Liouville-space descriptions for intense-field coherent electromagnetic interactions

Abstract

Liouville-space (reduced-density-operator) descriptions are developed for resonant and coherent electromagnetic interactions of quantized electronic systems, taking into account environmental decoherence and relaxation phenomena. Applications of interest include electromagnetically-induced transparency and related pump-probe optical phenomena in many-electron atomic systems (in electron-ion beam interactions, gases, and high-temperature plasmas) and semiconductor materials (bulk crystals and nanostructures). Time-domain (equation-of-motion) and frequency-domain (resolvent-operator) formulations are developed in a unified manner. The standard Born (lowest-order perturbationtheory) and Markov (short-memory-time) approximations are systematically introduced within the framework of the general non-perturbative and non-Markovian formulations. A preliminary semiclassical description of the entire electromagnetic interaction is introduced. Compact Liouville-space operator expressions are derived for the linear and the general (n'th order) non-linear electromagnetic-response tensors occurring in a perturbation-theory treatment of the semiclassical electromagnetic interaction. These expressions can be evaluated for coherent initial electronic excitations and for the full tetradic-matrix form of the Liouville-space self-energy operator representing the environmental interactions in the Markov approximation. Intense-field electromagnetic interactions are treated by means of an alternative, non-perturbative method, which is based on a Liouville-space Floquet-Fourier representation of the reduced density operator. Electron-electron quantum correlations are treated by the introduction of a cluster decomposition of the reduced density operator and a coupled hierarchy of reduced-density-operator equations.