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     

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.     

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     

Influence of the helium autoionization structures on the single/double ionization signal

Calculations of intense field (around 10¹⁶ W/cm²) single- and double-ionization processes in helium at XUV wavelengths are presented. The laser wavelength is chosen near the | 2s2p ¹ P autoionization structure and the dynamics are explored. Single and double ionization yields, as well as the photoelectron energy spectrum for photon energies around the autoionization structure are calculated. In the case of a pulse of few femtoseconds duration, no significant enhancement of the double ionization yield has been found in tuning the photon frequency around the peak of the resonance. It is also shown that in the case of a long pulse (and hence narrow compared with the relevant autoionization width), the branching ratio of double to single ionization yield can be relatively enhanced by tuning to the absorption minimum of the resonance. Received 19 February 2002 / Received in final form 2 May 2002 Published online 19 July 2002     

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.     

autoionizing levels in Ca: laser optogalvanic spectroscopy and theoretical analysis

We report the even parity J =4,5 autoionizing spectra of calcium below the 3d threshold, investigated by two-step laser excitation from the 3d4s metastables through the 3d4p , intermediate states and subsequent optogalvanic detection. The 3d4s states are populated by electronic collisions in a d.c. glow discharge sustained in a Ca heat-pipe. More than a hundred resonant transitions have been measured with an accuracy of for the narrow ones using standard laser calibration techniques. The high lying levels are assigned to all expected autoionizing series. Moreover, some levels are observed. The theoretical interpretation is achieved by a combination of the nearly ab initio eigenchannel R-matrix and multichannel quantum-defect (MQDT) methods as well as by an empirical determination of the MQDT parameters in the phase-shifted formulation. Theoretical energy level positions and excitation profiles are compared with the experimental data confirming the identification of the observed structures. Strong mixing between series is found, while the ones do not couple with the series. Further insight into the strong channel mixing in the studied energy range is provided by a comprehensive review of the excitation profiles in the vicinity of the 4p5p perturber as obtained from a number of intermediate levels used in the present and in earlier experiments. Systematic electron correlation trends for series of , and are discussed. Received: 20 November 1997 / Accepted: 15 January 1998     

Elliptic dichroism in hydrogen ionization by a coherent superposition of two harmonics

The two-photon ionization of the hydrogen atom from its ground state by a two-colour electromagnetic field consisting of two odd harmonics of the same IR laser is analyzed. The influence of the state of polarization of the bichromatic field on the azimuthal angular distribution and the dependence of the elliptic dichroism on the photon frequencies are reported. Received 11 December 2002 Published online 29 April 2003 RID="a" ID="a"e-mail: fritz.ehlotzky@uibk.ac.at     

Ionization of a hydrogen atom from its ground state by a coherent bichromatic laser field

We study the “coherent phase control” between the three-photon ionization by a fundamental laser field and the one-photon ionization by its third harmonic for a hydrogen atom in its ground state. The relative phase δ of the harmonic field with respect to the fundamental laser radiation “modulates” the interference between the two ionization channels, which is important near the crossing points between the ionization rates of the two individual processes. Numerical results for the total ionization rate and for the angular distribution of the photoelectrons as a function of the phase δ are presented for frequencies located in the vicinity of the atomic resonances corresponding to the absorption of two laser photons. Received 31 August 2000 and Received in final form 6 February 2001     

Phase properties of a Jaynes-Cummings model with Stark shift and Kerr medium

Phase properties of the field interacting with a two-level atom in a lossless cavity Jaynes-Cummings model, taking into account the level shifts produced by Stark effect with an additional Kerr medium for one-mode are studied using the phase formalism of Pegg and Barnett. It is shown in particular that phase properties of the field reflect the collapse and revival phenomena. The results for the time evolution of the phase probability distribution and the phase fluctuations are obtained. The effect of Stark shift on the phase properties in both the absence and presence of a Kerr medium is analyzed. Phase localization is found for certain choice of the parameters. Received: 27 March 1998 / Revised: 8 June 1998 / Accepted: 9 June 1998     

High order harmonic generation optimization with an apertured laser beam

We report a systematic study of high order harmonic generation with an infrared laser apertured by an iris, as a function of the aperture size. Measurements were made of harmonic generation efficiency for different gas species, laser energies and focal geometries. Harmonic efficiencies as a function of aperture show a characteristic peaked shape, which is independent of gas species and harmonic order. A one dimensional, time dependent simulation of harmonic generation in a gas cell, taking into account experimentally measured transverse coherence of the laser, closely reproduces the observed behaviours. We show that the aperture diameter which maximizes harmonic yield is the result of a compromise between considerations of focal geometry and ionization (which favour small apertures); and harmonic dipole amplitude and phase (which favour large apertures). Received 31 May 2002 Published online 24 September 2002 RID="a" ID="a"e-mail: kazamias@ensta.fr RID="b" ID="b"UMR 7639 du CNRS     

