A numerical analysis scheme has been developed to extract dynamic information from experimental images by the three-dimensional sliced fluorescence imaging method. The present scheme is based on a generalized framework in analyzing fluorescence images from the photo-initiated dynamic process. Specifically, image quality optimization, noise reduction and numerical fitting codes have been implemented in the present scheme to determine differential cross sections of the state-to-state inelastic collisions between CN(A 2£S) and He. These codes are indispensable in extracting state-to-state dynamic information from experimental images in any photo-initiated collision experiment, no matter it is executed in the beam or bulb environment.

The quantum impulse approximation theory has been extended to the inelastic collision. The total inelastic cross sections for the degenerated states with different angular momenta was calculated. It was proved that summing over the transitions from nl to n' and from nl to n'l' would give us the total cross section of transition from n to n'. Rate coefficients were calculated for the common gases in the atmosphere being the third particle. The resonant effect of the rate coefficients had been observed. Recombination coefficients were then calculated in terms of rate coefficients. Previous calculations were carried out in compare with the net rate flow through certain excited levels, which were found to be more stable and reflected a clearer picture of the whole process. Results have been compared with the elastic collision. A dramatic decreasing of rates when temperature increased was also observed. More thermal energy increases the probability of electrons for being re-ionized. Similar calculations had been carried out for the upper atmosphere gases, such as N₂, O₂, CO, CO₂, and H₂O. The recombination coefficients for electron combining with metallic ion Na+ were also calculated.

京都大学 / 0048 / 新制・課程博士 / 博士(理学) / 甲第20161号 / 理博第4246号 / 新制||理||1611(附属図書館) / 京都大学大学院理学研究科物理学・宇宙物理学専攻 / (主査)教授 高橋 義朗, 教授 田中 耕一郎, 教授 川上 則雄 / 学位規則第4条第1項該当 / Doctor of Science / Kyoto University / DFAM

La collision entre l'ion hydroxyle (OH+) et l'atome d'hydrogène (H) joue un rôle majeur en physico-chimie de l'atmosphère et en astrophysique. Pour l'étude de ce système, nous avons générés la surface d'énergie potentielle tridimensionnelle (SEP-3D) globale doublet de la réaction H + OH+ --- H2O+ (X2B1)--- O + H2+. Les calculs électroniques ont été effectués au niveau MRCI avec la base aug-cc-pV5Z en incluant la correction des erreurs de superposition de base (BSSE). Cette SEP couvre la région moléculaire et les régions des longues portées pour les différents canaux : OH+ + H, O + H2+ et la réaction d'échange d'hydrogène. La qualité de la SEP a été validée après une comparaison des constantes spectroscopiques de H2O+ (X2B1) et des fragments diatomiques, des niveaux rovibroniques de H2O+ (X2B1), l'énergie de dissociation et de la barrière à linéarité pour H2O+ (X2B1) aux données expérimentales et théoriques existantes. Un bon accord est trouvé. Après avoir déterminé la SEP, nous avons utilisé les outils de la dynamique quantique indépendante du temps pour calculer les sections efficaces élastiques et inélastiques désexcitation de OH+ (v=0, j=1, 2, 3, 4, 5, 6 et 7) en collision avec l'atome d'hydrogène sur un large domaine d'énergie cinétique. Nous avons ainsi déterminé les taux désexcitation rotationnelle pour des températures allant de 10 à 200K. Nous avons également utilisé la surface quadruplet de Martinez et al. pour déduire ces taux désexcitation. Les résultats montrent que les sections efficaces inélastiques calculées sur la surface doublet sont en moyenne au moins deux à trois fois plus importantes que leurs correspondantes obtenues sur la surface quartet. Les potentiels à longue portée des deux surfaces étant identiques, ce résultat montre qu'un modèle basé sur la seule longue portée du potentiel ne pourrait pas rendre compte de la dynamique inélastique de ce système / The collision between the hydroxyl cation (OH+) and hydrogen atoms (H) plays a major role in physical chemistry of the atmosphere and astrophysics. To study this system, we generated the global three-dimensional potential energy surface (3D-PES) of the reaction H + OH+ ---- H2O+ (X2B1) ---- O + H2+. The electronic calculations were performed at the MRCI level with aug-cc-pV5Z basis including the basis set superposition error (BSSE) correction. This PES covers the molecular region and the long ranges close to the OH+ + H, O + H2+ and the hydrogen exchange channels. The quality of the PES is checked after comparison of the spectroscopic constants of H2O+ (X2B1) and of the diatomic fragments, the rovibronic levels, the dissociation energy, and the barrier to linearity of H2O+ (X2B1) to available experimental and theoretical data. A good agreement is found. Then, we used the tools of time-independent Quantum Dynamics to calculate the elastic and inelastic cross sections for the de-excitation of OH+ in collision with the hydrogen atom over a wide range of kinetic energy. We have thus determined the rotational de-excitation rate coefficients for temperatures ranging from 10 up to 200K. The results show that the inelastic cross sections on the doublet surface are on average at least two to three times larger than their cross section obtained on the previously computed cross sections using the quartet surface. Since, the long range parts of the doublet and the quartet PESs are identical, our work invalidates hence previous cross section determination. When only long range potentials are considered. Therefore, we recommend using fully the global 3D PES for scattering and reactive collision relevant for atmospheric and astrophysical studies

