Article ID Journal Published Year Pages File Type
5375959 Chemical Physics 2008 12 Pages PDF
Abstract
The properties of pulse-train induced multiphoton excitation in anharmonic progressions and the accumulation of population in a specific rung state are investigated by means of numerical simulations. It is shown how and under which conditions resonant π-pulses and multiple-π pulses can be split into trains of fractional π-pulses driving the same transition. Standardized train forms are considered with sub-pulses of equal (gaussian) shapes and equal, but tunable pulse-to-pulse delays and pulse-to-pulse phase shifts. The increased number of tuning parameters together with the handle on the number of sub-pulses gives rise to a remarkable variability in the control of state-specific population transfer, where simple zero-order estimates assist the determination of the parameters. Each π- or multiple-π pulse is replaced by a resonance locus in parameter space representing an infinite set of π-trains. The loci span extended frequency ranges that increase with increasing sub-pulse number. Their projection onto the frequency-field strength plane gives rise to elliptically shaped closed curves, termed resonance ridges, which replace the singular points mapped out by simple π- and multiple-π pulses. In the subspace of pulse-to-pulse delays and pulse-to-pulse phase shifts the resonance loci are characterized by phase recurrence relations, whose number and complexity increases with increasing numbers of sub-pulses. Our results indicate that pulse trains may be a powerful tool for the control of parallel or branching multiphoton transitions and for the elimination of background and intruder state population.
Related Topics
Physical Sciences and Engineering Chemistry Physical and Theoretical Chemistry
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