General control of atoms and molecules has long been a goal for atomic physicists and physical chemists. Techniques such as laser cooling have been a huge breakthrough in studying ultra cold atoms and BECs. Although laser cooling has been a remarkable tool, it is limited to small group of atoms on the periodic table. A general technique to control and manipulate the entire periodic table has been out of reach until now. In this thesis I describe two methods of general control of atoms in the contexts of stopping supersonic beams and of isotope separation. Both these methods take advantage of high flux supersonic beams and the fact that every atom has a magnetic moment in the ground state or a long-lived excited state which can be manipulated using magnetic field gradients. The first method uses a series of pulsed electomagnetic coils to slow and stop a supersonic beam of paramagnetic atoms and molecules. We have demonstrated the slowing of metastable neon and molecular oxygen using 64 coils from 446.5 m/s to 55.8 m/s for metastable neon, and from 389 m/s to 83 m/s for molecular oxygen respectively. The second method is a novel and efficient approach to isotope separation which utilizes the concept of Maxwell's Demon. We call this technique Single-Photon Atomic Sorting as it is closely related to Single-Photon Cooling, a cooling technique developed in our laboratory. Our method uses a laser beam to change the magnetic moment to mass ratio in such a way that the desired isotopes are guided through a multi-pole magnetic field and collected. We show simulation results for various test cases which highlight the general applicability of this method. / text

This dissertation discusses several recently developed experimental techniques for controlling the motion of neutral atoms. While laser cooling and evaporative cooling have been extremely successful and have been in widespread use for many years, these techniques are only applicable to a few atomic species. Supersonic beams provide a general method of producing cold atoms in the co-moving frame, but their speeds are typically several hundreds of meters per second in the lab frame. Methods to slow and control atoms cooled by supersonic expansion are detailed. A method for controlling the velocity of a cold beam of ground state helium using specular reflection from single crystal surfaces is demonstrated. The velocity of the beam is shown to be continuously tunable, and beam velocities as slow as 265m/s are created from an initial beam speed of 511 m/s. Magnetism is a nearly universal atomic phenomenon, making magnetic control of atomic motion a very general technique. Magnetic stopping of supersonic beams of metastable neon and molecular oxygen is demonstrated using a series of pulsed electromagnetic coils. Neon is slowed from 446 m/s to 56 m/s, and oxygen is slowed from 389 m/s to 83 m/s, removing over 95% of the kinetic energy. The experimental technique is described in detail, and the theory and principle are discussed. An experiment for slowing and trapping of atomic hydrogen isotopes at around 100 mK using a room temperature apparatus is described. A method for further cooling of magnetically trapped hydrogen ensembles, single-photon cooling, is proposed. / text

This thesis discusses two ensembles, the study of which was dependent upon the controllable production of cold gas-phase samples using supersonic beams. The experiments on DNA bases and base clusters were carried out in Germany at the Max Born Institute. The experiments anticipating the construction of a molecular beam slower were carried out in the United States at the University of Texas at Austin. Femtosecond pump-probe techniques were employed to study the dynamics and electronic character of DNA bases, pairs and clusters in the gas phase. Experiments on DNA base monomers confirmed the dominance of a particular relaxation pathway, the nπ* state. Competition between this state and another proposed relaxation pathway was demonstrated through observations of the DNA base pairs and base-water clusters, settling a recent controversy. Further, it was determined that the excited state dynamics in base pairs is due to intramolecular processes rather than intermolecular processes. Finally, results from base-water clusters confirm that microsolvation permits comparison with biologically relevant liquid phase experiments and with ab initio calculations, bridging a long-standing gap. A purely mechanical technique that does not rely upon quantum or electronic properties to produce very cold, very slow atoms and molecules would be more generally applicable than current approaches. The approach described here uses supersonic beam methods to produce a very cold beam of particles and a rotating paddle-wheel, or rotor, to slow the cold beam. Initial experiments testing the possibility of elastic scattering from a single crystal surface were conducted and the implications of these experiments are discussed. / text

