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Orientadores: Carlos Rettori, Pascoal José Giglio Pagliuso / Dissertação (mestrado) - Universidade Estadual de Campinas, Instituto de Física Gleb Wataghin / Made available in DSpace on 2018-08-22T06:56:36Z (GMT). No. of bitstreams: 1 Lesseux_GuilhermeGorgen_M.pdf: 14003739 bytes, checksum: b737fc7f0d847cdc75e895351974e1e2 (MD5) Previous issue date: 2013 / Resumo: Compostos nanoestruturados têm atraído cada vez mais atenção do ponto de vista tecnológico devido às inúmeras possibilidades em termos de aplicação nas mais diversas áreas. Além da motivação em termos de aplicação, o aumento da proporção de átomos na superfície em relação ao volume e a redução da dimensionalidade nestes compostos trazem consigo novas questões em física. Com base nisso, o estudo científico sistemático destas questões é fundamental para o desenvolvimento da nanociência e da nanotecnologia de forma geral. No presente trabalho são estudadas propriedades magnéticas de três tipos de nanopartículas (NPs): i) NPs de Au assistidas por óxidos do tipo R2O3 (R = Er e Y) que exibem propriedades ferromagnéticas; ii) NPs metálicas, Au e Ag, com a impureza magnética Er3+ diluída permitindo assim a sondagem microscópica de propriedades físicas por Ressonância de Spin Eletrônico; iii) E, por fim, NPs de NaYF4 mono e codopadas com os íons de terras raras RE = Yb3+, Er3+ e Tm3+ nas quais foi possível verificar o fenômeno de upconversion. Com base em adaptação de métodos estabelecidos na literatura, [1_3] foi desenvolvida uma rota química para a obtenção de NPs de Au com propriedades ferromagnéticas acentuadas pela incorporação de óxidos. A partir da magnetização de saturação em 2 K e baseado em uma análise termogravimétrica (TGA) estimou-se um momento magnético efetivo de aproximadamente 0.2 µB por átomos de Au na superfície das NPs. Além da caracterização magnetometrica típica, observou-se uma linha intensa de ESR em banda-X desde 370 K até 4.2 K. Esta ressonância possui intensidade praticamente constante caracterizando a ressonância observada como ferromagnética (FMR). Estes resultados são interpretados com base na ligação entre a capa orgânica (capping), o óxido R2O3 e os átomos de Au gerando uma hibridização efetiva dos orbitais 5d-6s dos elétrons do Au. Esta hibridização seria, então, responsável por tornar a camada 5d do Au magnética devido a spins não compensados nos orbitais 5d. As NPs metálicas com impurezas de Er3+ foram obtidas por uma variação do método utilizado para as NPs de Au ferromagnéticas. Os valores de g e as estruturas hiperfinas observadas indicam que o íon Er3+ está em um sítio cúbico tanto nas partículas de Ag como nas de Au. Os espectros de ESR mostram que não há deslocamento de g e relaxação tipo Korringa devido à interação de troca entre os spins do Er3+ e os dos elétrons de condução, sugerindo assim que esta interação de troca não ocorre em NPs metálicas. Por fim, as NPs de NaYF4 dopadas com RE = Yb3+, Er3+ e Tm3+ foram obtidas por um método estabelecido na literatura. [4, 5] A incorporação, o estado de oxidação e a concentração dos íons magnéticos Er3+ e Yb3+ foram confirmados por medidas de magnetização dc e de ESR. Observou-se emissão visível no verde e no azul para amostras codopadas com 20%Yb3+ / 2%Er3+ e 30%Yb3+ / 0.5%Tm3+, respectivamente, devido ao fenômeno conhecido como upconversion / Abstract: Nanostructured compounds have attracted growing attention from the technological point of view due to numerous possibilities in terms of application in several areas. Besides, the large surface/volume atoms ratio and the reduced dimensionality of these nanocompounds raised new fundamental physical issues. Therefore, a detailed and systematic scientific study regarding these phenomena is crucial for the sake of nanoscience and nanotechnology development. In this dissertation, we thoroughly investigated the magnetic properties of three different types of nanoparticles (NPs): i) Au NPs assisted by oxides R2O3 (R = Er and Y) which present unexpected ferromagnetic properties; ii) diluted magnetic Er3+ impurities in Ag and Au NPs, which allow Electron Spin Resonance to study several microscopic local physical properties and, finally, iii) single and co-doped Yb3+, Er3+ and Tm3+ NaYF4 NPs that allowed to verify the up-conversion phenomena in these NPs. After adapting and improving already established methods reported in the literature, [1_3] we developed a