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Physical Review Letters

Coherent Pulse Propagation and the Dynamics of Rydberg Wave Packets

Jochen Arlt, Carsten Weiss, G. Torosyan, R. Beigang

Published Dec 15, 1997• 15 citations
Publisher

Abstract

The pulse reshaping of femtosecond laser pulses tuned to Rydberg transitions of strontium vapor is observed experimentally. We show theoretically that their shape closely reflects the dynamics of Rydberg wave packets induced by the pulses. The decay and compression of Rydberg wave packets excited by both Fourier limited and chirped fs pulses is presented.

DOI
10.1103/physrevlett.79.4774

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Introduction

Jeffrey W. Krause

When a coherent superposition of Rydberg states is excited by a laser pulse, a Rydberg wave packet is created. These wave packets are supremely quantum mechanical objects. However, they can be constructed to display classical, nearly classical, or semiclassical behavior, and thus serve as a natural bridge between the microscopic and mesoscopic worlds. In addition, their comparative simplicity allows detailed studies of the fundamental interactions of light with matter. The authors of this focus issue were invited to submit papers that reflect both the range of dynamical behavior exhibited by Rydberg wave packets, and the depth of understanding of them that is possible with current experiments and theory. In particular, the papers in this issue illustrate the possibility that emerging laser technology can be used not only to observe quantum behavior, but also to control it.

Optics Express•Sep 29, 1997•1 citation
The pulse reshaping of femtosecond laser pulses tuned to Rydberg transitions of strontium vapor is observed experimentally. We show theoretically that their shape closely reflects the dynamics of Rydberg wave packets induced by the pulses. The decay and compression of Rydberg wave packets excited by both Fourier limited and chirped fs pulses is presented.
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.
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.
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.
When a coherent superposition of Rydberg states is excited by a laser pulse, a Rydberg wave packet is created. These wave packets are supremely quantum mechanical objects. However, they can be constructed to display classical, nearly classical, or semiclassical behavior, and thus serve as a natural bridge between the microscopic and mesoscopic worlds. In addition, their comparative simplicity allows detailed studies of the fundamental interactions of light with matter. The authors of this focus issue were invited to submit papers that reflect both the range of dynamical behavior exhibited by Rydberg wave packets, and the depth of understanding of them that is possible with current experiments and theory. In particular, the papers in this issue illustrate the possibility that emerging laser technology can be used not only to observe quantum behavior, but also to control it.