In this thesis we explore in particular the dynamics of a special type of quasi-particle in pi-conjugated materials termed polaron, the origin of which is intimately related to the strong interactions between the electronic and the vibrational degrees of freedom within these systems. In order to conduct such studies with the particular focus of each appended paper, we simultaneously solve the time-dependent Schrödinger equation and the lattice equation of motion with a three-dimensional extension of the famous Su-Schrieffer-Heeger (SSH) model Hamiltonian. In particular, we demonstrate in Paper I the applicability of the method to model transport dynamics in molecular crystals in a region were neither band theory nor perturbative treatments such as the Holstein model and extended Marcus theory apply. In Paper II we expand the model Hamiltonian to treat the revolution of phenylene rings around the sigma-bonds and demonstrate the great impact of stochastic ring torsion on the intra-chain mobility in conjugated polymers using poly[phenylene vinylene] (PPV) as a model system. Finally, in Paper III we go beyond the original purpose of the methodology and utilize its great flexibility to study radiationless relaxations of hot excitons. / Report code: LiU-TEK-LIC-2007:4.

<p>In this thesis we explore in particular the dynamics of a special type of quasi-particle in pi-conjugated materials termed polaron, the origin of which is intimately related to the strong interactions between the electronic and the vibrational degrees of freedom within these systems. In order to conduct such studies with the particular focus of each appended paper, we simultaneously solve the time-dependent Schrödinger equation and the lattice equation of motion with a three-dimensional extension of the famous Su-Schrieffer-Heeger (SSH) model Hamiltonian. In particular, we demonstrate in Paper I the applicability of the method to model transport dynamics in molecular crystals in a region were neither band theory nor perturbative treatments such as the Holstein model and extended Marcus theory apply. In Paper II we expand the model Hamiltonian to treat the revolution of phenylene rings around the sigma-bonds and demonstrate the great impact of stochastic ring torsion on the intra-chain mobility in conjugated polymers using poly[phenylene vinylene] (PPV) as a model system. Finally, in Paper III we go beyond the original purpose of the methodology and utilize its great flexibility to study radiationless relaxations of hot excitons.</p> / Report code: LiU-TEK-LIC-2007:4.

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La Méthode de la Trajectoire Adiabatique Contrainte est développée dans le but de résoudre globalementl’équation de Schrödinger. Cette méthode utilise le formalisme de Floquet et une décomposition de Fourier pourdécrire les dépendances temporelles. Elle transforme ainsi un problème dynamique en un problème aux valeurspropres partiel dans un espace de Hilbert étendu au temps. Cette manipulation requiert l’application decontraintes sur les conditions initiales de l’état propre de Floquet recherché. Les contraintes sont appliquées parl’intermédiaire d’un opérateur absorbant artificiel. Cet algorithme est adapté à la description de systèmes dirigéspar des hamiltoniens dépendant explicitement du temps. Il ne souffre pas de l’accumulation d’erreurs au cours dutemps puisqu’il fournit une solution globale ; les erreurs éventuelles proviennent de la non-complétude des basesfinies utilisées pour la description moléculaire ou temporelle et de l’imperfection du potentiel absorbant dépendantdu temps nécessaire pour fixer les conditions initiales. Une forme générale de potentiel absorbant a étédéveloppée pour être en mesure d’intégrer un problème avec une condition initiale quelconque. Des argumentsrelatifs au suivi adiabatique dans le cas de Hamiltoniens non-hermitiens sont également présentés. Nous insistonssur le rôle des facteurs de phase géométrique. Les méthodes développées sont appliquées à des systèmesatomiques ou moléculaires soumis à des impulsions laser intenses, en relation avec la problématique du contrôlemoléculaire. Nous considérons plusieurs exemples : modèles d’atomes à deux ou trois niveaux, ion moléculairehydrogène et molécules froides de sodium. / The Constrained Adiabatic Trajectory Method (CATM) allows us to compute global solutions of the time-dependent Schrödinger equation using the Floquet formalism and Fourier decomposition. The dynamical problem is thustransformed into a “static” problem, in the sense that the time will be included in an extended Hilbert space. Thisapproach requires that suitable constraints are applied to the initial conditions for the relevant Floquet eigenstate.The CATM is well suited to the description of systems driven by Hamiltonians with explicit and complicated timevariations. This method does not have cumulative errors and the only error sources are the non-completeness ofthe finite molecular and temporal basis sets used, and the imperfection of the time-dependent absorbing potentialwhich is essential to impose the correct initial conditions. A general form is derived for the absorbing potential,which can reproduce any dispersed boundary conditions. Arguments on adiabatic tracking in the case of nonhermitianHamiltonians are also presented. We insist on the role of geometric phase factors. The methods areapplied to atomic and molecular systems illuminated by intense laser pulses, in connection with molecular controlproblems. We study several examples : two or three-level atomic models, hydrogen molecular ion, cold sodiummolecules.

