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Physical Review A

Semiclassical dynamics of circular-orbit Rydberg wave packets

Mark Mallalieu, Carlos R. Stroud

Published Apr 1, 1994• 32 citations
Publisher

Abstract

A semiclassical propagator is applied to describe the dynamics of circular-orbit wave packets which are initially well localized in three dimensions. A sum over classical Kepler trajectories for the wave-packet autocorrelation function is obtained which is extremely accurate well past the classical regime of the evolution regime of the wave packet. The nonclassical nature of the wave-packet evolution at long times is associated with the interference between amplitudes from classical paths at different energies. The time scale of the wave-packet revivals is related to the shearing rate of the corresponding classical ensemble.

DOI
10.1103/physreva.49.2329

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A semiclassical propagator is applied to describe the dynamics of circular-orbit wave packets which are initially well localized in three dimensions. A sum over classical Kepler trajectories for the wave-packet autocorrelation function is obtained which is extremely accurate well past the classical regime of the evolution regime of the wave packet. The nonclassical nature of the wave-packet evolution at long times is associated with the interference between amplitudes from classical paths at different energies. The time scale of the wave-packet revivals is related to the shearing rate of the corresponding classical ensemble.
A semiclassical approximation is derived from the autocorrelation function describing the excitation and detection of Rydberg wave packets by pairs of phase-locked laser pulses. The resulting expression is in terms of a sum over Kepler trajectories, and provides a direct explanation of the periodicity and spreading of the wave packet at short times when the evolution is classical. More surprisingly, this solution also provides an accurate description of the complex revival behavior of the wave packets, which is nonclassical. The phases of the wave packets, which are detected by the pulse-locking scheme, are also accurately given by analytical expressions derived from the semiclassical sum. The phase of the wave packets at short times have a simple interpretation as the phases of Bohr-Sommerfeld, and are related to Berry's phase. The semiclassical expression for the phases of the nonclassical revival wave packets is simpler than the corresponding quantal solution.
We study the dynamics of a circular-orbit wave packet1 and find that it has both classical and quantum features. A circular-orbit wave packet consists of aligned, standard hydrogenic eigenstates of maximum angular momentum (l = in = n − 1), superimposed with a Gaussian weighting function. We calculate the uncertainty products in all three degrees of freedom and find that, as the quantum numbers of the constituent eigenstates increase, the uncertainty products tend toward h/2. The classical aspect of the dynamics displays itself during revivals, when a well-localized wave packet travels along a Kepler orbit, obeying the classical equations of motion. Spreading and revivals (including fractional revivals2) of the wave packet, which are manifestations of its quantum nature, are related to the nonlinearity of the hydrogen atom Hamiltonian. We study fractional revivals of the wavepacket in detail.
We demonstrate that the quantum coherence of mesoscopic very-high- n , n ∼305, Rydberg wave packets travelling along nearly circular orbits can be maintained on microsecond time scales corresponding to hundreds of classical orbital periods. The coherence is probed through collapses and revivals of periodic oscillations in the average electron position. The temporal interferences of spatially separated Schrödinger cat-like wave packets are also observed. A novel hybrid quantum–classical trajectory method is employed to simulate the wave packet dynamics.
A semiclassical method is discussed for propagating wave packets that incorporates nonlinear classical dynamical information through the use of multiple reference trajectories. We apply the theory to obtain an analytic approximation for the autocorrelation function in the Coulomb potential which is extremely accurate in many circumstances in spite of the Coulomb singularity. All the detailed quantum behavior is reproduced including the long time revivals and the spectrum. The evolving phase space structure of the classical analog reveals how well a particular case will be approximated.
Quantum mechanical wave packet states can approach the classical ideal of a spatially localized particle traveling along a well-defined trajectory. These states offer a system in which the classical limit of quantum atomic theory can be studied. In this work, a wave packet that is radially localized and whose radial motion occurs at the classical orbital period is studied. Despite these strong classical features, the long-term evolution displays the quantum nature of the state. As the wave packet evolves, it becomes dispersed, and the radial motion becomes irregular. However, the wave packet does not remain dispersed, and classical motion returns with the return of the spatial localization. Both the collapse and revival of the wave packet occur because of the quantized nature of the atom. In this experiment, the wave packet was excited to the Rydberg slates by a short, ultraviolet pulse from the ground state of potassium. The probe pulse delay was scanned, and the resulting photo-ionization signal displayed the evolution of the wave packet. The collapse and revival of the radial wave packet were observed.1