No description available.

A new class of electrodes with nanometer-scale contact spacing can be produced at the edge of patterned metal/insulator/metal this film structures. A key challenge is to produce insulator layers with low leakage current and have pristine metal contacts for controlled molecular contacts. Atomic layer deposition of high quality Al2O3 thin films onto Au electrodes was enabled by surface modification with a self-assembled monolayer of -OH groups that react with a monolayer of trimethylaluminum gas source. Ar ion milling was then used to expose the edge of the Au/dielectric/Au structure for molecular electrode contacts. The junctions are characterized by atomic force microscope and tunnel current properties. The Au/self-assembled monolayer/Al2O3/Au tunnel junction, with a very thin oxide insulator layer (15.4 Å), is stable and has a small tunneling current density of about 0.20 ~ 0.75 A/cm2 at 0.5 V. Organometalic cluster molecules were attached to bridge the electrodes. Through tunnel current modeling, low temperature and photo current measurements, molecular current was found to be consistent with direct tunneling through the organic tethers to available states at the metal center. This novel electrode was also used to study the efficiency of organic conducting thin films where the photovoltaic efficiency can be improved when the electrode separation distance is below the exciton diffusion length. Copper (II) phthalocyanine (CuPc) was thermally evaporated between the nano-gap electrodes formed by Au/Al2O3/Au tunnel junctions. A large photocurrent enhancement over 50 times that of bulk CuPc film was observed when the electrode gap distance approached 10 nm. CuPc diffusion length is seen to be 10 nm consistent with literature reports. All devices show diode I-V properties due to a large Schottky barrier contact resistance between the small top Au electrode and the CuPc film. To add another dimension of nm-scale patterning, nanowires can be used as line-of-sight shadowmasks provided that nanowire location and diameter can be controlled. Lateral ZnO nanowires were selectively grown from the edge of a Si/Al2O3/Si multi-layer structure for potential integration into devices utilizing Si processing technology. Microstructural studies demonstrate a 2-step growth process in which the tip region, with a diameter ~ 10 nm, rapidly grew from the Al2O3 surface. Later a base growth with a diameter ~ 22 nm overgrew the existing narrow ZnO nanowire halting further tip growth. Kinetics studies showed surface diffusion on the alumina seed surface determined ZnO nanowire growth rate.

abstract: In this research, our goal was to fabricate Josephson junctions that can be stably processed at 300°C or higher. With the purpose of integrating Josephson junction fabrication with the current semiconductor circuit fabrication process, back-end process temperatures (>350 °C) will be a key for producing large scale junction circuits reliably, which requires the junctions to be more thermally stable than current Nb/Al-AlOx/Nb junctions. Based on thermodynamics, Hf was chosen to produce thermally stable Nb/Hf-HfOx/Nb superconductor tunnel Josephson junctions that can be grown or processed at elevated temperatures. Also elevated synthesis temperatures improve the structural and electrical properties of Nb electrode layers that could potentially improve junction device performance. The refractory nature of Hf, HfO2 and Nb allow for the formation of flat, abrupt and thermally-stable interfaces. But the current Al-based barrier will have problems when using with high-temperature grown and high-quality Nb. So our work is aimed at using Nb grown at elevated temperatures to fabricate thermally stable Josephson tunnel junctions. As a junction barrier metal, Hf was studied and compared with the traditional Al-barrier material. We have proved that Hf-HfOx is a good barrier candidate for high-temperature synthesized Josephson junction. Hf deposited at 500 °C on Nb forms flat and chemically abrupt interfaces. Nb/Hf-HfOx/Nb Josephson junctions were synthesized, fabricated and characterized with different oxidizing conditions. The results of materials characterization and junction electrical measurements are reported and analyzed. We have improved the annealing stability of Nb junctions and also used high-quality Nb grown at 500 °C as the bottom electrode successfully. Adding a buffer layer or multiple oxidation steps improves the annealing stability of Josephson junctions. We also have attempted to use the Atomic Layer Deposition (ALD) method for the growth of Hf oxide as the junction barrier and got tunneling results. / Dissertation/Thesis / Ph.D. Materials Science and Engineering 2013

