Relativistic R-matrix close-coupling calculations for photoionization of Ne-like Al IV

We present relativistic close-coupling photoionization calculations of Al IV using the Breit-Pauli R-matrix method to obtain photoionization cross-section of Al IV from the ground state and the lowest two J=0 (even) excited states. A multi-configuration eigenfunctions expansion of the core Al V is employed with spectroscopic configurations 2s²2p⁵, 2s2p⁶, 2s²2p⁴3s, 2s²2p⁴3p, 2s²2p⁴3d and 2s²2p⁴4s. We have included, for the first time, the lowest 68 level target states of Al V in the photoionization calculations of Al IV. Extensive configuration interaction wavefunctions are used to describe both the initial Al IV states and the final Al V states. Cross-sections are compared from three level calculations including only 2s² 2p^{5 2}P^o _3/2, _1/2 and 2s 2p^{6 2}S_1/2 levels of Al V. The present calculation using the lowest 68 target levels of Al V are presented for the first time and should provide reasonably complete database for practical application for photoionization cross-section for Al IV, where high-energy cross-sections along with near-threshold photoionization cross-section is required.     

Temporal coherent control induced by wave packet interferences in one and two photon atomic transitions

The interaction of a sequence of two identical ultrashort laser pulses with an atomic system results in quantum interferences as in Ramsey fringes experiments. These interferences allow achievement of temporal coherent control of the excitation probability. We present the results of a temporal coherent control experiment on two different atomic systems: one-photon absorption in K (4s-4p) and two-photon absorption in Cs (6s-7d). In K, the quantum interferences between the two excitation paths associated with the laser pulses are revealed through rapid oscillations of the excitation probability as a function of the time delay between the two pulses. These oscillations take place at the transition frequency (period T = 2.56 fs). The interferences are modulated by beats (at about 580 fs) resulting from the doublet structure of the excited state (4p (² P _1/2 , ² P _3/2 )). Three complementary interpretations of this experiment are presented: in terms of beats of quantum interferences, of variation in the spectrum intensity, and of wave packet interferences. Whenever the two laser pulses are temporally overlapped, optical interferences are superimposed on to the quantum interferences. The distinction between these two types of interference is clearly revealed in the two-photon excitation scheme performed on Cs (6s-7d (² D _3/2 , ² D _5/2 )) because quantum interferences occur at twice the frequency of the optical interferences. Received: 30 December 1997 / Revised: 28 February 1998 / Accepted: 4 March 1998     

Near-threshold electron-impact ionization of calcium atoms

The electron-impact ionization of calcium atoms is studied in the near-threshold energy range (from 6.11 to 16 eV). Experiments were performed by the method of intersecting electron and atomic beams with the recording of formed positive calcium ions. The electron beam (ΔE _1/2 = 0.15 eV) was formed using a hypocycloidal electron monochromator. An analysis of the specific features of ionization cross sections revealed a contribution from the excitation and decay of low-lying autoionization atomic states, which converge to the excitation thresholds of the 3d, 4p, and 5s ionic levels, and resonances (long-lived states of negative ions). The specific features of cross sections are identified using the experimental and theoretical data on photoionization (photoabsorption).     

Experimental study of autoionizing states of AuI

This paper describes the investigation of the autoionizing states of AuI by exciting the states of 6d ² D _3/2 and 6d D _5/2 with tunable dye lasers by means of a resonance ionization time-of-flight mass spectrometer (RI-TOFMS). Many new autoionizing states were found, a few of which have narrow-linewidths of about 0.1 cm^–1. The photoionization efficiencies for different channels were compared. Among the autoionizing states found so far, the highest photoionization yield is given by two newly obtained states from the state 6d ² D _5/2, 3683.6 cm^–1 and 4636.5 cm^–1 above the first ionization limit. In addition, the Shore-Fano profile parameters of several autoionizing resonances were determined by a nonlinear fitting program.     

