Ultrafast carrier and gain dynamics in strongly confined semiconductor quantum dots.

Abstract

This thesis investigates the carrier and gain dynamics of semiconductor quantum dots in the strong quantum confinement regime (i.e. the dot radius is smaller than the bulk excitonic Bohr radius). The materials under investigation are InP and CdSe. We can summarize our findings as follows: For the first time, the quantum confined ground state in InP quantum dots has been observed at room temperature by femtosecond spectral holeburning. This is the first confirmation of the observation of a strongly confined quantum dot made of III-V semiconductor materials. In CdSe quantum dots with a radius of half the bulk exciton Bohr radius, the carrier and gain dynamics have been investigated. The predicted phonon bottleneck, which should slow down carrier relaxation up to nanoseconds, has not been found. The carrier relaxation rates are rather on the order of 1 eV/ps. Gain has been found for the first time in strongly confined quantum dots. The existence of gain was proven by spectral holeburning in the gain region. The gain buildup and decay dynamics have been studied on a femtosecond and picosecond timescale. A multi-level model including biexcitons accounts for the gain formation. The model has been confirmed by three-beam spectral holeburning experiments and femtosecond pump-probe experiments with circularly polarized light. Some quantum dots did not show gain under high optical excitation but instead exhibited photodarkening. The carrier separation and localization dynamics of this photodarkening process has been studied on a femtosecond timescale. For the first time, the shift of the bleaching towards lower energy during the localization process could be observed on a femtosecond timescale. Finally, pulse propagation in bulk CdSe at multiple Pi-pulses has been studied. For the first time, strong evidence for the observation of self induced transparency in semiconductors has been found. Also, optical precursors, probably of nonlinear nature, have been found.