Abstract
Quantum control of the S(2)-->S(1) internal conversion in a complete 24-mode dimensionality model of pyrazine is demonstrated. The fully quantum mechanical study makes use of the recently developed "QP algorithm" for performing accurate computations of projected quantum dynamics and the role of overlapping resonances in control. The results are extremely encouraging, demonstrating active control over internal conversion so as to almost completely suppress the process over time scales of approximately 50-100 fs [well in excess of the natural internal conversion times (approximately 20 fs)] or to accelerate it to complete internal conversion in less than 5 fs. A number of new diagnostics are introduced to demonstrate the significance of overlapping-resonance contributions to control. Control is far better than for a reduced dimensionality model of pyrazine, presumably because of the increased degree of overlap between bound state resonances existing in the full dimensionality case.
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