Photoionization cross-section measurements from the 2p, 3d and 3s excited states of lithium

The photoionization cross-sections from the 2p²P_{1/2, 3/2}, 3d²D_{3/2, 5/2} and 3s²S_1/2 excited states of lithium have been measured at different ionizing laser wavelengths, above the first ionization threshold. The experiments are performed by using a thermionic diode working in the space charge limited mode and the cross-sections are measured by employing the saturation technique. By changing the ionization photon energy, a smooth frequency dependence of the cross-sections has been observed for the 2p and 3d states. The cross-section from the 3s excited state has been measured at a single photon energy. The measured values of the photoionization cross are compared with the available data.     

Near threshold photoionization of excited alkali atoms Ak(np) (Ak = Na, K, Rb, Cs; n = 3-6)

The effect of the polarization of the atomic core by the outer electron on near threshold photoionization of excited alkali atoms Ak(np) (Ak = Na-Cs; n=3-6) is investigated. Partial and total cross-sections for photo-ionization of the np-electron were computed utilizing the configuration interaction technique with Pauli-Fock atomic orbitals (CIPF) and including the long range core polarization potential (CP). To calculate the core polarization potential the variational principle is applied. Comparison with previous theoretical results and with available experimental data is made for the total cross-section , for the electron angular distribution parameter , for the ratio of the reduced electric dipole matrix elements and for the phase shift difference , associated with the d-wave and s-wave continua, respectively. In the comparison, new experimental results for , , and , measured for laser-excited, polarized ³⁹K(4p _3/2) atoms, have been included. Received 21 July 1999 and Received in final form 14 October 1999     

Two-color photoionization spectroscopy of uranium in a U–Ne hollow cathode discharge tube

A U–Ne hollow cathode discharge tube is used as a source of uranium atomic vapors as well as a photoelectron/photoion detector for carrying out two-color three-photon photoionization spectroscopy of uranium. Using the uranium excitation transition 0 cm⁻¹ (⁵L ₆ ⁰ ) → 16 900.38 cm⁻¹ (⁷M₇) at 591.5-nm laser wavelength as a first step transition and scanning the wavelength of a second laser from 558 to 568 nm, high-lying odd-parity atomic levels of uranium are studied in the energy region 34 500–34 813 cm⁻¹. All the expected 21 odd-parity atomic levels identified by various researchers in this region are observed in a single spectrum, demonstrating the high sensitivity achieved therein. In addition to this, we have identified eight autoionization resonances of uranium starting from its odd-parity atomic level at 33 801.06 cm⁻¹ pumped by two-photon excitation. Four out of these eight autoionization resonances are observed for the first time.     

Measurements of photoionization cross sections from the 4p, 5d and 7s excited states of potassium

New measurements of the photoionization cross sections from the 4p ²P_1/2,3/2, 5d ²D_5/2,3/2 and 7s ²S_1/2 excited states of potassium are presented. The cross sections have been measured by two-step excitation and ionization using a Nd:YAG laser in conjunction with a thermionic diode ion detector. By applying the saturation technique, the absolute values of the cross sections from the 4p ²P_3/2 and 4p ²P_1/2 states at 355 nm are determined as 7.2±1.1 and 5.6±0.8 Mb, respectively. The photoionization cross section from the 5d ²D_5/2,3/2 excited state has been measured using two excitation paths, two-step excitation and two-photon excitation from the ground state. The measured values of the cross sections from the 5d ²D_5/2 state by two-photon excitation from the ground state is 28.9±4.3 Mb, whereas in the two-step excitation, the cross section from the 5d ²D_3/2 state via the 4p ²P_1/2 state and from the 5d ²D_5/2,3/2 states via the 4p ²P_3/2 state are determined as 25.1±3.8 and 30.2±4.5 Mb, respectively. Besides, we have measured the photoionization cross sections from the 7s ²S_1/2 excited state using the two-photon excitation from the ground state as 0.61±0.09 Mb.     