The dynamics of a THz Rydberg wavepacket

An optically excited Rydberg wavepacket can be generated by exciting the electron from a low-lying state to a coherent superposition of high-lying states with a short broadband optical pulse. A special kind of Rydberg wavepacket is generated in the case of a interaction of a weak THz half cycle pulse with a stationary Rydberg state, called the THz wavepacket. This THz wavepacket is a coherent superposition of the initial Rydberg state and its neighbouring states. We have investigated the time evolution of THz wavepackets by measuring the impact of two in time delayed half cycle pulses ( ≈ 200 V cm^-1) on the population of a stationary (n = 40) Rydberg state in rubidium. The first half cycle pulse creates the THz wavepacket and the second half cycle pulse probes the dynamics of the THz wavepacket. We support our experimental data by numerically solving the Schr?dinger equation and with a semi-classical picture. Whereas an optically excited wavepacket is initially localized, a THz wavepacket is initially delocalized and becomes localized after half a revival time. Received 23 August 2000 and Received in final form 27 March 2001     

The multiphoton ionization rate and the energy shift of atoms interacting with weak dichromatic fields with commensurate frequencies are simple functions of the phase difference

By implementing a time-independent, nonperturbative many-electron, many-photon theory (MEMPT), cycle-averaged complex eigenvalues were obtained for the He atom, whose real part gives the field-induced energy shift, Δ(ω ₁, F ₁;ω ₂, F ₂,ϕ), and the imaginary part is the multiphoton ionization rate, Γ(ω ₁, F ₁;ω ₂, F ₂,ϕ), where ω is the frequency, F is the field strength and ϕ is the phase difference. Through analysis and computation we show that, provided the intensities are weak, the dependence of Γ(ω ₁, F ₁;ω ₂, F ₂,ϕ) on ϕ is simple. Specifically, for odd harmonics, Γ varies linearly with cos(ϕ) whilst for even harmonics it varies linearly with cos(2ϕ). In addition, this dependence on ϕ holds for Δ(ω ₁, F ₁;ω ₂, F ₂,ϕ) as well. These relations may turn out to be applicable to other atomic systems as well, and to provide a definition of the weak field regime in the dichromatic case. When the combination of (ω ₁, F ₁) and (ω ₂, F ₂) is such that higher powers of cos(ϕ) and cos(2ϕ) become important, these rules break down and we reach the strong field regime. The herein reported results refer to Γ(ω ₁, F ₁;ω ₂, F ₂,ϕ) and Δ(ω ₁, F ₁;ω ₂, F ₂,ϕ) for He irradiated by a dichromatic ac-field consisting of the fundamental wavelength λ = 248 nm and its 2nd, 3rd and 4th higher harmonics. The intensities are in the range 1.0×10¹²-3.5×10¹⁴ W/cm², with the intensity of the harmonics being 1-2 orders of magnitude smaller. The calculations incorporated systematically electronic structure and electron correlation effects in the discrete and in the continuous spectrum, for ¹S, ¹P, ¹D, ¹F, ¹G, and ¹H two-electron states of even and odd parity. Received 9 July 2000 and Received in final form 2 November 2000     

Isotope shifts and hyperfine structure in calcium 4snp and 4snf F Rydberg states

Isotope shifts and hyperfine structure have been measured in 4snp ¹ P₁ and Rydberg states for all stable calcium isotopes and the radioisotope ⁴¹Ca using high-resolution laser spectroscopy. Triple-resonance excitation via Rydberg state was followed by photoionization with a CO₂ laser and mass selective ion detection. Isotope shifts for the even-mass isotopes have been analyzed to derive specific mass shift and field shift factors. The apparent isotope shifts for ⁴¹Ca and ⁴³Ca exhibit anomalous values that are n-dependent. This is interpreted in terms of hyperfine-induced fine-structure mixing, which becomes very pronounced when singlet-triplet fine-structure splitting is comparable to the hyperfine interaction energy. Measurements of fine-structure splittings for the predominant isotope ⁴⁰Ca have been used as input parameters for theoretical calculation of the perturbed hyperfine structure. Results obtained by diagonalizing the second-order hyperfine interaction matrices agree very well with experimentally observed spectra. These measurements allow the evaluation of highly selective and sensitive methods for the detection of the rare ⁴¹Ca isotope. Received 17 December 1999 and Received in final form 29 March 2000     

