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2D materials have recently demonstrated a strong potential for spintronic applications. This has been further reinforced by the discovery of ferromagnetic 2D layers. Nevertheless, the fragility of ...

International audience; We report on the integration of atomically thin 2D insulating hexagonal boron nitride (h-BN) tunnel barriers into magnetic tunnel junctions (2D-MTJs) by fabricating two illustrative systems (Co/h-BN/Co and Co/h-BN/Fe) and by discussing h-BN potential for metallic spin filtering. The h-BN is directly grown by chemical vapor deposition on prepatterned Co and Fe stripes. Spin-transport measurements reveal tunnel magneto-resistances in these h-BN-based MTJs as high as 12% for Co/h-BN/h-BN/Co and 50% for Co/h-BN/Fe. We analyze the spin polarizations of h-BN/Co and h-BN/Fe interfaces extracted from experimental spin signals in light of spin filtering at hybrid chemisorbed/ physisorbed h-BN, with support of ab initio calculations. These experiments illustrate the strong potential of h-BN for MTJs and are expected to ignite further investigations of 2D materials for large signal spin devices.

International audience; Spintronic devices based on pure spin currents have drawn a lot of attention during the last few years for low energy device design. One approach to generate pure spin currents is to combine a metallic or insulating ferromagnetic layer with a non-magnetic metallic layer with a large spin-orbit coupling. A recent controversy has arisen in the possible role of magnetic proximity effects at ferromagnetic/ non-magnetic interfaces, which can hamper the understanding of pure spin current generation mechanisms. While magnetic proximity effects have been frequently observed at ferromagnetic metal/non-magnetic interfaces, there are only a few studies on ferromagnetic insulator/non-magnetic interfaces. Regarding the use of ferromagnetic insulators, the focus has been mainly on yttrium iron garnet (YIG). However, investigation of induced magnetic moments at YIG/Pt interfaces has engendered contradictory results. Here, we propose to study insulating ferrites for which electronic and magnetic properties can be modulated. Magnetic proximity effects have been investigated at MnFe 2 O 4 /Pt, CoFe 2 O 4 /Pt, and NiFe 2 O 4 /Pt interfaces by X-ray circular magnetic dichroism (XMCD) measurements at the Pt L 3 edge. Although hybridization with Pt seems to be different among the ferrites, we do not detect any XMCD signal as the signature of an induced magnetism in Pt. We have then studied the Fe 3 O 4 ferrite below and above the Verwey transition temperature. No XMCD signal has been measured in the insulating or conducting phase of Fe 3 O 4. This suggests that the absence of magnetic proximity effects at ferrite/Pt interfaces is not linked to the insulating character or not of the ferrites.

We report on the integration of atomically thin 2D insulating hexagonal boron nitride (h-BN) tunnel barriers into Co/h-BN/Fe magnetic tunnel junctions (MTJs). The h-BN monolayer is directly grown by chemical vapor deposition on Fe. The Conductive Tip Atomic Force Microscopy (CT-AFM) measurements reveal the homogeneity of the tunnel behavior of our h-BN layers. As expected for tunneling, the resistance depends exponentially on the number of h-BN layers. The h-BN monolayer properties are also characterized through integration into complete MTJ devices. A Tunnel Magnetoresistance of up to 6% is observed for a MTJ based on a single atomically thin h-BN layer.

International audience; We have studied the boron B diffusion in MgO/CoFeB bilayer by x-ray photoelectronspectroscopy depth analysis. A large concentration of B B/Mg=0.16 was found to diffuse into theMgO barrier after 350 °C annealing. The boron in MgO is in a highly oxidized B3+ state and ishomogenously distributed in the whole barrier. The important B diffusion in MgO could be relatedto the CoFeB crystallization process which begins from the under CoFeB/Ru interface and pushesboron atoms to diffuse into the MgO barrier during annealing.

International audience; We report a study of Co-doped La0.37Sr0.63TiO3−δ thin films grown by pulsed laser deposition in various oxygen pressure conditions. X-ray absorption spectroscopy and magnetic circular dichroism measurements at the Co L2,3 edges reveal that the cobalt mainly substitutes for the titanium and is in an ionic state. Nevertheless, in some films, indications of additional cobalt metallic impurities were found, suggesting that the intrinsic character of this magnetic system remains questionable.

