In recent years, impressive advances have been made in coherent control. Most current experiments rely on adaptive feedback control, which often generates optical fields too complicated to allow for mechanistic interpretation. We will use sophisticated models based on Multichannel Quantum Defect Theory (MQDT) to simulate experiments in benchmark molecules H2, NO, H2O, HCO and NO2 with spectroscopic accuracy. This will allow us to examine control mechanisms in detail and develop analytic tools for a broad range of time-resolved and ultrafast experiments. Initial studies will aim to control the branching ratio between dissociation and ionization in NO, in collaboration with experiments by Dr. Pratt at ANL (USA) and Prof. Fielding at UCL (UK). We will also simulate recent experiments by Prof. Suzuki at RIKEN (JP), who observed the time-resolved photoelectron distribution from dynamically aligned NO molecules. Subsequently, we will extend the theoretical model to include explicitly the effect of static electric fields and the dynamics associated with long-range vibrational states. The former will allow us to simulate a new category of quantum control experiments being developed, while the latter will allow analysis of recently observed spectra in H2 by Prof. Ubachs at VU (NE), and may open the door to coherent control experiments in that spectral region. The final, and main, stage of the project will investigate weak and strong field coherent control and ultrafast spectroscopy in polyatomic molecules, such as HCO, H2O and NO2. These polyatomic systems provide a major step towards real chemical complexity, and, in addition to competition between ionization and dissociation, rotational alignment and selective dynamics, they offer an example of chemical rearrangement reactions. We should be able to compare our calculations directly with experiments done by Dr. Pratt in order to uncover the underlying principles of quantum dynamics and coherent control.
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