Dans cette thèse, nous avons étudié la dynamique d'aimantation selon deux échelles de temps en utilisant la technique pompe-sonde magnéto-optique résolue en temps. A l'échelle de la picoseconde, la précession de l'aimantation est induite par des impulsions acoustiques dans des structures multicouches composées de deux couches ferromagnétique séparées par une couche métallique (Ni/Au/Py) avec différentes épaisseurs. La synchronisation de la précession des couches ferromagnétiques couplées a été observée. La modification de la précession de l'aimantation d'une couche de Ni est due l'interaction d'échange intercouche avec la couche Py. A l'échelle de 50fs, nous avons étudié la dynamique magnéto-optique cohérente, athermale, thermale et la relaxation des charges et des spins dans (Ni, Co et Fe) par impulsions de 11 fs dans un régime de faible perturbation. L'interaction spin-orbite et l'interaction d'échange jouent un rôle significatif dans la désaimantation ultrarapide. / In this thesis, we have investigated the magnetization dynamics at picosecond and femtosecond time scale using time resolved magneto-optical pump probe technique. At picosecond time scale, the magnetization precession is induced by ultrafast acoustic pulses in a three layered structure with two ferromagnetic layers separated by varying thickness of metallic spacer layer (Ni/Au/Py). The magnetization precession dynamics of the Ni layer is modified due to the interlayer exchange interaction with the Py layer and the synchronized precession of the coupied ferromagnetic layers has been observed. At the timescale of 50fs, coherent magneto-optical, non-thermal, thermal and relaxation dynamics of charges and spins in ferromagnetic transition metals (Ni, Co and Fe) is studied by using 11fs optical pulses in a very low perturbation regime. The spin orbit interaction and exchange interaction play a significant role in the demagnetization of the ferromagnetic metals induced by femtosecond pulses.

Doctor of Philosophy / Department of Physics / B.D. DePaola / In recent years, coherent excitation techniques have focused on the ability to efficiently prepare atomic or molecular systems into a selected state. Such population control plays a key role in cutting-edge research taking place today, such as in the areas of quantum information and laser-controlled chemical reactions. Stimulated Raman adiabatic passage (STIRAP) is a widely-used coherent excitation technique that provides a relatively robust control mechanism for efficiently exciting a target population into a desired state. While the technique is well proven, current experimental techniques yield little information on the population dynamics taking place throughout the excitation process, and experimentalists rely solely on final excited-state measurements to determine the efficiency of population transfer. This dissertation presents a unique diagnostic tool to measure multilevel coherent population transfer on a short (nanosecond) timescale. The technique described here uses magneto-optical trap recoil ion momentum spectroscopy (MOTRIMS) as a noninvasive probe of a coherently-controlled system. It provides extremely detailed information about the excitation process, and highlights some important characteristics seen in excited populations that would otherwise be misleading or completely overlooked if one were to use more traditional diagnostic techniques. This dissertation discusses both the theoretical and experimental results applied to three-level coherently excited target populations of Rb-87.