One and two-photon detachment cross-sections of Ps-

We present detailed calculations for one- and two-photon above-threshold detachment (ATD) cross-sections of the negative positronium ion Ps ^- ( e ⁺ e ^- e ^- ), below the threshold of Ps(n = 2), using a configuration interaction (CI) method on a B splines basis. Both the one- and two-photon detachment cross-sections have a form similar to the corresponding spectra of the H^- ion, scaled accordingly. The peak value of the one-photon cross-section agrees very well with the calculations by Bathia and Drachman [1], while it differs from those by Igarashi et al. [2], which give a value of 15% lower. Two-photon detachment cross-sections are also reported. Received 24 January 2002 / Received in final form 9 April 2002 Published online 19 July 2002     

Helium atom in the monochromatic electromagnetic field

We apply a non-perturbative procedure for the calculation of the total photoionization cross-section of two-electron atomic systems. The procedure is based on the Floquet-Fourier representation of the time-dependent Schr?dinger equation. With the use of the Hylleraas-type basis functions, the total photoionization cross-sections obtained are within the accuracy of a fraction of a percent, which, we believe, is the most accurate estimate for the cross-sections available. The total photoionization cross-sections for neutral helium deviate notably from the benchmark experimental data [J.A.R. Samson et al., J. Phys. B 27, 887 (1994)].     

Resonant widths, line intensities and lineshapes for MQDT models with two or more open channels

Approximate analytical formulae describing the energy variation of line intensities, autoionization widths and lineshape asymmetries, are derived for a Phase-Shifted Multichannel Quantum Defect Theory model composed of two closed interacting channels coupled to two effective continua. This is accomplished by putting the two compatibility equation solutions, for the common phase shifts of the two open channels, in such a form so the resonant behavior is attributed to one of them, the other accounting for an energy dependent background. Then, the well-known procedures for the simpler case where only one continuum is considered are applied, using only the resonant solution. The method is quite general and applicable to any MQDT model with two or more open channels. The resulting analytical formulae are tested on experimental spectra of Sr, Ba and Cu and it is shown that they are valid as long as: i) The resonances are non-overlapping, ii) The direct closed channel coupling is much stronger than the indirect one through the continua and (when excitation matrix elements are involved) iii) The open channels excitation strength is smaller or at least comparable to the closed channels one. Received: 26 May 1998 / Accepted: 1st July 1998     

A coincidence technique for the study of intense laser atom interactions

A new device for charged particle coincidence experiments in strong-field, short pulse laser-atom/molecule interactions is presented. The device consists of a single time of flight spectrometer, common for both positive and negative charge detection. Experimental parameters required for the use of the device in the high intensity regime are discussed. A demonstration of electron-ion coincidence measurements in the interaction of Xe atoms with 60 fs laser pulses at 800 nm and an intensity of W/cm² is reported. Received 22 November 1999     

Two-step laser excitation of the highly excited even-parity states of atomic mercury

We report term energies and quantum defects of highly excited even-parity states of mercury in the 83 876–84 140 cm^-1 energy range, employing a two-step laser excitation scheme via the S₀↦6s6p³P₁ inter-combination transition. Two dye lasers, pumped by a common Nd:YAG laser, were frequency doubled by BBO crystals and used to record the spectra in conjunction with a thermionic diode ion detector. Our new observations include the much extended D₂ (22 ≤n ≤52) series and a few members of the S₁ (24 ≤n ≤30) Rydberg series. Members of the D₂ Rydberg series with such a high n value are reported for the first time. The relative intensities of the D₂ and S₁ transitions (m = 4, 5 and 6) of group II-B elements excited from the P₁ inter-combination states are also discussed.     

Ionization of Rydberg atoms in THz-laser fields at the transition from low to high scaled frequencies

We have studied the ionization of Rydberg-excited xenon atoms in THz-laser fields and by quantum dynamical calculations. The experimental threshold laser field strength for 10% ionization probability follows an n^*-1.68 (1.04 THz) dependence (n^* effective principal quantum number) with additional weak resonance structures and shows that ionization does not occur by a Landau-Zener mechanism. At scaled frequencies of to 5.6 the simulated threshold fields for ionization in oscillatory fields show a dependence on the principal quantum number n of n^-4.1 to n^-1.35. Received: 17 February 1998 / Revised: 20 April 1998 / Accepted: 21 April 1998     

Floquet study of ionization and high-order harmonic generation for a hydrogen atom in high-frequency laser fields

In this paper, we investigate the dynamics of a hydrogen atom in high-frequency (several atomic units) super strong (up to several tens of atomic units) laser fields within the high frequency Floquet theory framework. The ionization rate, ionization spectrum, angular distribution and high-order harmonic generation are all investigated. Our studies reveal the universal behavior of the total ionization rate, excess-photon ionization spectrum and angular distribution of the ionization rate in the stabilization regime, and achieve a deep insight into the dynamics of high-order harmonic generation in the stabilization regime. Received 6 June 2001 and Received in final form 31 August 2001