A cylindrical arrangement of electrodes, together with control electronics, is described that provides uniform electric fields over cm3 volumes in a vacuum, whose angle and magnitude can be switched on a μs time scale. Full 360° field rotation is achieved, and the device allows access for particle or light beams from all sides. Both numerical and analytic descriptions of the general fields are given. Extension to full three-dimensional field control and other variations are described. The device, which was originally designed for crossed-beam collision experiments with keV energy ions and laser-excited Rydberg atoms in field-directed Stark states or coherent-elliptic states, may be more generally useful in atom trapping and cold collisions or in materials and surface science.
A cylindrical arrangement of electrodes, together with control electronics, is described that provides uniform electric fields over cm3 volumes in a vacuum, whose angle and magnitude can be switched on a μs time scale. Full 360° field rotation is achieved, and the device allows access for particle or light beams from all sides. Both numerical and analytic descriptions of the general fields are given. Extension to full three-dimensional field control and other variations are described. The device, which was originally designed for crossed-beam collision experiments with keV energy ions and laser-excited Rydberg atoms in field-directed Stark states or coherent-elliptic states, may be more generally useful in atom trapping and cold collisions or in materials and surface science.
Total electron capture by K+ or Cs+ from a Na Rydberg n=24 extremal Stark state, aligned with a weak external electric field, has been measured as a function of the angle between the atoms’ electric dipole moment and the projectile beam in the reduced-velocity range ṽ=0.15 to 1.05. A novel “Stark barrel” is described that produces the arbitrarily directed uniform electric field, smoothly switchable in both magnitude and direction in under 2 μs. The results illustrate the importance of spatial effects as opposed to velocity matching for a full understanding of electron capture near ṽ=1.
A device is described and mathematically analyzed which creates electrostatic multipole potentials at least up to rank 3 in a 2 cm diam spherical region. The fields in the Stark ball are produced by the application of programmed voltages to 24 conducting rods that are inserted symmetrically in an empty 5 cm conducting cavity. Three mutually orthogonal unobstructed paths through the center of the device between the rods are provided for access of light and particle beams, and four other tetrahedrally located openings can be added for beams, detectors, or imaging. The device is intended for application in atom or molecule trapping and cooling, recoil-ion momentum spectroscopy, particulate analysis, reactive scattering, and coherent control. Potential distributions can be established, altered, and rotated on subnanosecond time scales, and frequencies higher than 20 GHz can be introduced via the same electrodes. Uniform fields, i.e., first-rank multipoles, quadrupole, and octupole potentials can be programmed and superposed with arbitrary and independent time profiles, so that the device may be applied to the study of orientational properties of complex anisotropic molecules, pollens, grains of dust, and other particulates. The device is nonmagnetic. An extensive analysis of fields in the center region, fringing fields, and multipole purity up to rank 7 has been carried out, and recipes are given for pure (l,m)=(1,0), (2,0), and (3,0) multipoles. The principles and methods laid out here and applied to a “truncated octahedron” can be applied to the design of electrostatic environments having fewer or more independent electrodes in any polyhedral geometry.
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.
Quantum computing and quantum simulation with ultracold neutral atoms require Rydberg excitation of individual atoms in atomic arrays. Rydberg states are extremely sensitive to external electric fields, therefore precise three-dimensional control of the electric field is essential. We performed a spectroscopic study of three-photon Rydberg excitation of a single Rb atom in an optical dipole trap in the presence of an external DC electric field. The field was generated by eight electrodes deposited on the inner surfaces of an ultrahigh-vacuum glass cell. The used three-photon scheme of laser excitation of Rydberg \textit{nP} states allows the Stark shift and the splitting of the resonances to be observed simultaneously, which simplifies calibration of the electric field. In addition, in the commonly used two-photon Rydberg excitation schemes, the light shifts can complicate accurate determination of the DC Stark shift, particularly when the external electric field is scanned across different spatial directions, and different Stark components are excited. These shifts are absent in the three-photon excitation scheme used in our experiment. We demonstrated the ability to independently tune the electric field along all three spatial directions and to compensate for stray electric fields. The measured three-photon spectra exhibit Stark shifts and splittings of the three-photon resonance that are in good agreement with theoretical calculations. These results are also of interest for Rydberg electrometry.
