First-Principles-Based Development of Kinetic Mechanisms in Chemically Active Light-Emitting Nonthermal Plasmas and Gases

Abstract

Recent progress in several related research areas such as first‐principles electronic‐structure calculations of atoms and diatomic molecules, theory of elementary processes, kinetics, and numerical engineering, and also continued exponential growth in computational resources enhanced by recent advances in massively parallel computing have opened the possibility of directly designing kinetics mechanisms to describe chemical processes and light emission in such complex media as nonequilibrium plasmas and reacting gases. It is important that plasma and combustion kinetics can be described in the framework of this direct approach to a sufficiently high accuracy, which makes it an independent predictive research tool complementary to experimental techniques. This paper demonstrates the capabilities of the first‐principles based approach to develop kinetic mechanisms. Two examples are discussed in detail: (1) the mechanism of hydrocarbon fuel combustion at high temperatures and (2) light emission in non‐thermal glow discharge plasma of metal halides; special attention is paid to a comparison of the results obtained at every level of system description with the appropriate experimental data. In house software tools that can be used in such multilevel theoretical works are discussed as well.