2009
- Accession Number
- ADA548167
Entities
People
- George C. Schatz
Organizations
- Northwestern University