novel chemical route to obtain Au-NPs with enhanced ferromagnetic properties by oxide incorporation. Based on the saturation magnetization at 2 K and thermogravimetric analysis (TGA), we estimated an effective magnetic moment of µeff ¿ 0.2 µB per Au atom on the surface of the NPs. Besides the typical magnetometric characterization, we also carried out X-band ESR experiments. An intense ESR line was observed in the range of 4.2K = T = 370K with an integrated signal intensity which is almost constant in the entire T-range. Based on our results, the observed ESR signal is attributed to a ferromagnetic resonance (FMR). These results are discussed in terms of bonds between the NP-capping ligands and the Au atoms, which give rise to an effective hybridization between the 5d-6s electrons at the surface of the AuNPs. This hybridization might be the responsible mechanism for the Au 5d shell to become magnetic due to uncompensated spins in the 5d orbitals. The metallic Er3+ doped Ag and Au NPs were obtained by a slightly modified method used to get the ferromagnetic Au -NPs. The ESR g-values and observed hyperfine splitting indicate a cubic symmetry for the Er3+ ions in the Ag and Au NPs. Furthermore, we observed no g-shift and Korringa relaxation due to the exchange interaction between the magnetic rare-earth impurities and the conduction electron spins. This fact suggests that such an exchange interaction is negligible in metallic NPs. Finally, the Er3+, Yb3+ and Tm3+ doped NaYF4 NPs were obtained by a method already established in the literature. [4, 5] The incorporation of the Er3+ and Yb3+ ions as well as their oxidation state and concentration were confirmed by T-dependent magnetization and ESR measurements. For the co-doped NaYF4 NPs, we observed by naked eye the expected green and blue emitted lights of Yb/Er and Yb/Tm, respectively, due to a phenomenon known as upconversion / Mestrado / Física / Mestre em Física

京都大学 / 0048 / 新制・課程博士 / 博士(理学) / 甲第21554号 / 理博第4461号 / 新制||理||1640(附属図書館) / 京都大学大学院理学研究科物理学・宇宙物理学専攻 / (主査)教授 石田 憲二, 教授 前野 悦輝, 教授 松田 祐司 / 学位規則第4条第1項該当 / Doctor of Science / Kyoto University / DFAM

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Les parois de domaines dans les films ferromagnétiques ultra-minces sont au cœur de nombreux systèmes émergents pour le traitement et le stockage de l’information. L’observation de ces textures d’aimantation reste cependant délicate, notamment en raison des très faibles densités de moments magnétiques mises en jeu dans ces matériaux magnétiques, épais de quelques couches atomiques seulement. Dans cette thèse, nous proposons l’utilisation d’une nouvelle technique d’imagerie magnétique pour étudier les parois de domaines, la microscopie à balayage de centre NV. Cette technique, qui repose sur la mesure du déplacement Zeeman de l’énergie du spin électronique unique d’un centre coloré NV du diamant, combine des caractéristiques sans équivalent, permettant de mesurer le champ magnétique de manière quantitative dans un volume de détection de taille atomique. Le début du manuscrit vise à introduire les parois de domaines magnétiques dans les films ultra-minces, en regard de leurs potentielles applications. Nous dressons ensuite un état de l’art des techniques permettant d’observer ces objets, en soulignant leurs avantages et leurs inconvénients. L’expérience de microscopie magnétique à balayage de centre NV est alors décrite, et nous montrons que ses caractéristiques sont idéales pour l’imagerie des parois de domaines dans les couches ferromagnétiques ultra-minces. Dans la suite du manuscrit nous développons trois exemples en lien avec ces objets, pour lesquels la microscopie à centre NV permet d’apporter des informations nouvelles. Nous commençons par étudier l’interaction des parois avec les défauts du matériau, en observant la dynamique de sauts de Barkhausen thermiquement activés. Nous étudions ensuite le matériau plus en détail, en introduisant une mesure quantitative de la densité de moments magnétiques résolue à des échelles submicroniques. Enfin, nous présentons une méthode permettant de déterminer la structure interne des parois de domaines par la mesure de leur champ magnétique de fuite. Cette méthode est appliquée à diverses couches ferromagnétiques ultra-minces, afin d’étudier l’influence de l’interaction interfaciale de Dzyaloshinskii-Moriya sur la structure de la paroi. L’ensemble des résultats obtenus grâce à la microscopie à