Optimization of Generalized Multichannel Quantum Defect reference functions for Feshbach resonance characterization

This work stresses the importance of the choice of the set of reference functions in the Generalized Multichannel Quantum Defect Theory to analyze the location and the width of Feshbach resonance occurring in collisional cross-sections. This is illustrated on the photoassociation of cold rubidium atom pairs, which is also modeled using the Mapped Fourier Grid Hamiltonian method combined with an optical potential. The specificity of the present example lies in a high density of quasi-bound states (closed channel) interacting with a dissociation continuum (open channel). We demonstrate that the optimization of the reference functions leads to quantum defects with a weak energy dependence across the relevant energy threshold. The main result of our paper is that the agreement between the both theoretical approaches is achieved only if optimized reference functions are used.Comment: submitte to Journal of Physics

Coherent Control of Isotope Separation in HD+ Photodissociation by Strong Fields

The photodissociation of the HD+ molecular ion in intense short- pulsed linearly polarized laser fields is studied using a time- dependent wave-packet approach where molecular rotation is fully included. We show that applying a coherent superposition of the fundamental radiation with its second harmonic can lead to asymmetries in the fragment angular distributions, with significant differences between the hydrogen and deuterium distributions in the long wavelength domain where the permanent dipole is most efficient. This effect is used to induce an appreciable isotope separation.Comment: Physical Review Letters, 1995 (in press). 4 pages in revtex format, 3 uuencoded figures. Full postcript version available at: http://chemphys.weizmann.ac.il/~charron/prl.ps or ftp://scipion.ppm.u-psud.fr/coherent.control/prl.p

Resonance structures in the multichannel quantum defect theory for the photofragmentation processes involving one closed and many open channels

The transformation introduced by Giusti-Suzor and Fano and extended by Lecomte and Ueda for the study of resonance structures in the multichannel quantum defect theory (MQDT) is used to reformulate MQDT into the forms having one-to-one correspondence with those in Fano's configuration mixing (CM) theory of resonance for the photofragmentation processes involving one closed and many open channels. The reformulation thus allows MQDT to have the full power of the CM theory, still keeping its own strengths such as the fundamental description of resonance phenomena without an assumption of the presence of a discrete state as in CM.Comment: 7 page

Dissociation spectrum of H2+_2^+ from a short, intense infrared laser pulse: vibration structure and focal volume effects

The dissociation spectrum of the hydrogen molecular ion by short intense pulses of infrared light is calculated. The time-dependent Schr\"odinger equation is discretized and integrated in position and momentum space. For few-cycle pulses one can resolve vibrational structure that commonly arises in the experimental preparation of the molecular ion from the neutral molecule. We calculate the corresponding energy spectrum and analyze the dependence on the pulse time-delay, pulse length, and intensity of the laser for $\lambda \sim 790$nm. We conclude that the proton spectrum is a both a sensitive probe of the vibrational dynamics and the laser pulse. Finally we compare our results with recent measurements of the proton spectrum for 55 fs pulses using a Ti:Sapphire laser ($\lambda \sim 790$nm). Integrating over the laser focal volume, for the intensity $I \sim 3 \times 10^{15}$W cm$^{-2}$, we find our results are in excellent agreement with these experiments.Comment: 17 pages, 8 figures, preprin

Nuclear classical dynamics of H2_2 in intense laser field

In the first part of this paper, the different distinguishable pathways and regions of the single and sequential double ionization are determined and discussed. It is shown that there are two distinguishable pathways for the single ionization and four distinct pathways for the sequential double ionization. It is also shown that there are two and three different regions of space which are related to the single and double ionization respectively. In the second part of the paper, the time dependent Schr\"{o}dinger and Newton equations are solved simultaneously for the electrons and the nuclei of H$_2$ respectively. The electrons and nuclei dynamics are separated on the base of the adiabatic approximation. The soft-core potential is used to model the electrostatic interaction between the electrons and the nuclei. A variety of wavelengths (390 nm, 532 nm and 780 nm) and intensities ($5\times10^{14}$ $Wcm^{-2}$ and $5\times10^{15}$ $Wcm^{-2}$) of the ultrashort intense laser pulses with a sinus second order envelope function are used. The behaviour of the time dependent classical nuclear dynamics in the absence and present of the laser field are investigated and compared. In the absence of the laser field, there are three distinct sections for the nuclear dynamics on the electronic ground state energy curve. The bond hardening phenomenon does not appear in this classical nuclear dynamics simulation.Comment: 16 pages, 7 figure