International audience; Spin-conserving hopping transport through chains of localized states has been evidenced by taking benefit of the high degree of spin-polarization of CoFeB-MgO-CoFeB magnetic tunnel junctions. In particular, our data show that relatively thick MgO barriers doped with boron favor the activation of spin-conserving inelastic channels through a chain of three localized states and leading to reduced magnetoresistance effects. We propose an extension of the Glazman-Matveev theory to the case of ferromagnetic reservoirs to account for spin-polarized inelastic tunneling through nonmagnetic localized states embedded in an insulating barrier.

We report on the electronic and magnetic properties of Co-doped ZnO thin films investigated by x-ray absorption spectroscopies and element selective magnetometry. For a low Co concentration (around 5%), we evidence a paramagnetic phase clearly correlated to Co2+ ions substituted to Zn in the ZnO matrix. For higher Co concentrations (around 25%), we demonstrate the coexistence of both paramagnetic and ferromagnetic phases. The use of advanced element and orbital selective techniques allows us through the distinct spectral signature of Co in ionic or metallic states to assign the ferromagnetic phase to the presence of Co in a metallic state as a consequence of Co metal clustering in our films.

We have performed a layer-resolved, microscopic study of interactions between domain walls in two magnetic layers separated by a non-magnetic one, using high-resolution x-ray photoemission electron microscopy. Domain walls in the hard magnetic Co layer of a Co/Al2O3/FeNi trilayer with in-plane uniaxial anisotropy strongly modify the local magnetization direction in the soft magnetic FeNi layer. The stray fields associated to the domain walls lead to an antiparallel coupling between the local Co and FeNi moments. For domain walls parallel to the easy magnetization axis this interaction is limited to the domain wall region itself. For strongly charged (head-on or tail-to-tail) walls, the antiparallel coupling dominates the interaction over radial distances up to several micrometers from the centre of the domain wall., Comment: Published version, J. Phys.: Condens. Matter 19, 476204 (2007)

In the present thesis, the properties at ferromagnet/semiconductor interfaces, relevant for semiconductor spintronics applications, are addressed. Semiconductor spintronics refers to the possibility of storing information using the electron spin, additional to the electron charge, for enhanced flexibility in nanoscale semiconductor devices. The system under focus is the Fe/ZnSe(001) heterostructure, where ZnSe is a wide gap semiconductor ideally compatible with GaAs. The heterostructures are grown on GaAs(001) substrates by molecular beam epitaxy. From various electron-beam based diffraction, spectroscopy and microscopy techniques, it is shown that Fe grows epitaxially and predominantly in a layer-by-layer mode on ZnSe(001) with no presence of chemically reacted phases or interdiffusion. An in-plane uniaxial magnetic anisotropy (UMA) is detected for thin Fe films on ZnSe(001) by magnetometry, thus opposing the cubic symmetry of bcc Fe. From first principles calculations, the unidirectional sp3-bonds from ZnSe are shown to induce this uniaxiality. Moreover, an in-plane anisotropic lattice relaxation of Fe is found experimentally, seemingly as a consequence of the sp3-bonds, giving an additional UMA contribution via magneto-elastic coupling. It is proposed that these two effects are responsible for the much-debated UMA observed in Fe/semiconductor structures in general. The interface magnetism is probed by x-ray magnetic circular dichroism and Mossbauer spectroscopy. It is found that the magnetic moment at the interface is comparable or even enhanced with respect to the bulk Fe. These two experiments are believed to provide the first unambiguous proof of a persistent bulk magnetic moment at a transition metal/semiconductor interface. Spin-polarised transport measurements are performed on Fe/ZnSe/FeCo magnetic tunnel junctions. A magnetoresistance of 16% is found at low temperature, which evidences both the existence of interface spin polarisation, as inferred from the bulk magnetic moment above, and that the spin polarisation can be transmitted across the semiconductor barrier layer.

Nanoparticles of cobalt and nickel embedded in AlN matrix have been prepared by ion implantation or sputter deposition with average diameters ranging from 0.8 to 9 nm. The average magnetic moment per atom versus the average cluster diameter was measured either by x-ray magnetic circular dichroism and/or by SQUID magnetometry. The resulting values are always smaller than the bulk ones. An interpretation is given in terms of an interaction between the atoms located at the cluster surface and the AlN matrix, leading to a magnetically dead layer about 0.1 nm thick.