balayage de centre NV dans les couches ultra-minces ferromagnétiques démontrent les potentialités de la technique, et ouvrent de nombreuses perspectives quant à l’utilisation de cette nouvelle technique pour les études en nanomagnétisme. / Domain walls in ultra-thin ferromagnetic films are the cornerstones of many emerging devices, for both information processing and data storage. However, observing such magnetization patterns remains challenging, notably because the number of magnetic moments is particularly low in these atomic-thick layer. In this thesis, we propose to use a new imaging technique for studying domain walls, namely the NV centre scanning microscopy. This technique relies on the measurement of the energy shifts caused by the Zeeman effect on the electronic spin of a single NV colour centre in diamond, and combines unequalled characteristics for measuring the magnetic field in a quantitative fashion and with an atomic detection volume. The beginning of the thesis introduces domain walls in ultra-thin ferromagnetic films, in regard to their potential applications. In the following, we depict different techniques at the state of the art for observing these objects, stressing on their advantages and on their drawbacks. The experimental setup of scanning NV microscopy is then described, and we show that is characteristics are ideal for imaging domain walls in ultra-thin ferromagnetic films. The end of the thesis is focused on three problems linked with these objects, for which NV microscopy can bring new insights. Firstly, we begin with studying the interaction between a domain wall and defects by observing the dynamics of thermally activated Barkhausen jumps. Secondly, we study the material more in details, by introducing a new way to measure the magnetic moment density at a submicron scale. Lastly, we describe a method allowing for the determination of the inner structure of a domain wall, through a stray magnetic field measurement. This method is applied to different ultra-thin ferromagnetic layers, in order to study the influence of the interfacial Dzyaloshinskii-Moriya interaction on the domain wall structure. All the results obtained by scanning NV microscopy demonstrate the potentiality of the technique, and open many new perspectives for using this new technique to solve nanomagnetism issues.

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Within the exciting current trend to explore novel low-dimensional systems, the possibility to inject pure spin currents in graphene and other two-dimensional crystals has attracted considerable attention in the past few years. The theoretical prediction of large spin relaxation times and experimentally observed mesoscopic-scale spin diffusion lengths places graphene as a promising base system for future spintronics devices. This is due to the unique characteristics intrinsic to the two-dimensional lattice of carbon atoms forming graphene, such as the lack of nuclear spins and weak spin-orbit coupling of the charge carriers. Interestingly for some spintronic applications, the latter can be chemically and physically engineered, with large induced spin-orbit couplings found in functionalized graphene sheets. Understanding spin injection, spin current and spin dynamics in graphene is of a great interest, both from the fundamental and applied points of view. This thesis presents an experimental study of dynamical generation of spin currents in macroscopic graphene sheets by means of spin pumping from the precessing magnetization of an adjacent ferromagnet. The spin pumping characteristics are studied by means of ferromagnetic resonance (FMR) measurements in Permalloy/graphene (Py/Gr) bilayers. Changes in the FMR linewidth induced by the presence of graphene (when compared to studies with only Py films) correspond to an increase in the Gilbert damping in the ferromagnetic layer (proportional to the FMR linewidth) and interpreted as a consequence of spin pumping at the Py/Gr interface driven by the Py magnetization dynamics (i.e., magnetic induced by the microwave stimulus). FMR experiments are performed on different FM/Gr interfaces, completing a set of studies designed to systematically identify and eliminate damping enhancement arising from processes other than spin pumping. Remarkably, a substantial enhancement of the Gilbert damping observed in Py/Gr strips with graphene protruding a few micrometers from the strip sides is univocally