This thesis describes the design and construction of a novel molecule-surface scattering apparatus. The setup combines a Stark decelerator with a state-of- the-art surface scattering chamber, and allows background-gas free scattering of packets of velocity-controlled polar molecules in selected quantum states from well-defined surfaces with unprecedented energy resolution. Results for scattering of CO (a3Π) in different vibrational quantum states from a clean Au(111) surface are presented. CO is co-expanded with Xe or Ar to yield a supersonic molecular beam which produces fast, internally cold molecules. Excitation of CO to the long-lived electronically excited a3Π1 state makes it accessible to manipulation with electric fields due to the state’s large dipole moment. The complete removal of both carrier gas and remaining ground- state CO is achieved by focusing and deflecting the metastable CO with a switched electrostatic hexapole state selector. The 131-stage Stark decelerator is used to tune the velocity of a part of the metastable CO pulse, with an initial velocity of 360 m/s, in the range from (512 ± 4) m/s – (50 ± 4) m/s, corresponding to an incident translational energy between (307 ± 5) cm-1 and (3.0 ± 0.5) cm-1, respectively.This range can be extended up to (1300 ± 25) m/s, corresponding to an energy of(1980 ± 80) cm-1, by simple modifications to the setup. Prior to collision, the molecules can be laser- prepared in different vibrational and rotational quantum states. State- selective detection of the scattering products makes it possible to determine the quantum state, the scattering angle, and the kinetic energy of the scattered molecules. Therefore, detailed information about the scattering process can be obtained. The design of the machine allows for flexible laser access near the surface, such that a variety of different preparation and detection schemes can be employed. Ultra-high vacuum conditions in the scattering chamber are achieved by baking the entire apparatus, including the decelerator and the hexapole. Because of the carrier gas removal and a total of three differential pumping stages, no pressure rise is detected in the scattering chamber due to the incident molecular beam. Scattering experiments of CO (a3Π) on Au(111) have been performed. The scattering process leads to electron emission because the metastable excitation energy exceeds the work function of the surface. The electron emission yield, i.e. the number of electrons emitted per incident metastable particle, has been measured to be 0.13 ± 0.05. A laser ionization-depletion method is used which makes it possible to directly compare the intensity of the metastable CO ionization signal to the intensity decrease of the electron emission signal. It was also shown that vibrationally excited metastable CO leads to a higher electron emission yield. By preparing different vibrational distributions of CO in the a3Π electronic state via Franck-Condon pumping, the electron emission yield was determined for groups of vibrational levels. The first three vibrationally excited levels have an increased electron emission yield which on average is a factor of 1.5 larger than that of the vibrational ground state. Averaged over the vibrational levels with quantum number v = 4, 5, 6 , this factor is approximately 2.6 . In the range between 93 m/s and 512 m/s, the electron emission was observed to be independent of the velocity of the incident molecules. When the surface temperature is raised from 250 K to 900 K, the intensity of the electron emission signal increases by 27 %. These results are not in agreement with the models currently used to describe the de-excitation of electronically excited molecules at metal surfaces. This demonstrates the need for more theoretical work to incorporate the role of vibration into the description of the de-excitation mechanism.
A three-dimensional trap for Rydberg atoms in selected Stark states has been realized experimentally. H atoms seeded in a supersonic expansion of Ar are excited to the low-field seeking n=30, k=25, |m|=0, 2 Rydberg-Stark states, decelerated from a mean initial velocity of 665 m/s to zero velocity in the laboratory frame and loaded into a three-dimensional electrostatic trap. The motion of the cold Rydberg atom cloud in the trap and the decay of the trapped atoms have been studied by pulsed electric field ionization and imaging techniques.