A quantitative theory-versus-experiment comparison for the intense laser dissociation of H2+

A detailed theory-versus-experiment comparison is worked out for H$_2^+$ intense laser dissociation, based on angularly resolved photodissociation spectra recently recorded in H.Figger's group. As opposite to other experimental setups, it is an electric discharge (and not an optical excitation) that prepares the molecular ion, with the advantage for the theoretical approach, to neglect without lost of accuracy, the otherwise important ionization-dissociation competition. Abel transformation relates the dissociation probability starting from a single ro-vibrational state, to the probability of observing a hydrogen atom at a given pixel of the detector plate. Some statistics on initial ro-vibrational distributions, together with a spatial averaging over laser focus area, lead to photofragments kinetic spectra, with well separated peaks attributed to single vibrational levels. An excellent theory-versus-experiment agreement is reached not only for the kinetic spectra, but also for the angular distributions of fragments originating from two different vibrational levels resulting into more or less alignment. Some characteristic features can be interpreted in terms of basic mechanisms such as bond softening or vibrational trapping.Comment: submitted to PRA on 21.05.200

Femtosecond laser pulse shaping for enhanced ionization

We demonstrate how the shape of femtosecond laser pulses can be tailored in order to obtain maximal ionization of atoms or molecules. For that purpose, we have overlayed a direct-optimization scheme on top of a fully unconstrained computation of the three-dimensional time-dependent Schrodinger equation. The procedure looks for pulses that maintain the same total length and integrated intensity or fluence as a given pulse that serves as an initial guess. It allows, however, for changes in frequencies -- within a certain, predefined range -- and overall shape, leading to enhanced ionization. We illustrate the scheme by calculating ionization yields for the H2+ molecule when irradiated with short (~5 fs), high-intensity laser pulses

Correlation dynamics between electrons and ions in the fragmentation of D2_2 molecules by short laser pulses

We studied the recollision dynamics between the electrons and D$_2^+$ ions following the tunneling ionization of D$_2$ molecules in an intense short pulse laser field. The returning electron collisionally excites the D$_2^+$ ion to excited electronic states from there D$_2^+$ can dissociate or be further ionized by the laser field, resulting in D$^+$ + D or D$^+$ + D$^+$, respectively. We modeled the fragmentation dynamics and calculated the resulting kinetic energy spectrum of D$^+$ to compare with recent experiments. Since the recollision time is locked to the tunneling ionization time which occurs only within fraction of an optical cycle, the peaks in the D$^+$ kinetic energy spectra provides a measure of the time when the recollision occurs. This collision dynamics forms the basis of the molecular clock where the clock can be read with attosecond precision, as first proposed by Corkum and coworkers. By analyzing each of the elementary processes leading to the fragmentation quantitatively, we identified how the molecular clock is to be read from the measured kinetic energy spectra of D$^+$ and what laser parameters be used in order to measure the clock more accurately.Comment: 13 pages with 14 figure

Mécanismes de formation des ions en phase gazeuse

La formation d'ions atomiques et moléculaires en phase gazeuse met en jeu une grande variété de mécanismes, selon le processus d'excitation, le mécanisme primaire d'ionisation, et enfin les processus en compétition.Ces différents mécanismes ainsi que les principales techniques de détection sont présentés, en introduction à des exposés plus spécialisés. Les méthodes d'étude théorique utilisées dans le cas de la photoionisation sont brièvement décrites. Enfin, on indique les développements récents et les perspectives dans ce domaine