Magnetic nozzles, like Laval nozzles, are observed in several natural systems and have application in areas such as electric propulsion and plasma processing. Plasma flowing through these nozzles is inherently tied to the field lines and must separate for momentum redirection or particle transport to occur. Plasma detachment and associated mechanisms from a magnetic nozzle are investigated. Experimental results are presented from the plume of the VASIMR® VX-200 device flowing along an axisymmetric magnetic nozzle and operated at two ion energies to explore momentum dependent detachment. The argon plume expanded into a 150m3 vacuum chamber where the background pressure was low enough that charge-exchange mean-free-paths were longer than experiment scale lengths. This magnetic nozzle system is demonstrated to hydrodynamically scale up to astrophysical plasmas, particularly the solar chromosphere, implying general relevance to all systems. Plasma parameters were mapped over a large spatial range using measurements from multiple plasma diagnostics. The data show that the plume does not follow the magnetic field lines. A mapped integration of the ion flux shows the plume may be divided into three regions where 1) the plume briefly follows the magnetic flux, 2) diverges quadratically before 3) expanding with linear trajectories. Transitioning from region 1→2, the ion flux departs from the magnetic flux suggesting ion detachment. An instability forms in region 2 driving an oscillating electric field that causes ions to expand before enhancing electron cross-field transport through anomalous resistivity. Transitioning from region 2→3 the electric field dissipates, the trajectories linearize, and the plume effectively detaches. A delineation of sub-to-super Alfvénic flow aligns well with the inflection points of the linearization without a change in magnetic topology. The detachment process is best described as a two part process: First, ions detach by a breakdown of the magnetic moment when the quantity |v/fcLB| becomes of order unity. Second, the turbulent electric field enhances electron transport up to a factor of 4±1 above collisional diffusion; electron cross-field velocities approximate that of the ions and depart on more centralized field lines. Electrons are believed to detach by breakdown of magnetic moment further downstream in the weaker magnetic field.

La physique moderne repose sur deux théories fondamentales distinctes, la relativité générale et la mécanique quantique. Toutes les deux décrivent d’une part les phénomènes macroscopiques et cosmologiques tels que les ondes gravitationnelles et les trous noirs et d’autre part les phénomènes microscopiques comme la superfluidité ou le spin des particules. L’unification de ces deux théories reste, jusqu’à présent, un problème non résolu. Il est intéressant de noter que les différentes théories de gravité quantique prédisent une violation des principes de la relativité générale à différents niveaux.Il est donc hautement intéressant de détecter les violations de ces principes et de déterminer à quel niveau elles se produisent.De récentes propositions pour effectuer des tests du principe d’ équivalence d’Einstein suggèrent une amélioration spectaculaire des performances en utilisant des capteurs atomiques `a ondes de matière.Dans ce contexte, il est nécessaire de concevoir des états d’entrée de l’interferomètre avec des conditions initiales bien définies. Un test de pointe de l’universalité de la chute libre (Universality of FreeFall en anglais (UFF) ) nécessiterait, par exemple,un contrôle des positions et des vitesses avec une précision de l’ordre de 1 μm et 1 μm.s⁻¹ , respectivement.De plus, les systématiques liées à la taille du paquet d’ondes limitent le taux d’expansion maximum possible à 100 μm.s⁻¹. La création initiale des états d’entrée de l’interféromètre doit être assez rapide,de l’ordre de quelques centaines de ms au maximum,pour que le temps de cycle de l’expérience soit pertinent d’un point de vue métrologique. Dans cette thèse j’ai développé des séquences optimisées s’appuyant sur l’excitation du centre de masse et de la taille d’un ou plusieurs ensembles d’atomes refroidis ainsi que dégénérés. Certaines séquences proposé dans cette thèse ont déjà été implémenté dans des expériences augmentant de manière significative le contrôle des ensembles atomiques. / Modern physics relies on two distinct fundamental theories, General Relativity and Quantum Mechanics. Both describe on one hand macroscopic and cosmological phenomena such as gravitational waves and black holes and on the other hand microscopic phenomena as superfluidity or the spin of particles. The unification of these two theories remains, so far, an unsolved problem. Interestingly, candidate Quantum Gravity theories predict a violation of the principles of General Relativity at different levels. It is, therefore, of a timely interest to detect violations of these principles and determine at which level they occur. Recent proposals to perform Einstein Equivalence Principle tests suggest a dramatic performance improvement using matter-wave atomic sensors. In this context, the design of the input states with well defined initial conditions is required. A state-of-the-art test of the universality of free fall (UFF) would, for example, require a control of positions and velocities at the level of 1 µm and 1 µm.s⁻¹, respectively. Moreover, sizerelated systematics constrain the maximum expansion rate possible to the 100 µm.s⁻¹level. This initial engineering of the input states has to be quite fast, of the order of few hundred ms at maximum, for the experiment’s duty cycle to be metrologically-relevant. In this thesis I developed optimized sequences based on the excitation of the center of mass and the size excitation of one or two cooled atomic sample as well as degenerated gases. Some sequences proposed in this thesis have already been implemented in experiments and significantly increase the control of atomic ensembles.