A investigação das propriedades ópticas e sua relação com as propriedades magnéticas dos semicondutores é de grande interesse para a comunidade científica, em virtude da enorme demanda por novas tecnologias e funcionalidades que podem surgir dessas pesquisas. Os calcógenos de európio são semicondutores intrinsecamente magnéticos, transparentes na região visível do espectro eletromagnético e integráveis em matrizes de silício e nitreto de gálio, sendo assim fortes candidatos a aplicações tecnológicas envolvendo magnetismo e óptica. Neste trabalho são investigados os espectros de absorção e fotoluminescência dos calcógenos de európio, com base no modelo 4f -> 5d(\'t IND. 2g\') da transição óptica de dipolo elétrico, o qual mostrou-se totalmente adequado para a descrição da absorção óptica nos calcógenos de európio em função do campo magnético aplicado, explicando a presença de linhas de absorção estreitas e dicróicas nos espectros em campo alto e a forma larga dos espectros de absorção em campo nulo. Nos espectros de fotoluminescência do EuTe, entretanto, foram detectados estados eletrônicos não contemplados pelo modelo 4f -> 5d(\'t IND. 2g\') , em especial uma banda de emissão denominada \'MX IND. 0\', acoplada a modos vibracionais da rede. Uma linha zero-fônon correspondente a uma transição que não produz fônons pôde ser bem definida e a partir do deslocamento dessa linha em função do campo magnético foi possível detectar inequivocamente a formação de polarons magnéticos no EuTe pela primeira vez; o raio polarônico foi estimado como R = 3.6a, onde a é o parâmetro de rede e a energia de ligação desse polaron foi estimada em \'E IND. p\' = 45 meV, um resultado que foi confirmado através de medidas do deslocamento da linha zero-fônon em função da temperatura. Adicionalmente procurou-se identificar o estado eletrônico associado à emissão \'MX IND. 0\': a partir de medidas da intensidade da fotoluminescência em função da potência de excitação foi possível sugerir que a emissão \'MX IND. 0\' provem de estados eletrônicos ligados a defeitos da rede e foi possível estimar a concentração desses defeitos como menor que 0.1 ppm. / Investigation of optical properties and their relation to magnetic properties of semiconductors is of great interest to scientific community, due to the large demand for new technologies and features that can arise from these studies. Europium chalcogenides are intrinsically magnetic semiconductors, transparent in the visible region of electromagnetic spectrum and integrable into silicon and gallium nitride matrices, beeing strong candidates for technological applications involving magnetism and optics. The present study investigates absorption and photoluminescence spectra of europium chalcogenides, based on the 4f -> 5d(t2g) model of the electric dipole optical transition, which proved to be entirely appropriate to describe polarized optical absorption in europium chalcogenides as a function of magnetic field, explaining the presence of narrow dichroic lines at high fields and the broad shape of the zero-field absorption spectrum. However, in photoluminescence spectra of EuTe, electronic states not covered by the 4f -> 5d(t2g) model were detected, in particular an emission band labeled MX0, which is coupled to vibrational modes of the lattice. A transition without production of phonons, corresponding to a zero-phonon line, could be well resolved and from the displacement of the zero-phonon line as a function of magnetic field the formation of magnetic polarons in EuTe could be detected unambiguously for the first time. The polaronic radius is estimated as R = 3:6a, where a is the lattice parameter, and the polaron binding energy is estimated as Ep = 45 meV, a result that was confirmed by measurements of zero-phonon line displacement as a function of temperature. Additionally, we sought to identify the electronic state associated with MX0 emission: from measurements of the photoluminescence intensity as a function of excitation power, it was possible to suggest that MX0 emission comes from an electronic state coupled to lattice defects of low concentration, which we estimate to be of less than 0.1 ppm.

