This thesis has focused on functionalising heterometallic [nPr2NH2][Cr7NiF8(O2CtBu)16], {Cr7Ni}, clusters, which are candidates for qubits in quantum information processing, by substitution of the peripheral carboxylic acids to produce [nPr2NH2][Cr7NiF8(O2CtBu)16-x(O2CR)], where R is a group with the desired functionality. The use of pyridyl and carboxylic acid containing groups has been investigated for the purposes of linking {Cr7Ni} units, either through metal sites and metallic clusters. The work has resulted in the synthesis of multi-component, polymetallic, nano-scale constructs where in some cases where the individual building blocks have been pre-synthesised and isolated prior to synthesis, with examples of three, four and six {Cr7Ni} units bound to a variety of metal clusters. A selection of aromatic functionalised carboxylic acids has also been successfully substituted onto the ring periphery with the prospect of binding to aromatic surfaces such as graphene and carbon nanotubes. These include fluorenylmethyloxycarbonyl protected amino acids, which opens a potential avenue to grafting of peptide chains to the periphery.

Nanoscale systems have sizes intermediate between atomic and macroscopic ones. Therefore their treatment often requires a combination of methods from atomic and condensed matter physics. The conventional Landau-Zener theory, being a powerful tool in atomic physics, often fails to predict correctly nonadiabatic transition probabilities in various nanostructures because it does not include many-body effects typical for mesoscopics. In this research project the generalizations of the Landau-Zener theory that solve this problem were studied. The multistate, multiparticle and nonunitary extensions of the theory have been proposed and investigated. New classes of exactly solvable models have been derived. I discuss their applications in problems of the molecular condensate dissociation and of the driven charge transport. In application to the physics of nanomagnets new approaches in modeling the influence of the environment on the Landau-Zener evolution are proposed and simple universal formulas are derived for the extensions of the theory that include the coupling to noise and the nuclear spin bath.

Nanoscale systems have sizes intermediate between atomic and macroscopic ones. Therefore their treatment often requires a combination of methods from atomic and condensed matter physics. The conventional Landau-Zener theory, being a powerful tool in atomic physics, often fails to predict correctly nonadiabatic transition probabilities in various nanostructures because it does not include many-body effects typical for mesoscopics. In this research project the generalizations of the Landau-Zener theory that solve this problem were studied. The multistate, multiparticle and nonunitary extensions of the theory have been proposed and investigated. New classes of exactly solvable models have been derived. I discuss their applications in problems of the molecular condensate dissociation and of the driven charge transport. In application to the physics of nanomagnets new approaches in modeling the influence of the environment on the Landau-Zener evolution are proposed and simple universal formulas are derived for the extensions of the theory that include the coupling to noise and the nuclear spin bath.

Quantum mechanics has a long history of helping computer science. For a long time, it provided help only at the hardware level by giving a better understanding of the properties of matter and thus allowing the design of ever smaller and ever more efficient components. For the last few decades, much research has been dedicated to finding whether one can change computer science even more radically by using the principles of quantum mechanics at both the hardware and algorithm levels. This field of research called Quantum Information Processing (QIP) has rapidly seen interesting theoretical developments: it was in particular shown that using superposition of states leads to computers that could outperform classical ones. The experimental side of QIP however lags far behind as it requires an unprecedented amount of control and understanding of quantum systems. Much effort is spent on finding which particular systems would provide the best physical implementation of QIP concepts. Because of their nearly endless versatility and the high degree of control over their synthesis, organic materials deserve to be assessed as a possible route to quantum computers. This thesis studies the QIP potential of spin degrees of freedom in several such organic compounds. Firstly, a study on low-spin antiferromagnetic rings is presented. It is shown that in this class of molecular nanomagnets the relaxation times are much longer than previously expected and are in particular long enough for up to a few hundred quantum operations to be performed. A detailed study of the relaxation mechanisms is presented and, with it, routes to increasing the phase coherence time further by choosing the suitable temperature, isotopic and chemical substitution or solvent. A study of higher-spin systems is also presented and it is shown that the relaxation mechanisms are essentially the same as in low-spin compounds. The route to multi-qubit system is also investigated: the magnetic properties of several supermolecular assemblies, in particular dimers, are investigated. Coupling between neighbouring nanomagnets is demonstrated and experimental issues are raised concerning the study of the coherent dynamics of dimers. Finally a study of the purely organic compound phenanthrene is reported. In this molecule the magnetic moment does not result from the interactions between several transition metal ions as in molecular nanomagnets but from the photoexcitation of an otherwise diamagnetic molecule. The interest of such a system in terms of QIP is presented and relaxation times and coupling to relevant nuclei are identified.

L'objectif de cette thèse était de développer un magnétomètre à force de Faraday pour mesurer des valeurs absolues de l'aimantation à très basse température (30 mK) et fort champ magnétique (16 T) avec une haute sensibilité (10-5 emu). Ce magnétomètre sera principalement utilisé pour sonder les propriétés induites sous champ dans les systèmes magnétiques frustrés.Dans une première partie, je détaille le développement de ce magnétomètre. Cela comprend l'optimisation du réfrigérateur à dilution et de bobines de gradient de champ ainsi que le développement d'une détection capacitive avec un étage amplificateur à froid pour améliorer la sensibilité de la mesure. Les mesures magnétiques préliminaires sont présentées. Les changements nécessaires pour rendre le magnétomètre opérationnel sont discutés.Dans une seconde partie, je présente l'étude expérimentale de systèmes magnétiques frustrés: des grenats de Gadolinium, décrits par des spins classiques, et des composés moléculaires frustrés à base de Cuivre, pour sonder les effets quantiques. Ces mesures ont été réalisées entre 70 mK et 300 K sur les magnétomètres existant à l'Institut Néel.Dans Gd3Ga5O12, nous avons complété le diagramme de phases H-T. Nous avons montré la robustesse de ce diagramme de phases par notre étude sur le composé isomorphe GGd3Al5O12. Nous avons mis en évidence la convergence de toutes les phases observées en un unique point dans les deux systèmes.Dans les systèmes quantiques, nous avons réalisé des études préliminaires sur des clusters Cu44 à base de tétraèdres, et un système triangulaire Cu3. Bien que prometteuses, nous n'avons pas approfondi ces études à cause de problèmes d'échantillons. / The objective of this work was to develop a Faraday force magnetometer to measureabsolute values of the magnetization at very low temperatures (30 mK) andhigh applied magnetic fields (16 T) with a high sensitivity (10-5 emu). This magnetometer will be especially dedicated to the study of the field induced properties of frustrated magnets.In a first part, I present the development of this magnetometer. It involves the optimization of the dilution refrigerator and field gradient coils, and the development of a capacitive detection with a cold amplifier stage to improve the measurement sensitivity. Preliminary magnetic measurements are shown. The changes in the design required to make the magnetometer operational are discussed.In a second part, I focus on experimental studies of frustrated magnets: Gadolinium garnets, described by classical spins, and Copper based frustrated molecular compounds, to probe quantum effects. These measurements were performed from 70 mK to 300 K, with the existing magnetometers at the Institut Neel.In Gd3Ga5O12, we have complemented the H-T phase diagram. This phase diagram was proven to be robust by our study on the isomorphous compound, Gd3Al5O12. We evidence the convergence of all the observed phases to a unique point in both samples.In quantum systems, we performed preliminary studies on Cu44 clusters with tetrahedral motives, and on a triangular system Cu3. Although promising, these studies were not pursued due to sample problems.