Coherent excitation of Rydberg atoms in an ultracold gas

We demonstrate two schemes for the coherent excitation of Rydberg atoms in an ultracold gas of rubidium atoms employing the three-level ladder system 5S_1/2-5P_3/2-n?_j. In the first approach rapid adiabatic passage with pulsed laser fields yields Rydberg excitation probabilities of 90% in the center of the laser focus. In a second experiment two-photon Rydberg excitation with continuous-wave fields is applied which results in Rabi oscillations between the ground and Rydberg state. The experiments represent a prerequisite for the control of interactions in ultracold Rydberg gases and the application of ultracold Rydberg gases for quantum information processing.     

Observations and analysis of resonant laser ablation of GaAs

Laser ablation of solid GaAs samples has been studied using one tunable pulsed dye laser. At relatively low laser power, enhancements of up to several hundred times have been observed in the yield of resonantly ionised Ga using laser wavelengths corresponding to the atomic transition 4² P _1/2-4² D _3/2. The influences of laser power and target geometry, on the ion yield and spectral profile, are discussed. It is argued that the resonant excitation and ionisation processes occur in the gas phase of the atoms ablated from the sample surface, and the observed asymmetric spectral profile results from laser-induced collisional processes, e.g., optical collisions, under conditions of relatively high atomic density in the interaction region. Potential applications are foreseen for resonant laser ablation in trace analysis.     

Polyatomic molecules formed with a Rydberg atom in an ultracold environment

We investigate properties of ultralong-range polyatomic molecules formed with a Rb Rydberg atom and several ground-state atoms whose distance from the Rydberg atom is of the order of n²a₀, where n is the principle quantum number of the Rydberg electron. In particular, we put emphasis on the splitting of the energy levels, and elucidate the nature of the splitting via the construction of symmetry-adapted orbitals.     

Atomic beam deflection by coherent momentum transfer and the dependence on weak magnetic fields

The deflection of Ne atoms in the metastable state ³ P ₂ by coherent transfer of the momenta of 4 or 8 photons is demonstrated, based on the technique developed for coherent population transfer with delayed pulses (STIRAP). After deflection the intensity profile of the isotope of mass 20 is fully seperated from that for the undeflected atoms of mass 22. It is furthermore shown, how the interplay of Larmor precession of the electronic magnetic moment and the sequential deflection in two spatially separated zones can be used to measure the magnetic field, integrated over the flight-path between the transfer zones. Received: 1 October 1997 / Revised: 22 December 1997 / Accepted: 11 March 1998     

Ionization of fast rydberg atoms in longitudinal and transverse electric fields

The main properties of longitudinal and transverse electric field ionizers for fast Rydberg atoms n=21–40 have been investigated. The dispersion and the background due to collisional processes between fast atoms and residual gas molecules have been measured and calculated. The kinetic energy spread of ions formed by field ionization of Rydberg atoms and their trajectories have been calculated. The potassium beam energy was 3.9 keV.     

Two-color three-photon resonant excitation spectrum of strontium in the autoionization region

We report new studies of the odd parity autoionizing Rydberg series of strontium attached to the 4d( ² D _{3/2, 5/2}) ionic limits possessing J = 1-3 based on the two-color three photon resonant excitation technique in conjunction with an atomic beam apparatus. Using the 4d ²³ P ₀ intermediate levels, we have been able to record the autoionizing Rydberg series of J = 1 whereas, from the 4d ²³ P ₂ intermediate level the series of Rydberg levels possessing J = 1, 2 and 3 have been observed. The level assignments and the line shapes simulations of the autoionizing resonances have been made using the multichannel quantum defect theory. Received 21 November 2001 / Received in final form 2 May 2002 Published online 19 July 2002     

Oscillator strength measurements of the 3p ↦ nd Rydberg transitions of sodium

We report new measurements of the oscillator strengths of the 3p ²P_3/2 ↦nd ²D_{5/2, 3/2} and 3p ²P_1/2 ↦ nd ²D_3/2 Rydberg transitions of sodium using a thermionic diode ion detector in conjunction with the Nd:YAG pumped dye lasers. The ns ²S_1/2 and nd ²D_5/2,3/2 Rydberg series have been recorded via two-step excitation, from the 3p ²P_3/2 and 3p ²P_1/2 intermediate states. Employing the saturation technique, the photoionization cross sections from the 3p ²P_3/2 and 3p ²P_1/2 intermediate states at the first ionization threshold are determined as 7.9(1.3) Mb and 6.7(1.1) Mb respectively. The f-values of the Rydberg transitions are calibrated with the photoionization cross section measured at the first ionization threshold and compared with the earlier data.     