associated to spin pumping at the quasi-onedimensional interface between the Py strip edges and graphene. This increase in the FMR linewidth compares with observations in other bilayer systems, in where thick (thicker than the spin diffusion length) layers of heavy metals with strong spin-orbit coupling are employed as the non-magnetic layer, indicating that spin relaxation in chemically grown graphene must be greatly enhanced in order to account for the losses of angular momentum lost by the ferromagnet. The fundamental implications of the results presented in this thesis point to a non-trivial nature of the spin pumping mechanism owing to the two-dimensionality of the non-magnetic layer (i.e., graphene). In addition, a spintronics device designed to interconvert charge and spin currents has been designed. A high-frequency microwave irradiation lock-in modulation technique is employed to detect the small electrical voltages generated by the inverse spin Hall effect (ISHE). As a proof of principle, a successful spin-charge interconversion in Py/Pt-based devices is experimentally demonstrated in this thesis. The challenges associated with the spin-charge interconversion in twodimensional devices are discussed and systematically addressed, and a potential device geometry for measuring the ISHE in Py/Gr-based systems is provided.

Magnetic nanoparticles and molecules, in particular ferromagnetic noble metal nanoparticles, molecular magnet and single-molecule magnets (SMM), are perfect examples to investigate the role of quantum mechanics at the nanoscale. For example, SMMs are known to reverse their magnetization by quantum tunneling in the absence of thermal excitation and show a number of fundamental quantum mechanical manifestations, such as quantum interference effects. On the other hand, noble metal nanoparticles are found to behave ferromagnetically for diameters below a few nanometers. Some of these manifestations are still intriguing, and novel research approaches are necessary to advance towards a more complete understanding of these exciting nanoscale systems. In particular, the ability to study an isolated individual nanoscale system (i.e just one molecule or nanoparticle) is both challenging technologically and fundamentally essential. It is expected that accessing to the energy landscape of an isolated molecule/nanoparticle will allow unprecedented knowledge of the basic properties that are usually masked by collective phenomena when the systems are found in large ensembles or in their crystal form. Several approaches to this problem are currently under development by a number of research groups. For instance, some groups are developing deposition techniques to create patterned thin films of isolated magnetic nanoparticles and molecular magnets by means of optical lithography, low-energy laser ablation, or pulsed-laser evaporation or specific chemical functionalization of metallic surfaces with special molecular ligands. However, it is still a challenge to access the properties of an individual molecule or nanoparticle within a film or substrate. iv I have studied molecular nanomagnets and ferromagnetic noble metal nanoparticles by means of a novel experimental approach that mixes the chemical functionalization of nano-systems with the use of single-electron transistors (SETs). I have observed the Coulomb-blockade single-electron transport response through magnetic gold nanoparticles and single-molecule magnet. In particular, Coulomb-blockade response of a Mn4-based SET device recorded at 240 mK revealed the appearance of two diamonds (two charge states) with a clear switch between one and the other is indicative of a conformational switching of the molecule between two different states. The excitations inside the diamonds move with magnetic field. The curvature of the excitations and the fact of having them not going down to zero energy for zero magnetic field, indicated the presence of magnetic anisotropy (zero-field splitting) in the molecule. In addition, the high magnetic field slope of the excitations indicates that transitions between charge states differ by a net spin value equal to 9 (|∆S| = 9), as expected from the behavior of Mn4 molecules in their crystalline form. Anticrossings between different excitations are indicative of quantum superpositions of the molecular states, which are observed for the first time in transport measurements through and individual SMM.