Magnetism of isolated Mn12 single-molecule magnets detected by magnetic circular dichroism: Observation of spin tunneling with a magneto-optical technique

We report magnetic and magneto-optical measurements of two Mn12 single-molecule magnet derivatives isolated in organic glasses. Field-dependent magnetic circular dichroism (MCD) intensity curves (hysteresis cycles) are found to be essentially identical to superconducting quantum interference device magnetization results and provide experimental evidence for the potential of the optical technique for magnetic characterization. Optical observation of magnetic tunneling has been achieved by studying the decay of the MCD signal at weak applied magnetic field

Blue luminescence at room temperature in defective MgO films

Luminescence spectroscopy has been used to characterize MgO films prepared by rf-sputtering. A clear correlation is found between the appearance of an emission peak centered at approximately 460 nm and the detection of ferromagnetic ordering in the samples. We suggest that cationic vacancies are responsible for the blue-light emission by introducing p states into the electronic band-gap. In accordance with this, our results strongly indicate that cationic vacancies are at the heart of the appearance of long-range magnetic ordering in MgO films.

Magnetism of isolated Mn12 single-molecule magnets detected by magnetic circular dichroism: Observation of spin tunneling with a magneto-optical technique

We report magnetic and magneto-optical measurements of two Mn12 single-molecule magnet derivatives isolated in organic glasses. Field-dependent magnetic circular dichroism (MCD) intensity curves (hysteresis cycles) are found to be essentially identical to superconducting quantum interference device magnetization results and provide experimental evidence for the potential of the optical technique for magnetic characterization. Optical observation of magnetic tunneling has been achieved by studying the decay of the MCD signal at weak applied magnetic field

Controlling the spin of metal atoms adsorbed on oxide surfaces: Ni on regular and defective sites of the MgO(001) surface

We have analyzed the relative energy of nonmagnetic and magnetic low-lying electronic states of Ni atoms adsorbed on regular and defective sites of the MgO(001) surface. To this end cluster and periodic surface models are used within density functional theory. For Ni atoms adsorbed on oxygen vacancies at low coverage, the interaction energy between the metal and the support is much larger than on regular sites. Strong bonding results in a diamagnetic adsorbed species and the energy required to reach the high-spin state increases. Moreover, a correlation appears between the low-spin to high-spin energy difference and the interaction energy hypothesizing that it is possible to prepare the surface to tune the high-spin to low-spin energy difference. Magnetic properties of adsorbed thin films obtained upon increasing coverage are more difficult to interpret. This is because the metallic bond is readily formed and dominates over the effect of the atoms directly bound to the vacancy.

Ferromagnetism in transparent thin films of MgO

We show both theoretical and experimental evidences of the appearance of ferromagnetism in MgO thin films. First-principles calculations allow predicting the possibility of the formation of a local moment in MgO, provided the existence of Mg vacancies which create holes on acceptor levels near the O 2p-dominated valence band. Magnetic measurements evidence of the existence of room-temperature ferromagnetism in MgO thin films. High-resolution transmission electron microscopy demonstrates the existence of cation vacancies in our samples. Finally, by applying the element specificity of the x-ray magnetic circular dichroism technique, we also demonstrate that the magnetic moments of the system arise from the spin polarization of the 2p electrons of oxygen atoms surrounding Mg vacancies.