Ce travail de thèse porte sur l’étude des propriétés optiques de boites quantiques anisotropes de (Cd,Mn)Te insérées dans des nanofils de ZnTe. Les boites quantiques étudiées contenant 10% de Mn sont allongées suivant l’axe du fil ce qui tend à favoriser un état fondamental à trou léger ayant une susceptibilité de spin perpendiculaire à l’axe du fil. L’objectif principal de la thèse est l’étude de la formation du Polaron Magnétique dans ces boites et la détermination de leur anisotropie magnétique.Nous avons étudié en premier les propriétés optiques de nanofils de ZnTe et de nanofils coeurs-coquilles ZnTe/(Zn,Mg)Te. Ces études nous ont amené à modéliser les contraintes élastiques dans le cœur, dans la coquille et dans des boites allongées insérées dans les nanofils. Ce modèle nous a permis d’estimer les splittings entre les niveaux de trou lourd et de trou léger dans la boite et dans le fil.Nous avons étudié ensuite des nanofils contenant des boites magnétiques et non magnétiques par spectroscopie magnéto-optique. Dans les boites magnétiques, les interactions d’exchange entre les porteurs localisés et les spins de Mn induisent un très fort décalage Zeeman de la raie excitonique (Effet Zeeman Géant). Pour extraire des paramètres quantitatifs, nous avons combiné différentes techniques expérimentales sur le même nanofil (photo et cathodoluminescence, analyse dispersive en énergie du rayonnement X). Nous avons utilisé différentes orientations du champ magnétique pour déterminer l’anisotropie du trou dans la boite. Les valeurs expérimentales sont plus petites que les valeurs théoriques ce qui suggère un mauvais confinement du trou dans la boite.Afin d’obtenir un meilleur confinement du trou, nous avons étudié des boites de (Cd,Mn)Te entourées d’une coquille de (Zn,Mg)Te. Grace au meilleur confinement du trou, nous avons réussi à observer la formation du Polaron Magnétique excitonique. Des mesures de photoluminescence résolues en temps sur des nanofils uniques nous ont permis d’extraire l’énergie et le temps de formation du Polaron Magnétique entre 5K et 50K. La raie d’émission des boites présente un effet Zeeman géant inhabituel caractéristique d’un Polaron Magnétique à trou léger. Nous avons développé un modèle théorique pour décrire la formation du Polaron Magnétique excitonique dans les boites quantiques. Ce model, basé sur l’énergie libre et valable pour des températures et des champs magnétiques arbitraires, a été utilisé pour rendre compte de l’ensemble des données expérimentales. Ce modèle a permis de déterminer les paramètres caractéristiques du polaron magnétique à trou léger (énergie, orientation and amplitude du moment magnétique, volume d’échange, anisotropie du trou). / In this PhD work we study the optical properties of anisotropic (Cd,Mn)Te magnetic quantum dots inserted in ZnTe nanowires. The quantum dots containing typically 10% of Mn spins are elongated along the nanowire axis which tend to stabilize a light hole ground state with a spin susceptibility perpendicular to the nanowire axis. The main goal was to study the formation of exciton Magnetic Polarons in such quantum dots and to determine their magnetic anisotropy.We investigate first the optical properties of ZnTe and ZnTe/(Zn,Mg)Te core shell nanowires. We model the elastic strain profile in core-shell nanowires and in elongated quantum dots. From the strain profiles, we estimate the value of the light hole heavy hole splitting expected in the dot and in the nanowire.In a second step we study single nanowires containing magnetic and non magnetic quantum dots by magneto-optical spectroscopy. The exchange interactions between confined carriers and Mn spins induce a large Zeeman shift of the exciton line (Giant Zeeman Effect). To extract quantitative parameters, we combine different experimental techniques (photo and cathodoluminescence, energy dispersive X ray spectroscopy) on the same nanowire. We use also different magnetic field orientations in order to determine the hole anisotropy in the dot. The experimental values are smaller than the theoretical ones suggesting a weak confinement of the holes in the dot due to a small (Cd,Mn)Te/ZnTe valence band offset.In a third step we study nanowires containing (Cd,Mn)Te quantum dots surrounded by a (Zn,Mg)Te alloy. Thanks to the better hole confinement induced by the (Zn,Mg)Te alloy, the formation of exciton magnetic polarons can be observed. We perform time resolved photoluminescence studies on single nanowires in order to determine the energy and the formation time of magnetic polarons from 5K to 50K. The quantum dot emission line shows an unusual Zeeman shift, characteristic of a light hole magnetic polaron. We develop a theoretical model describing the formation of exciton magnetic polaron in quantum dots. We use this model, based on the free energy and valid for any temperature and magnetic field, to fit the whole set of experimental data. It allows us to determine the characteristic parameters of the light hole magnetic polarons (energy, orientation and magnitude of the magnetic moment, exchange volume, hole anisotropy).

