The CoFe2O4 nanocrystals are highly attractive due to their magnetic properties - large coercivity (up to 2 T at low temperatures) with moderate saturation magnetization (80 A.m2.kg-1), remarkable chemical stability and mechanical hardness. Upon RE doping, a significant change of the properties is expected. This thesis is focused on investigation of Co1-LaxFe2O4, x = 0.05 - 0.5 and CoLaxFe2-x O4 x = 0.05 - 0.2 nanoparticles prepared by sol-gel and microemulsion method, respectively, with varying particle size according to the final heat treatment. In the former case, the particles were embedded in amorphous SiO2 matrix, while in the latter case, the samples were matrix-free. The samples were characterized using X-ray diffraction and Mössbauer spectroscopy. Measurements of the temperature dependence of the ZFC-FC magnetization revealed that the blocking temperature is above the room temperature. The values of coercivity and saturation magnetization strongly depend on particles size determined by method of preparation. The higher coercivity values of about 2 T at 10 K show the samples prepared by the sol-gel method. The obtained results are discussed in the context of preparation method, particle size and level of La doping.

京都大学 / 0048 / 新制・課程博士 / 博士(理学) / 甲第20890号 / 理博第4342号 / 新制||理||1623(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 前野 悦輝, 教授 佐藤 昌利, 教授 石田 憲二 / 学位規則第4条第1項該当 / Doctor of Science / Kyoto University / DFAM

The magnetization dynamics in ferromagnetic materials will depend on the specific shape of the system’s energy landscape. In most systems, the energy landscapes can be approximated as paraboloids, resulting in a typical ellipti- cal precession of the magnetization. However, this model is not always appli- cable to more complex potentials, which can present exotic precessions. The aim of this project was to measure the magnetization dynamics in a system where a non-parabolic potential was expected. From the dynamics, it would then be possible to estimate the energy potential of the system. In order to measure magnetization dynamics, time-resolved MOKE (magneto-optic Kerr effect) measurements were performed using a pump-and-probe tech- nique. A permalloy (Fe20Ni80) thin film with an uniaxial in-plane anisotropy was used as a sample, presumably presenting a bistable energy potential with two close minima at certain applied external magnetic fields. By measuring one component of the magnetization in the plane of the sample, the shape of the precession in this landscape could be extracted. The results show the expected parabolic precessions at higher external fields, from which energy landscapes could be constructed. The dynamics measured at one particular field also indicate a bistable energy potential although no exotic precessions were found.

Skeletal muscle performs essential functions, including movement and posture. Musculoskeletal disorders can disrupt these functions, leading to temporary or permanent impairment. As most muscle abnormalities will cause morphological and physiological changes in skeletal muscle, identifying diseased or injured skeletal muscle relies on having a frame of reference, i.e. a correct characterization of what is considered healthy or 'normal' skeletal muscle. Non-invasive Magnetic Resonance Imaging (MRI) techniques such as 1H Magnetic Resonance Spectroscopy (1H-MRS) to assess the biochemical environment, Magnetization Transfer (MT) to study water dynamics and Blood Oxygen Level Dependent (BOLD) signal to study blood flow and relative (de)oxy-Hb concentration have yet to be extensively explored in skeletal muscle. Therefore, to improve the knowledge of the biochemical environment of skeletal muscle, a series of experiments were performed using these techniques in calf muscles. 