Photoelectron angular distributions from strong-field coherent electronic excitation

Photoelectron Angular Distributions (PADs) resulting from nonperturbative excitation of potassium atoms using shaped femtosecond laser pulses are presented. We study control exerted by (1) the polarization of an unshaped, i.e., a bandwidth-limited light pulse, (2) shaped linearly polarized light, and (3) a combination of both degrees of freedom, i.e., polarization-shaped laser pulses. A theoretical approach to describe PADs from nonperturbative Resonance Enhanced Multi-Photon Ionization (REMPI) with ultrashort polarization-shaped laser pulses is presented and compared to experimental results. Applications of this technique to the generation and observation of atomic ring currents are discussed.     

Synchronization of Raman transitions in highly excited hydrogen atoms: A new proposal for measuring the Rydberg constant

We present an analysis of the Raman interaction between a Rydberg atom and ultrashort light pulses. An application of the synchronization of quantum transitions to a simple atomic system (the hydrogen atom) is demonstrated. This is a direct way of measuring times and frequencies of microwave transitions between the high-lying atomic states using ultrashort light pulses. The results and analysis represent a new method for measuring the Rydberg constant.     

Generalized Pseudospectral Method for Solving the Time-Dependent Schrödinger Equation Involving the Coulomb Potential

We present an accurate and efficient generalized pseudospectral method for solving the time-dependent Schrödinger equation for atomic systems interacting with intense laser fields. In this method, the time propagation of the wave function is calculated using the well-known second-order split-operator method implemented by the numerically exact, fast transform between the grid and spectral representations. In the grid representation, the radial coordinate is discretized using the Coulomb wave discrete variable representation (CWDVR), and the angular dependence of the wave function is expanded in the Gauss-Legendre-Fourier grid. In the spectral representation, the wave function is expanded in terms of the eigenfunctions of the field-free zero-order Hamiltonian. Calculations on the high order harmonic generation and ionization dynamics of hydrogen atom in strong laser pulses are presented to demonstrate the accuracy and efficiency of the present method. This new algorithm will be found more computationally attractive than the close-coupled wave packet method using CWDVR and/or methods based on evenly spaced grids.     

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.     

Saturation intensity for ultrashort-pulse X-ray laser schemes

Analytic expressions are obtained for the saturation intensity in X-ray laser schemes based on short-pulse high-intensity drivers. For field-ionized plasma schemes, the specific mean saturation intensityJ _sat is time independent and depends only on atomic transition probabilities, level degeneracies, and transition energies. The analytic expression is found to be in good agreement with a detailed numerical calculation. Integrating over space and frequency gives a saturation intensityI _sat of order 2 × 10¹¹ W/cm² for lasing in Li-like Ne at 98 . The low input energy requirements for this scheme (< 1 J), associated with using a confocal geometry, give energy efficiencies of order 10^–6 and greater. For inner-shell photo-ionization schemes, an accurate expression for a time-dependent saturation intensity is obtained. This scheme is calculated to have high saturation intensities,I _sat 10¹³ W/cm², at short wavelengths (5–15 ). The requirement of a line focus geometry leads to higher input energies (5 J) and the short duration of lasing (50 fs) results in lower energy efficiencies ( 10^–7). Repetition rates are important in determining appropriate applications for both schemes.     

Absorption and ionization of molecular nitrogen by UV femtosecond laser pulses

Mechanisms of non-linear absorption and ionization of molecular nitrogen gas by UV femtosecond laser pulses were studied using photogalvanic and photoacoustic techniques. The effect of the intermediate Rydberg resonance, its dynamic Stark perturbation and ponderomotive upshift of the first ionization potential of nitrogen molecules by the intense laser pulses has been revealed by observing an increase of a power slope of ion yield from three to four at increasing laser intensity.     

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.     

Simplified Model for Analysing Ion/Photoelectron Images

Based on the Onion-Peeling algorithm （OPA） principle, we present a simplified model for analysing photoion and photoelectron images, which allows the analysis of experimental raw images. A three-dimensional distribution of the nascent charged particles, from which the radial and angular distributions are deduced, can be obtained more easily by this model than by the commonly used procedures. The analysis results of Xe photoelectron images by this model are compared with those from the standard Hankel-Abel inversion. The results imply that this model can be used for complicated （many peaks） and ＇ditffcult＇ （low signal-to-noise） images with cylindrical symmetries, and can provide a reliable reconstruction in some cases when the commonly used Haukel Abel transform method fails.     

Classical Effects of Carrier--Envelope Phase on Nonsequential Double Ionization

A classical microcanonical 1＋1-dimensional model is used to investigate the ion momentum distributions in nonsequential double ionization with linearly polarized few-cycle pulses. We find that the ion momentum distribution has a strong dependence on the carrier-envelope phase of the few-cycle pulse, which is consistent with the experimental results qualitatively. Back analysis shows that the ionization probability of the first electron at different phases and its returning kinetic energy play the main role on the ion momentum distributions.     

Systematics of inner-shell photo-ionization X-ray lasers with constant pump rates

Population-rate equations are analytically solved for constant pump rates. Conditions for population inversions are developed for this simplified case. Numbers appropriate for inner-shell photo-ionization of magnesium and neon are used. These allow back-of-the envelope calculations for predicting lasing duration. Pump-rate thresholds are also given which permit lasing for the duration of the pumping. Blackbody-source temperatures associated with such pump rates are calculated. A method of using the solution of the small-signal population-rate equations to determine the saturated intensity when the lower lasing level has a decay channel is given. This method is applied to the case of constant pump rates. An analytic expression for the saturated intensity is developed for this case.     