Coherent population trapping involving Rydberg states in xenon probed by ionization suppression

We report the observation of pronounced coherent population trapping and dark resonances in Rydberg states of xenon. A weak two-photon coupling with radiation of = 250 nm is induced between the 5p^{6 1} S ₀ ground state of xenon and state 5p ⁵6p[1/2]₀, leading to (2+1) resonantly enhanced three-photon ionization. The state 5p ⁵6p[1/2]₀ is strongly coupled by radiation with ≃ 600 nm to 5p ⁵ ns[J _C]₁ or 5p ⁵ nd[J _C]₁ Rydberg states with principal quantum numbers n in the range 18 ?n? 23 and with the rotational quantum number of the ionic core J _C = 1/2 or J _C = 3/2. The ionization is monitored through observation of the photoelectrons with an energy resolution ΔE = 150 meV which is sufficient to distinguish the ionization processes into the two ionization continua. Pronounced and robust dark resonances are observed in the ionization rate whenever is tuned to resonance with one of the ns- or nd-Rydberg states. The dark resonances are due to efficient population trapping in the atomic ground state 5p^{6 1} S ₀ through the suppression of excitation of the intermediate state 5p ⁵6p[1/2]₀. The resolution is sufficient to resolve the hyperfine structure of the ns-Rydberg levels for odd xenon isotopes. The hyperfine splitting does not vary significantly with n in the given range. Results from model calculations taking the natural isotope abundance into account are in good agreement with the observed spectral structures. Pronounced dark resonances are also observed when the dressing radiation field with is generated from a laser with poor coherence properties. The maximum reduction of the ionization signal clearly exceeds 50%, a value which is expected to be the maximum, when the dip is caused by saturation of the transition rate between the intermediate and the Rydberg state due to incoherent radiation. This work demonstrates the potential of dark resonance spectroscopy of high lying electronic states of rare gas atoms. Received 7 May 2000 and Received in final form 25 June 2001     

Spin-polarized Dirac-Slater calculations on the energies of hollow argon atom

In this work, the multiplet splitting in terms of a spin-dependent model is analyzed. The spin-polarized and unpolarized single configuration Dirac-Fock-Slater wavefunctions have been used in the evaluation of the total energies of highly ionized argon with different L shell population The transition energies of hollow argon atom with initial configurations 1s ⁰ _1/22s ^m _1/22p ⁿ _1/22p ^l _3/2 with m = 0 to 2 and n + l varying from 6 to 1 are reported in this work. The calculations have been carried out by taking into account a relativistic exchange potential in the Dirac-Slater potential. To account for the correlation effects, a correction term has also been considered perturbatively. The present calculations show that the spin-polarized technique which is mainly applied to the ground states of atoms may also be applied to atoms ionized in the inner shells with a good degree of accuracy. Received 5 December 2000 and Received in final form 9 April 2001     

Back and forth transfer and coherent coupling in a cold Rydberg dipole gas

Coupling by the resonant dipole-dipole energy transfer between cold cesium Rydberg atoms is investigated using time-resolved narrow-band deexcitation spectroscopy. This technique combines the advantage of efficient Rydberg excitation with high-resolution spectroscopy at variable interaction times. Dipole-dipole interaction is observed spectroscopically as avoided level crossing. The coherent character of the process is linked to back and forth transfer in the np + np <--> ns + (n + 1)s reaction. Decoherence in the ensemble has two different origins: the atom motion induced by dipole-dipole interaction and the migration of the s-Rydberg excitation in the environment of p-Rydberg atoms.     

Experimental evidence for molecular ultrafast dissociation in O<Subscript>2</Subscript> clusters

Resonant Auger spectra of O₂ clusters excited at the O1s edge are reported. After excitation to the repulsive 1s^-13σ^* state, the resulting resonant Auger spectrum displays features that remain constant in kinetic energy as the photon energy is detuned. The shift between known atomic fragment features and these features is consistent with that observed for atoms and clusters in singly charged states in direct photoemission. These findings are strong evidence for the existence of molecular ultrafast dissociation processes within the clusters or on their surface.     

