In this PhD thesis, we study the interplay between symmetry-breaking order and quantum-disordered phases in the milieu of frustrated quantum magnets, and further show how the excitation process of long-wavelength (semi-)classical modes in spin-orbit coupled antiferromagnets crucially depends on the nature and interactions of the underlying quantum quasiparticles. First, we focus on Kitaev's exactly solvable model for a Z2 spin liquid as a building block for constructing novel phases of matter, utilizing Majorana mean-field theory (MMFT) to map out phase diagrams and study occurring phases. In the Kitaev Kondo lattice, conduction electrons couple via a Kondo interaction to the local moments in the Kitaev model. We find at small Kondo couplings a fractionalized Fermi liquid (FL*) phase, a stable non-Fermi liquid where conventional electronic quasiparticles coexist with the deconfined excitations of the spin liquid. The transition between FL* and a conventional Fermi liquid is masked by an exotic (confining) superconducting phase which exhibits nematic triplet pairing, which we argue to be mediated by the Majorana fermions in the Kitaev spin liquid. We moreover study bilayer Kitaev models, where two Kitaev honeycomb spin liquids are coupled via an antiferromagnetic Heisenberg interaction. Varying interlayer coupling and Kitaev coupling anisotropy, we find both direct transitions from the spin liquid to a trivial dimer paramagnet as well as intermediate 'macrospin' phases, which can be studied by mappings to effective transverse-field Ising models. Further, we find a novel interlayer coherent pi-flux phase. Second, we consider the stuffed honeycomb Heisenberg antiferromagnet, where recent numerical studies suggest the coexistence of collinear Néel order and a correlated paramagnet, dubbed 'partial quantum disorder'. We elucidate the mechanism which drives the disorder in this model by perturbatively integrating out magnons to derive an effective model for the disordered sublattice. This effective model is close to a transition between two competing ground states, and we conjecture that strong fluctuations associated with this transition lead to disorder. Third, we study the generation of coherent low-energy magnons using ultrafast laser pulses in the spin-orbit coupled antiferromagnet Sr2IrO4, inspired by recent pump-probe experiments. While the relaxation dynamics of the system at long time scales can be well described semi-classically, the ultrafast excitation process is inherently non-classical. Using symmetry analysis to write down the most general coupling between electric field and spin operators, we subsequently integrate out high-energy spin fluctuations to derive induced effective fields which act to excite the low-energy magnon, constituting a generalized 'inverse Faraday effect'. Our theory reveals a tight relationship between induced fields and the two-magnon density of states.:1 Introduction 1.1 Frustrated antiferromagnets 1.2 Quantum spin liquids 1.3 Fractionalization and topological order 1.4 Spin-orbit coupling 1.5 Outline I Novel phases by building on Kitaev’s honeycomb model 2 Kitaev honeycomb spin liquid 2.1 Microscopic spin model and constants of motion 2.2 Majorana representation of spin algebra 2.3 Exact solution 2.3.1 Ground state 2.3.2 Correlations and dynamics 2.3.3 Thermodynamic properties 2.4 Z2 gauge structure 2.5 Toric code 2.6 Topological order 2.6.1 Superselection sectors and ground-state degeneracy 2.6.2 Topological entanglement entropy 2.6.3 Symmetry-enriched and symmetry-protected topological phases 3 Mean-field theory 3.1 Generalized spin representations 3.1.1 Parton constructions 3.1.2 SO(4) Majorana representation 3.2 Projective symmetry groups 3.3 Mean-field solution of the Kitaevmodel 3.4 Comparisonwithexactsolution 3.4.1 Spectral properties 3.4.2 Correlation functions 3.4.3 Thermodynamic properties 3.5 Generalized decoupling 3.6 Comparison to previous Abrikosov fermion mean-field theories of the Kitaev model 3.7 Discussion 4 Fractionalized Fermi liquids and exotic superconductivity in the Kitaev Kondo lattice 4.1 Metals with frustration 4.2 Local-moment formation and Kondo effect 4.2.1 Single Kondo impurity 4.2.2 Kondo lattices and heavy Fermi liquids 4.3 Fractionalized Fermi liquids 4.4 Construction of the Kitaev Kondo lattice 4.4.1 Hamiltonian 4.4.2 Symmetries 4.5 Mean-field decoupling of Kondo interaction 4.5.1 Solution of self-consistency conditions 4.6 Overview of mean-field phases 4.7 Fractionalized Fermi liquid 4.7.1 Results from mean-field theory 4.7.2 Perturbation theory beyond mean-field theory 