Conselho Nacional de Desenvolvimento Científico e Tecnológico / Magnetic tunnel junctions (MTJ) ofCoFeB=MgO=CoFeB and multilayers of (CoFeB=MgO)x3 were produced using the technique of magnetron sputtering, where the insulating film was grown in an atmosphere reactive Ar +O. Multilayers were produced on measures of X-ray difraction and magnetization. Junctions for transport measurements. All curves IxV, nonlinear, were measured at room temperature, and adjustments made using the Simmons model for symmetric barrier. Adjustments were made firt for the positive voltages and then to negative voltages, where the height and thickness of the barrier and the effective area of tunneling was always considered free parameters. Since the effective area of tunneling, much smaller than the area produced during deposition,thus indicating the existence of points where the current tunneling through the barrier,due to fluctuations in the thickness of the insulation. The post was seen exponential growth of the resistance multiplied by the effective area of tunneling as a function of thickness, using only the values calculated from the simulation curves IxV. We also observed the curve of conductance versus voltage, for the investigation of oxidation or not the interface between electrode and barrier, showing that almost 100% of samples of the tunnel junctions was low oxidation of the electrode (positive). / Junções túnel magnéticas (MTJ) deCoFeB=MgO=CoFeB e multicamadas deCoFeB=MgO)x3 foram produzidas utilizando a técnica de magnetron sputtering, onde o filme isolante foi crescido em atmosfera reativas, Ar+O. As multicamadas foram produzidas visando medidas de difração de raio-X (XRD) e magnetização. As junções, para medidas de transporte. Todas as curvas IxV, não lineares, foram medidas a temperatura ambiente, e os ajustes realizados utilizando o modelo de Simmons para barreira simétrica. Os ajustes foram realizados primeiro para as tensões positivas e depois para tensões negativas, onde a altura e a espessura da barreira, e a área efetiva de tunelamento foram considerados parâmetros livres sempre. Sendo a área efetiva de tunelamento, muito menor, do que a área produzida durante a deposição, indicando assim a existência de pontos onde a corrente de tunelamento atravessa a barreira, devido a flutuações na espessura do isolante. A posteriori foi verificado o crescimento exponencial da resistência multiplicada pela área efetiva de tunelamento em função da espessura, utilizando somente valores calculados através das simulações das curvas IxV. Também foi verificada a curva de condutância versus a tensão, para a investigação da oxidação ou não da interfase entre eletrodo e barreira, mostrando que quase 100% das amostras das junções túnel ocorreu oxidação do eletrodo de baixo (positivo).

Le sujet de cette thèse concerne la spintronique moléculaire. Des jonctions tunnel magnétiques formées par une barrière tunnel moléculaire (monocouche auto-assemblée) insérée entre deux électrodes métalliques ferromagnétiques ont été étudiées. Afin de fabriquer les dispositifs, un procédé de greffage des molécules sur des substrats ferromagnétiques a été mis en place et une technique de lithographie a été développée pour définir des jonctions de taille submicronique. L’ensemble de ce travail expérimental a permis l’obtention de jonctions non court-circuitées et mesurables, où le transport électronique est bien du transport par effet tunnel.Les mesures de magnétotransport de ces échantillons ont amené des résultats intéressants et nouveaux : les jonctions, dont la barrière est formée par des alcanes-thiols, présentent de la magnétorésistance à température ambiante, allant jusqu’à 12%. Une partie de la thèse s’attelle à la compréhension des différents comportements magnétorésistifs observés : un modèle de barrière tunnel à deux niveaux est proposé pour les décrire.La dernière partie du travail présente des résultats préliminaires obtenus lorsque la barrière moléculaire est formée par des molécules aromatiques ou commutables et met en évidence des phénomènes nouveaux par rapport au cas précédent.L’ensemble des résultats prouve le fonctionnement de jonctions tunnel magnétiques à base de monocouches moléculaires à température ambiante et ouvre la voie à l’utilisation de molécules plus complexes pour une électronique de spin moléculaire multifonctionnelle. / This thesis work enters within the molecular spintronic fields. Magnetic tunnel junctions based on molecular self assembled monolayers have been investigated. The devices structure is a molecular monolayer inserted between two ferromagnetic electrodes.A process to graft molecules on a ferromagnet’s surface and a lithography technique have been developed to define the junctions. This experimental work has led to non short-circuited and measurable junctions, in which an electronic tunnel transport has been demonstrated.Interesting and new results have been found out from magnetoresistance measurement of the samples: junctions made with alkanes-thiols barrier have shown magnetoresistance signal at room temperature (up to 12%). In order to explain the magnetoresistive behaviour, a simple model where the barrier is discribed by two levels has been proposed.The last part of the thesis reports preliminary results obtained when the barrier is made of aromatic molecules or switchable molecules and it points out new phenomenons compared to the alkanes case.The overall work proves that devices made from magnetic tunnel junctions with self-assembled monolayers work at room temperature. It is then possible to consider switchable molecules to build multifunctional molecular spintronics devices.

