The unique physical properties and low temperature solution processability of organic semiconductors have enabled many applications such as light emitting diodes, flexible logic and solar cells, they are unexploited in their potential for use in solid state devices for spintronics and spin-based information processing. Organic semiconductors composed of mainly light elements appeal to the field of spintronics due to their long spin lifetime originating from their weak spin-orbit coupling. The significant progress in improving carrier mobility of organic semiconductors in the past decade may lead to organic spin transport materials with both long spin diffusion length and spin lifetime which is important for spintronics applications. This dissertation explores the spin transport in organic semiconductors using a variety of experimental techniques from all electrical spin injection and detection to ferromagnetic resonance spin pumping and ISHE spin detection. Non-local spin valves and novel all electrical spin transport device architectures based on high mobility conjugated polymers were studied systematically. The intrinsic roadblocks for electrical spin injection-based measurements were identified as the current spreading effect (electrical cross-talk between the injector and detector electrodes) and the hopping conduction in organic semiconductors which makes all electrical nonlocal spin injection and detection measurements extremely challenging if not impossible for organic semiconductors. In addition, spin current transmission in the out of plane direction of organic semiconductors was studied by tri-layer spin pumping technique where the spin transport properties of organic semiconductors are correlated with their molecular structure and charge transport properties. Spin pumping, a charge-free spin injection method together with ISHE spin detection successfully overcome the impedance mismatch problem and the intrinsic roadblocks imposed by electrical spin injection-based techniques and enabled lateral spin current transport in organic semiconductors to be detected electrically. The lateral spin diffusion length of up to a micrometre was observed in doped conjugated polymers in agreement with theoretical calculations based on exchange mediated spin diffusion model and parameters obtained from first principle. Moreover, this non-local spin transport device structure provides a platform for studying spin transport in a wide range of organic semiconductors where the spin current propagates along the high mobility direction and could potentially be used as building blocks for high performance flexible spintronics devices.

This thesis explores the use of 2D materials (graphene and hBN) for spintronics. Interest on these materials in spintronics arose from theoretical predictions of high spin filtering in out-of-plane transport through graphene and hBN sandwiched by ferromagnets. Similarly, 5-layer graphene was forecast to be a perfect spin filter. In the case of in-plane spin transport, graphene was expected to be an excellent material due to its low spin-orbit coupling and low number of defects. Although there already exist experimental works that attempted to explore the aforementioned predictions, they have failed so far to comply with the expected results. Earlier experimental works in graphene and hBN out-of-plane spin transport achieved low spin filtering on the order of a few percent; while spin relaxation parameters in graphene for in-plane spin transport remained one or two orders of magnitude below the predicted values. In the case of vertical devices, the failure to meet the theoretical expectations was attributed to the oxidation of the ferromagnets and the lack of an epitaxial interface between the later and the graphene or hBN. Similarly, the exact mechanisms that lead to high spin relaxation for in-plane spin transport in graphene are not completely understood, in part due to the low-quality of the explored devices. In this thesis we analyze new architectures and procedures that allowed us to fabricate ultraclean and oxidation-free interfaces between ferromagnets and graphene or hBN. In these devices we encountered negative and reversible magnetoresistance, that could not be explained with the previous theoretical models. We propose a new model based on a thorough characterization of the devices and well-known properties of graphene that were not taken into account in the previous model. We also employed a novel type of contact to graphene (1D-contacts) and applied it for the first time to achieve spin-injection in graphene. The main advantage of this type of contact is the full encapsulation of graphene with hBN, which leads to high quality graphene spintronic devices.