Master's thesis deals with vehicles collisions within an environment of logistic distribution storehous. The aim is to avoid potential collisions that can occur between these vehicles. In the first chapter are detailed collisions of particles and elements impact for the law of conservation of energy and momentum. In further sections is carried out detailed research of elastic and inelastic collisions in an ideal environment, which are the theoretical basis for the simulation of the real environment. Collisions are supported by detailed calculations and added pictures. The second chapter deals with the development of double-layer application simulating elastic collisions in an ideal environment. In subchapters are descriptions of the classes and methods for computing prediction of collisions with examples of source code. The last section describes the software platform JavaFX and used animation classes that are required for visualization issues. The last chapter, which is the main goal of the work is done by the expansion of the existing design environment of storehouse and vehicles. Particular chapters then describe the cases of various types of collisions their detection and avoidance. There is an application designed to address this issue, with a description of the classes and methods. Used methods are supported with flowcharts for easier understanding.

Le travail de cette thèse porte sur l’étude expérimentale de la diffusion d’atomes d’hydrogène sur des surfaces et sous incidence rasante. L’énergie des atomes et des ions varie de quelques centaines d’eV à quelques keV, tandis que les surfaces étudiées sont des isolants et des semi-métaux. En particulier on a étudié la formation de l’ion H- sur du graphite pyrolytique dit HOPG (highly oriented pyrolytic graphite) et sur une surface de LiF(001). Pour ce dernier système, nous avons étudié en détail la diffraction d’atomes H° et d’ions H+. Ces expériences ont été réalisées sur un montage expérimental utilisant un faisceau pulsé et permettant de détecter en coïncidence les particules diffusées et les électrons secondaires. L’ensemble permet de connaître la charge finale de la particule diffusée, sa perte d’énergie, son angle de diffusion, le tout en corrélation avec la statistique et l’énergie des électrons émis.Le résultat de ce travail a révélé que la diffraction persiste dans le régime inélastique. En effet, nous observons un motif de diffraction après la neutralisation de proton sur la surface de LiF(001). Un modèle est proposé pour expliquer ces résultats qui semblent en contradiction avec ceux publiés par le groupe de H. Winter sur la diffraction d’atomes d’hydrogène sur cette même surface. Concernant la formation d’ion négatif sur HOPG, nous avons mis en évidence un taux de H- (~10%) sur une surface propre. C’est le plus haut taux de H- jamais observé avec ce type d’expérience en incidence rasante. C’est encore plus élevé qu’avec des isolants ioniques, ces derniers donnant un taux déjà 10 fois plus grand que celui observé sur métaux propres. Ces résultats confirment l’efficacité du graphite à convertir des ions et des atomes en ions négatifs. En exploitant les données fournies par la technique des coïncidences, nous avons pu élucider le mécanisme à l’œuvre dans cette conversion. Du fait de la structure électronique particulière de HOPG, avec une bande interdite projetée dans la direction Gamma, seuls les électrons localisés sigma contribuent à la formation de l’ion négatif, donnant au HOPG un caractère isolant du point de vue de la capture électronique. Les électrons pi contribuant de manière efficace à la perte d’énergie par collisions binaires, donnant de ce point de vue au HOPG son caractère métallique. / In this thesis, we have investigated experimentally the scattering of hydrogen atoms and ions on solid surfaces at grazing incidence. The projectile energy ranges from several hundred eV to few keV. The formation of H- ions is studied on highly oriented pyrolytic graphite (HOPG) surface; and surface diffraction is carried out on LiF(001) surface with H° and H+ particle scattering. Both experiments were performed in the same experimental setup (see Figure 1.2 and 2.1)—with grazing scattering geometry and a PSD (position sensitive detector) located downstream to record scattered particles. For charge state analysis a set of electrostatic plates is inserted between sample and PSD. During the experiment, coincident measurement technique is used to identify the energy loss associated to 0, 1, 2…electrons emission. Clear evidence of diffraction with inelastic scattering by proton on LiF(001) has been obtained, which has not been observed before. Indeed, the group of H. Winter reported that no diffraction exists with inelastic scattering of H° on LiF(001). However, according to our result, a coherence scattering factor still exists even though the electron capture by the proton is an inelastic process. For negative ion formation on HOPG surface, we report here the highest fraction of H- (~10%) measured in grazing scattering experiments; it is larger than those obtained on ionic insulators, the latter being typically 10 times larger than those measured on clean metals. These results confirm the high yields of negative hydrogen ions from graphite reported in the literature. Electron emission and energy loss of scattered beam have also been deciphered via coincidence measurement. Due to the special structure of HOPG, two kinds of electron emissions (σ and π-band electron) and energy losses (cycles and metal-like energy loss) have been measured. Furthermore, the total electron emission on HOPG with insulator-like behavior and total energy loss with metal-like are the most representative property of HOPG which have been first presented in this thesis.