Studies in chemical reaction engineering: (a) The generation of temperature- and pressure-dependent absolute rate constants, (b) Local and global optimization of complex models, and (c) Turbulent reactive flows

This thesis is a study of three aspects of chemical reaction engineering. The first aspect concerns the computation of the absolute rate constants of elementary gas-phase reactions as a function of temperature and pressure. An inverse Laplace methodology is presented that derives microcanonical rate coefficients as function of vibrational and rotational energies from thermal data. The effect of pressure on multiple-well, multiple-channel elementary gas-phase reactions is studied by setting forth a full theoretical analysis of the master equation for intermolecular and intramolecular energy transfer. The second aspect of the thesis concerns optimization of functions. In regard to this aspect of the thesis an efficient dynamic programming method for the optimal control of large-scale problems is presented. Also presented is a new Bayesian method of global optimization of multimodal functions. The third and final aspect of the thesis is in regard to chemically reactive turbulent flow. Two stochastic Lagrangian models of turbulent flow are examined. The first lumps the hydrodynamics while treating the chemical-kinetics in detail. The second lumps the chemical-kinetics while treating the hydrodynamic flow-field in detail. The models are used to simulate the turbulence chemistry interactions in methane flames.