Études de l’effet tunnel des spins quantiques macroscopiques

Dans cette thèse, nous présentons quelques analyses théoriques récentes ainsi que des observations expérimentales de l’effet tunnel quantique macroscopique et des tran- sitions de phase classique-quantique dans le taux d’échappement des systèmes de spins élevés. Nous considérons les systèmes de spin biaxial et ferromagnétiques. Grâce à l’approche de l’intégral de chemin utilisant les états cohérents de spin exprimés dans le système de coordonnées, nous calculons l’interférence des phases quantiques et leur distribution énergétique. Nous présentons une exposition claire de l’effet tunnel dans les systèmes antiferromagnétiques en présence d’un couplage d’échange dimère et d’une anisotropie le long de l’axe de magnétisation aisé. Nous obtenons l’énergie et la fonc- tion d’onde de l’état fondamentale ainsi que le premier état excité pour les systèmes de spins entiers et demi-entiers impairs. Nos résultats sont confirmés par un calcul utilisant la théorie des perturbations à grand ordre et avec la méthode de l’intégral de chemin qui est indépendant du système de coordonnées. Nous présentons aussi une explica- tion claire de la méthode du potentiel effectif, qui nous laisse faire une application d’un système de spin quantique vers un problème de mécanique quantique d’une particule. Nous utilisons cette méthode pour analyser nos modèles, mais avec la contrainte d’un champ magnétique externe ajouté. La méthode nous permet de considérer les transitions classiques-quantique dans le taux d’échappement dans ces systèmes. Nous obtenons le diagramme de phases ainsi que les températures critiques du passage entre les deux régimes. Nous étendons notre analyse à une chaine de spins d’Heisenberg antiferro- magnétique avec une anisotropie le long d’un axe pour N sites, prenant des conditions frontière périodiques. Pour N paire, nous montrons que l’état fondamental est non- dégénéré et donné par la superposition des deux états de Néel. Pour N impair, l’état de Néel contient un soliton, et, car la position du soliton est indéterminée, l’état fondamen- tal est N fois dégénéré. Dans la limite perturbative pour l’interaction d’Heisenberg, les fluctuations quantiques lèvent la dégénérescence et les N états se réorganisent dans une bande. Nous montrons qu’à l’ordre 2s, où s est la valeur de chaque spin dans la théorie des perturbations dégénérées, la bande est formée. L’état fondamental est dégénéré pour s entier, mais deux fois dégénéré pour s un demi-entier impair, comme prévu par le théorème de Kramer

Studies on Fluxon Dynamics in Coupled Josephson Junctions

The thesis deals with detailed theoretical analysis of fluxon dynamics in single and in coupled Josephson junctions of different geometries under various internal and external conditions. The main objective of the present work is to investigate the properties of narrow Long Josephson junctions (LJJs) and to discuss the intriguing physics. In this thesis, Josephson junctions of three types of geometries, viz, rectangular, semiannular and quarter annular geometries in single and coupled format are studied to implement various fluxon based devices. Studies presented in this thesis reveal that mulistacked junctions are extremely useful in the fabrication of various super conducting electronic devices. The stability of the dynamical mode and therefore the operational stability of the proposed devices depend on parameters such as coupling strength, external magnetic fields, damping parameters etc. Stacked junctions offer a promising way to construct high-TC superconducting electronic components. Exploring the complex dynamics of fluxons in coupled junctions is a challenging and important task for the future experimental and theoretical investigations

Studies on Chaos and Synchronization in ac-driven Josephson junctions

The main goal of this thesis is to study the dynamics of Josephson junction system in the presence of an external rf-biasing.A system of two chaotically synchronized Josephson junction is studied.The change in the dynamics of the system in the presence of at phase difference between the applied fields is considered. Control of chaos is very important from an application point of view. The role Of phase difference in controlling chaos is discussed.An array of three Josephson junctions iS studied for the effect of phase difference on chaos and synchronization and the argument is extended for a system of N Josephson junctions. In the presence of a phase difference between the external fields, the system exhibits periodic behavior with a definite phase relationship between all the three junctions.Itdeals with an array of three Josephson junctions with a time delay in the coupling term. It is observed that only the outer systems synchronize while the middle system remain uncorrelated with t-he other two. The effect of phase difference between the applied fields and time-delay on system dynamics and synchronization is also studied. We study the influence of an applied ac biasing on a serniannular Josephson junction. It is found the magnetic field along with the biasing induces creation and annihilation of fluxons in the junction. The I-V characteristics of the junction is studied by considering the surface loss term also in the model equation. The system is found to exhibit chaotic behavior in the presence of ac biasing.

