Computational Prediction of Kinetic Rate Constants

A core component of aerospace manufacturing is based on cutting-edge materials used in extreme environments. Chemical kinetics models are vital for interpreting experimental measurements and predicting the behavior of these complex systems. For many applications, the reaction rates for all required chemical processes are unknown. We propose a versatile user-friendly computational package for calculating chemical rate constants based on electronic structure theory, reaction dynamics, and transition state theory. This will be accomplished by enhancing the Extensible Computational Chemistry Environment (Ecce), a state-of-the-art graphical user interface, to integrate kinetics calculations based on the electronic structure code NWChem, the dynamics code VENUS, the transition state theory code POLYRATE, and the quantum state specific quasiclassical trajectory method. Together, this set of codes will allow the user to calculate rate constants from high-level quantum calculations within a single environment, while providing a realistic prediction of the inherent calculation errors. In Phase I, we will demonstrate proof of principle by computing reaction rate constants through an enhanced Ecce. In Phase II, we will integrate chemical rate constant predictions into Ecce forming the Ab initio Transition state Or Molecular dynamics Simulations for Chemical Rate Constants (ATOMS-CRC) Toolkit.