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La technique Storing Matter a pour objectif d’améliorer la sensibilité et la quantification des analyses par SIMS. Elle consiste à découpler la phase de pulvérisation de l’échantillon de la phase d’analyse. Pour cela, la matière pulvérisée par bombardement ionique est déposée en sous-monocouche sur un collecteur optimisé. Le dépôt est ensuite analysé par SIMS. La probabilité d’ionisation de la matière ne dépend plus de son environnement initial (“effet de matrice”), mais de la surface du collecteur. Le choix du collecteur permet un gain de sensibilité et la quantification des concentrations de l’échantillon initial. L’efficacité de la technique dépend du choix du collecteur et d’un facteur de collection ? caractérisant la phase de pulvérisation-dépôt. Dans ce travail, nous avons étudié la pulvérisation et l’émission de la matière sous bombardement ionique pour optimiser ce facteur ?. Nous avons mis au point un dispositif expérimental ainsi qu’un protocole d’analyse par SIMS qui nous a permis d’étudier la distribution angulaire sous un bombardement d’ions Cs+ avec une incidence oblique pour différents paramètres d’impact. L’étude menée sur quatre cibles (Si, Ge, InP et GaAs) a montré que la distribution angulaire est de forme cosn (?-?Max) pour une énergie et un angle d’impact de respectivement 2 à 10 keV et 30° à 60°. L’exposant n est ~2 tandis que la direction d’émission préférentielle ?Max varie de la normale à la surface (0°) jusqu’à un angle d’émission de 35° dans la direction spéculaire au faisceau en fonction de l’énergie d’impact et de l’angle d’incidence. Ces résultats appliqués à Storing Matter ont permis de déterminer la configuration optimum pour une collection maîtrisée en fonction du bombardement / The Storing Matter technique aims at optimising the sensitivity and quantitativeness of SIMS analysis. It consists in decoupling the sputtering of the specimen from the subsequent analysis step. The specimen is sputtered by means of an ion beam. The emitted particles are deposited at a sub-monolayer level on an optimised collector. The deposit is subsequently analysed in a SIMS instrument. The ionisation probability in SIMS does not depend anymore on the initial sample composition (“Matrix effect”), but on the collector surface chemistry. The collector is chosen in order to increase the sensitivity and to quantify the specimen. The efficiency of this new technique depends on the collector choice and on the collection factor ? characterising the sputter-deposition step. In this work, the sputtering and emission processes under ionic bombardment have been studied in order to optimise this factor ?. We developed an experimental set-up and an analysis protocol based on SIMS that allows us to study the angular distribution under Cs+ bombardment with an oblique incidence for different impact parameters. Four targets (Si, Ge, InP and GaAs) were studied. The results show that the angular distribution is shaped as a cosine function cosn (?-?Max) for impact energies between 2 and 10 keV and for incidence angles from 30 to 60°. Under these conditions, the exponent n is ~2 and the preferential direction of emission ?Max varies from the normal to the surface to 35° in the specular direction in function of the impact energy and the incidence angle. The results allowed to find the best settings for the Storing Matter technique to control the sputtered matter collection in function of the bombardment parameters

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Doctor of Philosophy / Department of Physics / Uwe Thumm / Although the latest and most powerful supercomputer today, Tianhe-2 in China, can finish 33.86 quadrillion floating-point operations per second (www.top500.org), it is still a big challenge to simulate the simplest few-electron system - the helium atom - a threebody system with one nucleus and two electrons. Within the fixed-nucleus approximation and time-dependent close coupling (TDCC) approach, we developed software to solve the time-dependent Schrödinger equation (TDSE) accurately, implementing the finite-element discrete-variable representation (FE-DVR) scheme. The general idea of the method is to expand the wave functions in the eigenvectors of the angular momentum operator, which further transform the six-dimensional TDSE to a set of infinite two-dimensional coupled equations. Although there are infinitely many coupled equations, they can be truncated to a finite number of equations by applying selection rules and physical requirements, and solved with our current computational resources. By numerically solving the TDSE in full dimensionality, we investigate the double photoionization of helium atoms in external fields. In co-planar emission geometry with and without the presence of a comparatively weak infrared (IR) laser pulse, we discuss the double ionization (DI) dynamics of helium atoms irradiated by ultrashort pulses of extreme ultraviolet (XUV) laser light. We first investigate the degree of electronic correlation by correlated photoelectron angular distributions for two-photon double ionization (TPDI) of helium atoms in the sequential and non-sequential DI regime. We quantify sequential and non-sequential contributions to TPDI driven by an XUV pulse with central photon energy hw[subscript]xuv near the sequential DI threshold. If the spectral width of the XUV pulse is broad enough, both the sequntial (hw[subscript]xuv > 54.4 eV) and non-sequential (hw[subscript]xuv < 54.4 eV) channels are open. Therefore, the sequential and non-sequential DI mechanisms are difficult to distinguish. By tracking the DI asymmetry in joint photoelectron angular distributions, we introduce the forward-backward-emission asymmetry as a measure that allows the distinction of sequential and non-sequential contributions. Specifically, for hw[subscript]xuv = 50 eV pulses with a sine-squared temporal profile, we find that the sequential DI contribution is the largest at a pulse length of 650 as (1 as = 10[superscript]−18 s), due to competing temporal and spectral constraints. In addition, we validate a simple heuristic expression for the sequential DI contribution in comparison with ab initio calculations. We then investigate the influence of the laser field on the DI of helium by a single XUV pulse. For IR-laser-assisted single-XUV-photon DI our joint angular distributions show that the IR-laser field enhances back-to-back electron emission and induces a characteristic splitting in the angular distribution for electrons that are emitted symmetrically relative to the identical linear polarization directions of the XUV and IR pulse. These IR-pulse-induced changes in photoelectron angular distributions are (i) imposed by different symmetry constraints for XUV-pulse-only and laser-assisted XUV-photon DI, (ii) robust over a large range of energy sharing between the emitted electrons, and (iii) consistent with the transfer of discrete IR-photon momenta to both photoelectrons from the assisting IR-laser field. While selection-rule forbidden at equal energy sharing, for increasingly unequal energy sharing we find back-to-back emission to become more likely and to compete with symmetric emission. To obtain a high level of accuracy, accurate quantum-mechanical calculations of three Coulomb interacting particales exposed to an intense XUV and weak IR field are at the limit of current computational power. Any direct extension (such as strong laser-field intensity, elliptically-polarized field, and laser-induced DI) of our approach to more complicated systems appears to be currently out of reach. At the end of this thesis, we give suggestions on how to improve the efficiency of TDSE calculations for simulations of these complicated many-photon processes.

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Made available in DSpace on 2014-10-09T12:24:10Z (GMT). No. of bitstreams: 0 / Made available in DSpace on 2014-10-09T14:08:22Z (GMT). No. of bitstreams: 1 00931.pdf: 2473042 bytes, checksum: d56b30414065c63c73322142142d66e6 (MD5) / Dissertacao (Mestrado) / IEA/D / Instituto de Fisica, Universidade de Sao Paulo - IF/USP