Nanomagnetic devices are highly energy efficient and non-volatile. Because of these two attributes, they are potential replacements to many currently used information processing technologies, and they have already been implemented in many different applications. This dissertation covers a study of nanomagnetic devices and their applications in various technologies for information processing – from simulating and analyzing the mechanisms behind the operation of the devices, to experimental investigations encompassing magnetic film growth for device components to nanomagnetic device fabrication and measurement of their performance. Theoretical sections of this dissertation include simulation-based modeling of perpendicular magnetic anisotropy magnetic tunnel junctions (p-MTJ) and low energy barrier nanomagnets (LBM) – both important devices for magnetic device-based information processing. First, we propose and analyze a precessionally switched p-MTJ based memory cell where data is written without any on-chip magnetic field that dissipates energy as low as 7.1 fJ. Next, probabilistic (p-) bits implemented with low energy barrier nanomagnets (LBMs) are also analyzed through simulations, and plots show that the probability curves are not affected much by reasonable variations in either thickness or lateral dimensions of the magnetic layers. Experimental sections of this dissertation comprise device fabrication aspects from the basics of material deposition to the application-based demonstration of an extreme sub-wavelength electromagnetic antenna. Magnetic tunnel junctions for memory cells and low barrier nanomagnets for probabilistic computing, in particular, require ultrathin ferromagnetic layers of uniform thickness, and non-uniform growth or variations in layer thickness can cause failures or other problems. Considerable attention was focused on developing methodologies for uniform thin film growth. Lastly, micro- and nano-fabrication methods are used to build an extreme sub-wavelength electromagnetic antenna implemented with an array of magnetostrictive nanomagnets elastically coupled to a piezoelectric substrate. The 50 pW signal measured from the approximately 250,000-nanomagnet antenna sample was 10 dB above the noise floor.

No description available.

Elastic and inelastic interactions are studied in tunnel junctions of a superconducting nanoelectromechanical setup and in response to resent experimental superconducting scanning tunneling microscope findings on a paramagnetic molecule. In addition, the electron density of molecular graphene is modeled by a scattering theory approach in very good agreement with experiment. All studies where conducted through the use of model Hamiltonians and a Green function formalism. The nanoelectromechanical system comprise two fixed superconducting leads in-between which a cantilever suspended superconducting island oscillates in an asymmetric fashion with respect to both fixed leads. The Josephson current is found to modulate the island motion which in turn affects the current, such that parameter regions of periodic, quasi periodic and chaotic behavior arise. Our modeled STM setup reproduces the experimentally obtained spin excitations of the paramagnetic molecule and we show a probable cause for the increased uniaxial anisotropy observed when closing the gap distance of tip and substrate. A wider parameter space is also investigated including effects of external magnetic fields, temperature and transverse anisotropy. Molecular graphene turns out to be well described by our adopted scattering theory, producing results that are in good agreement with experiment. Several point like scattering centers are therefore well suited to describe a continuously decaying potential and effects of impurities are easily calculated.