La communication quantique vise la génération, la distribution et le stockage de qubits afin d'établir de véritables réseaux quantiques. Le stockage cohérent, efficace et réversible d'états photoniques dans des mémoires atomiques est donc nécessaire et représente actuellement un enjeu majeur de la science de l'information quantique. Ainsi, de nombreux supports de stockage, tels que les ensembles d'atomes froids ou à l'état solide, sont envisagés afin de satisfaire au mieux les propriétés attendues d'une mémoire quantique. Les travaux présentés dans ce manuscrit s'inscrivent dans ce contexte et décrivent la réalisation expérimentale d'une mémoire basée sur le protocole DLCZ dans un ensemble d'atomes froids de 87Rb. Un dispositif de double piège magnéto-optique permet de refroidir et de confiner cet ensemble au sein d'un piège dont le temps de vie est ~15 s, et de le manipuler en vue du stockage quantique. Nous disposons ainsi d'un nuage présentant une épaisseur optique à résonance de l'ordre de 5, et dont les atomes sont refroidis à une dizaine de µK. La mise en place du protocole DLCZ dans cet ensemble atomique consiste à créer des états cohérents de la matière puis à les relire, à partir de diffusions Raman qui s'accompagnent de la génération de photons uniques corrélés en impulsion. Les premiers résultats obtenus montrent des corrélations non-classiques, affichant une violation forte de l'inégalité de Cauchy-Schwarz, pour une efficacité de lecture de l'ordre de 4% et un temps de cohérence de l'état stocké de ~800 ns. Cette mémoire, utilisée comme une source de photons uniques annoncés, fait partie d'un projet pour lequel une interface basée sur de l'optique non-linéaire / Quantum communication aims at generating, distributing and storing qubits between distant locations, in view of implementing actual quantum networks. Coherent, efficient and reversible storage of photonic states in atomic memories is thus necessary and represents a major challenge in quantum information science. Several storage medium, such as cold atomic or solid-state ensembles, are considered so as to satisfy at best the different benchmarks of a quantum memory. In this context, the work presented in this manuscript describes the experimental realization of a memory based on the DLCZ protocol in cold atomic ensemble of 87Rb. A double magneto-optical trap system allows cooling and confining this ensemble within a trap showing a lifetime of 15 s, and to manipulate it for quantum storage. This cloud shows a resonant optical thickness of about 5, and atoms are cooled down to 10 µK. The implementation of the DLCZ protocol in this atomic ensemble consists in creating coherent states of matter and then to read them, using Raman scattering events which come along with the generation of pairs of single photons correlated in momentum. First results show non-classical correlations, which exhibit a strong violation of the Cauchy-Schwarz inequality, with a read-out efficiency of about $4\%$ and a coherence time of the stored state on the order of 800 ns. This memory, used as a heralded single photon source, is part of a project in which an interface based on non-linear guided wave optics has been built and caracterized so as to convert the 795 nm single photons generated by the memory to the telecom wavelength of 1560 nm. Both elements, combined with a entangled photon source withi

This thesis is divided into three main sections that deal with optical and magnetic thin films properties and their measurements techniques. Principles of the spectroscopic reflectometry and measurements of optical properties are described in the first part. Results of imaging reflectometry are most important. This technique is based on in situ monitoring of optical properties of SiO2 thin films during etching over the area cca 10 × 13 mm2. In next section magnetic properties of thin films and new apparatus built on the Institute of Physical Engineering of BUT are shown. Magnetic properties were observed by longitudinal magneto-optical Kerr effect. The construction of the device is based on a light beam with rectilinear polarization reflected from magnetic material with turned polarization. For investigation of local magnetic properties of microstructures a microscope objective focusing laser beam on the sample is used. The last part of the thesis is aimed on improving of a spin valve structure Co/Cu/NiFe. This work was done within the frame of the Erasmus project in Laboratoire Louis Néel in Grenoble. The goal was to achieve the value of GMR (Giant Magnetoresistance) as high as possible by changing of deposition parameters. This value describes the rate of resistances in different mutual directions of magnetization in trilayers.

