Dynamic and geometric alignment of molecules induced by intense laser fields

We present a method to discuss simultaneously the relative importance of molecular dynamic and geometric alignment induced by intense laser fields in theoretical view. This method divides the process of molecular alignment into three steps, which are tightly correlated with that of molecular multielectron dissociative ionization and Coulomb explosion. A fourth-order Runge-Kutta algorithm and a developed counting approach are used to calculate the angular distribution of molecules in the first and second steps of molecular alignment. The last step is described by a field-ionization, Coulomb explosion model. The angular distribution of molecules at the critical distance originated from geometric alignment is obtained by calculating the volume of shells associated with a series of particular angle. The final angular distributions of molecules are obtained by properly weighting the results of three steps. The numerical results of distinguishing between dynamic and geometric alignment for certain conditions are presented and discussed. Our computational results show that the alignment mechanism, which dominates the observed anisotropy of angular distributions of ionic fragments for a given condition, is determined by the dependences of the extent of dynamic and geometric alignment on laser parameters and molecular parameters.     

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.     

Fragmentation of CO in Femtosecond Laser Fields

Fragmentation of CO in a linearly polarized femtosecond laser field within the intensity order of 10^14 W.cm^-2 at 820nm is investigated experimentally by using velocity mapping technique. According to the observed kinetic energy and angular distributions of different charged fragment ions, fragmentation channels of CO are proposed. The angular distributions provide helpful information for assigning the dissociation channels.     

Photoelectron angular distributions of molecules in bichromatic laser fields of circular polarization

Photoelectron angular distributions (PADs) from above-threshold ionization of O₂ and N₂ molecules irradiated by a bichromatic laser field of circular polarization are studied. The bichromatic laser field is specially modulated such that it can be used to mimic a sequence of one-cycle laser pulses. The PADs are greatly affected by the molecular alignment, the symmetry of the initial electronic distribution, and the carrier-envelope phase of the laser pulses. Generally, the PADs do not show any symmetry, and become symmetric about an axis only when the symmetric axis of laser field coincides with the symmetric axis of molecules. This study shows that the few-cycle laser pulses can be used to steer the photoelectrons and perform the selective ionization of molecules.     

Structural Deformation of CO22+ in Intense Femtosecond Laser Fields

The angular distributions of CO^＋ from the dissociation of CO2^2＋ and CO2^＋ in intense femtosecond laser fields （45 fs, about 5 × 10^15 W/cm^2） are studied at a laser wavelength of 800nm based on the time-of-flight mass spectra of CO^＋ fragment ions. The experimental results show that structural deformation occurs in the charge state of CO2^2＋ and the CO^＋ maintains linear geometrical structure.     

Dipole traps with mode-locked lasers

We investigate the properties of two separate dipole traps, realised using a cw mode-locked Ti:sapphire laser and a cw mode-locked Nd:YVO₄ laser, red-detuned by 25 nm and 284 nm, respectively. Approximately 10³ laser-cooled ⁸⁵Rb atoms were confined in the traps at ≈50 μK, with no observable heating after initial loading. The lifetimes of the traps were consistent with limitations imposed by wavelength-dependent photoassociation losses and collisions with background vapour. Determination of the ac Stark shift of the 780 nm cooling transition using a weak probe beam showed no observable difference between using narrow-bandwidth or mode-locked trapping light. Techniques for trapping and focusing of atoms based on the dipole force of blue and uv light become much more accessible through efficient doubling, tripling and quadrupling of mode-locked sources. This opens up the possibility of manipulating more technologically interesting species. Received: 30 September 1999 / Revised version: 21 December 1999 / Published online: 24 March 2000     

Theory of Tunnel Ionization in Complex Systems

We present a detailed derivation of the Ammosov-Delone-Krainov theory of tunnel ionization in complex systems （CS-ADK）. A few mistakes in the previous works have been found and corrected. The theory is then applied to CO2, showing that CS-ADK yields better agreement with experiment than the molecular ADK theory.     