Coverage effects on the magnetism of Fe/MgO(001) ultrathin films

Different aspects of the structure-magnetism and morphology-magnetism correlation in the ultrathin limit are studied in epitaxial Fe films grown on MgO(001). In the initial stages of growth the presence of substrate steps, intrinsically higher than an Fe atomic layer, prevent the connection between Fe islands and hence the formation of large volume magnetic regions. This is proposed as an explanation to the superparamagnetic nature of ultrathin Fe films grown on MgO in addition to the usually considered islanded, or Vollmer-Weber, growth. Using this model, we explain the observed transition from superparamagnetism to ferromagnetism for Fe coverages above 3 monolayers (ML). However, even though ferromagnetism and magnetocrystalline anisotropy are observed for 4 ML, complete coverage of the MgO substrate by the Fe ultrathin films only occurs around 6 ML as determined by polar Kerr spectra and simulations that consider different coverage situations. In annealed 3.5 ML Fe films, shape or configurational anisotropy dominates the intrinsic magnetocrystalline anisotropy, due to an annealing induced continuous to islanded morphological transition. A small interface anisotropy in thicker films is observed, probably due to dislocations observed at the Fe¿MgO(001) interface.

Spin filtering through ferromagnetic BiMnO3 tunnel barriers

We report on experiments of spin filtering through ultrathin single-crystal layers of the insulating and ferromagnetic oxide BiMnO3 (BMO). The spin polarization of the electrons tunneling from a gold electrode through BMO is analyzed with a counterelectrode of the half-metallic oxide La2/3Sr1/3MnO3 (LSMO). At 3 K we find a 50% change of the tunnel resistances according to whether the magnetizations of BMO and LSMO are parallel or opposite. This effect corresponds to a spin-filtering efficiency of up to 22%. Our results thus show the potential of complex ferromagnetic insulating oxides for spin filtering and injection.

Magnetism of isolated Mn12 single-molecule magnets detected by magnetic circular dichroism: Observation of spin tunneling with a magneto-optical technique

We report magnetic and magneto-optical measurements of two Mn12 single-molecule magnet derivatives isolated in organic glasses. Field-dependent magnetic circular dichroism (MCD) intensity curves (hysteresis cycles) are found to be essentially identical to superconducting quantum interference device magnetization results and provide experimental evidence for the potential of the optical technique for magnetic characterization. Optical observation of magnetic tunneling has been achieved by studying the decay of the MCD signal at weak applied magnetic field

Anisotropia magnética (110) em Nanofilmes de Permalloy sobre MgO(100)

The study and fabrication of nanostructured systems composed of magnetic materials has been an area of great scientific and technological interest. Soft magnetic materials, in particular, have had great importance in the development of magnetic devices. Among such materials we highlight the use of alloys of Ni and Fe, known as Permalloy. We present measurement results of structural characterization and magnetic films in Permalloy (Ni81Fe19), known to be a material with high magnetic permeability, low coercivity and small magneto- crystalline anisotropy, deposited on MgO (100) substrates. The Magnetron Sputtering technique was used to obtain the samples with thicknesses varying between 9 150 nm. The techniques of X- ray Diffraction at high and low angle were employed to confirm the crystallographic orientation and thickness of the films. In order to investigate the magnetic properties of the films the techniques of Vibrant Sample Magnetometry (VSM), Ferromagnetic Resonance (FMR) and Magnetoimpedance were used. The magnetization curves revealed the presence of anisotropy for the films of Py/MgO (100), where it was found that there are three distinct axis - an easy-axis for θH = 0°, a hard-axis for θH = 45° and an intermediate for θH = 90°. The results of the FMR and Magnetoimpedance techniques confirm that there are three distinct axes, that is, there is a type C2 symmetry. Then we propose, for these results, the interpretation of the magnetic anisotropy of Py/MgO ( 100 ) is of type simple C2, ie a cubic magnetic anisotropy type ( 110 )

Crescimento de filmes nanométricos monocristalinos de Fe/MgO(100) por "SPUTTERING" DC

