Non-resonant dynamic stark control of vibrational motion with optimized laser pulses.

J Chem Phys

Department of Chemistry, Technical University of Denmark, Building 207, DK-2800 Kongens Lyngby, Denmark.

Published: June 2016

The term dynamic Stark control (DSC) has been used to describe methods of quantum control related to the dynamic Stark effect, i.e., a time-dependent distortion of energy levels. Here, we employ analytical models that present clear and concise interpretations of the principles behind DSC. Within a linearly forced harmonic oscillator model of vibrational excitation, we show how the vibrational amplitude is related to the pulse envelope, and independent of the carrier frequency of the laser pulse, in the DSC regime. Furthermore, we shed light on the DSC regarding the construction of optimal pulse envelopes - from a time-domain as well as a frequency-domain perspective. Finally, in a numerical study beyond the linearly forced harmonic oscillator model, we show that a pulse envelope can be constructed such that a vibrational excitation into a specific excited vibrational eigenstate is accomplished. The pulse envelope is constructed such that high intensities are avoided in order to eliminate the process of ionization.

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http://dx.doi.org/10.1063/1.4954663DOI Listing

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