Les oscillateurs à transfert de spin (STO) sont des oscillateurs nanométriques (~100nm) prometteurs pour les applications radiofréquence. Ils reposent sur la précession de l'aimantation d'une couche magnétique mince induite par transfert de spin (STT). Un dispositif STO basé sur jonction tunnel magnétique (MTJ) fournira typiquement un signal électrique de l'ordre d'une dizaine de GHz et d'une puissance de plusieurs nW. Comparés aux oscillateurs contrôlés en tension (VCO) utilisés actuellement pour la génération de microondes, les STO ont l'avantage d'être hautement accordables en fréquence. Malgré cela, les critères requis en termes de qualité de signal ne sont pas encore remplis par les STO pour être compétitifs.Deux approches existent pour améliorer la qualité du signal de sortie : (i) optimisation de l'empilement magnétique d'un dispositif STO unique et (ii) synchronisation de plusieurs STOs. C'est la deuxième approche qui a été retenue dans le cadre de cette thèse : ici nous nous intéressons à la synchronisation électrique d'un STO à une source de courant RF stabilisée, dit « injection-locking ». Le cas d'un STO à aimantation homogène, de type précession dans le plan (IPP) est étudié.En particulier, la synchronisation d'un STO à 2f, c'est-à-dire lorsque la fréquence du courant injecté est proche du double de la fréquence de génération du STO, est favorisée par rapport à la synchronisation à f. Les résultats expérimentaux obtenus par plusieurs groupes montrent à la fois une gamme de synchronisation et une réduction de largeur de raie plus prononcées à 2f qu'à f.Ce comportement singulier est examiné dans un premier temps par une étude analytique de la dynamique de l'aimantation couplée aux simulations numériques macrospin dans le but d'identifier les mécanismes de synchronisation qui prennent effet au sein du système.En effet, les modèles actuels (formalisme auto-oscillateur KTS) décrivent la synchronisation d'un STO à un courant RF sans faire de distinction entre la synchronisation à f et 2f, et les prédictions qui en découlent s'avèrent être insuffisantes pour la synchronisation à 2f. Pour combler à cela, nous mettons en évidence par extension du formalisme existant les clés du processus de synchronisation à 2f : l'ajustement de fréquence par ajustement de l'amplitude d'oscillation via la non-linéarité, ainsi que la modification du terme d'anti-damping se faisant par l'intermédiaire de la différence de phase.La caractérisation expérimentale du régime synchronisé pour un STO basé sur jonction tunnel magnétique est également détaillée dans le manuscrit. Grâce aux techniques de mesures en domaine temporel et fréquentiel développées spécialement, les grandeurs caractéristiques (gamme de synchronisation et différence de phase) du système sont extraites et comparées aux prédictions théoriques. Enfin, les effets de l'injection du courant RF sur la cohérence du signal de sortie sont discutés. / Spin transfer oscillators (STOs) are promising nanometer scaled oscillators (~100nm) for radiofrequency applications. They rely on the steady precession of the magnetization of a thin magnetic layer induced by spin-transfer torque (STT). A STO device based on a magnetic tunnel junction (MTJ) will typically generate an electrical signal with a frequency of the order of ten GHz and an output power of several nW. Compared to voltage controlled oscillators (VCO) used today for microwave generation, STOs have the advantage of having an important frequency tunability with current. However, criteria in terms of the quality of the output signal are not yet fulfilled for STO to be competitive.To enhance the STO signal properties, two suggestions are proposed: (i) optimization of the magnetic stack within a single STO device and (ii) synchronization of several STOs. The second approach was examined during this thesis: here we look at the electrical synchronization of a STO to a stabilized RF current source, or “injection-locking”. The case of a STO with homogenous magnetization of in-plane precession (IPP) type is investigated.Interestingly, synchronization of a STO at 2f, i.e. when the frequency of the injected current is close to twice the generation frequency of the STO, is favored compared to synchronization at f. The experimental results from several groups have shown both enhanced synchronization range and a more pronounced linewidth reduction at 2f.This singular behavior is examined first through an analytical study of magnetization dynamics along with numerical macrospin simulations, in order to identify synchronization mechanisms taking effect in the system.Indeed, current models (in particular the KTS auto-oscillator formalism) describe synchronization of a STO with making a clear distinction between synchronization at f and 2f, and the resulting predictions turn out to be insufficient at 2f. Here, by extension of the KTS formalism, the keys to the synchronization process at 2f are presented: frequency adjustment by adjustment of the oscillation amplitude via the STO non-linearity and modification of the anti-damping term through the phase-difference.The experimental characterization of the synchronized regime in a MTJ-based STO is also detailed in the manuscript. Utilizing experimental signal processing techniques in both frequency and temporal domain, we extract characteristic quantities for synchronization such as the locking-range and the phase-difference, and we compare these quantities with the analytical predictions. Finally, the effects of current injection on the coherence of the output signal are also discussed.

