Control of diabatic versus adiabatic field dissociation in a heavy Rydberg system

A novel phenomenon is observed in the dynamics of laser-prepared coherent wave packets, bound by the Coulombic 1/r potential of an ion-pair system. After exciting weakly bound (approximately 3 meV) H(+)(-) wave packets in a Stark field, and permitting them to evolve in time, control of field dissociation via adiabatic and diabatic routes is demonstrated by applying delayed pulsed-electric fields, involving a zero-field crossing. Control manifests itself through the production of ions from each pathway at a different instant in time. This phenomenon is applied to map the oscillatory behavior of an angular momentum wave packet in a heavy Rydberg system. The characteristic frequencies of the observed Stark oscillations verify predicted mass-scaling laws for heavy Rydberg systems.     

Measuring the degree of unitarity for any quantum process

The state transfer from cesium nS (n = 45?53) states to Stark (product) states induced by a weak electric field (WEF) pulse was investigated using the state-selective field ionization method in a standard magneto-optic trap (MOT). The WEF pulse shifts the nS Rydberg states that anticross with the (n ? 4) hydrogen-like manifolds, causing state transitions from the initial excited nS state to the Stark states. The mechanism of transfer was investigated by changing the rising and falling time of the WEF pulse and the switching off time of the external field pulse had an important role during the evolution process of product states. The population of the product states is also measured as a function of the principal quantum number and Rydberg densities.     

Entangling quantum gate in trapped ions via Rydberg blockade

We present a theoretical analysis of the implementation of an entangling quantum gate between two trapped Ca⁺ ions which is based on the dipolar interaction among ionic Rydberg states. In trapped ions, the Rydberg excitation dynamics is usually strongly affected by mechanical forces due to the strong couplings between electronic and vibrational degrees of freedom in inhomogeneous electric fields. We demonstrate that this harmful effect can be overcome using dressed states that emerge from the microwave coupling of nearby Rydberg states. At the same time. these dressed states exhibit long-range dipolar interactions which we use to implement a controlled adiabatic phase gate. Our study highlights a route toward a trapped ion quantum processor in which quantum gates are realized independently of the vibrational modes.     

Stark shift and dissociation process of an ionized donor bound exciton in spherical quantum dots

The effect of an electric field on the ground state energy of an exciton bound to an ionized donor (D⁺, X) was studied in CdSe spherical quantum dots where quantum confinement is described by an infinitly deep potential. Calculations have been performed in the framework of the effective mass approximation using a variational method by choosing an appropriate sixty-terms wave function taking into account different interparticles correlations and symetry distorsion induced by the electric field. It appears that the Stark shift is significant even for low fields and depends strongly of spherical dot sizes. The competition between the confinement effect and the Stark effect is discussed as function of the spherical dot size and the applied electric field strength. The (D⁺, X) Stark shift is estimated and its behavior is discussed as a function of the dot radius and electric field strength. The electron and hole average distances have also been calculated and the role of the ionized donor in the excitonic dissociation is established.     

铯Rydberg原子Stark态的避免交叉

在磁光阱中利用双光子激发制备49S铯Rydberg原子,研究了超冷49S态原子在外加电场中的Stark效应和nS态原子与(n-4)多重态之间的避免交叉现象.利用态选择脉冲场电离方法测量并获得了避免交叉点附近的离子谱,测量了避免交叉点附近离子谱的变化情况,并观察到避免交叉点附近由相互作用导致的态转移现象.     

Three photon resonant ionization in atomic potassium via S,P, D and F series Rydberg states

Single colour three photon resonant ionization (2 + 1) is observed in atomic potassium vapour in a heat pipe oven using an excimer laser pumped dye laser. Using wavelengths between 570 nm and 603 nm various²S and²D Rydberg states are populated by two photon excitation. Third photon of the same wavelength ionizes the atoms. Rydberg states up ton ⋍ 50 are observed. Electric field as low as 1 V/cm causes extensive Stark mixing of the states. This results in progressively higher three photon ionization signals via the perturbed²P and²F Rydberg states. The three photon ionization process is studied using both linearly and circularly polarized incident light. The experiment shows qualitatively that the²P Rydberg states are perturbed primarily by the²D states in the prescence of an external electric field and to a much smaller extent by²S states. This is also explained theoretically by calculating the Stark mixing coefficients under the Bates and Daamgard (1949) approximation. Implication for a similar effect in other alkali elements is discussed.     

