New experiments and theory contributing to the understanding of the dynamics and control of molecular Rydberg wave packets are presented. An intuitive scheme for controlling the rotational quantum state of a Rydberg molecule is demonstrated experimentally. We determine the accumulated phase difference between the various components of a molecular electron wave packet, and then employ a sequence of phase-locked optical pulses to selectively enhance or depopulate specific rotational states. The angular momentum composition of the resulting wave packet, and the efficiency of the control scheme, is determined by calculating the multipulse response of the time dependent Rydberg populations. The dynamics of predissociating Rydberg electron wavepackets are observed using the optical Ramsey method. The time-resolved spectra are hydrogenic and are very well modeled by assuming that only one p Rydberg series contributes to the dynamics. This is in contrast with previous observations of autoionising Rydberg electron wave packets which show quite dramatic deviations from hydrogenic behaviour above the Born-Oppenheimer limit. The origin of these deviations lies in the interplay between electronic and molecular phase. By exploiting these phases we are able to control the ratio of predissociaton to autoionisation A multichannel quantum defect theory analysis of the Rydberg state of NO is undertaken. The analysis takes into account all the accessible series with / < 3 and all documented interseries interactions. This analysis is the most complete description of NO to date and will aid in the design of future coherent control experiments.

L’essor des procédés de micro et nano-fabrications rend aujourd’hui accessible la synthèse contrôlée de nanoparticules métalliques (typiquement de 3 à 200nm) offrant de larges résonances d’absorption et de diffusion dont les fréquences peuvent être contrôlées finement en variant judicieusement leur géométrie et leur composition. Dans ce travail de thèse relevant de l’électrodynamique classique établit par Maxwell, nous étudions numériquement l’intérêt de ces particules pour la problématique du (dé)couplage de la lumière piégée dans un film mince diélectrique - une géométrie de référence permettant de rendre compte du phénomène de piégeage qui limite considérablement l’efficacité de dispositifs électroluminescents et de certaines cellules solaires. Pour ce faire, nous proposons quelques règles de conception de nanoparticules capables d’extraire efficacement la lumière piégée. Pour un émetteur seul, environ 20% de la lumière émise est rayonnée hors du guide (rad~0.2). L’ajout d’une monocouche (~50nm d’épaisseur) composée d’un ensemble de particules « optimisées » et aléatoirement positionnées autour de l’émetteur permet d’accroître cette efficacité jusqu’à 70% en moyenne statistique sur le désordre. D’intéressants effets de cohérences liés à la nature du désordre au sein de ladite couche sont également mis en évidence. / Metallic nanoparticles (MNps) exhibit strong plasmonic resonances in their absorption and scattering spectra. Recent advances in micro- and nano-fabrication processes allow scientists to control the particle shape; and thus to tune these resonances on the visible and near-IR spectrum - opening unprecedented applications ranging from imaging techniques to solar cells improvement. In the present work, we numerically investigate the capacity of MNps to (de)couple the light that is confined in guided modes of dielectric thin films—a relevant system to analyze, understand and reduce the light trapping phenomenon that strongly lowers the efficiency of some electroluminescent devices. To this end, we propose, by the control of its polarization state, to optimize the quantity of light that a nanoparticle extracts during a scattering event. For a sole source embedded in the guide, barely 20% of the light is extracted (rad~0.2). The addition of an ultra-thin layer composed of hundreds of randomly deposited engineered-nanoparticles shows promising results with rad ~0.7 (in realistic configurations). Interesting coherence effects arising from the randomness of the disorder are also evidenced.