Ce travail de doctorat porte sur la croissance par ablation laser pulsée de films ultrafins de Grenat de Fer et d’Yttrium dopés au Bismuth (BiYIG). Ces films d’épaisseur nanométriques sont caractérisés puis utilisés pour des applications magnon-spintroniques. Cette thèse englobe deux thématiques différentes de la physique : la science des matériaux et les applications magnon-spintroniques.La motivation de cette thèse repose sur le besoin, venant de la communauté magnon-spintronique, d’un nouveau matériau magnétique ultrafin à anisotropie ajustable. En effet, au court des dernières années, une avancée majeure dans le domaine a été l’obtention d’auto-oscillations magnétiques induites par un courant de charge dans un isolant magnétique. Ce résultat a été rendu possible grâce à l’utilisation d’un film ultrafin (20 nm) de Grenat de Fer et d’Yttrium (YIG) possédant de très faibles pertes magnétiques. Ces films ultrafins de YIG sont également intéressants pour la magnonique puisqu’il est aussi possible d’y propager et de manipuler des ondes de spin sur de grandes distances. Cependant, la direction facile d’aimantation dans ces films est fixée par l’anisotropie de forme et n’est pas un paramètre ajustable. Pour pousser plus loin les possibilités dans le domaine de la magnon-spintronique un matériau ultrafin, présentant des pertes magnétiques similaires au YIG, dans lequel il serait possible de stabiliser une anisotropie perpendiculaire serait désirable.La croissance par épitaxie en phase liquide de films de YIG substitués de plusieurs microns d’épaisseur a permis de mettre en évidence que l’anisotropie magnétique pouvait être modifiée par dopage. Notamment que la substitution des atomes d’Yttrium par les atomes de Bismuth sur les sites atomiques dodécaédriques permet d’obtenir une direction facile d’aimantation hors du plan, le BiYIG est également reconnu pour sa forte activité magnéto-optique. Cette thèse présente la croissance par ablation laser pulsée de films ultrafins (7 à 50 nm d’épaisseur) de BiYIG. Dans ces films l’anisotropie magnétique a deux origines : l’anisotropie de croissance et l’anisotropie de contrainte. Dans ces films grâce à la contrainte les deux types anisotropies magnétique (planaire ou perpendiculaire) peuvent être obtenues. La caractérisation dynamique des films montre que la substitution d’Yttrium par le Bismuth n’augmente pas les pertes magnétiques et que l’amortissement de Gilbert dans le BiYIG est comparable à celui du YIG. De plus l’augmentation de l’activité magnéto optique du BiYIG par rapport à celle du YIG rend ce nouveau matériau très intéressant pour des techniques expérimentales impliquant l’interaction lumière/ moment magnétique (BLS, Kerr microscope…).Pour observer des phénomènes spintronique nous avons déposé une couche de Pt. Des mesures de transport comme la magnetoresistance Hall de spin, l’effet Hall de spin inverse ou l’effet Hall anormal témoignent d’un transfert de courant de spin a l’interface BiYIG-Pt. Grâce à l’anisotropie perpendiculaire, il est également possible d’observer de nouveaux phénomènes comme la génération d’onde de spin cohérent à partir d’auto-oscillations. Ce nouvel isolant magnétique combinant une faible épaisseur, un faible amortissement magnétique et une anisotropie magnétique modifiable est donc un matériau prometteur pour des applications magnon-spintroniques et ouvre de nouvelles possibilités pour le domaine. / This PhD work focuses on the Pulsed Laser Deposition (PLD) growth of Bismuth doped Iron Garnet nanometer thick films. Those films are charcterised and used for magnon-spintronics applications. This PhD has two main focuses : material science and magnon-spintronics applications.The aim of this PhD is to fill up the need in the magnon-spintronics community of an ultrathin magnetic material combining low magnetic losses and tunable magnetic anisotropy. Indeed the recent breakthrough in the domain was the ability of generating magnetic auto-oscillations from a charge current in a magnetic insulator. This result has been obtained by using an 20 nm thick film of Yttrium Iron Garnet (YIG) with low magnetic losses (α=2⋅〖10〗^(-4) ). Those ultrafin films of YIG can also be used for spin waves propagation over micrometeter distances. However the easy magnetic axis in those films is set to in plane due to the shape anisotropy and it is not a tunable parameter. To go further in terms of magnon-spintronics applications a perpendicularly easy magnetized low losses ultra-thin magnetic material would be desirable. Liquid Phase Epitaxy growth of micrometer thick doped YIG during the 70’s evidenced that the magnetic anisotropy could be modified by doping or substitution. Especially the substitution of Yttrium atoms by Bismuth ones on the dodecaedric atomic sites allows to stabilise out of plane magnetic anisotropy. Morevover the BiYIG is also known to posses high magneto optical activity.This PhD presents the growth by Pulsed Laser Deposition of ultrathin BiYIG films (7 to 50 nm thick). In those films the uniaxial magnetic anisotropy has two main origins : the magneto elastic and the growth induced anisotropy. Using the strain in those films it is possible to obtain both out of plane and in plane magnetic anisotropy. The dynamical characterisation shows that magnetic losses in the perpendicular easy magnetized films are comparable to the one of YIG ultrathin films. The high magneto optical activity in those films makes the BiYIG ultrathin films suitable for ligth based detection technics involving ligth/magnetism interaction. By sputtering a Pt sublayer on the top of BiYIG ultra thin films we could observ different spintronic phenomena evidencing the transfer of spin current from the metal to the insulator. Low losses and nanometer thickness in perpendicularly easy magnetized BiYIG films allow to observ current induced magnetic auto oscillation in the same fashion as what was previously done with ultrathin YIG. The perpendicular magnetic anisotropy allows however to couple those auto oscillation to spin waves, which was not possible for in plane magnetized YIG fims. This new phenomena is related to the unique properties of the ultrathin BiYIG.BiYIG ultrathin films are thus opening new perspectives in the magnon spintronic commnutiy due to their low thickness and tunable magnetic anisotropy.

