Picosecond nonlinear optical studies of exciton relaxation in multiple quantum well structures.

This work presents new results of experimental studies of exciton relaxation in GaAs/AlGaAs multiple quantum well materials, using transient nonlinear laser spectroscopy techniques. In the low excitation regime, effective optical Bloch equations similar to the density matrix formalism of a two-level system describe the response. Solutions of these equations appropriate for three-pulse scattering studies are presented, along with a discussion of new experimental techniques used in this work. Non-ideal conditions present in the molecular beam epitaxy growth process introduce monolayer fluctuations in the quantum well thickness, leading to inhomogeneous broadening and exciton localization at sites of minimum energy. Localized excitons are separated in energy from extended, quasi-delocalized states by the mobility edge. Studies of localized exciton relaxation indicate that these excitons relax on a much slower timescale than delocalized excitons. The temperature dependence of the localized exciton relaxation rate shows that above 15K, the excitons are thermally activated to extended states above the mobility edge. Below 15K the excitons relax by phonon assisted migration between localization sites. For temperatures above 5K, and for exciton energies greater than 1 meV below line center, an extra dephasing mechanism characterizes the exciton relaxation. The inhomogeneous broadening of the exciton leads to the emission of stimulated photon echoes in the experimental geometry used in this work. The time-resolved emission demonstrates the stimulated photon echo nature at low excitation densities. At higher excitation densities, the decay dynamics is more complex. The time-resolved emission shows the presence of a stimulated photon echo and a free polarization decay. This unusual result suggests that both a homogeneous and an inhomogeneous exciton distribution comprise the exciton resonance. Exciton relaxation at low excitation densities represents the interaction of the exciton with the lattice. At higher excitation densities, exciton-exciton and exciton-free carrier interactions modify the relaxation rates. The dependence of the exciton relaxation rate on excitation density shows that many-body effects play an important role in the exciton physics. Free carrier interactions are more efficient at increasing the exciton relaxation rate; both types of interactions are more important in quantum well systems than in bulk materials.PhDPhysicsUniversity of Michigan, Horace H. Rackham School of Graduate Studieshttp://deepblue.lib.umich.edu/bitstream/2027.42/105307/1/9116322.pdfDescription of 9116322.pdf : Restricted to UM users only