Le développement de différentes techniques pour contrôler les degrés de liberté internes et externes des molécules et pour produire (ultra-) froide, piège des moléculaire ensembles ouvrir des voies différentes à la physique et la chimie dans le régime de basse température. Il s'agit notamment de nombreux territoires en physique comme, phases quantiques de la matière, traitement de l'information quantique, les froides collisions moléculaires, les chimies froides et aussi de divers tests de haute précision pour la physique fondamentale. Cette thèse décrit diverses expériences de guidage et de décélération des faisceaux supersoniques d'atomes paramagnétiques à l’aide de champs magnétique inhomogène dépendent du temps. Ces champs magnétiques inhomogènes ont été utilisés pour exercer une force sur les atomes ou les molécules paramagnétiques, qui résultent de l'effet Zeeman. Le principe du ralentisseur Zeeman nouvellement développé est de produire un déplacement tridimensionnel du piège magnétique, à la vitesse initiale du faisceau. Le contrôle de la dépendance temporelle du champ magnétique nous permet de contrôler la vitesse du piège magnétique co-mobile, procurant ainsi une décélération d'une classe de vitesse du faisceau supersonique. Le piège magnétique co- mobile est déduit à partir d'une onde magnétique mobile, offrant un minimum de distorsion du piège lors de sa propagation. Les propriétés transverses du piège sont réglables grâce à un champ magnétique transversal quadrupolaire, qui peut être ajusté indépendamment des propriétés de vitesses et l'accélération du piège. Une grande part du travail de thèse a été consacrée à la conception, la réalisation et la construction du montage expérimental, consistant en un jet supersonique et en un dispositif complexe de bobines pour réaliser l’onde magnétique progressive, formant un piège magnétique mobile. Le jet froid pulsé d'atomes métastables est produit par expansion supersonique à travers une valve refroidie à l'azote liquide, excités dans l'état métastable par une décharge électrique. Nous avons guidé le jet d'argon au travers d’un tube capillaire le guidage et la décélération ont été démontrés. Le piège magnétique mobile est formé par la combinaison d'un champ magnétique quadrupolaire et d'un champ magnétique axial modulé spécialement. Le champ quadrupolaire est continu et un gradient de champ est dirigé seulement dans la direction transverse du jet. Le circuit plan produit une onde magnétique sinusoïdale avec un gradient de champ dans la direction axiale. Avec l'électronique fabriquée au laboratoire, ou peut produire une onde magnétique progressive d'amplitude 0.69T (avec un courant AC de 300A) et de fréquence 40 kHz. On obtient ainsi une onde qui se déplace à une vitesse de 464m/s. Plusieurs expériences de principe ont été réalisées en utilisant le jet froid pulsé d'argon métastable. Nous avons étudié les propriétés de guidage du quadrupole pour divers courants et pour différents atomes (hélium et argon) et comparé les résultats aux prédictions théoriques de simulations numériques. Le jet d'argon métastable a été guidé en 3D à des vitesses variées (464m/s, 400m/s, 392m/s) avec un décélérateur de 28cm de long. La température observée du paquet guidé est de 100mK. L'expérience de décélération a été réalisée avec le jet d'argon métastable depuis la vitesse de 400m/s jusqu’à 370m/s et depuis la vitesse de 392m/s jusqu’à 365m/s. Les résultats expérimentaux sont comparés avec les simulations numériques. / The development of various techniques to control both the internal and external degrees of freedom of molecules and to produce (ultra-) cold, trapped molecular ensembles open various avenues to physics and chemistry in the low temperature regime. These include many territories in physics like, quantum phases of matter, quantum information processing, cold molecular scattering, cold chemistry and also various high precision tests for fundamental physics.This thesis describes various guiding and deceleration experiments of supersonic beams of paramagnetic atoms using inhomogeneous time-dependent magnetic fields. Inhomogeneous magnetic fields have been used to exert a force on paramagnetic atoms or molecules, which derives from the Zeeman effect. The principle of the newly developed Zeeman decelerator is to produce a moving tridimensional magnetic trap, which moves at the initial velocity of the beam. The control of the time dependence of the magnetic field allows us to control the velocity of the so-called co-moving magnetic trap, thereby affording for a deceleration of a velocity class of the supersonic beam. The co-moving magnetic trap is inferred from a moving magnetic wave, offering a minimal distortion of the trap during its propagation. The transverse properties of the trap are tunable through a transverse quadrupolar magnetic field, which can be adjusted independently of the velocity and acceleration properties of the trap.Much of this thesis was devoted to the design, development and construction of the experimental setup consisting of a supersonic beam and complex coils to achieve a traveling magnetic wave. Using home-made electronics operating 300A AC currents at frequencies up to 40 kHz, the coils can produce a magnetic wave of amplitude 0.7T, moving at a controllable velocity up to 464m/s. Several proof-of-principle experiments have been carried out using a pulsed, cold beam of metastable atoms, excited in metastable states by an electric discharge during the supersonic expansion. We have studied the guiding properties of the quadrupolar magnetic field alone on two atomic beams (metastable helium and argon) and compared with the theoretical prediction of tridimensional numerical simulations. A supersonic beam of metastable argon atoms has been trapped in a co-moving trap at a constant velocity (464m/s, 400m/s, and 392m/s) using a 28cm-long prototype decelerator. The temperature of the guided beam packet is observed to be 100mK. Finally, Zeeman deceleration experiments have been done on metastable argon beams with an initial velocity of 400m/s, decelerated to various final velocities (392m/s, 370m/, and 365m/s). The experimental results are compared with tridimensional numerical simulations.Keywords: Supersonic beams, metastable atoms, cold molecules, atoms in inhomogeneous magnetic fields, transverse magnetic guide, co-moving magnetic trap, tridimensional guiding, Zeeman deceleration.