Two groups of magnetic oxides were investigated in this thesis. Thin films of La2/3Sr1/3MnO3 (LSMO) deposited by pulsed laser deposition (PLD) on SrTiO3 (STO) substrates were characterized by polar and longitudinal magneto-optical (MO) Kerr spectroscopy. Experimental results were compared to theoretical calculations based on the transfer matrix formalism. A very good agreement between experimental and theoretical data revealed high magnetic ordering down to 5 nm of film thickness as well as a mechanism of suppression of double exchange interaction near the LSMO/STO interface. Magnetically doped Ce1-xCoxO2-δ films deposited by PLD on MgO (x = 0.05 and 0.10) and oxidized Si (x = 0.20) substrates were studied by combination of spectroscopic ellipsometry and MO Faraday and Kerr spectroscopy. Both diagonal and off-diagonal permittivity tensor components were obtained and verified by theoretical calculations confronted with experimental data. Diagonal spectra revealed two optical transitions from oxygen to cerium states. Off-diagonal spectra revealed two paramagnetic transitions involving cobalt ions. An essential influence of cobalt doping on the resulting ferromagnetic properties of CeO2 was observed.

Two important mechanisms in preparation of ultrathin films of magnetic oxides were systematically investigated in this work. First, influence of epitaxial strain on resulting magneto-optical properties of La2/3Sr1/3MnO3 (LSMO) ultrathin films was studied. The investigated films were grown by pulsed laser deposition on four different substrates, providing a broad range of induced epitaxial strains. Magnetic properties were found to deteriorate with increasing value of the epitaxial strain, as expected due to the unit cell distortion increasingly deviating from the bulk and effect of the magnetically inert layer. A combination of spectroscopic ellipsometry and magneto-optical Kerr effect spectroscopy was used to determine spectra of the diagonal and off-diagonal elements of permittivity tensor. The off-diagonal elements confirmed presence of two previously reported electronic transitions in spectra of all films. Moreover, they revealed another electronic transition around 4.3 eV only in spectra of films grown under compressive strain. We proposed classification of this transition as crystal field paramagnetic Mn t2g → eg transition, which was further supported by ab initio calculations. A key role of strain in controlling electronic structure of ultrathin perovskite films was demonstrated. Dynamic application of...

This diploma thesis studies magneto-optical (MO) response of epitaxial thin films of Co-doped ceria. Thin films were characterized by XPS, LEED, STM, spectroscopic ellipsometry and measurement of MO activity. The work focuses on studying MO response of the films depending on film thickness, cobalt concentration, oxidation state of cerium and chemical state of cobalt. Spectra of MO response consist of low energy region where the MO activity is mediated by transitions from defect induced states to conduction band and high energy region where a peak of MO activity appears which we attribute to transitions from valence band to conduction band. In this work we qualitatively explain the effects of the physico- chemical states of the thin films on the structure of the obtained MO spectra, mainly on the appearance of the MO activity in the low energy region, and on the changes of the position of the MO peak. Compared to other preparation methods the epitaxial thin films allow achieving a shift of the MO peak in the direction of higher photon energy.

Title: Optical and magneto-optical studies of ferrimagnetic garnets for photonic and spintronic applications Author: RNDr. Lukáš Beran Department: Intitute of Physics of Charles University Supervisor: RNDr. Martin Veis, PhD., Institute of Physics of Charles University Abstract: This doctoral thesis is devoted to fabrication and systematic char- acterization of physical properties of thin films of iron garnets with potential applications in photonic and spintronic devices. Investigated samples were pre- pared by metallo-organic decomposition and pulsed laser deposition. The study was focused on structural and magnetic characterizaiton along with optical and magneto-optical properties. Obtained experimental results were further con- fronted with theoretical calculations. The application potencial of garnets for photonic devices was discussed based on determined Figure of Merit (Faraday rotation to optical loss ratio). High values were achieved for single crystal thin film of Ce doped yttrium iron garnet on galium gadolinium garnet substrate as well as for pollycrystalline Bi doped yttrium iron garned on silicon substrate. Furthermore, new rare-earth garnets were prepared with attempt to achieve per- pendicular magnetic anisotropy of these film. This was achieved for three di erent materials, which were not...