Second and fourth order stark shifts in the 6snd 1 D 2 barium rydberg series

Stark splittings of⁶ snd ¹ D ₂ Rydberg states were measured betweenn=10 and 24 by quantum beat spectroscopy at very low electric field strengths, allowing the determination of tensor polarizabilities and atn=14, 19, and 24 the determination of tensor hyperpolarizabilities. The irregular behaviour of the tensor polarizabilities was explained by Coulomb approximation calculations. The fourth order contributions to the Stark Hamiltonian were written as effective operators. Representation in spherical tensor form gives tensors of rank zero, two, and four. The associated scalar and tensor hyperpolarizabilities were derived. Using these formulae, theoretical values for the hyperpolarizabilities were calculated.     

分子里德伯态的电子能级结构——一些小分子及分子离子的里德伯能级结构

本文在独立电子近似的基础上,利用多重散射自洽场理论方法,计算了He₂,H₂等分子和He₂⁺分子离子的里德伯能级结构。根据分子的电子组态极限,确定了各里德伯系列初始态的主量子数,阐明了这些分子和分子离子里德伯能级结构的变化规律。理论计算的结果同已有的实验数据符合良好,从而为超越独立电子近似的计算打下了基础。     

Dissociation energies of the I(3/2g) and I(1/2g) states of Ar+ 2

Rotationally resolved pulsed-field-ionization zero-kinetic-energy (PFI-ZEKE) photoelectron spectra of ⁴⁰Ar₂ and ³⁶Ar₂ have been recorded between 124650cm^?1 and 127 150cm^?1 following resonant two-photon excitation via the 0⁺ _u (v¹= 0) Rydberg state located below the Ar (¹S₀) + Ar?((3p)⁵4s′ [1/2]₁) dissociation limit. Four overlapping vibrational progressions were observed and attributed to transitions to the I(1/2u) u⁺ = 35–50, I(3/2g) u⁺ = 0–10, I(1/2g) v⁺ = 0–6 and I(3/2u) v⁺ = 0–2 vibronic states of Ar⁺ ₂. The vibrational quantum numbers of the ionic states were derived from an analysis of the isotopic shifts, and the dissociation energies of the I(3/2g) (D⁺ ₀(⁴⁰Ar⁺ ₂:) = 1509.4 ± 1.2cm^?1) and the I(1/2g) (D⁺ ₀(⁴⁰Ar⁺ ₂) = 616.3 ± 1.2cm^?1) states were determined.     

Measurement of the three-dimensional velocity distribution of Stark-decelerated Rydberg atoms

The full three-dimensional velocity distributions of decelerated and accelerated particles in a Stark decelerator for Rydberg atoms and molecules have been measured. In the experiment, argon atoms in a supersonic beam are excited to low-field and high-field seeking Stark states with principal quantum number in the range n=15 to 25 and are decelerated in a 3 mm long decelerator consisting of four electrodes on which time-dependent voltages are applied. The time dependence of the resulting inhomogeneous electric field is chosen such that the decelerating force acting on the high-field seeking states is maximized at each point along the trajectories. The three-dimensional velocity distribution of the atoms before and after the deceleration is determined by measuring times of flight and two-dimensional images of the atomic cloud on the detector. Under optimal deceleration conditions, the decrease in kinetic energy in the longitudinal dimension amounts to 1.0×10^-21 J and the increase in mean kinetic energy in the transverse dimensions is only 1.0×10^-23 J. The corresponding temperatures of 100 mK and 300 mK in the two transverse dimensions are sufficiently low that trapping can be envisaged. The possibility of focusing a Rydberg atom beam is demonstrated experimentally.     

Exact expressions for the potential functions of a molecule in terms of the probability amplitudes of electron transitions and their utilization in the inverse spectroscopic problem

The frequencies of 5s ³ S ₁-np ³ P ₁ Rydberg transitions, quantum defects for n=15–50, and energies of high-lying P states of the Zn atom were measured by three-step laser excitation with subsequent ionization by a pulsed electric field. Free Zn atoms were produced through effusion of Zn vapor from an atomizer during the thermal dissociation of ZnS molecules. The evaporation kinetics was studied, and the ZnS vapor pressure was measured by the detection of photoionic signals of Zn.     

