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The Journal of Chemical Physics

Deflection and deceleration of hydrogen Rydberg molecules in inhomogeneous electric fields

Yoshihiro Yamakita, Simon R. Procter, A L Goodgame, T. P. Softley, Frédéric Merkt

Published Jul 6, 2004• 87 citations
Publisher

Abstract

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.

DOI
10.1063/1.1763146

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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 novel theoretical study of the control of translational motion of atomic and molecular Rydberg states in inhomogeneous static electric fields is presented. Simulations have been carried out demonstrating that, under realistic conditions, the deflection and focusing of Rydberg atoms and molecules should be achievable. Advantage is taken of the high susceptibility of the Rydberg states to external electric fields, allowing the use of much smaller fields than would be necessary for ground state neutrals. The simulations presented are for trajectories of Rydberg states with n = 18-20 in the fields of an electric dipole, quadrupole and hexapole. A deflection of 7 mm is predicted for n = 18 Rydberg states travelling parallel to the dipole after 100 µs time of flight. In the hexapole n = 20 Rydberg states are refocused to a spot size of the order of the laser beam waist (10 µm) after 20 µs. It is demonstrated that the hexapole can also act as a cylindrical lens if its axis is perpendicular to the Rydberg beam direction. Spontaneous emission and black-body decay rates are also calculated, and their variation with the applied field is investigated. The potential applications of this work might include the use of focusing and deflection for controlled low-energy collisions of Rydberg molecules with surfaces.
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.
The controlled deflection of Rydberg atoms in an inhomogeneous electric field is demonstrated and shown to be in agreement with predictions based on a well-defined Stark map. Krypton atoms in a supersonic beam are excited in a two-colour multiphoton process to selected Stark states with n = 16-19 and undergo deflections in the field of an electrostatic dipole. The spatial distribution of the deflected atoms is monitored by ion imaging. The atoms travelling ~10 cm in the beam direction after excitation are deflected from the beam axis by distances of up to 3 mm, the interaction with the field taking place over 40 µs. Simulations of the trajectories agree well with the experimental results, demonstrating that the detected Rydberg atoms are those which have not undergone decay processes in the 40 µs applied field.
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.
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 large electric dipole moments associated with highly excited Rydberg states of atoms and molecules make gas-phase samples in these states very well suited to deceleration and trapping using inhomogeneous electric fields. The methods of Rydberg-Stark deceleration with which this can be achieved are reviewed here. Using these techniques, the longitudinal motion of beams of atoms and molecules moving at speeds as high as 2500 m/s have been manipulated, with changes in kinetic energy of up to |Δ E kin|=1.3×10−20 J (|Δ E kin|/e=80 meV or |Δ E kin|/h c=650 cm −1) achieved, while decelerated and trapped samples with number densities of 106– 107 cm −3 and translational temperatures of ∼150 mK have been prepared. Applications of these samples in areas of research at the interface between physics and physical chemistry are discussed.