Deux mécanismes importants reliant la préparation des couches ultraminces d’oxydes magnétiques à leurs propriétés physiques ont été étudiés dans ce travail. En premier lieu, l’influence de la contrainte épitaxiale sur les propriétés magnéto-optiques de la manganite La₂/₃Sr₁/₃MnO₃ (LSMO) a été étudiée. Les couches ultraminces ont été déposées par ablation laser pulsé sur quatre substrats différents, ce qui a fourni différentes valeurs statiques de la contrainte épitaxiale. Les propriétés magnétiques ont été révélées comme se détériorant avec l’augmentation de la contrainte, ce qui était prévisible à cause de la distorsion grandissante de la maille unitaire ainsi qu’à cause de l’effet de la couche magnétiquement inerte. La combinaison de l’ellipsométrie spectroscopique et de la spectroscopie Kerr magnéto-optique a été utilisée afin de déterminer les spectres des éléments diagonaux et non diagonaux du tenseur de permittivité. L’étude des éléments non-diagonaux a confirmé la présence déjà rapportée de deux transitions électroniques dans les spectres de toutes les couches. De plus, elle a révélé une autre transition électronique autour de l’énergie de 4.3 eV, mais seulement dans les spectres des couches déposées avec une contrainte compressive. Nous avons proposé la classification de cette transition comme une transition paramagnétique du champ cristallin Mn t2g → eg. Cette classification a été confortée par des calculs ab initio. Nous avons ainsi montré le rôle clé de la contrainte dans le contrôle des propriétés magnéto-optiques des couches pérovskites ultraminces. En revanche, l’application dynamique de la contrainte par l’utilisation d’une sous-couche piézoélectrique est restée peu concluante. Le transfert de la contrainte entre la sous-couche piézoélectrique et la couche LSMO nécessite des améliorations ultérieures. En second lieu, l’influence de la désorientation du substrat a été étudiée par rapport à la dynamique de l’aimantation dans l’oxyde SrRuO₃ (SRO). Comme attendu, nous avons trouvé qu’un grand angle de désorientation mène à la suppression de la croissance de plusieurs variants cristallographiques du SRO. Au moyen de la microscopie à force magnétique, nous avons montré que la présence de plusieurs variants de SRO mène à l’augmentation de la densité de défauts agissant comme points d’ancrage ou de nucléation pour les domaines magnétiques. Nous avons donc montré que l’emploi d’un substrat vicinal est important pour la fabrication des couches ultraminces de SRO de haute qualité, avec une faible densité de défauts cristallographiques et d’excellentes propriétés magnétiques. / Two important mechanisms in preparation of ultrathin films of magnetic oxides were systematically investigated in this work. First, influence of epitaxial strain on resulting magneto-optical properties of La₂/₃Sr₁/₃MnO₃ (LSMO) ultrathin films was studied. The investigated films were grown by pulsed laser deposition on four different substrates, providing a broad range of induced epitaxial strains. Magnetic properties were found to deteriorate with increasing value of the epitaxial strain, as expected due to the unit cell distortion increasingly deviating from the bulk and effect of the magnetically inert layer. A combination of spectroscopic ellipsometry and magneto-optical Kerr effect spectroscopy was used to determine spectra of the diagonal and off-diagonal elements of permittivity tensor. The off-diagonal elements confirmed presence of two previously reported electronic transitions in spectra of all films. Moreover, they revealed another electronic transition around 4.3 eV only in spectra of films grown under compressive strain. We proposed classification of this transition as crystal field paramagnetic Mn t2g → eg transition, which was further supported by ab initio calculations. A key role of strain in controlling electronic structure of ultrathin perovskite films was demonstrated. Dynamic application of strain via use of piezoelectric underlayer remained inconclusive, requiring further improvement of the strain transfer from the piezoelectric layer into the LSMO. Second, influence of substrate miscut on magnetization dynamics in SrRuO₃ (SRO) was studied. As expected we found that high miscut angle leads to suppression of multi-variant growth. By means of magnetic force microscopy we showed that presence of multiple SRO variants leads to higher density of defects acting as pinning or nucleation sites for the magnetic domains, which consequently results in deterioration of magnetic properties. We demonstrated that use of vicinal substrate with high miscut angle is important for fabrication of high quality SRO ultrathin films with low density of crystallographic defects and excellent magnetic properties.