The research behind this master dissertation started with the installation of a DC sputtering system, from its first stage, the adaptation of a refrigerating system, passing by the introduction of a heating system for the chamber using a thermal belt, until the deposition of a series of Fe/MgO(100) single crystal nanometric film samples. The deposition rates of some materials such as Fe, Py and Cu were investigated through an Atomic Force Microscope (AFM). For the single crystal samples, five of them have the same growth parameters and a thickness of 250Å, except for the temperature, which varies from fifty degrees from one to another, from 100ºC to 300ºC. Three other samples also have the same deposition parameters and a temperature of 300ºC, but with thickness of 62,5Å, 150Å, and 250Å. Magneto-optical Kerr Effect (MOKE) of the magnetic curves measurements and Ferromagnetic Resonance (FMR) were made to in order to study the influence of the temperature and thickness on the sample s magnetic properties. In the present dissertation we discuss such techniques, and the experimental results are interpreted using phenomenological models, by simulation, and discussed from a physical point of view, taking into account the system s free magnetic energy terms. The results show the growth of the cubic anisotropy field (Hac) as the sample s deposition temperature increases, presenting an asymptotic behavior, similar to the characteristic charging curve of a capacitor in a RC circuit. A similar behavior was also observed for the Hac due to the increase in the samples thicknesses. The 250˚A sample, growth at 300°C, presented a Hac field close to the Fe bulk value

Propriedades fisicas do monocristal fe/mgo(100) e estudo da expansao termica da superficie da ag(100)

In this work we have developed a way to grow Fe/MgO(100) monocrystals by magnetron sputtering DC. We investigated the growing in a temperature range among 100 oC and 300 oC. Structural and magneto-crystalline properties were studied by different experimental techniques. Thickness and surface roughness of the films were investigated by atomic force microscopy, while magneto-crystalline properties were investigated by magneto-optical Kerr effect and ferromagnetic resonance. Our results show that as we increase the deposition temperature, the magneto-crystalline anisotropy of the films also increases, following the equation of Avrami. The best temperature value to make a film is 300 oC. As the main result, we built a base of magnetoresistence devices and as an aplication, we present measurements of Fe/Cr/Fe trilayer coupling. In a second work we investigated the temperature dependence of the first three interlayer spacings of Ag(100) surface using low energy electron diffraction. A linear expansion model of crystal surface was used and the values of Debye temperatures of the first two layers and thermal expansion coefficient were determinated. A relaxation of 1% was found for Ag(100) surface and these results are matched with faces (110) and (111) of the silver. iv

Petrography, magnetic susceptibility and geochemistry of the Rio Branco Granite, Carajás Province, southeast of Pará, Brazil

Petrografia, suscetibilidade magnética e geoquímica do Granito Rio Branco, Província Carajás, sudeste do Pará, Brazil. O Granito Rio Branco é um stock paleoproterozoico intrusivo no biotita-monzogranito arqueano Cruzadão. Ocorre a oeste da cidade de Canaã dos Carajás, nas proximidades da mina de cobre do Sossego na Província Carajás. É constituído por sienogranitos não deformados e isotrópicos, hololeucocráticos, em geral de granulação média. A mineralogia é formada por feldspato alcalino pertítico, quartzo e plagioclásio. A biotita, intensamente cloritizada, é a principal fase máfica, acompanhada por flluorita, allanita, zircão, pirita e calcopirita como minerais acessórios. Albitização e, com menor intensidade greisenização, afetaram o granito, sendo a mineralogia secundária albita, fluorita, topázio, clorita, muscovita, siderofilita e óxidos e/ou hidróxidos de ferro. O Granito Rio Branco apresenta valores sistematicamente baixos de suscetibilidade magnética (SM) variando de 1,3 x 10^-5 a 6,96 x 10^-4 (SI). Geoquimicamente, é metaluminoso a peraluminoso, possui altas razões FeOt/(FeOt + MgO) e mostra afinidades com granitos ferrosos, tipo-A do subtipo A2. Os padrões dos ETR revelam um ligeiro enriquecimento de ETR leves em relação ao ETR pesados e anomalia negativa acentuada de Eu (Eu/Eu* = 0,08 - 0,13), resultando feição em "gaivota", característica de granitos evoluídos. O conjunto de dados obtidos demonstra o caráter evoluído do Granito Rio Branco e sua derivação a partir de líquidos reduzidos e enriquecidos em voláteis, causadores das transformações hidrotermais tardias. O estudo comparativo deste corpo com aqueles das suítes anorogênicas da Província Carajás sugere que o Granito Rio Branco possui maior afinidade com os granitos das suítes Velho Guilherme e, em menor grau, Serra dos Carajás. Por outro lado, é claramente distinto da Suíte Jamon. Embora apresente características similares às dos granitos especializados em estanho, não há mineralizações desta natureza associadas ao corpo.