A investigação das propriedades ópticas e sua relação com as propriedades magnéticas dos semicondutores é de grande interesse para a comunidade científica, em virtude da enorme demanda por novas tecnologias e funcionalidades que podem surgir dessas pesquisas. Os calcógenos de európio são semicondutores intrinsecamente magnéticos, transparentes na região visível do espectro eletromagnético e integráveis em matrizes de silício e nitreto de gálio, sendo assim fortes candidatos a aplicações tecnológicas envolvendo magnetismo e óptica. Neste trabalho são investigados os espectros de absorção e fotoluminescência dos calcógenos de európio, com base no modelo 4f -> 5d(\'t IND. 2g\') da transição óptica de dipolo elétrico, o qual mostrou-se totalmente adequado para a descrição da absorção óptica nos calcógenos de európio em função do campo magnético aplicado, explicando a presença de linhas de absorção estreitas e dicróicas nos espectros em campo alto e a forma larga dos espectros de absorção em campo nulo. Nos espectros de fotoluminescência do EuTe, entretanto, foram detectados estados eletrônicos não contemplados pelo modelo 4f -> 5d(\'t IND. 2g\') , em especial uma banda de emissão denominada \'MX IND. 0\', acoplada a modos vibracionais da rede. Uma linha zero-fônon correspondente a uma transição que não produz fônons pôde ser bem definida e a partir do deslocamento dessa linha em função do campo magnético foi possível detectar inequivocamente a formação de polarons magnéticos no EuTe pela primeira vez; o raio polarônico foi estimado como R = 3.6a, onde a é o parâmetro de rede e a energia de ligação desse polaron foi estimada em \'E IND. p\' = 45 meV, um resultado que foi confirmado através de medidas do deslocamento da linha zero-fônon em função da temperatura. Adicionalmente procurou-se identificar o estado eletrônico associado à emissão \'MX IND. 0\': a partir de medidas da intensidade da fotoluminescência em função da potência de excitação foi possível sugerir que a emissão \'MX IND. 0\' provem de estados eletrônicos ligados a defeitos da rede e foi possível estimar a concentração desses defeitos como menor que 0.1 ppm. / Investigation of optical properties and their relation to magnetic properties of semiconductors is of great interest to scientific community, due to the large demand for new technologies and features that can arise from these studies. Europium chalcogenides are intrinsically magnetic semiconductors, transparent in the visible region of electromagnetic spectrum and integrable into silicon and gallium nitride matrices, beeing strong candidates for technological applications involving magnetism and optics. The present study investigates absorption and photoluminescence spectra of europium chalcogenides, based on the 4f -> 5d(t2g) model of the electric dipole optical transition, which proved to be entirely appropriate to describe polarized optical absorption in europium chalcogenides as a function of magnetic field, explaining the presence of narrow dichroic lines at high fields and the broad shape of the zero-field absorption spectrum. However, in photoluminescence spectra of EuTe, electronic states not covered by the 4f -> 5d(t2g) model were detected, in particular an emission band labeled MX0, which is coupled to vibrational modes of the lattice. A transition without production of phonons, corresponding to a zero-phonon line, could be well resolved and from the displacement of the zero-phonon line as a function of magnetic field the formation of magnetic polarons in EuTe could be detected unambiguously for the first time. The polaronic radius is estimated as R = 3:6a, where a is the lattice parameter, and the polaron binding energy is estimated as Ep = 45 meV, a result that was confirmed by measurements of zero-phonon line displacement as a function of temperature. Additionally, we sought to identify the electronic state associated with MX0 emission: from measurements of the photoluminescence intensity as a function of excitation power, it was possible to suggest that MX0 emission comes from an electronic state coupled to lattice defects of low concentration, which we estimate to be of less than 0.1 ppm.

