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Frontiers in Optics

Coherent control on molecular systems by polarization shaped laser pulses

Albrecht Lindinger

Published Jan 1, 2011• 0 citations
Publisher

Abstract

Polarization pulse shaping is presented for coherent control of multi-photon ionization of alkali dimers. Sub-pulse parameters including polarization are controlled. These pulses are also transmitted through a photonic crystal fiber which is valuable for endoscopy.
DOI
10.1364/fio.2011.fwd5

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We demonstrate that the use of time-dependent light polarization opens a new level of control over quantum systems. With potassium dimer molecules from a supersonic molecular beam, we show that a polarization-shaped laser pulse increases the ionization yield beyond that obtained with an optimally shaped linearly polarized laser pulse. This is due to the different multiphoton ionization pathways in K2 involving dipole transitions which favor different polarization directions of the exciting laser field. This experiment is a qualitative extension of quantum control mechanisms which opens up new directions giving access to the three-dimensional temporal response of molecular systems.
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A femtosecond laser pulse can be tailored to control the two-photon transitions using the ultra-fast pulse-shaping technique. This paper theoretically and experimentally demonstrates that two-photon transitions in molecular system with broad absorption line can be effectively controlled by square phase-modulation in frequency domain, and the influence of all parameters characterizing the square phase-modulation on two-photon transitions is systemically investigated and discussed. The obtained results have potential application in nonlinear spectroscopy and molecular physics.