Dynamics of O(3P) Reactions with Gaseous Liquid and Solid Hydrocarbons
Abstract
Prof. Hase has studied the reaction dynamics of oxygen atoms (triplet P state) with alkane hydrocarbons. In the initial phase, highly accurate ab initio quantum chemistry calculations (CASSCF, CASPT2, MRCI, with cc-pVTZ and cc-pVQZ basis sets) were applied to model reactions, including 0 + ethane and related reactions. In the second phase, a semiempirical quantum chemistry method, PM3-SRP, was developed by modifying and reparametrizing the standard PM3 method to fit the ab initio data. In the application phase, PM3-SRP was used in quasiclassical trajectory calculations to compute the dynamics of O + ethane at 5 eV collision energy, and propane monomer and tetramer at less than 2 eV collision energy. The trajectory results are in good agreement with experiment where comparison is possible. The O + ethane calculations at 5 eV predict the formation of a large number of products, many of which result from unimolecular decomposition of initially formed products. In the low energy 0 + propane calculations, the predicted distribution of vibrational and rotation energy in the OH product is in excellent agreement with experiment. In addition, energy transfer and physisorption of 0 atoms on self-assembled alkane monolayers were studied by computing inelastic scattering dynamics.
Document Details
- Document Type
- Technical Report
- Publication Date
- Mar 01, 2006
- Accession Number
- ADA448198
Entities
People
- William L Hase
Organizations
- Texas Tech University Department of Chemistry and Biochemistry