1H-MRS investigations showed high repeatability of metabolite quantification within and across scanning sessions despite its challenges due to the high structural organization of skeletal muscle. Furthermore, differences in the metabolic profile between endurance vs. power-oriented participants at rest were found, suggesting 1H-MRS could be used as a non-invasive technique to assess muscle fiber composition. A multimodal MT, and BOLD study were performed on exercised skeletal muscle to complement the metabolic understanding of skeletal muscle. It was shown that high-quality data could be obtained in simultaneous studies of BOLD/EMG. In addition, during a multimodal MT and BOLD acquisition, MT signal showed a decrease after exercise and was linearly correlated to the BOLD signal activation. The ability of MT to distinguish between highly/lowly activated muscle groups during exercise opens the opportunity to non-invasively investigate muscle group recruitment with a higher spatial resolution compared to EMG, and lower scanning times compared to BOLD. Overall, the main purpose of this thesis was to investigate, characterize and provide unique metrics to study the functional and metabolic profile of healthy skeletal muscle at rest and during exercise. / Thesis / Master of Applied Science (MASc) / Skeletal muscle performs vital functions such as movement, heat generation, and posture. The impact of musculoskeletal disorders, which can disrupt these functions and cause temporary or permanent impairment of physical activity and movement, is expected to grow in the future. Correctly characterizing healthy or 'normal' skeletal muscle is necessary to identify diseased or injured skeletal muscle, as most muscle abnormalities cause changes in morphology and physiology. Non-invasive MRI techniques to assess the biochemical environment, water dynamics, blood flow and relative (de)oxy-Hb concentration have yet to be extensively explored in healthy skeletal muscle. Thus, the primary purpose of this thesis was to investigate, characterize and provide unique metrics to study the functional and metabolic profile of healthy skeletal muscle at rest and during exercise. The metrics investigated can be used to establish a baseline to detect abnormal skeletal muscle.

This dissertation is focused on ferromagnetic, multiferroics, and two-dimensional (2D) perovskites, exploring different unique collective magnetic and ferroic characters: (1) ferromagnetic thin film Co/Pd multilayers, (2) BaTiO3-BiFeO3 (BTO-BFO) a magneto-electric materials system, and (3) CuCl4 halide organic-inorganic perovskites. Low-power all-optical memory offers a unique opportunity to achieve ultra-fast magnetic switching in which the switching dynamics are not thermally mediated and occur on the order of the laser pulse. However, it is challenging to achieve a low-power optically excited magnetization precession angle above 90 degrees, which is required for magnetic switching. Co/Pd thin film multilayers were investigated for their potentially large perpendicular magnetic anisotropy (PMA) with three differing regimes of magnetic anisotropy: in-plane, weakly out-of-plane, and out-of-plane. Utilizing the time-resolved magneto-optical Kerr effect (TR-MOKE), we observed clear magnetic precession (on the order of a few GHz) with magnetic precession angle increasing (up to 4.5 degrees) for thinner Co samples which demonstrated stronger PMA. We observed a clear connection between PMA strength and precession amplitude as well as a large efficiency of energy transfer between spin and orbital subsystems for our strongest PMA sample. BTO-BFO is a strong room-temperature multiferroic with enhanced magneto-electric properties compared to BFO. We utilized time-resolved differential reflectivity (TR-DR) and TR-MOKE to observe strong coherent acoustic phonons in thin films as well as nanorods. Our nanorods showed additional modes (a new 20 GHz and 6 GHz mode) not observed in thin films including the fast 33 GHz mode which showed some weak tunability with high magnetic fields (up to 10 T). The observed tunability of these modes in an external magnetic field shows interesting coupling between magnetic moment and phononic modes which may be caused by the breaking of the spin-cycloid at the interface of the nanorods and the surface of the nanorods. We also observed second harmonic generation (SHG) emission which demonstrated a large enhancement in our nanorod structures with further observation of wavelength dependence. Finally, ferromagnetic