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Physical Review A

Rydberg atoms in far-infrared radiation fields. II. Wave packet dynamics

J. H. Hoogenraad, Rutger B. Vrijen, Lambertus D. Noordam

Published Jun 1, 1998• 8 citations
Publisher

Abstract

The short-pulse dynamics of excitation and stimulated emission between highly excited states $(15<n<60)$ is studied with picosecond far-infrared pulses (40--60 $\ensuremath{\mu}\mathrm{m}$) originating from a free electron laser. We measured the excitation of a Rydberg wave packet in rubidium around $n=40$ excited from a deeper bound $(n\ensuremath{\approx}20)$ Rydberg state by a picosecond far-infrared laser pulse. Moreover, starting from a stationary $n=40$ state we found that upon irradiating with a short far-infrared laser pulse, adjacent Rydberg states are populated by resonant Raman transfer via a deeper $(n=20)$ bound state. Finally, we discuss the dynamics of wave-packet excitation at a Cooper minimum in lithium, where sign change of the excitation matrix elements causes excitation at large distances from the atomic core. Possible measurement methods for this effect are discussed and found to yield different information.

DOI
10.1103/physreva.57.4546

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The short-pulse dynamics of excitation and stimulated emission between highly excited states (15<n<60)(15<n<60)(15<n<60) is studied with picosecond far-infrared pulses (40--60 \ensuremathμm\ensuremath{\mu}\mathrm{m}\ensuremathμm) originating from a free electron laser. We measured the excitation of a Rydberg wave packet in rubidium around n=40n=40n=40 excited from a deeper bound (n\ensuremath≈20)(n\ensuremath{\approx}20)(n\ensuremath≈20) Rydberg state by a picosecond far-infrared laser pulse. Moreover, starting from a stationary n=40n=40n=40 state we found that upon irradiating with a short far-infrared laser pulse, adjacent Rydberg states are populated by resonant Raman transfer via a deeper (n=20)(n=20)(n=20) bound state. Finally, we discuss the dynamics of wave-packet excitation at a Cooper minimum in lithium, where sign change of the excitation matrix elements causes excitation at large distances from the atomic core. Possible measurement methods for this effect are discussed and found to yield different information.
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Multiphoton excitation and ionization studies of the Li 23s23s23s state by 20 ps far-infrared laser pulses originating from the free-electron laser FELIX are presented. The two-photon ionization cross section of highly excited Rydberg sss states is small, due to a newly discovered Cooper minimum in the bound-bound $ns\ensuremath{-}{n}^{\ensuremath{'}}p$ transitions. Instead of this lowest-order process, ionization proceeds via a remarkable multiphoton bypass starting with stimulated emission to a lower-lying state. The measurements are interpreted with calculations of the Cooper minimum and a Floquet analysis of the states involved in the bypass.
We have studied the evolution of Rydberg wave packets in the presence of interatomic dipole-dipole interactions in a frozen Rb gas. Rb atoms in a magneto-optical trap (MOT) are first laser excited to nsnsns Rydberg eigenstates. A picosecond THz pulse further excites them into coherent superposition states involving the initial-level and neighboring npnpnp states. A second, identical, time-delayed THz pulse probes the wave-packet dynamics. As the wave packets evolve they are influenced by dipole-dipole interactions, predominantly pairwise excitation-exchange processes of the form $|s\ensuremath{\rangle}|p\ensuremath{\rangle}\ensuremath{\leftrightarrow}|p\ensuremath{\rangle}|s\ensuremath{\rangle}$. The coherent electronic evolution of the ensemble dephases due to the variation in dipole-dipole coupling strength between atom pairs in the MOT. The experimental results are in good agreement with numerical calculations that simulate the interactions between nearest neighbors in a frozen gas.