L'objectif principal de ma thèse porte sur les composés à base d'europium, une des terres rares qui est magnétique et qui forme des semiconducteurs magnétiques. Le but premier était de mesurer les corrélations magnétiques dans l'EuB6 à l'aide de la technique diffraction de neutrons à petits angles SANS (small angle neutron scattering en anglais), plus précisément de mesurer la longueur de corrélation des polarons magnétiques. La raison de sonder les polarons magnétiques dans l'EuB6 est que leur présence pourrait expliquer la grande magnétorésistance proche de la transition Curie associée avec l'ordre ferromagnétique. Ceci est une tâche particulièrement difficile puisque l'europium est un très grand absorbeur de neutrons, affectant donc la durée d'acquisition. De longs temps d'exposition étaient nécessaires pour obtenir un bruit de fond adéquat. Suite à l'analyse des données, nous avons pu conclure que les polarons magnétiques sont définitivement présents. De plus, leur présence augmente de façon non négligeable les fluctuations magnétiques. Par contre, la présence de ces fluctuations magnétiques rend la tâche de mesurer la longueur de corrélation plus difficile. La plus grande découverte de mon doctorat a été la phase nématique dans le EuB6 grâce à des mesures de magnétorésistance en fonction de l'angle. Ceci se manifestait avec une brisure de symétrie du cristal seulement dans les propriétés électroniques. Ces données m'ont permis de mieux comprendre le rôle que jouent les polarons magnétiques dans ce système. En dopant le système au calcium, nous avons confirmé la présence d'une transition vers un ordre de verre de spins à partir d'une concentration de 30% de calcium. Ce composé semble posséder la même phase nématique que le EuB6. Toutefois, cette phase est bien plus concentrée autour de la transition à cause du manque de fluctuations magnétiques au-dessus de celle-ci. / The main objective of my thesis is about Europium, a magnetic rare earth, based compounds which produces magnetic semiconductors. The primary goal was to measure magnetic correlations in the EuB6 using SANS (small angle neutron scattering) technique, more precisely, to measure the correlation length of magnetic polarons. The raison for studying magnetic polarons in EuB6 is that their presence can explain the large magnetoresistance near the Curie transition associated to a ferromagnetic order. This is a particularly difficult task since Europium (Eu2+) is a very strong neutron absorber, thus affecting the acquisition time. Long exposure times were necessary to obtain adequate background. After the analysis of the data, we have finally been able to conclude that magnetic polarons are definitely present. In addition, their presence increases significantly magnetic fluctuations. On the other hand, the presence of these magnetic fluctuations makes the task of measuring the correlation length more difficult. The biggest discovery of my Ph.D. was the nematic phase in the EuB6 using angle-based magneto-resistance measurements. The nematic phase is caracterized by a breaking of symmetry only in the electronic properties. These data have allowed me to better understand the role played by magnetic polarons in this system. By doping the system with calcium, we confirmed the presence of a transition to a spin glass order from a concentration of 30% calcium. This compound seems to have the same nematic phase as its parent compound. However, this phase is much more concentrated around the spin glass transition because of lack of magnetic fluctuations above it.