Electric field induced anomalies in frequency shift and collisional perturbations in the 5snd D2 Rydberg series of strontium in a heatpipe setup with ionization detection

We have examined the effect of weak DC electric field (2-20 V/cm) complimented by foreign gas collisions on the bound J = 2 even-parity 5snd ¹D₂ Rydberg states of neutral strontium. We use resonant two-photon transverse excitation, employing a narrow bandwidth tunable dye laser and an atomic jet in a heatpipe setup with ionization detection. In this paper we report certain anomalies in the observed spectra covering principal quantum number range n = 27-42 indicating a frequency shift reversal with nearly quadratic dependence on the field strength above an anti-resonance region. Furthermore, we have observed the emergence of highly localized doubly-excited 4d² states, including a remarkably broad perturber with large angular momentum, uncovering orbital contraction effect. This non-Rydberg excitation, which intrudes upon the two-photon spectrum with large energy overlap is due to single-photon excitations from the 5s5p ¹P₁ resonance level following molecular dissociation of the Sr₂ dimers suitably governed by binary atomic collisions. Our study which involves laser excitation complimented by electric field and collisions using inexpensive home-made setup opens up the possibilities for a new class of experiments, with considerable simplicity in the choice of excitation schemes for both Rydberg and non-Rydberg transitions, to reach states lying at high energies which cannot otherwise be accessed from the ground state due to parity and selection rules, while allowing one to probe localization properties of atomic wave functions.     

Detection and study of Rb I Rydberg states

We describe the details of an experiment using an atomic beam of rubidium which allowed us to detect by field ionization techniques the np Rydberg states from n = 28 up to n = 78, to detect also ns and nd states using a Stark mixing, and for all of these detected states to check the classical law E_c = [16n^*4]^?1 concerning the critical ionizing electric field E_c. It turns out that for n as high as 65 this law is quite well verified.     

Influence of the surface electric field in ion-beam-surface interaction at grazing incidence

We have measured the polarization of light emitted after ion surface scattering at small angle of incidence. The measurements are carried out with H⁺-, H ₂ ⁺ - and He⁺-ions under UHV-conditions with mono- and polycrystalline targets. We explain the typical variation of the polarization as “post collision Stark interaction” (PCSI) in the surface electric field, which can force transitions between nearly degenerate terms. The electric field is composed of two different contributions, a strong but short range surface field which is “seen” by atomsand ions and a long range but weak field due to the image charge which is “seen” to first orderonly by ions. The influence of the electric field on H-Balmer radiation is negligible at typical survival distances r_s≧0.35nm. But in contrast to H-atoms He⁺-ions feel the additional influence of the image field leading to a strong alteration of the polarization of the emitted light. The polarization of the Balmer-radiation stemming from Coulomb exploding H ₂ ⁺ -beams is observed to be modified by the electric field of the “spectator proton”.     

Sr原子里德堡态的电场效应

用ππ偏振光分步激发方法测量了Sr原子n=12和n=13附近里德堡态的Stark结构。Stark图显示Sr原子在低电场区Stark簇的线性特征。讨论了能级的交叉与抗交叉结构及其与量子亏损的关系。 关键词：     

Atomic and molecular ions in intense ultra-fast laser fields

The interaction of a 60 fs 790 nm laser pulse with beams of Ar⁺, C⁺, H₂ ⁺, HD⁺ and D₂ ⁺ are discussed. Intensities up to 10¹⁶ Wcm^-2 are employed. An experimental z-scanning technique is used to resolve the intensity dependent processes in the confocal volume.Received: 6 January 2003, Published online: 15 July 2003PACS: 32.80.Fb Photoionization of atoms and ions - 33.80.Rv Multiphoton ionization and excitation to highly excited states (e.g., Rydberg states) - 42.50.Hz Strong-field excitation of optical transitions in quantum systems; multiphoton processes; dynamic Stark shift     

Perturbation theory for the intensity of Stark lines of a hydrogen atom

Perturbation theory for the wave function of a hydrogen-like atom in a homogeneous electric field of strength F makes it possible to obtain the Rayleigh-Schrödinger series with the coefficients of F ^N (N=0, 1, 2,...) being linear combinations of the Sturm function, which represents the unperturbed state, with 8N ² functions of the corresponding complete set with indices adjacent to the parabolic quantum number of the initial level. A method for recursive analytic calculation of the coefficients of the linear combination for any order N is developed. General expressions for corrections to the matrix elements and intensities of the radiation transitions between Stark sublevels are obtained. Analytic formulas and numerical values of the corrections up to the fourth order for the Lyman and Balmer series are presented. A comparison with the available data for transitions between the Stark components of Rydberg states is given.     

Continuous wave field ionization laser spectroscopy

A new technique is described which allows Doppler-free, isotope-selective excitation of atoms by continuous wave laser radiation and continuous ionization of the atoms by an electric field. The atoms are excited to high Rydberg states in an electric-field-free region of a collimated atomic beam. Because the lifetimes of Rydberg atoms are long they can reach a spatially separated region of the atomic beam where they are ionized by a continuous electric field with a probability of unity. In the case of lithium we obtained a 10³ times larger ion signal by field ionization of Rydberg atoms than by direct photoionization from low excited states.