Depuis le début du XX siècle, la thématique de transport a concentré l’attentionde nombreux chercheurs. L’objectif étant alors d’identifier et de comprendre lesdifférentes sources de diffusions prenant part à la résistivité de la matière. Les deuxpremières sources diffusives mises en évidence ont été les phonons dépendant de latempérature, et les défauts du réseau cristallin. Dans les années 1950, l’étude des semiconducteursa fait émerger une troisième source de diffusion, la diffusion magnétique.Dès la mise en évidence du rôle joué par le magnétisme sur la résistivité de certainsmatériaux, il a rapidement été établi que la résistivité magnétique R est tributaire dela stabilité de l’ordre magnétique du réseau. A basse température T, la diffusion desélectrons s’ opère par l e biais des ondes de spins. A haute température, R est proportionnelleaux corrélations spin-spin. Cependant, les mécanismes de diffusion ayant lieuau voisinage de la température de transition ordre/désordre magnétique restent encoremal comprise. L’objectif de cette thèse a consisté à étudier ce problème à l’aide d’uneapproche nouvelle basée sur la simulation Monte Carlo. En effet, les théories existantessont toutes construites avec des hypothèses sur les mécanismes à l’origine du comportementde résistance tels que : fonction corrélation spin-spin, longueur de localisation.Elles utilisent beaucoup d’approximations au cours du calcul telles que théorie du champmoyen, approximation du temps de relaxation, la portée des fonctions de corrélation. Lesprincipaux handicaps de ces théories sont de n’être valables que pour certaines gammesde températures, et d’être tributaires du type de magnétisme porté par les réseaux cristallins.Notre approche offre quant à elle une procédure unifiée concernant l’étude desrésistivités magnétiques fonction de la température. Cette méthode peut s’appliquer `atout type de matériaux, tout ordre magnétique (ferromagnétique, antiferromagnétique,ferrimagnétique, verre de spin, ...), tout type de modèle de spins (Ising, Heisenberg, XY,...), enfin tout type de réseau cristallin. Seule la connaissance du Hamiltonien permet defaire la simulation, et de reproduire des mesures expérimentales avec la possibilité d’unecomparaison quantitative.Dans un premier temps, nous traitons de structures ferromagnétiques et interprétons les différents mécanismes de diffusion en fonction de la température. Nousétendons ensuite l´étude aux systèmes antiferromagnétiques, frustrés et non-frustrés. Cessystèmes n’ont fait l’objet que de peu d’études. Dans le cas des systèmes antiferromagnétiques non-frustrés, nous sommes en mesure de contredire une prédiction théoriquefaite par Haas en 1968, concernant la forme de la résistance magnétique à la transition dephase . Dès lors, nous nous consacrerons à l’étude des mécanismes de transport dansdes systèmes antiferromagnétiques frustrés. Ces travaux ont permis de mettre en évidencedes comportements nouveaux des transitions de phases des résistances magnétiques : nousmontrons que ces résistances subissent une transition du premier ordre , mais qu’ilest également possible par le contrôle d’un paramètre du modèle, de choisir le sens de latransition : des hautes résistances vers les basses résistances ou inversement .Pour finir, nous confrontons nos résultats de simulations avec des mesures expérimentalesen réalisant une étude de transport sur un matériau semiconducteur antiferromagnétique :MnTe. Il résulte de cette étude un bon accord entre nos résultats de simulations et lesmesures expérimentales . / ....

