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Quantum Electronics and Laser Science Conference

Rotational wave packets observed via coherent pulse propagation

Stefan Marzenell, G. Torosyan, R. Beigang

Published Nov 13, 2002• 0 citations
Publisher

Abstract

Summary form only given. The formation and dynamics of wave packets has been investigated by means of various experimental techniques. In particular, the reshaping of femtosecond pulses transmitted through an atomic vapor was interpreted in terms of contracting and decaying wave packets in the case of atomic Rydberg wave packets excited in strontium vapor with femtosecond UV pulses.In this contribution we report on the observation of coherent pulse propagation in molecular vapors in the mid infrared spectral region. The coherent excitation of a whole manifold of rotational transitions in CO and N/sub 2/O vapor led to the formation of rotational wave packets.

DOI
10.1109/qels.2001.961898

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Summary form only given. The formation and dynamics of wave packets has been investigated by means of various experimental techniques. In particular, the reshaping of femtosecond pulses transmitted through an atomic vapor was interpreted in terms of contracting and decaying wave packets in the case of atomic Rydberg wave packets excited in strontium vapor with femtosecond UV pulses.In this contribution we report on the observation of coherent pulse propagation in molecular vapors in the mid infrared spectral region. The coherent excitation of a whole manifold of rotational transitions in CO and N/sub 2/O vapor led to the formation of rotational wave packets.
Summary form only given. A small-area femtosecond pulse propagates in a dispersive medium in a coherent fashion, if the relaxation times of the medium are compared with the pulse length for a long time. As a result, the pulse will be reshaped. This has been described by linear dispersion theory. Using Rydberg states of a molecular or an atomic gas as dispersive medium, the large spectral width of the femtosecond pulse can overlap with more than one level simultaneously. In this case, the shape of the propagated pulse reflects the temporal evolution of the Rydberg wave packet formed by the resonant Rydberg states.
The observation of an atomic wave packet by use of a coherent, nonlinear-optical process is reported. Wave packets formed in K or Rb vapor by two-photon excitation of ns and (n-2)dstates (n=8 for K; n=11 , 12 for Rb) with red (~620-nm) , 80-100-fs pulses were detected by four-wave mixing in pump-probe experiments. The temporal behavior of the wave packet is observed by monitoring the coherent UV radiation generated near the alkali mp(2)P? (2)S(1/2) (7</=m</=12 for Rb; 5</=m</=7 for K) resonance transitions when a probe pulse is scattered by the wave packet established by the earlier (identical) pump pulse. The spatial and spectral characteristics of the UV emission are well described by axially phase-matched four-wave mixing, and all the prominent frequency components of the wave packets are associated with energy differences between pairs of excited states for which Diota=0 or Diota=2 . These results demonstrate that the wave packet modulates chi((3))of the medium, thus rendering the wave packet detectable.
We experimentally investigate various processes present in the photoassociative interaction of an ultracold atomic sample with shaped femtosecond laser pulses. We demonstrate the photoassociation of pairs of rubidium atoms into electronically excited, bound molecular states using spectrally cut femtosecond laser pulses tuned below the rubidium D1 or D2 asymptote. Time-resolved pump-probe spectra reveal coherent oscillations of the molecular formation rate, which are due to coherent transient dynamics in the electronic excitation. The oscillation frequency corresponds to the detun-ing of the spectral cut position to the asymptotic transition frequency of the rubidium D1 or D2 lines, respectively. Measurements of the molecular photoassociation signal as a function of the pulse energy reveal a non-linear dependence and indicate a non-perturbative excitation process. Chirping the association laser pulse allowed us to change the phase of the coherent transients. Furthermore, a signature for molecules in the electronic ground state is found, which is attributed to molecule formation by femtosecond photoassociation followed by spontaneous decay. In a subsequent article [A. Merli et al., submitted] quantum mechanical calculations are presented, which compare well with the experimental data and reveal further details about the observed coherent transient dynamics.
We report the observation of coherent UV light pulses by the coherent scattering of IR pulses from atomic rubidium vapor. Rubidium atoms were first excited by a 100 fs pulse from the 5S ground state to the 5D state via a two-photon transition. The atoms were then pumped by an IR pulse resonant to the 5D–12P transition. The presence of the IR pulse triggered the instantaneous emission of a UV light pulse on the 12P–5S transition. The pulse had a time duration of tens of picoseconds, which was measured by a picosecond-resolution streak camera. The temporal shape of the generated light is explained by a simplified atom–field interaction theory.