The shapes of Auger decay lines in photoelectron satellite spectra

The theory of the shapes of Auger decay lines of satellite two-hole-one particle states accompanying photoionization based on the Green's function method is developed. The lineshapes of Auger decay of satellite states [2 s 2 p ]( ^1,3 P )3 s ( ² P ), [2 s 2 p ]( ¹ P )4 s ( ² P ) and [3 s 3 p ]( ³ P )4 s ( ² P ) in valence p-photoelectron spectra of Ne and Ar atoms are calculated (hole states are indicated by square brackets throughout). It is shown that in some cases the Auger lineshapes reproduce the shape of the photoelectron satellite line, but in other cases Auger line may be narrower then the photoelectron line and may have opposite direction of asymmetry. The theoretical results are in agreement with experimental low-energy Auger spectra. Received: 25 May 1998 / Accepted: 2 October 1998     

High resolution measurement and MQDT analysis of the 5d<Superscript>9</Superscript> 6s<Superscript>2</Superscript> np,nf (J = 1) autoionizing resonances of mercury

We report new high resolution photoabsorption measurements of the 5d-subshell excitation spectra of mercury using a 3-meter normal incidence spectrograph equipped with a 6000 line/mm holographic grating and synchrotron radiation emitted by the Bonn 2.5 GeV electron accelerator as the background source of continuum. The observed spectra reveal autoionizing resonances attached to the 5d⁹(²D_5/2)6s² and 5d⁹(²D_3/2)6s² parent ion levels of mercury. We have analysed the line shapes of the lower members of the 5d⁹6s² np and nf J = 1 autoionizing resonances using the phase shifted formulation of the MQDT and extracted the interaction parameters.     

Investigation of auto-ionizing states in xenon by resonantly enhanced multi-photon ionization

We have examined the autoionization spectrum of xenon by resonantly enhanced three-photon ionization (2 + 1 REMPI) involving intermediate states 5p ⁵6p[J = 0, 2]. The properties of the observed autoionization resonances change significantly with the choice of the intermediate state. For ionization via an intermediate state with predominantly 5p ⁵(²P_3/2) core character, a strong continuum with embedded window-type 5p ⁵(²P _1/2)nd'-autoionization resonances is observed. For intermediate states, predominantly with 5p ⁵(²P_1/2) core character, both 5p ⁵(²P _1/2)nd'- as well as 5p ⁵(²P _1/2)ns'-resonances are present in the spectrum as overlapping, nearly symmetric peaks on a rather weak continuum. Calculations confirm the significant dependence of the spectral lineshapes upon the excitation pathway to the autoionizing state. The ionization data are compared with spectra obtained by monitoring third-harmonic generation via autoionizing states without resonant excitation of intermediate states. These spectra also exhibit the signature of both the nd'- and ns'-resonances. Received 30 September 2002 Published online 28 January 2003 RID="a" ID="a"Permanent address: Rostov State University of Transport Communication, 344038, Rostov-on-Don, Russia. RID="b" ID="b"e-mail: halfmann@physik.uni-kl.de     

Rb atomic absorption line reference for single Sr+ laser cooling systems

85 Rb, 5s²S_1/2(F”=2)→6p²P_1/2(F’=2,3) absorption resonance with the ⁸⁸Sr⁺, 5s²S_1/2→5p²P_1/2 transition is exploited to provide a simple, effective frequency reference for a laser cooling/fluorescence excitation source applied to single Sr⁺ ions. A modulation-free frequency stabilization system has been designed which uses the differential signal from two frequency-displaced beams traversing a Rb cell and which probe the Doppler-broadened Rb S–P lineshape at microwatt power levels. The method is applied to frequency lock a 422-nm frequency-doubled diode laser system that is used for excitation of a single ⁸⁸Sr⁺ ion. Stable, long-term laser cooling and fluorescence are achieved using the frequency-stabilized 422-nm source resulting in observed ion confinement times without adjustment of over 8 h, together with an improvement in single-ion loading efficiency. Received: 12 February 1998     

