MULTI-STRUCTURAL AND MULTI-PATH VARIATIONAL TRANSITION STATE THEORY FOR PREDICTING RATE CONSTANTS FOR MECHANISTIC STUDDES OF BIOFUELS COMBUSTION

摘要

The atomistic simulation of reactions of complex molecules, such as those involved in biofuel combustion, requires one to treat anharmonic, coupled torsions in both reactants and transition states, along with the accompanying torsional anharmonicity, and to consider reaction along more than one reaction path. We have developed methods for including multiple structures, torsional anharmonicity, and multiple paths in reaction rate calculations that include both variationally optimized transition states and multidimensional tunneling. I will review the theory and present selected applications based on our recently developed density functional approximations such as M08-HX.