Aux basses températures, les matrices dopées aux ions terre-rare sont des systèmes prometteurs pour la réalisation de mémoires quantiques. Parmi elles, le système Er³⁺:Y₂SiO₅ a l'avantage de posséder une transition aux longueurs d'onde Télécom, adaptée aux réseaux de communication actuels. Cependant, aucun stockage quantique n'a pu être réalisé de manière efficace durant un temps suffisamment long dans ce matériau. L'objectif de cette thèse est de mieux comprendre les interactions limitant la cohérence du système aux faibles champs magnétiques. Dans ce cadre là, les interactions dominantes sont les basculements réciproques entre deux spins électroniques opposés des ions erbium et l'interaction super-hyperfine entre ces spins et les spins nucléaires des ligands yttrium. J'ai calculé la force et les caractéristiques de ces deux couplages dipolaires en incluant la grande anisotropie de la matrice Y₂SiO₅. J'ai alors pu vérifier l'effet de cette anisotropie sur les basculements réciproques des spins des ions erbium à l'aide de deux techniques optiques, le creusement de trou spectral et l'excitation transitoire. Le taux de ces basculements est maximisé lorsque le champ magnétique est orienté perpendiculairement à l'axe principal du tenseur caractérisant le spin effectif. Il augmente globalement comme le carré de la concentration en ions dopants et diminue avec le champ magnétique. Enfin, j'ai pu mesurer les caractéristiques des interactions super-hyperfines par le biais des modulations d'une décroissance d'écho de photon qu'elles provoquent. Il existe une configuration particulière où un couplage sélectif intervient entre les ions erbium et un unique yttrium de leurs environnements. Au contraire, le couplage à un nombre important d'ions ligands est responsable de la chute du temps de cohérence pour des champs magnétiques inférieurs à la dizaine de mT. / At low temperatures, rare-earth doped matrices are promising supports for the development of quantum memories. Among them, Er³⁺:Y₂SiO₅ is well adapted to the current communication networks because of its transition at Telecom wavelength. However, quantum storage has a very limited efficiency and a short duration in this material. In this thesis, I study the interactions that hinder the coherence at low magnetic fields. In this regime, the dominant processes are flip-flops between opposite electronic spins of erbium ions and the super-hyperfine interaction with nuclear spins of yttrium ligands. I have included the strong anisotropy of the Y₂SiO₅ matrix in the calculation of these two dipolar interactions. In order to check the anisotropy of the flip-flops between erbium spins, I have used two different optical techniques : spectral hole-burning and transient excitation. I have showed that their rate is maximum when the magnetic field is perpendicular to the principal axis of the effective spin tensor. Moreover, the flip-flop probability globally increases as the square of the doping concentration and as the inverse of the field. Then I have also checked the calculations of super-hyperfine interactions by measuring photon echo modulations. I have found a particular situation where an erbium ion is strongly coupled to a single yttrium. On the contrary, the coupling to several ligands at very low magnetic fields drastically reduces the coherence time.

La réalisation d’une mémoire quantique pour la lumière met en jeu les aspects les plus fondamentaux de l’interaction matière-rayonnement. Pour capturer l’information quantique portée par la lumière, le matériau doit être capable de se maintenir dans un état de superposition quantique. Le temps de stockage est limité par la durée de vie de cet état, caractérisée par le temps de cohérence. Les premières expériences ont été réalisées dans des vapeurs atomiques froides, bien connues. Plus récemment, les ions de terres rares en matrice cristalline (REIC) ont attiré l’attention par leurs long temps de cohérence, associés à de larges bandes passantes d’interaction. Pour exploiter ces bonnes propriétés, des protocoles spécifiques ont été proposés. Nous nous sommes tournés vers un dérivé prometteur de l’écho de photon, le Peigne Atomique de Fréquences (AFC, proposé en 2008), fondé sur la transmission du champ incident à travers un profil d’absorption spectralement périodique. Les premiers chapitres de ce manuscrit présentent ce protocole et les travaux effectués durant cette thèse pour en améliorer l’efficacité (i.e. la probabilité de capter et de restituer l’information incidente), en augmenter la bande passante et la capacité de multiplexage et en mesurer le bruit. Les chapitres suivants présentent un nouveau protocole, proposé dans notre groupe durant cette thèse, et baptisé ROSE (Revival Of Silenced Echo). Ce protocole, très proche de l’écho de photon, a été démontré et caractérisé expérimentalement. Il semble très prometteur en termes d’efficacité, de bande passante et de bruit. / The development of a quantum memory for light involves the most fundamental aspects of the light-matter interaction. To store the quantum information carried by light, the material has to be able to stay in a state of quantum superposition. The storage time is limited by the lifetime of this state, characterized by the coherence time. The first experiments involved the well-known cold atomic vapors. More recently, Rare Earth Ions doped Crystals (REIC) have drawn attention because of their remarkably long coherence time, combined with a large interaction bandwidth. Specific protocols have been proposed to take the most out of these properties. We have opted for a promising spin-off of the well-known photon echo, named the Atomic Frequency Comb (AFC, proposed in 2008), based on the transmission of the incoming field through a spectrally periodic absorption profile. The first chapters of this manuscript present this protocol and our works aimed at improving its efficiency (the probability for capturing and retrieving the incoming information), increasing its bandwidth and its multiplexing capacity and measuring its noise. The following chapters present a new protocol, proposed in our group during this thesis, and called Revival Of Silenced Echo (ROSE). This protocol, similar to the photon echo, have been demonstrated and characterized experimentally. It seems really promising in terms of efficiency, bandwidth and noise.

