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International Conference on Ultrafast Phenomena

Creation of an anti wavepacket in a Rydberg atom

Lambertus D. Noordam, Henrik Stapelfeldt, D. I. Duncan, Thomas F. Gallagher

Published Jan 1, 1992• 0 citations
Publisher

Abstract

At the 1990 UFP conference the observation of several kinds of wave packets was reported [1]. All these wavepackets have in common that the wavefunction is localised due to a coherent superposition of eigenstates. The localised ‘particle’ evolves in course of time. The oscillation time of the wavepacket is determined by the inverse spacing of the states out of which the wavepacket is formed. We reported on the localisation of an atomic electron wavefunction by coherent superposition of Rydberg states. Also the observation of exciton wavepackets was reported, as well as the observations of optic phonons in the time domain. At an earlier conference the CalTech group reported already the observation of the oscillation of vibrational wavepackets in diatomic molecules [2].

DOI
10.1364/up.1992.fd3

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At the 1990 UFP conference the observation of several kinds of wave packets was reported [1]. All these wavepackets have in common that the wavefunction is localised due to a coherent superposition of eigenstates. The localised ‘particle’ evolves in course of time. The oscillation time of the wavepacket is determined by the inverse spacing of the states out of which the wavepacket is formed. We reported on the localisation of an atomic electron wavefunction by coherent superposition of Rydberg states. Also the observation of exciton wavepackets was reported, as well as the observations of optic phonons in the time domain. At an earlier conference the CalTech group reported already the observation of the oscillation of vibrational wavepackets in diatomic molecules [2].
The authors have excited and detected a radially localized electronic wavepacket in atomic rubidium. The wavepacket is formed of an optically induced coherent superposition of Rydberg states with mean principal quantum number, n=62. The motion of the wavepacket on a classical trajectory is monitored in a time-delayed ionization experiment. The collapse and revival of the classical dynamics is observed. During the period of nonclassical behaviour they observe, for the first time, a partial revival of the wavepacket.
We demonstrate that atomic wavepackets can serve as sensitive detectors for investigating atomic and molecular dynamics. In concert with parametric four-wave mixing, the interference between coherent superpositions of atomic excited states produced by ultrafast (/spl sim/150 fs) pump and probe pulses provides a new and powerful tool with which fundamental processes, such as molecular dissociation and Rydberg-Rydberg atomic collisions, can be observed with the extraordinary sensitivity afforded by a coherent nonlinear optical process. Experiments are described in which the dissociation of an electronically excited molecule (Rb/sub 2/) and the distribution of atomic fragments into excited states spanning >10 000 cm/sup -1/ are observed. Also, resonant collisions between Rb atoms in the 7s and 5d states are detected by monitoring the shift in the frequency of an atomic wavepacket induced by the dipole-dipole interaction.
We report an observation of the long-term evolution of a radially localized electronic wave packet formed by the coherent superposition of Rydberg states of atomic potassium. Initially, the wave packet can be described classically. Subsequent dephasing of the discrete states in the superposition leads to a loss of spatial localization so that the evolution can no longer be described classically. However, the wave packet revives at a later time. Theory and experiment show good agreement including an accurate measurement of the phase shift of the wave packet on revival.
Experimental and theoretical work is presented on the control of wave packet dynamics in atomic and molecular systems. Using sequences of phase-locked optical pulses, the link between optical phase and quantum mechanical phase is explored in the Na atom and Naj dimer, representing a step towards the logical engineering of quantum states in more complicated systems. A novel apparatus, constructed to study and control the vibrational dynamics of vibrational wave packets on the Na ionic potential surface, is described in chapter 3. Theoretical simulations for proposed experiment are presented in chapter 4. Control is achieved by exploiting the phase-evolution of the constituent vibrational quantum states within the wave packet superposition. The phase relationship and the accumulated phase difference between the various components of the wave packet is determined, and a sequence of phase-locked optical pulses is employed to selectively enhance or depopulate specific vibrational states, or sets of vibrational states. The quantum state composition of the resulting wave packet, and the efficiency of the control scheme, is determined by calculating the multi-pulse response of the time-dependent vibrational state populations. In chapter 5, the quantum interference between Rydberg electron wave packets in the Na atom is investigated using pairs of phase-locked wave packets, allowing manipulation of 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 specific angular momentum compositions within the resultant wave packet to be engineered. Experimentally, this final quantum state distribution is analysed in the frequency domain using state selective field ionisation, 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.
Atoms in high-lying Rydberg states with large values of principal quantum number n, n ≥300, form a valuable laboratory in which to explore the control and manipulation of quantum states of mesoscopic size using carefully tailored sequences of short electric field pulses whose characteristic times (duration and/or rise/fall times) are less than the classical electron orbital period. Atoms react to such pulse sequences very differently than to short laser or microwave pulses providing the foundation for a number of new approaches to engineering atomic wavefunctions. The remarkable level of control that can be achieved is illustrated with reference to the generation of localized wavepackets in Bohr-like near-circular orbits, and the production of non-dispersive wavepackets under periodic driving and their transport to targeted regions of phase space. New protocols continue to be developed that will allow even tighter control with the promise of new insights into quantum-classical correspondence, information storage in mesoscopic systems, physics in the ultra-fast ultra-intense regime, and non-linear dynamics in driven systems.