Experimental and theoretical analysis of the 5 pnpJ =0 e , 1 e , 2 e autoionizing spectrum of Sr

The even parity 5 pnpJ = 0, 1 and 2 doubly excited autoionizing states of strontium were investigated both experimentally and theoretically. Sr atoms in an atomic beam were excited through the two-step Isolated Core Excitation (ICE) scheme 5s^{2 1} S ₀ -λ ₁ → 5 sn'p ¹ P ₁ ( n' = 12-16)-λ ₂ → [5 p _3/2 np ] _J . The final ICE transition probes the [5 p _3/2 np ] _J resonances. However, the [5 p _1/2 np ] _J series below the 5 p _1/2 threshold were excited also due to their mixing with the [5 p _3/2 np ] _J perturbers. An extended energy region was covered below and above the 5 p _1/2 ionization limit by saturating the central ICE lobe and recording as many as possible “red” and “blue” secondary lobes. J identification was achieved by using mutually parallel and perpendicular linear polarizations of the laser beams. The ICE spectra were compared to those obtained by employing a two-step excitation scheme using the bound 4 d 5 p ¹ P ₁ valence state as an intermediate one. Final identification for very complex structures was achieved after comparison with theoretical energy level positions and excitation profiles produced by the R-matrix method combined with the multichannel quantum defect theory (MQDT) method. The agreement between theoretical and observed structures is quite satisfactory. Received 31 May 2000     

Two dimension selective coherent population trapping controlled by a phase shift

Two-dimensional laser cooling based on velocity-selective coherent population trapping is investigated theoretically for the J _g=1J _e=0 atomic transition. Wavevectors and polarizations of three laser beams are chosen to realize a coherent superposition of three degenerate ground states. For the first time in laser cooling, use is made of the electric field phases to realize coherent population trapping selective in two dimensions. Numerical solutions and analytic estimates are presented for laser cooling of helium atoms.     

Polarization correlation in the two-photon decay of atomic hydrogen: nonlocality versus entanglement

From the work by Perrie et al. [Phys. Rev. Lett. 54, 1790 (1985)], photon pairs from the 2s _1/2 → 1s _1/2 (two-photon) decay of atomic hydrogen are known to be quantum mechanically correlated. In these experiments, the polarization states of the photons emitted in back-to-back geometry were shown to violate the Bell inequality as a qualitative sign of nonlocality and entanglement. In the present contribution, we analyze how these nonlocal quantum correlations, as given by the violation of the Bell inequality, differ from the concurrence as a true entanglement measure. Results are shown for both quantifiers in dependence of the decay geometry and the initial polarization of the atoms for the 2s _1/2 → 1s _1/2 and 3d _5/2 → 1s _1/2 two-photon decay of atomic hydrogen. These results display the difference between nonlocality and entanglement and, hence, may stimulate further experiments on nonlocal quantum correlations in atomic systems.     

On the strong influence of inner shell resonances upon the outer shell photoionization of endohedral atoms

It is demonstrated by the example of the Xe atom stuffed inside the C₆₀ fullerene, i.e., the endohedral Xe@C₆₀, that the so-called confinement resonances in 4d subshell strongly affect the photoionization cross section of outer 5p and subvalent 5s electrons near the 4d ionization threshold. It is a surprise that these narrow inner 4d shell resonances are not smeared out in the outer shell photoionization cross section. On the contrary; the inner shell resonances affect the outer cross section by enhancing them enormously. Close to its own photoionization thresholds, 5p and 5s photoionization cross sections of Xe@C₆₀ are dominated by their own confinement resonances greatly affected by the amplification of the incoming radiation intensity due to polarization by it of the C₆₀ electron shell. Between 4d and 5p thresholds, the effect of 4d is becoming stronger while own resonances of 5p and 5s are becoming much less important.     

