Femtosecond Transient Stimulated Emission Pumping: Theory and Experiment

Hunziker, Lukas E.; Ludowise, P.; Price, William S.; Morgen, Mike; Blackwell, Megan; Chen, Y.

doi:10.1142/9789812831880_0002

Cited by 3 publications

(1 citation statement)

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“…The fs probing and signal detection mechanism can be realized in various ways. These include, for probing, the methodology of laser-induced fluorescence (LIF), − absorption, mass spectrometry with multiphoton ionization (MPI), ,− photoelectron kinetic energy and ZEKE, and stimulated emission pumping . Nonlinear optical four-wave-mixing (FWM) techniques, like degenerate FWM (DFWM), provide an additional and significant probing method, especially for generalization of absorption techniques in gas-phase reaction dynamics.…”

Section: Introductionmentioning

confidence: 99%

Femtosecond Real-Time Probing of Reactions. 19. Nonlinear (DFWM) Techniques for Probing Transition States of Uni- and Bimolecular Reactions

1996

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Degenerate four-wave mixing (DFWM), using ∼60 femtosecond (fs) laser pulses, is introduced to study transition-state dynamics of chemical reactions in the gas phase. The ultrafast techniques are applied to a range of systems, atomic, unimolecular, and bimolecular. It is shown how fs DFWM can be incorporated in different temporal pulse schemes to extract the dynamics. The DFWM beams are configured in a folded boxcar geometry, producing a spatially separated, background-free, femtosecond signal pulse. Aspects of the technique, such as absorption, are investigated. We have taken advantage of the relatively broad spectral width of the fs pulses and extended the techniques to two-color grating experiments in the gas phase. The unimolecular system, NaI, provided a means of testing this new approach. Our experimental observations of the wave packet motion are in excellent agreement with results obtained using laser-induced fluorescence (LIF). A control experiment was also performed on this system, demonstrating the advantages of the nonlinear technique. Bimolecular reactions were initiated for the system Na+H 2 . Atomic sodium was investigated with fs DFWM and the oscillatory wave packet behavior (2 ps period) was observed, corresponding to the fine structure splitting of the 3p level (17.2 cm -1 ). We also explored the application of fs DFWM to the reactive and nonreactive collisions of the Na+H 2 system, which serves as a good model for studying dynamics of nonadiabatic quenching processes and collision complexes.

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Section: Introductionmentioning

confidence: 99%

Femtosecond Real-Time Probing of Reactions. 19. Nonlinear (DFWM) Techniques for Probing Transition States of Uni- and Bimolecular Reactions

1996

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Femtosecond real time probing of reactions XXII Kinetic description of probe absorption fluorescence depletion and mass spectrometry

ZEWAIL¹

1996

Molecular Physics

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Laser Ion Kinetics: Dynamics of Intramolecular Reactions in Substituted Benzalacetones

Heinicke

Grun

Grotemeyer

2000

Eur J Mass Spectrom (Chichester)

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Measurements of a single shot femtosecond laser pump-probe technique on substituted benzalacetones are reported. The technique is based on counter propagating femtosecond laser pulses in a supersonic beam of low density of sample molecules and simultaneous probe detection by ion or fragment ion formation through a reflectron time-of-flight mass spectrometer. It will be shown that the range of the pump-probe delays covers the time span between 100 fs and 10 ps depending on the pulse width of the laser used and the stability of the voltages of the mass spectrometer. The application of this technique to medium-sized organic molecules reveals some insight into the electron transfer process during ionisation through a 1 + 1 multi-photon absorption procedure. Furthermore it is demonstrated that this technique is also applicable to the investigation of ultra-fast isomerisation and fragmentation processes.

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Femtosecond Transient Stimulated Emission Pumping: Theory and Experiment

Cited by 3 publications

References 0 publications

Femtosecond Real-Time Probing of Reactions. 19. Nonlinear (DFWM) Techniques for Probing Transition States of Uni- and Bimolecular Reactions

Femtosecond Real-Time Probing of Reactions. 19. Nonlinear (DFWM) Techniques for Probing Transition States of Uni- and Bimolecular Reactions

Femtosecond real time probing of reactions XXII Kinetic description of probe absorption fluorescence depletion and mass spectrometry

Laser Ion Kinetics: Dynamics of Intramolecular Reactions in Substituted Benzalacetones

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