Long-Time Dynamical Behaviour of Alternative-Current Stark Effect

We report the long time dynamical behaviour of ac Stark effect in a simple quantum model in which two level atoms interact with quantized coherent radiation field. A new phenomenon of periodic quantum collapse and revival of the ac Stark shift of energy level due to ac Stark effect is expressed accurately by analysing the phase of transition probability amplitude. The analytic prediction is confirmed by the numerical results.     

Femtosecond laser-induced dynamic alignment in Coulomb explosion of CO: Roles of laser wavelength, intensity and pulse duration

Dependences of dynamic alignment of CO molecules induced by intense femtosecond laser fields on laser wavelength, intensity and pulse duration are investigated by numerical simulations. A counting approach and a fourth-order Runge-Kutta algorithm are used to calculate the angular distribution and the time evolution of molecules. A two-step Coulomb explosion model of diatomic molecules in intense laser fields is used to determine the instant that CO molecular dynamic alignment is over. Our calculating results show that the linear polarizability and the damping force play an important role in the angular rotation of CO molecule in conditions of 800 nm laser wavelength and 10¹⁵ W/cm² laser intensity. The contributions of the second-order field-induced dipole moment and the higher-order correction term to molecular rotation acceleration comparing to the linear polarizability and damping force are negligible. The extent of dynamic alignment of CO molecules reduces with the increasing of laser intensity. The dynamic alignment time of CO molecules is tightly connected to the laser pulse duration. The angular distributions of CO molecules as the laser pulse length varied from 50 to 250 fs at laser intensity of 3×10¹⁴ W/cm² are shown and discussed.     

Kilohertz extreme-ultraviolet light source based on femtosecond high-order harmonic generation from noble gases

A compact, versatile table-top kilohertz source of coherent extreme-ultraviolet (XUV) radiation in the wavelength region 18–100 nm, based on high-order harmonic generation from noble gases induced by a 40-femtosecond Ti:sapphire laser system, is presented. The XUV beamline delivers at its output 10⁸ photons/s at a wavelength of 23 nm. The monochromatized XUV radiation is directly focused onto a 10^-2-mm² spot by a toroidal grating, allowing one to reach intensities higher than 10⁶ W/cm². Optimization results are presented for a new XUV-generating geometry, utilizing a ‘semi-infinite’ quasi-static gas cell and strong focusing. In those conditions, we observe an anomalous inversion between the cutoffs of argon and krypton, with the krypton spectrum extending to much higher orders than expected in an adiabatic limit. Received: 9 July 2001 / Revised version: 1 August 2001 / Published online: 7 November 2001     

Improving Raman velocimetry of laser-cooled cesium atoms by spin-polarization

We study the performances of Raman velocimetry applied to laser-cooled, spin-polarized, cesium atoms. Atoms are optically pumped into the F = 4, m₄=0 ground-state Zeeman sublevel, which is insensitive to magnetic perturbations. High resolution Raman stimulated spectroscopy is shown to produce Fourier-limited lines, allowing, in realistic experimental conditions, atomic velocity selection to one-fiftieth of a recoil velocity.     

Three-photon interference spectra in four-level atomic systems

We have considered the interference spectra that occur at the three-photon generated frequency arising from the interaction of three laser fields with a four-level atom, where two of the laser fields are on two-photon resonance with the three levels forming a “λ” scheme while the third laser operates between the second ground and the second excited state of the atom. At low intensities of all three laser fields, the overall intensity of the peak at the three-photon generated frequency, describing the spectrum of an electron in the second excited state, depends on the strength of the combined field of the two laser fields that are on two-photon resonance and it takes negative values. This indicates that light amplification without population inversion is likely to occur at the three-photon generated frequency. The combined field of the three laser fields induces multiphoton excitations near the three-photon generated frequency, whose peaks are characterized by linewidths which are much less than the natural linewidths of the atoms. These excitations describe absorption or stimulating emission processes depending on the values of the detunings of the laser fields. The derived results are graphically presented and discussed. Received: 24 January 2001 / Published online: 8 June 2001     

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.     