This thesis targets the field of molecular spintronics and more particularly the new spin polarization tailoring opportunities, unachievable with inorganic materials, which arise from the ferromagnetic metal/molecule hybridization at the interface.: the new concept of Spinterface.In a first part we investigate Self-Assembled Monolayers (SAMs) based magnetic tunnel nanojunctions. This system appears to be a highly promising candidate to engineer the properties of spintronics devices at the molecular level since SAMs are the equivalent of a molecular LEGO building unit. We present the functionalization of the half-metallic manganite (La,Sr)MnO3 (LSMO) with alkyl phosphonic acids SAMs and the fabrication of LSMO/SAMs/Co magnetic tunnel nanojunctions with an area of few 10 nm2. MR of 30% to 50% is observed in most of the devices, while we report even up to 250% tunnel magnetoresistance (TMR) at low temperature. The most striking point is the robustness of the signal with bias voltage with still 20% TMR observed in the volt range. The influence of the molecular chain length is also investigated and represents a first step towards achieving molecular tailoring.In a second part we develop organic spintronics devices relying on high Curie temperature metallic ferromagnetic electrodes and standard organic semiconductor such as Co/Alq3/Co organic spin valves (OSVs). Junctions have a large area (section of 50 or 100 µm) and are fabricated in-situ by shadow mask. Magnetoresistance (MR) effects at room temperature are investigated with -4% MR observed in Co/Alq3/Co OSVs and +8% MR in Co/MgO/Alq3/Co OSVs. The role of the two interfaces on the spin polarization properties of the devices is also investigated. A stronger spin-dependent hybridization is found to occur at the bottom Co/Alq3 interface inverting the spin polarization on the first molecular layer. The observation of spin polarization inversion at room temperature demonstrates that spinterface effects can strive up to room temperature.; Cette thèse s’inscrit dans le domaine de la spintronique moléculaire. Elle s’intéresse plus précisément aux nouvelles opportunités de façonnage de la polarisation de spin qui découlent de l'hybridation métal ferromagnétique/molécule à l'interface : le nouveau concept de « spinterface ».Dans une première partie nous présentons l’étude de nanojonctions tunnel magnétiques à base de monocouches auto-assemblées (SAMs). Ce système est un des plus prometteur dans l’optique de moduler les propriétés des dispositifs de spintronique par ingénierie chimique, tel un LEGO moléculaire. Nous y présentons la fonctionnalisation de la manganite demi-métallique (La,Sr)MnO3 (LSMO) avec des SAMs d’acides alkylphosphoniques et la fabrication de nanojonctions LSMO/SAMs/Co avec une surface de quelque 10 nm2. Une magnétorésistance de 30% à 50% est observée dans la majorité des dispositifs avec une magnétorésistance tunnel (TMR) jusqu'à 250 % à basse température. Un point remarquable est aussi le comportement très robuste du signal avec la tension: environ 20% de TMR est encore observée au-dessus d’une tension de 1 V. L'influence de la longueur de la chaîne moléculaire a été aussi étudiée et représente un premier pas vers la modulation des dispositifs au niveau moléculaire. Dans une deuxième partie nous présentons l’étude des dispositifs organiques à base de métaux ferromagnétiques à haute TC (température de Curie) et semi-conducteurs organiques. Nous avons réalisé des vannes de spin de Co/Alq3/Co avec des sections de 50 ou 100 µm et fabriquées in-situ par « shadow mask ». Des mesures à température ambiante ont permis d’observer -4% de magnétorésistance (MR) dans une vanne de spin Co/Alq3/Co et +8% MR dans une vanne de spin de Co/MgO/Alq3/Co. Le rôle des deux interfaces sur les propriétés de polarisation de spin des dispositifs est aussi étudié et détaillé. Une forte hybridation métal/molécule dépendant du spin à l'interface inferieure de Co/Alq3, présentant un effet de spinterface (inversion de la polarisation en spin), est observée. Ces études montrent que les effets de spinterface, comme l’inversion de la polarisation de spin, peuvent persister dans un dispositif jusqu’à température ambiante.