Autoionization of an ultracold Rydberg gas through resonant dipole coupling

We investigate a possible mechanism for the autoionization of ultracold Rydberg gases, based on the resonant coupling of Rydberg pair states to the ionization continuum. Unlike an atomic collision where the wave functions begin to overlap, the mechanism considered here involves only the long-range dipole interaction and is in principle possible in a static system. It is related to the process of intermolecular Coulombic decay (ICD). In addition, we include the interaction-induced motion of the atoms and the effect of multi-particle systems in this work. We find that the probability for this ionization mechanism can be increased in many-particle systems featuring attractive or repulsive van der Waals interactions. However, the rates for ionization through resonant dipole coupling are very low. It is thus unlikely that this process contributes to the autoionization of Rydberg gases in the form presented here, but it may still act as a trigger for secondary ionization processes. As our picture involves only binary interactions, it remains to be investigated if collective effects of an ensemble of atoms can significantly influence the ionization probability. Nevertheless our calculations may serve as a starting point for the investigation of more complex systems, such as the coupling of many pair states proposed in [P.J. Tanner et al., Phys. Rev. Lett. 100, 043002 (2008)].     

铯47D精细能级超冷里德堡原子自由演化的动力学研究

用连续窄线宽激光器将超冷铯里德堡原子分别激发到47D_3/2, 47D_5/2精细态, 观察了处于里德堡精细态的铯原子向超冷铯等离子体自由演化的过程, 详细对比了不同精细态的铯里德堡原子预电离时间、电离速率以及等离子体的转化效率. 将里德堡原子快速转化为等离子体的过程解释为局域势阱内由预电离产生的电子与里德堡原子的快速碰撞导致的雪崩电离.     

Photoionization cross sections of Fe XXI

Total and partial photoionization cross sections for (Fe XXI+hν→Fe XXII+e) are presented for the ground and excited bound states with n?10 and l?9. Fe XXI is prevalent in high-temperature astrophysical plasmas as well as in photoionized plasmas excited by hard X-rays. Results are reported for the first time for the high-energy photoionization with core excitations to n=2,3 states. Details of photoionization, especially the high-energy features that often dominate considerably over the low energy ones, are illustrated. These prominent features will affect the photoionization and the recombination rates in high-temperature plasmas. Calculations are carried out in the close coupling (CC) approximation using the R-matrix method. A large CC wavefunction expansion for Fe XXII which includes the ground and 28 excited core states from n=2 and 3 complexes and spans over a wide energy range is used. A total of 835 discrete bound states of Fe XXI in the singlet, triplet, and quintet symmetries are obtained. Total photoionization cross sections, σ_PI(nLS), for ionization into all 29 states are presented for all 835 final bound states and partial photoionization cross sections, σ_PI(g,nLS), for ionization into the ground ²P⁰ state of the core are presented for 685 states. While the n=2 core excitations are at relatively lower energy range (within 15 Ry from the ionization threshold), the n=3 excitations lie at considerably higher energy, 73 Ry and above, yet introduce resonant features and enhancements more prominent than those of n=2 states. Larger numbers of resonances are formed due to Rydberg series of autoionizing states converging on to the 29 core states. However, most noticeable structures are formed in the excited state cross sections by the photoexcitation-of-core (PEC) resonances in the photon energy range of 73-82 Ry. All these high-energy features are absent in the currently available results. The present results should enable more accurate modeling of the emission spectrum of highly excited plasma from the optical to far-ultraviolet region.     

Ionization of barium through a coherent excitation of two bound intermediate states

We have investigated theoretically the asymmetrical photoionization yields into the 6s _1/2, 5d _3/2 and 5d _5/2 continuum channels of atomic barium observed by Wang, Chen and Elliott [Phys. Rev. Lett. 77, 2416 (1996)] in the study of coherent control through two-color resonant interfering paths. The atomic parameters obtained from a theoretical approach based on a combination of jj-coupled eigenchannel R-matrix and Multichannel Quantum Defect Theory are used to analyze the photoionization spectra from the and 6s7p states with polarized light beams. The studied energy range includes the 6p7p autoionizing resonances. The dynamics of the two-color photoionization is governed by the coherent excitation of the 6s6p and intermediate states. This excitation is described as an adiabatic process in the rotating wave approximation. The influence of the radiative decay, spatial distribution of the intensities of the laser beams and hyperfine interaction is discussed. Received 28 September 1999     