Molecular dissociative sequential excitation and ionization of strontium vapor

We report new measurements on laser-assisted molecular dissociative sequential excitation and ionization spectra of strontium vapor. A single Nd:YAG pumped dye laser in conjunction with an atomic beam apparatus have been used to investigate the even parity 5snd ^3,1 D ₂ Rydberg series resulting from the 5s5p ¹ P ₁ resonance level. The relative intensities changes among the 5snd ³ D ₂ and ¹ D ₂ Rydberg series are attributed to the interactions with the 4d6s ^1,3 D ₂ perturbers, respectively. The interchannel interactions between the 5snd ¹ D ₂ series and the 4d6s ¹ D ₂ level and among the 5snd ³ D _1,2,3 series and the 4d6s ³ D _1,2,3 intruders have been separately parameterized using the two-channel quantum defect theory. Received: 10 September 1998 / Received in final form: 16 December 1998     

Two-color pump-probe experiments in helium using high-order harmonics

A pump-probe technique has been applied for measuring the lifetimes and absolute photoionization cross-sections of excited He states. The 1s2p ¹P and 1s3p ¹P states of He are excited by using the 13th and the 14th harmonic, respectively, of a tunable 70 ps dye laser generated in a Kr gas jet. The states are ionized after a varying time delay, by absorption of probe photons with energies between 1.6 and 4.5 eV. Lifetimes of τ(1s2p) = 0.57 ns and τ(1s3p) = 1.76 ns are determined with a precision of about 15%. A significant enhancement of the number of ions present in the lifetime curves at zero time delay for pressures above 6×10^-5 mbar is attributed to direct two-photon ionization of He in combination with AC Stark broadening of the excited state and absorption of the XUV light in the medium. Absolute photoionization cross-sections from the He 1s2p ¹P and He 1s3p ¹P states in the threshold region are determined by measuring the saturation of the ionization process with a precision of ∼ 25%. In addition, the variation of the relative orientation between the polarization vectors of the pump and probe beams enables the determination of partial photoionization cross-sections. Received 3 June 2002 / Received in final form 14 August 2002 Published online 22 October 2002 RID="a" ID="a"Present address: Department of Biophysics, Leiden University, 2333 CA Leiden, The Netherlands. RID="b" ID="b"Present address: Continuum Electro-Optics Inc., 3150 Central Expressway, Santa Clara, CA 95051, USA. RID="c" ID="c"Present address: CEA/DRECAM/SPAM, CEN Saclay, 91105 Gif-sur-Yvette, France. RID="d" ID="d"Present address: Department of Physics, National University of Rwanda, Butare, Rwanda. RID="e" ID="e"Present address: CELIA, Université Bordeaux 1, 33405 Talence, France. RID="f" ID="f"Present address: MAX-Lab, Lund University, Box 118, 221 00 Lund, Sweden. RID="g" ID="g"e-mail: anne.lhuillier@fysik.lth.se     

Resonance-enhanced multiple-photon ionisation spectroscopy of excited sulphur atoms

Sulfur atoms are produced in the excited 3s ²3p ^{4 1} D ₂ and 3s ²3p ^{4 1} S ₀ levels by two-photon photodissociation of CS₂ in the gas phase in the region 285–305 nm. These excited atoms are detected by three-photon (two to resonance) ionisation at selected laser wavelengths. Many new transitions have been observed which have not been reported previously. The new dark states that have been accessed by two-photon absorption have been characterised and the energy levels with respect to the ground ³ P ₂ state have been determined. Configuration interaction between 6p ³ P ₁, 6p ⁵ P ₁, and 4p¹ P ₁ states, and also between 6p ³ P ₂, 6p ⁵ P ₂, and 4p¹ D ₂ states has been observed. It is found that intermediate states reached from the ¹ S ₀ level through two-photon absorption lie above the first ionisation potential of S⁺(⁴ S ⁰). It is proposed that autoionisation into the ⁴ S ⁰+e^– continuum is a dominant mechanism in the decay of these levels, although ionisation by a further photon absorption is not ruled out.     

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