Microwave devices mostly use ferrite circulators, which need an external magnetic bias. Cost and size of these circulators lead to study various materials in order to replace the ferrites. Among the candidates, irradiated polymer membranes, filled by oriented magnetic metallic nanowires, have already been used in an unbiased non-reciprocal device, which exhibits more than 10 dB insertion loss. Lower insertion loss is required to make efficient nanowired circulators. In this thesis, the nanowired membrane properties, useful for designing, modelling and making non-reciprocal devices, are studied. Contribution of the different loss factors can then be estimated, thus allowing to identify the key loss factor and then to propose solutions to reduce conductor loss, magnetic loss, and dielectric loss in new devices. Device modelling and measurement of these solutions are carried out. The performance improvement can then be quantified. Finally, new nanowired membrane technologies to be explored are suggested, as they could allow achieving the implementation of all the solutions into the same device.; L'objectif de cette thèse est d'étudier la possibilité d'utiliser des membranes chargées de nanofils métalliques magnétiques comme matériau non-réciproque dans des circulateurs hyperfréquence. Ces dispositifs utilisent très largement des ferrites polarisés par des aimants permanents, ce qui les rend coûteux et encombrants. Le remplacement de ces ferrites par des membranes de polymère irradié, chargées de nanofils métalliques magnétiques orientés, a déjà donné naissance à un dispositif présentant un effet non-réciproque sans polarisation externe, mais avec des pertes d'insertion de plus de 10 dB. La réduction des pertes d'insertion des dispositifs à membranes chargées de nanofils est recherchée. Dans le cadre de cette thèse, les propriétés du matériau utiles à la conception, à la simulation et à la réalisation de dispositifs non-réciproques sont étudiées. La contribution des différents facteurs de dissipation aux pertes d'insertion est évaluée, ce qui permet d'identifier les facteurs clés et de proposer des solutions réduisant les pertes conducteurs, les pertes magnétiques, et les pertes diélectriques par rapport au dispositif pré-existant. La pertinence de ces solutions est évaluée par les simulations et mesures de dispositifs. Enfin, de nouvelles technologies à explorer sont proposées pour la fabrication du diélectrique à nanofils magnétiques, elles permettraient d'appliquer conjointement les diverses solutions de réduction de pertes présentées dans cette thèse.

Microwave devices mostly use ferrite circulators, which need an external magnetic bias. Cost and size of these circulators lead to study various materials in order to replace the ferrites. Among the candidates, irradiated polymer membranes, filled by oriented magnetic metallic nanowires, have already been used in an unbiased non-reciprocal device, which exhibits more than 10 dB insertion loss. Lower insertion loss is required to make efficient nanowired circulators. In this thesis, the nanowired membrane properties, useful for designing, modelling and making non-reciprocal devices, are studied. Contribution of the different loss factors can then be estimated, thus allowing to identify the key loss factor and then to propose solutions to reduce conductor loss, magnetic loss, and dielectric loss in new devices. Device modelling and measurement of these solutions are carried out. The performance improvement can then be quantified. Finally, new nanowired membrane technologies to be explored are suggested, as they could allow achieving the implementation of all the solutions into the same device.; L'objectif de cette thèse est d'étudier la possibilité d'utiliser des membranes chargées de nanofils métalliques magnétiques comme matériau non-réciproque dans des circulateurs hyperfréquence. Ces dispositifs utilisent très largement des ferrites polarisés par des aimants permanents, ce qui les rend coûteux et encombrants. Le remplacement de ces ferrites par des membranes de polymère irradié, chargées de nanofils métalliques magnétiques orientés, a déjà donné naissance à un dispositif présentant un effet non-réciproque sans polarisation externe, mais avec des pertes d'insertion de plus de 10 dB. La réduction des pertes d'insertion des dispositifs à membranes chargées de nanofils est recherchée. Dans le cadre de cette thèse, les propriétés du matériau utiles à la conception, à la simulation et à la réalisation de dispositifs non-réciproques sont étudiées. La contribution des différents facteurs de dissipation aux pertes d'insertion est évaluée, ce qui permet d'identifier les facteurs clés et de proposer des solutions réduisant les pertes conducteurs, les pertes magnétiques, et les pertes diélectriques par rapport au dispositif pré-existant. La pertinence de ces solutions est évaluée par les simulations et mesures de dispositifs. Enfin, de nouvelles technologies à explorer sont proposées pour la fabrication du diélectrique à nanofils magnétiques, elles permettraient d'appliquer conjointement les diverses solutions de réduction de pertes présentées dans cette thèse.