Investigation of sub-Doppler cooling effects in a cesium magneto-optical trap

We present an investigation of sub-Doppler effects in a cesium magneto-optical trap. First, a simple one-dimensional theoretical model of the trap is developed for aJ _g = 1 J _e = 2 transition. This model predicts the size of the trapped atom cloud and temperature as a function of laser intensity and detuning. In the limit of small magnetic field gradients, the trap temperature is found to be equal to the molasses temperature and a minimum size for the trap is calculated. We then describe several experiments performed in a three-dimensional cesium trap to measure the trap parameters, spring constant, friction coefficient, temperature and density. Whilst the temperature of the trapped atoms is found to be equal to the molasses temperature, in agreement with theory, the trap spring constant is found to be two orders of magnitude smaller than the one-dimensional prediction, a value close to that predicted by Doppler models. The maximum density is found to be on the order of 10¹² atoms/cm³ or one atom per optical wavelength on average. When the number of trapped atoms becomes large, the temperature begins to increase dramatically. This excess temperature depends in a very simple way on the atom number, laser intensity and detuning, suggesting that its origin lies in multiple photon scattering within the trap.     

Acceleration of cold Rb atoms by frequency modulated light pulses

The displacement of Rb atoms in a magneto-optical trap (MOT) caused by the force of a finite time series of counter-propagating frequency modulated light pulse pairs is measured as a function of the chirp of the pulses. The frequency modulated light pulses induced ⁸⁵Rb 5²S_1/2 F=3 ↔ ⁸⁵Rb 5²P_3/2 F'=2, 3, 4 excitation and de-excitation of the atoms. The result of this excitation de-excitation process is a force causing the acceleration and, consequently, the displacement of the maximum of the spatial distribution of the trap atoms. The time dependence of the populations of the levels of the atom are calculated — including also the ⁸⁵Rb 5²S_1/2 F=2 and F'=1 states — as the result of the interaction with the finite train of counter propagating frequency modulated light pulses by the solution of the Bloch equations. As the result of the measurement the interval of the chirp of the frequency modulated light of given intensity where the transitions take place, are determined. The results of the experiment and the expectation on the basis of model calculations are in qualitative agreement.     

Coherent coupling of a single <Superscript>40</Superscript>Ca<Superscript>+</Superscript> ion to a high-finesse optical cavity

We demonstrate coherent coupling of the quadrupole S_1/2D_5/2 optical transition of a single trapped ⁴⁰Ca⁺ ion to the standing wave field of a high-finesse cavity. The dependence of the coupling on temporal dynamics and spatial variations of the intracavity field is investigated in detail. By precisely controlling the position of the ion in the cavity standing wave field and by selectively exciting vibrational state-changing transitions the ion’s quantized vibration in the trap is deterministically coupled to the cavity mode. We confirm coherent interaction of ion and cavity field by exciting Rabi oscillations with short resonant laser pulses injected into the cavity, which is frequency-stabilized to the atomic transition. Received: 23 August 2002 / Published online: 8 January 2003 RID="*" ID="*"Corresponding author. E-mail: christoph.becher@uibk.ac.at RID="**" ID="**"Present address: Time and Frequency Division, National Institute of Standards and Technology, Boulder, CO 80305, USA     

Detection of oxygen atoms in a high pressure surfatron microwave discharge via two-photon four-wave mixing

3 P_J) oxygen atoms are detected in a high pressure surface wave discharge driven at 2.45 GHz via two-photon resonant degenerate four-wave mixing spectroscopy (TP-DFWM) in the forward folded BOX configuration. The nonlinear optical signal provides a direct measure of the relative oxygen atom concentration with high spatial resolution inside the discharge up to pressures of 1 bar and without distortions due to linear absorption or saturation effects. The axial distribution of oxygen atom concentration is observed to depend sensitively on total pressure and gas flux. For total gas pressures up to 600 mbar both in case of a mixture of 10% O₂/He and 10% O₂/Ar the concentration of oxygen atoms increases linearly with pressure. At higher pressures an increase with larger slope is observed for 10% O₂/Ar, while the concentration remains constant for 10% O₂/He. This is interpreted by an increase of the three-body recombination rate in O₂/He mixtures. Received: 26 July 1996/Revised version: 15 November 1996     

Kinetic energy oscillations in annular regions of ultracold neutral plasmas

A study of ion equilibration in annular regions of ultracold strontium plasmas is reported. Plasmas are formed by photoionizing laser-cooled atoms with a pulsed dye laser. The experimental probe is spatially-resolved absorption spectroscopy using the ²S_1/2-²P_1/2 transition of the Sr⁺ ion. The kinetic energy of the ions is calculated from the Doppler broadening of the spectrum, and it displays clear oscillations during the first microsecond after plasma formation. The oscillations, which are a characteristic of strong coulomb coupling, are fit with a simple phenomenological model incorporating damping and density variation in the plasma.