Spintronics, also known as spin electronics, or magnetoelectronics, refers to the study of the role that electron and (less frequently) nuclear spins play in solid state physics, and a group of devices that specifically exploit both the intrinsic spin of the electron and its associated magnetic moment, in addition to its fundamental electronic charge. As a principal type of spintronic device, a spin-valve is a device that uses ferromagnetic electrodes to polarize and analyze the electronic spins. The electrical resistance of the device depends sensitively on the relative magnetization of its two ferromagnetic electrodes, a phenomenon referred to as Giant Magnetoresistance (GMR). Having been successfully applied in the field of data storage, GMR also shows potential for future logic devices. Organic semiconductors possess many advantages in electronic device applications. Therefore, using organic semiconductors in spintronics is very interesting and promising, in part, because of their exceptionally long spin-decoherence times. This thesis concerns itself with the scientific study of magnetic field and spin effects in organic spin valves (OSV) and organic light emitting diodes (OLED). Three projects were finished, achieving a better understanding of the transportation of charge and spin carriers inside organic films, and paving the way to enhancing the spin diffusion length and the organic magnetoresistance (OMAR) effect. Firstly, C60 films were used as the spin-transport layer of OSV devices, because of its low hyperfine coupling and high mobility, which prior work suggested to be beneficial. Subsequently we studied the spin injection and transport properties by measuring the devices' magnetoresistance (MR) response at various biasing voltages, V, temperatures, T and different C60 film thickness. But we do not observe a significantly increased spin-diffusion length compared to OSV devices based on other organic semiconductors. We propose conductivity mismatch as a likely cause of the loss of spin-valve signal with increasing C60 layer thickness. There exists some disagreement in the scientific literature regarding whether OSV operate in the so-called tunneling regime or the so-called injection regime. To shed light on this question, we fabricated spin-valve devices made of organic semiconductor thin films of rubrene sandwiched between ferromagnetic cobalt and iron electrodes. Current-voltage (I-V) characteristics in Co/AlOx/rubrene/Fe junctions with a rubrene layer thickness, d, ranging from 5-50 nm, were measured, and we found two different modes of conductivity. The first mode, tunneling, occurs in relatively thin junctions, d < 15 nm, and decays exponentially with increasing rubrene thickness. We determined the tunneling decay length to be 1 nm. The tunneling mode is also characterized by a weak temperature dependence and a nearly parabolic differential conductance. The second mode, injection followed by hopping, occurs in relatively thick devices, d ≥ 15 nm, and can be identified by strongly temperature dependent, highly non-linear I-V traces that are similar to those commonly measured in organic injection devices such as OLEDs. We observed MR in devices with a rubrene thickness of 5 nm and 10 nm. Those devices are clearly in the tunneling regime. For the 15 nm device, for which the tunneling current is just barely measurable we could not observe MR. In the third project, we show that the performance of both OMAR and OSV devices very sensitively depends on whether the metallic layers are deposited by thermal evaporation or electron-beam evaporation. A strongly reduced spin diffusion length and an enhanced OMAR response can be achieved in devices fabricated by electron-beam evaporation. Then we showed that the difference must be attributed to the generation of traps resulting from the exposure of the organic layer to X-ray bremsstrahlung that is generated during the e-beam evaporation process. We also used the thermally stimulated current technique (TSC) to characterize these traps.

京都大学 / 新制・課程博士 / 博士(工学) / 甲第23210号 / 工博第4854号 / 新制||工||1758(附属図書館) / 京都大学大学院工学研究科電子工学専攻 / (主査)教授 白石 誠司, 教授 木本 恒暢, 教授 引原 隆士 / 学位規則第4条第1項該当 / Doctor of Philosophy (Engineering) / Kyoto University / DGAM

京都大学 / 0048 / 新制・課程博士 / 博士(工学) / 甲第21109号 / 工博第4473号 / 新制||工||1695(附属図書館) / 京都大学大学院工学研究科電子工学専攻 / (主査)教授 白石 誠司, 教授 木本 恒暢, 教授 山田 啓文 / 学位規則第4条第1項該当 / Doctor of Philosophy (Engineering) / Kyoto University / DFAM

No description available.

The general theme of the thesis is the interplay between magnetization dynamics and spin transport. The main presentation is divided into three parts. The first part is devoted to deepening our understanding on magnetic damping of ferromagnetic metals, which is one of the long-standing issues in conventional spintronics that has not been completely understood. For a nonuniformly-magnetized ferromagnetic metal, we find that the damping is nonlocal and is enhanced as compared to that in the uniform case. It is therefore necessary to generalize the conventional Landau-Lifshitz-Gilbert equation to include the additional damping. In a different vein, the decay mechanism of the uniform precession mode has been investigated. We point out the important role of spin-conserving electron-magnon interaction in the relaxation process by quantitatively examining its contribution to the ferromagnetic resonance linewidth. In the second part, a transport theory is developed for magnons which, in addition to conduction electrons, can also carry and propagate spin angular momentum via the magnon current. We demonstrate that the mutual conversion of magnon current and spin current may take place at magnetic interfaces. We also predict a novel magnon-mediated electric drag effect in a metal/magnetic-insulator/metal trilayer structure. This study may pave the way to the new area of insulator-based spintronics. In the third part of thesis, particular attention is paid to the influence the spin orbit coupling on both charge and spin transport. We theoretically investigate magnetotransport anisotropy and the conversion relations of spin and charge currents in various magnetic systems, and apply our results to interpret recent experiments.

