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Physical Review Letters

Nonhydrogenic Effects in the Deceleration of Rydberg Atoms in Inhomogeneous Electric Fields

E. Vliegen, Hans Jakob Wörner, T. P. Softley, Frédéric Merkt

Published Jan 23, 2004• 104 citations
Publisher

Abstract

Argon atoms in Stark states at n approximately 25 have been decelerated and accelerated in inhomogeneous electric fields. The acceleration and deceleration behavior can be understood only by considering the adiabatic Landau-Zener dynamics that take place at the avoided crossings between the Stark states and the limited fluorescence lifetimes of approximately 10 micros.

DOI
10.1103/physrevlett.92.033005

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Argon atoms in Stark states at n approximately 25 have been decelerated and accelerated in inhomogeneous electric fields. The acceleration and deceleration behavior can be understood only by considering the adiabatic Landau-Zener dynamics that take place at the avoided crossings between the Stark states and the limited fluorescence lifetimes of approximately 10 micros.
Argon atoms in a pulsed supersonic expansion are prepared in selected Stark components of Rydberg states with effective principal quantum number in the range n * = 15–25. When traversing regions of inhomogeneous electric fields, these atoms get accelerated or decelerated depending on whether the Stark states are low- or high-field seeking states. Using a compact electrode design, which enables the application of highly inhomogeneous and time-dependent electric fields, the Rydberg atoms experience kinetic energy changes of up to 1.2 × 10 −21 J (i.e. 60 cm −1 in spectroscopic units) in a single acceleration/deceleration stage of 3 mm length. The resulting differences in the velocities of the low- and high-field seeking states are large enough that the corresponding distributions of times of flight to the Rydberg particle detector are fully separated. As a result, efficient spectral searches of the Rydberg states best suited for acceleration/deceleration experiments are possible. Numerical simulations of the particle trajectories are used to analyse the time-of-flight distributions and to optimize the time dependence of the inhomogeneous electric fields. The decay of the Rydberg states by fluorescence, collisions and transitions induced by black-body radiation takes place on a timescale long enough not to interfere significantly with the deceleration during the first ∼5 µs.
Argon and hydrogen atoms excited to Rydberg Stark states in supersonic expansions have been decelerated using inhomogeneous electric fields. In the case of hydrogen, the atoms have been decelerated from an initial velocity of 700 m/s to zero velocity in the lab frame using time-dependent inhomogeneous electric fields and subsequently stored in two- and three-dimensional traps. The dynamics of the Rydberg atoms in the traps and the phase-space characteristics of the decelerated atoms have been characterized by pulsed field ionization and imaging techniques. Multi-stage Zeeman deceleration of ground state H and D atoms has been demonstrated. Using this technique H atoms, traveling at 420 m/s, have been decelerated to half of their initial kinetic energy. © 2008 World Scientific Publishing Co. Pte. Ltd.
Hydrogen molecules are excited in a molecular beam to Rydberg states around n=17-18 and are exposed to the inhomogeneous electric field of an electric dipole. The large dipole moment produced in the selected Stark eigenstates leads to strong forces on the H2 molecules in the inhomogeneous electric field. The trajectories of the molecules are monitored using ion-imaging and time of flight measurements. With the dipole rods mounted parallel to the beam direction, the high-field-seeking and low-field-seeking Stark states are deflected towards and away from the dipole, respectively. The magnitude of the deflection is measured as a function of the parabolic quantum number k and of the duration of the applied field. It is also shown that a large deflection is observed when populating the (17d2)1 state at zero field and switching the dipole field on after a delay. With the dipole mounted perpendicular to the beam direction, the molecules are either accelerated or decelerated as they move towards the dipole. The Rydberg states are found to survive for over 100 micros after the dipole field is switched off before being ionized at the detector and the time of flight is measured. A greater percentage change in kinetic energy is achieved by initial seeding of the beam in helium or neon followed by inhomogeneous field deceleration/acceleration. Molecular dynamics trajectory simulations are presented highlighting the extent to which the trajectories can be predicted based on the known Stark map. The spectroscopy of the populated states is discussed in detail and it is established that the N+=2, J=1, MJ=0 states populated here have a special stability with respect to decay by predissociation.
A method is proposed to decelerate neutral atoms in a thermal beam for purposes of precision spectroscopy, atomic clocks, or loading into shallow traps. Rydberg atoms exhibit large electric dipole moments suggesting that inhomogenous fields can exert forces on them. The resultant change in kinetic energy is equal to the Stark shift of the Rydberg state. It has been found that a series of tandem electrode pairs can reduce atomic velocities by a factor of 10. Various limitations and constraints are discussed.
Hydrogen atoms in a cold supersonic expansion with an average velocity of 700 m s −1 have been excited to Rydberg Stark states with principal quantum number in the range n = 20–25 and subsequently decelerated and accelerated in time-independent inhomogeneous electric fields. Accelerations of up to 2 × 10 8 m s −2 have been achieved and the initial kinetic energy of atoms prepared in low (high)-field seeking Stark states could be more than quadrupled (halved) over a flight distance of only 3 mm and in a time of less than 5 µs. The control over the velocity of the Rydberg atoms is such that trapping can be envisaged.
The interaction between inhomogeneous electric fields and the large electric dipole moments of atoms and molecules in Rydberg states of high principal quantum number can be used to efficiently accelerate and decelerate atoms and molecules in the gas phase. We describe here how hydrogen atoms and molecules initially moving with velocities of ∼600 m/s in supersonic beams can be decelerated to zero velocity and loaded into electric traps. The long observation times that are made possible by the electrostatic trapping enables one to study slow relaxation processes. Experiments are presented in which we have observed photoionization processes and transitions between Rydberg states induced by blackbody radiation at temperatures between 10 K and 300 K on a time scale of several milliseconds. Comparison of these processes in Rydberg states of H and H(2) suggests the importance, in H(2), of collisional processes and of the process of blackbody-radiation-induced predissociation.