Stimulated emission at the difference-frequency generation

 We consider the stimulated emission process that occurs at the difference-frequency generation of a bichromatic field interacting with a three-level atom, where one of the laser fields is strong while the other is weak. It is shown that at the difference-frequency generation an induced peak occurs which can exhibit both gain and attenuation. Conditions under which this takes place are established and discussed herein. Received: 29 April 1996 / Accepted: 17 July 1996     

Simple and efficient photo-ionization loading of ions for precision ion-trapping experiments

We report a simple and efficient method to load a Paul trap with Ca⁺ ions. A beam of neutral atomic calcium is ionized in a two-step photo-ionization process using uv-diode lasers near 423 nm and 390 nm. Photo-ionization of a calcium beam for loading a Paul trap has first been demonstrated by Kjaergaard et al. The advantages of our method are the use of cheap and easily handled diode-laser systems and the large cross section for field ionization when exciting high-lying Rydberg states. Finally, we discuss the advantages of photo-ionization for ion generation compared to loading by electron bombardment. Received: 24 August 2001 / Revised version: 16 October 2001 / Published online: 23 November 2001     

Quantum interference spectra at the difference-frequency generation in four-level atomic systems

Analytical expressions of the spectral functions have been derived for a number of induced excitations that occur near the difference-frequency generation in a four-level atomic system interacting with three laser fields. The spectral heights and subnatural line widths of the induced peaks depend on the intensities of the laser fields involved. The maximum heights of the induced peaks take positive, zero and negative values, indicating that the processes of absorption (attenuation), dark resonance and stimulated emission (amplification) are likely to occur near the difference-frequency generation, respectively. Received: 15 March 2002 / Revised version: 17 June 2002 / Published online: 8 January 2003 RID="*" ID="*"Corresponding author. Fax: +1-613-954-5242     

Superradiant transitions between high-lying levels of Sr in an external electric field

Superradiant transitions were observed between high lying levels in Sr. The transitions react very sensitively to an external electric field. Superradiant cascades or one transition in a superradiant branching can be suppressed. The square root of the high of a superradiant pulse decreases with the second power of the electric field strength. This behaviour can be explained by calculations.Dedicated to Prof. Dr. Herbert Welling on the occasion of his 60th birthday     

Study on Non-Sequential Double Ionization of Aligned Diatomic Molecules in Strong Laser Fields

We develop a semiclassical model to describe the non-sequential double ionization of aligned diatomic molecules in an intense linearly polarized field. It is found that in the tunnelling regime, the oriented molecule shows geometric effects on double ionization process when aligned parallel and perpendicular to the external field. Our results are qualitatively consistent with the recent experimental observations.     

Absence of Charge-Resonance-Enhanced Ionization in Attosecond Pulse Photoionization： Numerical Result on One-Dimensional H2^＋

We present a numerical result of photoionization rate for the one-dimensional molecular hydrogen ion model exposed to intense light of 1 × 10^16-2×10^16 W/cm^2, 55-as pulse duration, and 800nm wavelength. In contrast to the previous calculation result of charge-resonance-enhanced ionization for lower intensity and much longer pulse, our result exhibits an ionization saturation. The numerical results are interpreted in the field-dressed potential picture as over-the-barrier liberation of electrons. This extremely short pulsewidth and relatively high field phenomenon requests experimental demonstration.     

Double-Exponentially Decayed Photoionization in CREI Effect： Numerical Experiment on 3D H2^＋

On the platform of the 3D H2^＋ system, we perform a numerical simulation of its photoionization rate under excitation of weak to intense laser intensities with varying pulse durations and wavelengths. A novel method is proposed for calculating the photoionization rate： a double exponential decay of ionization probability is best suited for fitting this rate. Confirmation of the well-documented charge-resonance-enhanced ionization （CREI） effect at medium laser intensity and finding of ionization saturation at high light intensity corroborate the robustness of the suggested double-exponential decay process. Surveying the spatial and temporal variations of electron wavefunctions uncovers a mechanism for the double-exponentially decayed photoionization probability as onset of electron ionization along extra degree of freedom. Henceforth, the new method makes clear the origins of peak features in photoionization rate versus internuclear separation. It is believed that this multi-exponentially decayed ionization mechanism is applicable to systems with more degrees of motion.