Summary: | The experimental work in this thesis is divided into two distinct parts. In both parts, broadband femtosecond laser pulses are "shaped" by adjusting the relative phase and amplitude of spectral components.
In the first set of experiments, time-dependent perturbation theory is used to show that the probability of a quantum transition in atomic rubidium can be substantially enhanced or suppressed using pulse shaping, compared to the probability of transition observed when a transform-limited or "flat phase" optical pulse is used. These enhancement or suppression effects are also demonstrated experimentally. As quantum interference (the material phase having been transferred from the optical phase) is used to enhance or diminish a particular final quantum state, this can be classified as a quantum coherent control experiment.
In the second set of experiments, an optical pulse is scattered into a train of pulses by a layered structure. The layered structure is used to simulate the effect of optical pulses travelling through certain types of complex media. One consequence of the disruption of a single pulse into a train of pulses is lower per-pulse peak intensity, and thus a greatly diminished nonlinear signal. It is shown that spectral pulse shaping (in phase only) is sufficient to pre-compensate for the scattering structure, allowing a single transform-limited pulse to be obtained at the output.
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