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Springer series in chemical physics

Ultrafast Two-Photon Free Induction Decay

Dorine Keusters, Peifang Tian, Warren S. Warren

Published Jan 1, 2003• 1 citation
Publisher
DOI
10.1007/978-3-642-59319-2_25

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Ultrafast Two-Photon Free Induction Decay

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Direct optical analogs of (two-dimensional) NMR experiments require detection of the phase of a coherence induced by a (series of) laser pulses, which is difficult [1]. Recently it was demonstrated that by using a phase coherent pulse pair created by an acousto optic pulse shaper (AOPS), this phase information can be detected conveniently and fast. [2, 3] This technique was demonstrated on the one-photon transitions in Rubidium [3]. The same technique can be used to detect a coherence that is induced by two photons simultaneously [4], as we demonstrate experimentally by detecting the two-photon free induction decay (TPFID) of Rb and coumarin. Since the two-photon transition in Rb is resonance enhanced, several types of coherences are induced in the two-photon process. An AOPS allows a separation of these types of coherences, and has potential advantages for suppressing scattered light.

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Ultrafast phase dynamics of coherent carriers in GaAs

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Ultrafast phase dynamics of free-induction decay for carriers in bulk GaAs is studied with differential-phase spectroscopy. The instantaneous phase shifts of the free-induction decay with respect to the excitation pulses are extracted from simultaneously recorded laser pulse autocorrelation and free-induction decay in GaAs. Ultrafast phase dynamics during and immediately after the femtosecond pulse excitation are numerically evaluated with optical Bloch equations using pump pulse and semiconductor exciton parameters as input. Good agreement of the theory with experiment is obtained.

Applied Physics Letters•Dec 7, 1998•13 citations
Direct optical analogs of (two-dimensional) NMR experiments require detection of the phase of a coherence induced by a (series of) laser pulses, which is difficult [1]. Recently it was demonstrated that by using a phase coherent pulse pair created by an acousto optic pulse shaper (AOPS), this phase information can be detected conveniently and fast. [2, 3] This technique was demonstrated on the one-photon transitions in Rubidium [3]. The same technique can be used to detect a coherence that is induced by two photons simultaneously [4], as we demonstrate experimentally by detecting the two-photon free induction decay (TPFID) of Rb and coumarin. Since the two-photon transition in Rb is resonance enhanced, several types of coherences are induced in the two-photon process. An AOPS allows a separation of these types of coherences, and has potential advantages for suppressing scattered light.
Ultrafast phase dynamics of free-induction decay for carriers in bulk GaAs is studied with differential-phase spectroscopy. The instantaneous phase shifts of the free-induction decay with respect to the excitation pulses are extracted from simultaneously recorded laser pulse autocorrelation and free-induction decay in GaAs. Ultrafast phase dynamics during and immediately after the femtosecond pulse excitation are numerically evaluated with optical Bloch equations using pump pulse and semiconductor exciton parameters as input. Good agreement of the theory with experiment is obtained.