Reduction of multi-photon ionization in dielectrics due to collisions

The collisional effect due to the multi-photon ionization process in dielectric material has been studied. We found that the breakdown threshold of fused silica is the same for both linearly and circularly polarized light at 55 fs and 100 fs, which we believe is an indication of the suppression of multi-photon ionization in solids. By numerically solving the time-dependent Schrödinger equation with scattering, for the first time, we have observed substantial reduction of the multi-photon ionization rate in dielectrics due to collisions.     

Harmonic Enhancement Mechanism of a Superposition State Atom Irradiated by Short Pulses

We investigate the high-order harmonic generation （HHG） of a model atom whose initial state is prepared in a superposition of its ground state and an excited state irradiated by different duration laser pulses. Compared to the HHG generated from an atom whose initial state is in its ground state, its conversion efficiency obtains some enhancement. The enhancement originates from the higher ionization rate （rather than the ionization yield） of the atom with superposition initial state.     

Resonantly enhanced three-photon excitation spectra of lithium

We present the first measurement on the resonantly enhanced three-photon excitation spectra of natural lithium using a Nd:YAG laser pumped dye laser in conjunction with a thermionic diode ion detector. Exploiting the linear and circular polarizations, the np ²P_3/2(8 ? n ? 11) and nf  ²F_7/2 (8 ? n ? 38) series have been observed via three-photon excitation from the ground state. The measured level energies reveal a dynamic shift from calculated values, which increases with an increase of the principal quantum number n. The ac stark shift and line broadening mechanisms are studied as a function of laser intensity. It is noted that the width increases and the line center shifts towards the higher energy side as the laser intensity is increased. The maximum observed shift for the 12f ²F_7/2 line is 0.33 cm⁻¹ corresponding to the laser intensity variation from 1.34 × 10¹² W/m² to 1.03 × 10¹³ W/m², whereas its width increases from 0.36 cm⁻¹ to 0.82 cm⁻¹.     

High-Order Above-Threshold Ionization of H2+ in Intense Laser Field

The nonperturbative quantum electrodynamies method proposed by Fu et al. [Phys. Rev. A 75 （2007） 063419] is employed to study the high-order above-threshold ionization （ATI） of a diatomic molecule. Based on this frequency-domain theory, the high-order ATI process can be regarded as ATI followed by laser-assisted collision, where the total transition amplitude is the coherent summation of the contributions from each ATI channel. The angular-resolved ATI spectrum, which agrees with the results by Becket et al. based on the time-domain method, is obtained by this frequency domain theory. Furthermore, it is demonstrated that the interference characteristics representing the molecular structure in the ATI spectrum originates from the recollision of the electron with two-centre ion in each ATI channel.     

Enhancement of Bichromatic High-Order Harmonic Generation by a Strong Laser Field and Its Third Harmonic

We investigate high-order harmonic generation （HHG） in a linearly polarized bichromatic field composed of a fundamental laser field with frequency w and an additional laser field with frequency 3w. The numerical results show that it is possible to enhance the intensity of most high harmonics in orders of magnitude. A most striking feature in the enhancement is that the intensity of several special high harmonics is practically impaired as compared with that in the monochromatic case. The qualitative explanation to the great enhancement is that the additional high-frequency field can provide new transition paths for electrons to reach the continuum. The relative phase between the fundamental field and its third harmonic field also affects the intensity of high-order harmonics near the cutoff efficiently.     

High-order above-threshold ionization with few-cycle laser pulses: Molecular improved strong-field approximation vs. molecular low-frequency approximation

We investigate high-order above-threshold ionization (HATI) of homonuclear diatomic molecules by a few-cycle laser pulse. In order to describe molecular HATI in ultrashort laser pulses we have modified our molecular improved strong-field approximation (MISFA), which was developed for long laser pulses and in which the rescattering of the ionized electron off the parent ion was described using the first-order Born approximation (1BA). Now, we introduce the so-called molecular low-frequency approximation (MLFA) in which the elastic rescattering amplitude is calculated exactly. The angle-resolved electron energy spectra for HATI of N₂ and O₂ obtained using the MLFA are compared with those obtained within the MISFA. The difference between these spectra becomes significant for larger (re)scattering angles. This is due to the fact that the exact scattering amplitude, used in the MLFA, has minima for some values of the rescattering angles that are absent in the 1BA. Also, the rescattering plateau is lower for the MLFA spectra. We investigate the influence of the carrier-envelope phase on the high-energy part of the molecular HATI spectra. As in the atomic case, the left-right (backward-forward) asymmetry is also observed in the molecular case.     

Numerical studies of the isomer selectivity of two- and three-step resonance ionization of niobium

Received: 24 March 1997/Revised version: 8 September 1997     

Ultrahigh Harmonic Generation from an Atom with Superposition of Ground State and Highly Excited States

We investigate the high-order harmonic generation from an atom prepared in a superposition of ground state and highly excited state. When the atom is irradiated by an ultrashort pulse, the cutoff position of the plateau in the harmonic spectrum is largely extended compared with the case that the atom is initially in the ground state. The physics of the extension of the high-order harmonic plateau can be interpreted by the spatial structure of the atomic initial wave packet. We can optimize the generation of high-order harmonics by substituting the excited state for a particular coherent superposition of some highly excited states to form a spatially localized excited wave packet.     

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     

Rydberg stabilization of atoms in strong fields: the “magic mountain” in the chaotic sea

We discuss the classical problem of an hydrogen atom interacting with a monochromatic field. We illustrate in particular, analytically and numerically, the stabilization mechanism and give theoretical expressions for the stabilization borders.