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Angular orientation of wave packets in molecules and atoms

Shapiro, E.

Published Mar 1, 2002• 2 citations
OpenAlex

Abstract

We discuss patterns of angular localization of various wave packets in molecules and Rydberg atoms, showing how one can easily predict spatial properties of superpositions of quantum eigenstates.

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The quantum theory of atoms is based on a Hamiltonian which is just that of the classical Kepler theory of planetary orbits. In spite of this common foundation, the predictions of the quantum theory ordinarily do not much resemble those of the classical theory. Even in the limit of large quantum numbers the energy eigenstates of quantum theory do not look at all like the classical elliptical orbits. Recently, Parker and Stroud1 showed that it is possible to excite a Rydberg atomic wave packet localized in the radial coordinate. Also, Yeazell and Stroud2 showed that a wave packet localized in the angular coordinates can be formed. Both wave packets exhibit an evolution describable, at least in part, by classical theory. However, neither wave packet truly corresponds to a wave packet traveling in a classical elliptical orbit. We discuss the manner in which such a wave packet might be formed using a short-pulsed laser and arf dressing field. The evolution of the resulting wave packet is compared with that of its classical counterpart.
The quantum theory of atoms is based on a Hamiltonian which is just that of the classical Kepler theory of planetary orbits. In spite of this common foundation, the predictions of quantum theory ordinarily do not much resemble those of classical theory. Even in the limit of large quantum numbers the energy eigenstates of quantum theory do not look at all like the classical elliptical orbits. Recently, Parker and Stroud1 have shown that it is possible to excite a Rydberg atom wave packet whose radial dependence resembles the classical ideal of a particle traveling in an elliptical orbit. In this paper we discuss the formation of a wave packet in the polar and azimuthal angles by the coherent excitation of Rydberg states with the same principal quantum, but with a distribution of the angular momentum quantum numbers. When this wave packet is formed of the Rydberg states of an alkali atom the connection with classical theory is again striking. The wave packet precesses due to the core polarization, just as the classical elliptical orbit precesses due to an added r–4 perturbing potential.
This paper presents an experimental and theoretical analysis of quantum interference between Rydberg wave packets in Na. Pairs of phase-locked wave packets manipulate the total orbital angular momentum of Na Rydberg atoms. Initially, the wave packet is composed of a superposition of s and d Rydberg series. Exploitation of the difference between the quantum defects of the two series allows one to predict the phase of the second wave packet required to engineer specific angular momentum compositions within the resultant wave packet. Experimentally, this final quantum state distribution is analysed in the frequency domain using state-selective field ionization and in the time domain using the optical Ramsey method. The theoretical calculations show how the phase difference between pairs of optical pulses is linked to the corresponding Rydberg frequency spectrum, therefore enabling the control of the quantum state composition of the wave packets. Finally, it is shown that by intuitively chirping one of the laser pulses it is possible to compensate for the dispersion of the wave packet and improve the effectiveness of the angular momentum control.