Fabrication of molecular spin devices with ferromagnetic electrodes coupled with a high spin molecule is an important challenge. This doctoral study concentrated on realizing a novel molecular spin device by the bridging of magnetic molecules between two ferromagnetic metal layers of a ferromagnetic-insulator-ferromagnetic tunnel junction on its exposed pattern edges. At the exposed sides, distance between the two metal electrodes is equal to the insulator film thickness; insulator film thickness can be precisely controlled to match the length of a target molecule. Photolithography and thin-film deposition were utilized to produce a series of tunnel junctions based on molecular electrodes of multilayer edge molecular electrodes (MEME) for the first time. In order to make a microscopic tunnel junction with low leakage current to observe the effect of ~10,000 molecules bridged on the exposed edge of a MEME tunnel barrier, growth conditions were optimized; stability of a ~2nm alumina insulator depended on its ability to withstand process-induced mechanical stresses. The conduction mechanism was primarily 1) tunneling from metal electrode to oranometalic core by tunneling through alkane tether that acts as a tunnel barrier 2) rapid electron transfer within the oranometalic Ni-CN-Fe cube and 3) tunneling through alkane tether to the other electrode. Well defined spin-states in the oranometalic Ni-CN-Fe cube would determine electron spin-conduction and possibly provide a mechanism for coupling. MEME with Co/NiFe/AlOx/NiFe configurations exhibited dramatic changes in the transport and magnetic properties after the bridging of oranometalic molecular clusters with S=6 spin state. The molecular cluster produced a strong antiferromagnetic coupling between two ferromagnetic electrodes to the extent, with a lower bound of 20 erg/cm,2 that properties of individual magnetic layers changed significantly at RT. Magnetization, ferromagnetic resonance and magnetic force microscopy studies were performed. Transport studies of this configuration of MEME exhibited molecule-induced current suppression by ~6 orders by blocking both molecular channels and tunneling between metal leads in the planar 25μm2 tunnel junction area. A variety of control experiments were performed to validate the current suppression observation, especially critical due to observed corrosion in electrochemical functionalization step. The spin devices were found to be sensitive to light radiation, temperature and magnetic fields. Along with the study of molecular spin devices, several interesting ideas such as ~9% energy efficient ultrathin TaOx based photocell, simplified version of MEME fabrication, and chemical switching were realized. This doctoral study heralds a novel molecular spin device fabrication scheme; these molecular electrodes allow the reliable study of molecular components in molecular transport.

Spin-dependent electron transport in submicron/nano sized magnetic thin film devices fabricated using the optical lithography, e-beam lithography and focused ion beam (FIB) was investigated with the primary aim to find the ballistic magnetoresistance (BMR) in thin film nanoconstrictions. All experimental results were analysed in combination with micromagnetic simulations. The magnetisation reversal processes were investigated in a submicron half-pinned NiFe stripe with a microconstriction. An asymmetric MR curve was observed, and micromagnetic simulations verified it was due to the exchange-bias on the left side, which changed the magnetic switching mechanism. The effects of different pinning sites on the magnetisation switching and domain wall displacement were studied in NiFe film and spin-valve based nanodevices. A sign of domain wall MR was seen on the transversal MR curve of the NiFe nanodevice due to the domain wall induced electron scattering. The size effect on the magnetisation switching and interlayer magnetostatic coupling was demonstrated and characterised in synthetic antiferromagnet (SAF)-pinned spin-valve nanorings. It has been clarified by micromagnetic simulations that these nanorings exhibit a double or single magnetisation switching process, which is determined by the magnetostatic coupling as a function of the ring diameter. The interlayer magnetostatic coupling was efficiently reduced in large SAF-pinned nanorings, resulting in a small shift of the minor MR curve, which is beneficial to the magnetic memory applications. In-situ MR measurements and the investigation of domain wall properties have been carried out in FIB patterned NiFe film nanoconstrictions. Spin-valve like sharp transitions were observed on the MR curves in the 80 nm/130 nm wide nanoconstriction devices. However, our analysis of the results by micromagnetic simulations and domain observations with scanning electron microscopy with polarisation analysis (SEMPA) concluded that these sharp MR transitions originated from the anisotropic magnetoresistance (AMR) effect, due to the fast magnetisation rotation in the nanoconstriction, and not from BMR. The numerical investigation has proved that a further reduction of the constriction width/length is necessary for large MR values.