NONLINEAR OPTICS OF SEMICONDUCTOR AND MOLECULAR NANOSTRUCTURES - A COMMON PERSPECTIVE

A unified microscopic theoretical framework for the calculation of opt ical excitations in molecular and semiconductor materials is presented . The hierarchy of many-body density matrices for a pair-conserving ma ny-electron model and the Frenkel exciton model is rigorously truncate d to a given order in the radiation field. Closed equations of motion are derived For five generating functions representing the dynamics up to third order in the laser field including phonon degrees of freedom as well as all direct and exchange-type contributions to the Coulomb, interaction. By eliminating the phonons perturbatively the authors ob tain equations that, in the case of the many-electron system, generali ze the semiconductor Bloch equations, are particularly suited for the analysis of the interplay between coherent and incoherent dynamics inc luding many-body correlations, and lead to thermalized exciton (rather than single-particle) distributions at long times. A complete structu ral equivalence with the Frenkel exciton model of molecular materials is established.