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Rydberg-Stark deceleration and trapping of atoms and molecules

Seiler, Christian

Published Jan 1, 2013• 2 citations
Publisher

Abstract

This thesis describes contributions to the development of a new method to control the translational motion of atoms and molecules in supersonic beams.This method, Rydberg-Stark deceleration, is in principle applicable to all atoms and molecules in the gas phase.It relies on the Stark effect exhibited by Rydberg states and enables the production of samples of translationally and internally cold atoms and molecules which have possible applications in high-resolution spectroscopic experiments, in the studies of collisions at low temperatures and in quantum information science.This method has been developed and tested in deceleration and trapping experiments on hydrogen and deuterium atoms, and hydrogen molecules initially moving in supersonic beams.Its power originates from the large dipole moments, easily exceeding 1000 Debye, induced in Rydberg states by electric fields.Large forces are exerted on Rydberg atoms and molecules

DOI
10.3929/ethz-a-010028679

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Rydberg-Stark deceleration of atoms and molecules

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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.

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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.

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Cooling effects in the Stark deceleration of Rydberg atoms/molecules with time-dependent electric fields

Yoshihiro Yamakita, R Takahashi, Koichi Ohno +3 more

This paper presents calculations for realizing the deceleration of H 2 Rydberg molecules with n = 16, where n is the principal quantum number. A double-dipole decelerator (Softley T P, Procter S R, Yamakita Y, Maguire G and Merkt F 2005 J. Elec. Spectrosc. Relat. Phenom. 144–147 113) operated with an optimum time-dependent electric field allows, in principle, complete deceleration of the Rydberg molecules to zero mean velocity. A bunch of molecules in a supersonic beam is decelerated from the initial velocity centered at ∼900 ms −1 and translational temperature 1 K to the final velocity 0 ms −1 and temperature 13 mK. The calculations are performed using the 4th-order symplectic integrator based on representations in phase space { q, p }, and show that an ensemble with narrow δ q 0 and broad δ p 0 distribution is converted to one at standstill with broad δ q and narrow δ p . Cooling effects are reinforced by field ionization in which the fast components that move to regions of high electric field are effectively filtered out.

Journal of Physics Conference Series•Sep 1, 2007•7 citations
This thesis describes contributions to the development of a new method to control the translational motion of atoms and molecules in supersonic beams.This method, Rydberg-Stark deceleration, is in principle applicable to all atoms and molecules in the gas phase.It relies on the Stark effect exhibited by Rydberg states and enables the production of samples of translationally and internally cold atoms and molecules which have possible applications in high-resolution spectroscopic experiments, in the studies of collisions at low temperatures and in quantum information science.This method has been developed and tested in deceleration and trapping experiments on hydrogen and deuterium atoms, and hydrogen molecules initially moving in supersonic beams.Its power originates from the large dipole moments, easily exceeding 1000 Debye, induced in Rydberg states by electric fields.Large forces are exerted on Rydberg atoms and molecules
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.
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 experimental realisation of a set of surface-based devices for controlling the positions and velocities of Rydberg atoms initially travelling in pulsed supersonic beams is described. The unique aspect of these devices is that they are based on the geometry of two-dimensional electrical transmission-lines and are therefore suited to integration with chip-based microwave circuits to realise a complete Rydberg laboratory on a chip. Such a chip-based laboratory could be exploited in hybrid approaches to quantum information processing, and for studies of collisions and decay processes of highly excited atoms and molecules. The devices operate through the generation of inhomogeneous electric fields and take advantage of the large electric dipole moments associated with high Rydberg states to exert forces on the atoms. In the experiments, helium atoms in Rydberg-Stark states with principal quantum numbers ranging from 48 to 52 and electric dipole moments of 10000 D are employed. The devices developed include electrostatic guides which permitted control over the transverse motion of beams of atoms. These were used to transport samples, initially travelling at 1950 m/s and deflect them away from their initial axis of propagation. The guided atoms were detected by pulsed electric field ionisation. To control the longitudinal motion of the samples, the transmission-lines were modified to permit the generation of sets of continuously moving electric traps. The resulting transmission-line decelerators were then employed to guide, accelerate and decelerate atoms trapped in three-dimensions. Accelerations up to 2.3 x 10^{7} m/s^{2} were applied to decelerate samples from 2000 m/s to zero-velocity in the laboratory-fixed frame of reference, leading to the removal of 80 meV of kinetic energy, the largest achieved in any Stark decelerator to date. The decelerated atoms were trapped in stationary electric traps and detected in situ. The phase-space acceptances of the decelerators were calculated to characterise the effects of acceleration and deceleration on the trapped atoms. The results of the calculations were employed in the interpretation of the experimental data, and to identify effects of collisions and blackbody transitions.
Hydrogen and deuterium Rydberg atoms, initially moving at velocities of 600 and 560 m s −1 , respectively, in pulsed supersonic beams, have been decelerated and electrostatically trapped following adiabatic 90° deflection from their initial axis of propagation to minimize collisions with the trailing edge of the gas pulses. The time evolution of the potential energy surfaces, over which the atoms undergoing deceleration travel during the trap-loading process, is analogous to that of a moving electrodynamic trap. It has been studied in the laboratory-fixed frame of reference and in the continuously moving frame of reference defined by the instantaneous position of the electric-field minimum around which the atoms are located. The importance of the quadratic Stark effect in the deceleration of samples in Rydberg states with principal quantum numbers above 35 has also been investigated by comparison of experimental results with predictions resulting from the numerical calculation of particle trajectories. The data presented for deuterium atoms represent the first application of Rydberg–Stark deceleration and trapping for this atom. Comparison of the rate of loss of n = 30 H and D atoms from the trap enables one to conclude that it is not affected by the particle dynamics during deceleration and trap loading.
A surface-electrode decelerator and deflector for Rydberg atoms and molecules has been developed with the goal of performing collisional experiments. Translationally cold H2{\mathrm{H}}_{2}H2​ molecules in a supersonic beam were excited to Rydberg-Stark states of principal quantum number n=31n=31n=31, loaded into electric traps moving at a predetermined speed above the surface of a bent printed circuit board, decelerated, and deflected from the original direction of the supersonic beam by an angle of ${10}^{\ensuremath{\circ}}$. The phase-space characteristics of the deflected beam were characterized by measuring the time-of-flight distribution and images of the Rydberg molecules and comparing them to the results of numerical particle-trajectory simulations. More than 1000 H2{\mathrm{H}}_{2}H2​ molecules were deflected per experimental cycle at a repetition rate of 25 Hz. The phase-space characteristics of the deflector make it attractive to study ion-molecule reactions at low collision energies.
This paper presents calculations for realizing the deceleration of H 2 Rydberg molecules with n = 16, where n is the principal quantum number. A double-dipole decelerator (Softley T P, Procter S R, Yamakita Y, Maguire G and Merkt F 2005 J. Elec. Spectrosc. Relat. Phenom. 144–147 113) operated with an optimum time-dependent electric field allows, in principle, complete deceleration of the Rydberg molecules to zero mean velocity. A bunch of molecules in a supersonic beam is decelerated from the initial velocity centered at ∼900 ms −1 and translational temperature 1 K to the final velocity 0 ms −1 and temperature 13 mK. The calculations are performed using the 4th-order symplectic integrator based on representations in phase space { q, p }, and show that an ensemble with narrow δ q 0 and broad δ p 0 distribution is converted to one at standstill with broad δ q and narrow δ p . Cooling effects are reinforced by field ionization in which the fast components that move to regions of high electric field are effectively filtered out.