resonance on our nanorod and thin film BTO-BFO structures indicated very weak Gilbert damping (on the order of 10−3), demonstrating the practicality of our structure for low-spin loss applications. Lastly, this dissertation focuses on a project around CuCl4 and CuCl2Br2 perovskites in which we observed time-dependent SHG. An increase in SHG as a function of infrared laser exposure is shown to coincide with changes in the crystal structure of the Cu perovskite materials. This increase in SHG was shown to last for a few days after hours of laser exposure indicating a slow hysteretic change to the crystal structure of the perovskites. / Doctor of Philosophy / Multifunctionality in materials is important for various applications including future mem- ory devices where ferromagnetism (collective magnetic order), ferroelectricity (collective electric polarization order), and piezoelectricity (collective strain order) can be implemented in a given device. This dissertation centers on three material systems for exploring ferroic orders: Co/Pd thin multilayers, BaTiO3-BiFeO3 (BTO-BFO) films and nano-rod arrays, and Cu halide organic-inorganic perovskite thin films and 2D structures. Co/Pd thin films demonstrate interesting ferromagnetic order with magnetic anisotropy in which the magnetization of the thin film has a preferred direction based on the thickness of the thin film. BTO-BFO demonstrates coupling between ferroelectric and antiferromagnetic order. The magnetic information may be controlled by applying electric fields or strain and Cu halide perovskites demonstrate potentially created ferroelectric order under long-term laser expo- sure with high ferroelectric switching speeds. Dynamics and nonlinear optical responses in these materials systems were explored with Ti:Sapphire pulsed lasers (∼ 100 fs). Our techniques allowed us for a better understanding of fast carrier and spin dynamics after optical excitation. Furthermore, nonlinear optics, in which two or more photons can be used to emit higher energy photons, were employed to explore the ferroelectric properties within these material systems. The results presented in this dissertation provided information on collective orders and fundamental interactions in several less-explored material systems.

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<p> It is believed that Sr2RuO4 is a triplet superconductor that breaks time reversal symmetry, and it is expected to have spontaneous magnetization both at the sample edge, as well as at domain walls. Recent magnetic microscopy results place upper limits on the magnetic fields differing from previous theoretical calculations by 2 orders of magnitude. Using a Ginzburg-Landau formalism we investigate the effects of a rough surface as well as parameter choices which differ from the typical weak coupling parameters on the magnitudes of the spontaneous supercurrents and magnetic fields. The dependance on surface roughness is found to be small resulting in only a 20% reduction for the weak coupling parameters. Changing the parameters from weak coupling in addition to pair breaking surface effects is also found to affect the magnitudes of the spontaneous fields weakly, except in certain unphysical parameter regimes. The effects of the surface stabilizing another non-magnetic order parameter are considered, and give rise to field distributions with similar features to those present at domain walls.</p> / Thesis / Master of Science (MSc)

Magnetismus ist ein Phänomen, das eine wichtige Rolle in einer Vielfalt technischer Anwendungen spielt. Ohne den Einsatz magnetischer Effekte und Materialen wäre der heutzutage erreichte technische Fortschritt unmöglich, da viele grundlegende Techniken wie Stromerzeugung, elektrischer Antrieb, Informationsübertragung und viele andere auf magnetische bzw. elektromagnetische Phänomene zurückzuführen sind. Dabei haben die ferromagnetischen Materialen stets zur Effizienz von elektrischen und elektronischen Anwendungen beigetragen, weswegen an diesen Materialen auch entsprechend viel geforscht worden ist. Moderne Technologien, insb. Massenspeicher basieren oft auf Ferromagneten und