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Applied Physics B

Coherent transients as a highly sensitive probe for femtosecond pulse shapers

Wendel Wohlleben, J. Degert, Antoine Monmayrant, B. Chatel, Marcus Motzkus, B. Girard

Published Jun 15, 2004• 20 citations
Publisher
DOI
10.1007/s00340-004-1555-x

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We demonstrate a method for femtosecond, phase sensitive detection of optical polarization, using an acousto-optic pulse shaper to create a sequence of up to several hundred phase coherent pulses. Essential to this method is the ability of the acousto-optic pulse shaper to update the phase relation of the pulses in the sequence on a nanosecond timescale. The method is demonstrated by measuring the optical free induction decay’ of rubidium vapor, and can be particularly useful for experiments involving very low or very high optical densities. It can easily be extended to multidimensional spectroscopy.
Femtosecond phase-coherent two-dimensional (2D) spectroscopy has been experimentally demonstrated as the direct optical analog of 2D nuclear magnetic resonance. An acousto-optic pulse shaper created a collinear three-pulse sequence with well-controlled and variable interpulse delays and phases,which interacted with a model atomic system of rubidium vapor. The desired nonlinear polarization was selected by phase cycling (coadding experimental results obtained with different interpulse phases). This method may enhance our ability to probe the femtosecond structural dynamics of macromolecules.
We present experiments demonstrating high-resolution and wide-bandwidth coherent control of a four-level atomic system in a diamond configuration. A femtosecond frequency comb is used to excite a specific pair of two-photon transitions in cold 87Rb. The optical-phase-sensitive response of the closed-loop diamond system is studied by controlling the phase of the comb modes with a pulse shaper. Finally, the pulse shape is optimized resulting in a 256% increase in the two-photon transition rate by forcing constructive interference between the mode pairs detuned from an intermediate resonance.