Conselho Nacional de Desenvolvimento Científico e Tecnológico / We analyze the possibility of using aluminum nitride (AlN) as a piezoelectric tunnel barrier in magnetic or non-magnetic tunnel junctions. Samples in the form of monolayers, bilayers, multilayers and tunnel junctions were produced by magnetron sputtering from an aluminum metal target. The insulating AlN barrier was grown in a reactive atmosphere of argon and nitrogen. Through the monolayers and bilayers we investigated the growth conditions of AlN onto different substrates, buffer, and cap layers. Using x-ray diffraction and transmission electronic microscopy it was possible to verify the excellent degree of texturing of AlN films with the direction <002> perpendicular the substrate plane. The multilayer showed that the use of AlN as a piezoelectric tunnel barrier is feasible, since the crystallographic structure remains when the thickness of the AlN is drastically reduced to a thickness so that quantum tunneling is possible. We also held magnetization measurements and tunnel magnetoresistance in magnetic tunnel junctions. It is important that the coercive fields of the electrodes are different, so that from the application of an external field can be obtained a situation where the magnetization of the electrodes point in opposite directions. The average thickness of the tunnel barrier in multilayers and tunnel junctions were obtained by x-ray diffraction and transmission electron microscopy. The nonlinear IxV curves of tunnel junctions were measured at room temperature and at lower temperatures, and showed a linear behavior at low voltages, and a nonlinear behavior for higher voltages. Measurements of tunnel magnetoresistance showed spin dependent tunneling. Simulations using the Simmons model for symmetric barrier allowed us to obtain the effective area of tunneling, effective thickness of the barrier, and the height of the barrier. Effective area values are some orders of magnitude smaller than the actual area of the junctions, and transmission electron microscopy pictures show that the tunnel transport occurs at some hot spots. In the measurements of the IxV curves we observe a minimum thickness of 6nm for the insulating barrier to be piezoelectric, as the polarization effect was detected. The curves have a shift to negative bias, both in magnetic and non-magnetic tunnel junctions. Using the results of the simulation we verified the exponential pattern of resistance, normalized by the effective area of tunneling, depending on the thickness of the insulator. For effective barrier thickness above 1nm, the barrier height increases with insulator thickness, as expected. For barrier thickness between 0;8 and 1nm, there is a decline in barrier height. We have not found recorded in the literature this type of behavior for normal insulating systems or for piezoelectric materials. / Nesta tese analizamos a possibilidade do uso de nitreto de alumínio (AlN) como barreira túnel piezoelétrica em junções túnel magnéticas ou não magnéticas. Amostras na forma de monocamadas, bicamadas, multicamadas e junções túnel foram produzidas pela técnica de "magnetron sputtering"a partir de um alvo metálico de alumínio. A barreira isolante de AlN foi crescida em uma atmosfera reativa de argônio e nitrogênio. Através das monocamadas e das bicamadas investigamos as condições de crescimento do AlN sobre diferentes substratos, e camadas "buffer"e camadas "cap". Utilizando difração de raio-x e microscopia eletrônica de transmissão foi possível verificar o excelente grau de texturização dos filmes de AlN com a direção <002> perpendicular ao plano do substrato. As multicamadas mostraram que a utilização do AlN como barreira túnel piezoelétrica é viável, pois a estrutura cristalográfica se mantém quando a espessura do AlN é drasticamente reduzida até uma espessura que ocorra o fenômeno de tunelamento quântico. Também foram realizadas medidas de magnetização e de magnetorresistência túnel em junções túnel magnéticas. Nestas, é importante que os campos coercivos dos eletrodos sejam diferentes, para que a partir da aplicação de um campo externo seja possível obter uma situação onde os momentos magnéticos dos eletrodos apontem em sentidos contrários. A espessura média da barreira túnel nas multicamadas e junções túnel foram obtidas através de difração de raio-x e de microscopia eletrônica de transmissão. As curvas IxV não lineares das junções túnel foram medidas a temperatura ambiente e a baixa temperatura, e apresentaram um comportamento linear a baixas tensões e uma relação não linear para tensões mais elevadas. Para a realização de simulações foi utilizado modelo de Simmons para barreira simétrica. Os parâmetros obtidos através deste modelo são, a área efetiva de tunelamento Se f , a espessura efetiva da barreria te f e a altura da barreira f0. Através da observação dos resultados da área efetiva que são algumas ordens de grandeza menores que a área real da junção, e das imagens de microscopia eletrônica de transmissão podemos afirmar que o transporte túnel se dá por "hot spots". Nas medidas das curvas IxV observamos uma espessura mínima de 6nm para a barreira isolante piezoelétrica onde o efeito de polarização foi detectado. As curvas sofrem um deslocamento para tensões negativas, isto ocorre tanto nas junções túnel magnéticas como nas não magnéticas. Utilizando os resultados dos ajustes foi possível verificar o caráter exponencial da resistência, normalizada pela área efetiva de tunelamento, em função da espessura do isolante. Para espessura efetiva da barreira, a partir de 1nm, a altura da barreira aumenta com a espessura do isolante. Resultado este esperado, mostrando uma tendência do crescimento da altura da barreia com a espessura. Para espessura de barreia entre 0;8 e 1nm, há presença de um declínio na altura da barreira. Não encontramos registro na literatura deste tipo de comportamento para sistemas isolantes normais nem para materiais piezoelétricos. Medidas de magnetorresistência túnel nas junções mostraram que o tunelamento é dependente de spin.