erfordern daher die weitere Erforschung und Anpassung ihrer Eigenschaften. Für die Funktionalität von Hochgeschwindigkeitsgeräten spielt das dynamische Verhalten dünner magnetischer Schichten eine kritische Rolle. In dieser Arbeit wird die Magnetisierungsdynamik dünner Schichtelemente mittels zeitaufgelöster Weitfeld- Kerrmikroskopie untersucht. Dies ist ein aktuelles Thema, an dem in den letzten Jahren sehr intensiv gearbeitet wird. Allerdings sind viele für die Anwendungen sehr wichtige Details des magnetischen Schaltens wegen ihre Vielfältigkeit und Komplexität doch nicht vollständig untersucht und verstanden. In dieser Arbeit werden überwiegend experimentelle Ergebnisse vorgestellt, die einen zusätzlichen Beitrag zum aktuellen Wissenstand leisten. In einem ferromagnetischen Körper bilden sich Bereiche mit spontaner Magnetisierung, die man als Domänen bezeichnet. Die spontane Magnetisierung entsteht aufgrund der Spin-Spin Wechselwirkung, und die Domänen bilden sich aufgrund der Energieminimierung des magnetisierten Körpers. Langsame Magnetisierungsprozesse werden im Wesentlichen getragen von Domänenumordnungen und Domänengrenzenverschiebungen. Solche Prozesse bezeichnet man als quasistatisch, da sich der Körper durch deren Langsamkeit immer im Gleichgewicht oder zumindest sehr nahe daran befindet. Mit zunehmender Anregungsgeschwindigkeit gilt diese Annahme nicht mehr, da die Präzessionsbewegung der magnetischen Momente das Schaltverhalten in diesem Fall definiert. Die Untersuchung der Magnetisierungsdynamik setzt die Möglichkeit voraus, nicht-unterbrochene Prozesse beobachten zu können. Dieses Ziel kann mittels stroboskopischer Abbildung erreicht werden. Dabei wird derselbe Prozess kontinuierlich wiederholt (vorausgesetzt, dass die Prozesse sich reproduzierbar wiederholen lassen), und zu definierten Zeitpunkten werden die entsprechenden Kerraufnahmen gemacht. Dafür wird eine CCD Kamera mit einem Photoverstärker benutzt, welcher als optischer Schalter fungiert. Die Zeitauflösung dieses Systems und damit auch das Vermögen, die Hochfrequenzvorgänge abzubilden, beträgt 250 ps. Die Eigenschaften des magnetischen Umschaltens hängen stark von der Elementgeometrie ab. Diese Unterschiede sind auf unterschiedliche Entmagnetisierungsfaktoren, und damit auf Unterschiede in den effektiven Feldern zurückzuführen. Solche Unterschiede werden auf zwei Weisen initiiert: ein quadratisches Element wird entlang unterschiedlicher Richtungen (entlang der Seite und der Diagonalen) angeregt; die Form des Elementes wird zwischen Quadrat und Rechteck mit unterschiedlichen Seitenverhältnissen variiert. Die beobachteten Schaltvorgänge werden miteinander verglichen und die Ergebnisse dargestellt. Dabei werden auch die dynamischen Vorgänge immer mit den quasistatischen verglichen. Aus dem Vergleich folgt, dass ein steigendes Seitenverhältnis zur geringeren Schaltgeschwindigkeit führt, und dass die dabei entstehenden Domänen zunehmend komplexer werden. Dabei gibt es wesentliche Unterschiede zwischen den dynamischen und quasistatischen Domänen, vor allem in der Domänenwandstruktur. Das Schalten an sich unterscheidet sich auch sehr stark. Quasistatisches Schalten erfolgt überwiegend durch Domänenwandbewegung, während das dynamische Schalten durch inkohärente Rotation der Magnetisierung im ganzen Element erfolgt. Das Hochfrequenzverhalten am Prototypen eines Mikroinduktors wird untersucht. Der Induktor besteht aus vielen magnetischen Elementen, die eine induzierte uniaxiale Anisotropie besitzen. Diese ist bei der Hälfte der Elemente entlang des Magnetfeldes, und bei der anderen Hälfte senkrecht zum Magnetfeld der Spule ausgerichtet. Das dynamische Verhalten der beiden Elementtypen unterscheidet sich stark, vor allem die Ummagnetisierungsgeschwindigkeit. Diese Unterschiede können zu einer Phasenverschiebung im elektrischen Signal führen, was die Effizienz des Induktors senkt. Durch die Untersuchung der Magnetisierungsdynamik in Wechselfeldern unterschiedlicher Frequenz ist auch festgestellt worden, dass bis 100 MHz die Magnetisierungsvorgänge überwiegend durch Domänenwandbewegung erfolgen, während ab 200 MHz- Rotationsprozesse stattfinden.