Neste trabalho estudamos teórica e experimentalmente o efeito de Conjugação de Fase por Mistura Degenerada de Quatro Ondas (CFMD40) e Modulação Transversal de Fase em cristais dopados com Cr+3. Estudamos a CFMD40 em Al2O3:Cr+3 (rubi) e GdAlO3:Cr+3 com um laser de Ar (em λ=514nm) obtendo um bom acordo entre os resultados experimentais e os teóricos (nestes cálculos usamos os valores de n2 de um trabalho anterior [1]). O modelo teórico que fizemos explica muito bem o comportamento de saturação da eficiência da CFMD40 que não era compreendido em trabalhos anteriores [47,48.2]. Usando os mesmos valores de n2 obtivemos um bom acordo entre os resultados experimentais e teóricos para o efeito de Modulação Transversal de Fase. Também fizemos um modelo teórico para o efeito de Modulação Transversal de Fase em CFMD40 que explica nossas observações [2]. A não linearidade destes materiais foi investigada usando-se três técnicas experimentais diferentes [1.2] e por dois outros grupos [61.62] (para o rubi) através de mistura de duas ondas não degeneradas. Todas estas medidas estão em bom acordo. Na alexandrita (BeAl2O 4:Cr+3) estudamos o espectro de χ(3) (ou n2) em ressonância das linhas R. Nos atribuímos a forma assimétrica do espectro como sendo oriunda de duas contribuições para susceptibilidade, onde um termo é devido a interação ressonante com o sistema de dois níveis e o outro devido a mudança de polarizabilidade causada pela população do estado excitado (esta é a primeira vez que este efeito foi observado). / In this work we studied theoretical and experimentally the effects of Phase Conjugation by Degenerate Four Wave Mixing and Transversal Phase (PCD4WM) Modulation in Cr+3 doped crystals. We studied the PDC4WM in Al2O3:Cr+3 (ruby) and GdAlO3:Cr+3 with on Ar laser (at λ= 514 nm) and obtained a good agreement between our experimental and theoretical results (in these ca1culations we used the nonlinear refractive index n 2 values from a previous paper [1]. The theoretical model that we developed explains very well the saturation behaviour of the PDC4WM efficiency that was not understood in previous papers [47.48,2]. These values of n2 are also in good agreement with our results in Transverse Phase Modulation. We also developed a theoretical model for the effect of Transverse Phase Modulation in PCDFWM that explains our observations [2]. The nonlinearity ?n IND.2? from these materials was investigated by us using three different techniques [1.2], by other two groups [61.62] (for the ruby) in nondegenerate two-wave mixing and all those measurements are in good agreement. In alexandrite (BeAl2O4:Cr +3) we studied the χ(3) (or n2) spectrum in resonance with the R lines. We attributed the asymetric shape of the spectrum by the effect of two differents contributions, one term due to the resonant interaction of the two-level system and the other due to the polarizability change caused by excited state population (this is the first observation of this kind of effect.

Neste trabalho estudamos teórica e experimentalmente o efeito de Conjugação de Fase por Mistura Degenerada de Quatro Ondas (CFMD40) e Modulação Transversal de Fase em cristais dopados com Cr+3. Estudamos a CFMD40 em Al2O3:Cr+3 (rubi) e GdAlO3:Cr+3 com um laser de Ar (em λ=514nm) obtendo um bom acordo entre os resultados experimentais e os teóricos (nestes cálculos usamos os valores de n2 de um trabalho anterior [1]). O modelo teórico que fizemos explica muito bem o comportamento de saturação da eficiência da CFMD40 que não era compreendido em trabalhos anteriores [47,48.2]. Usando os mesmos valores de n2 obtivemos um bom acordo entre os resultados experimentais e teóricos para o efeito de Modulação Transversal de Fase. Também fizemos um modelo teórico para o efeito de Modulação Transversal de Fase em CFMD40 que explica nossas observações [2]. A não linearidade destes materiais foi investigada usando-se três técnicas experimentais diferentes [1.2] e por dois outros grupos [61.62] (para o rubi) através de mistura de duas ondas não degeneradas. Todas estas medidas estão em bom acordo. Na alexandrita (BeAl2O 4:Cr+3) estudamos o espectro de χ(3) (ou n2) em ressonância das linhas R. Nos atribuímos a forma assimétrica do espectro como sendo oriunda de duas contribuições para susceptibilidade, onde um termo é devido a interação ressonante com o sistema de dois níveis e o outro devido a mudança de polarizabilidade causada pela população do estado excitado (esta é a primeira vez que este efeito foi observado). / In this work we studied theoretical and experimentally the effects of Phase Conjugation by Degenerate Four Wave Mixing and Transversal Phase (PCD4WM) Modulation in Cr+3 doped crystals. We studied the PDC4WM in Al2O3:Cr+3 (ruby) and GdAlO3:Cr+3 with on Ar laser (at λ= 514 nm) and obtained a good agreement between our experimental and theoretical results (in these ca1culations we used the nonlinear refractive index n 2 values from a previous paper [1]. The theoretical model that we developed explains very well the saturation behaviour of the PDC4WM efficiency that was not understood in previous papers [47.48,2]. These values of n2 are also in good agreement with our results in Transverse Phase Modulation. We also developed a theoretical model for the effect of Transverse Phase Modulation in PCDFWM that explains our observations [2]. The nonlinearity ?n IND.2? from these materials was investigated by us using three different techniques [1.2], by other two groups [61.62] (for the ruby) in nondegenerate two-wave mixing and all those measurements are in good agreement. In alexandrite (BeAl2O4:Cr +3) we studied the χ(3) (or n2) spectrum in resonance with the R lines. We attributed the asymetric shape of the spectrum by the effect of two differents contributions, one term due to the resonant interaction of the two-level system and the other due to the polarizability change caused by excited state population (this is the first observation of this kind of effect.