4.8 Heavy Fermi liquid 4.9 Superconducting phases 4.9.1 Spontaneously broken U(1) phase rotation symmetry 4.9.2 Excitation spectrum and nematicity 4.9.3 Topological triviality 4.9.4 Group-theoretical classification 4.9.5 Pairing glue 4.10 Comparison with a subsequent study 4.11 Discussion and outlook 5 Bilayer Kitaev models 5.1 Model and stacking geometries 5.1.1 Hamiltonian 5.1.2 Symmetries and conserved quantities 5.2 Previous results 5.3 Mean-field decoupling and phase diagrams 5.3.1 AA stacking 5.3.2 AB stacking 5.3.3 σAC stacking 5.3.4 σ ̄AC stacking 5.4 Quantum phase transition in the AA stacking 5.4.1 Perturbative analysis 5.5 Phase transition in the σAC stacking 5.6 Macro-spin phases 5.6.1 KSL-MAC transition: Effective model for Kitaev dimers 5.6.2 DIM-MAC transition: Effective theory for triplon condensation 5.6.3 Macro-spin interactions and series expansion results 5.6.4 Antiferromagnet in the AB stacking 5.7 Stability of KSL and the interlayer-coherent π-flux phase 5.7.1 Perturbative stability of the Kitaev spin liquid 5.7.2 Spontaneous interlayer coherence near the isotropic point 5.8 Summary and discussion II Partial quantum disorder in the stuffed honeycomb lattice 6 Partial quantum disorder in the stuffed honeycomb lattice 6.1 Definition of the stuffed honeycomb Heisenberg antiferromagnet 6.2 Previous numerical results 6.3 Derivation of an effective model 6.3.1 Spin-wave theory for the honeycomb magnons 6.3.2 Magnon-central spin vertices 6.3.3 Perturbation theory 6.3.4 Instantaneous approximation 6.3.5 Truncation of couplings 6.3.6 Single-ion anisotropy 6.3.7 Discussion of most dominant interactions 6.4 Analysis of effective model 6.4.1 Classical ground states 6.4.2 Stability of classical ground states in linear spin-wave theory 6.4.3 Minimal model for incommensurate phase 6.4.4 Discussion of frustration mechanism in the effective model 6.5 Partial quantum disorder beyond the effectivemodel 6.5.1 Competition between PD and the (semi-)classical canted state 6.5.2 Topological aspects 6.5.3 Experimental signatures 6.6 Discussion 6.6.1 Directions for further numerical studies 6.6.2 Experimental prospects III Optical excitation of coherent magnons 7 Ultrafast optical excitation of magnons in Sr2IrO4 7.1 Pump-probe experiments 7.2 Previous approaches to the inverse Faraday effect and theory goals 7.3 Sr2IrO4 as a spin-orbit driven Mott insulator 7.4 Spin model for basal planes in Sr2IrO4 7.4.1 Symmetry analysis 7.4.2 Classical ground state and linear spin-wave theory 7.4.3 Mechanism for in-plane anisotropy 7.5 Pump-induced dynamics 7.5.1 Coupling to the electric field: Symmetry analysis 7.5.2 Keldysh path integral 7.5.3 Low-energy dynamics 7.5.4 Driven low-energy dynamics 7.6 Derivation of the induced fields 7.6.1 Perturbation theory 7.6.2 Evaluation of loop diagram 7.6.3 Analytical momentum integration in the continuum limit 7.6.4 Numerical evaluation of effective fields 7.7 Analysis of induced fields 7.7.1 Polarization and angular dependence 7.7.2 Two-magnon spectral features 7.8 Applications to experiment 7.8.1 Predictions for experiment 7.8.2 Magnetoelectrical couplings 7.9 Discussion and outlook 8 Conclusion and outlook 8.1 Summary 8.2 Outlook IV Appendices A Path integral methods B Spin-wave theory B.1 Holstein-Primakoff bosons B.2 Linear spin-wave theory B.2.1 Diagonalization via Bogoliubov transformation B.2.2 Applicability of linear approximation B.3 Magnon-magnon interactions B.3.1 Dyson's equation and 1/S consistency B.3.2 Self-energy from quartic interactions in collinear states on bipartite lattices C Details on the SO(4) Majorana mean-field theory C.1 SO(4) Matrix representation of SU(2) subalgebras C.2 Generalized SO(4) Majorana mean-field theory for a Heisenberg dimer (Chapter 3) C.3 Dimerization of SO(4) Majorana mean-field for the Kitaev model (Chapter3) C.4 Mean-field Hamiltonian in the Kitaev Kondo lattice (Chapter 4) C.5 Example solutions in the superconducting phase for symmetry analysis (Chapter4) D Linear spin-wave theory for macrospin phase in the bilayer Kitaev model (Chapter 5) D.1 Spin-wave Hamiltonian and Bogoliubov rotation D.2 Results and discussion E Extrapolation of the effective couplings for the staggered field h -> 0 (Chapter 6) E.1 xy interaction E.1.1 Leadingorder ~ S0 E.1.2 Subleadingorder ~ S^(−1) E.2 z-Ising interaction F Light-induced fields by analytical integration (Chapter 7) F.1 Method F.2 Results Bibliography

No description available.

Das Standart-Modell zur Beschreibung von Observablen magnetischer Moleküle ist das Heisenberg-Modell. In diesem wird der Magnetismus des Superaustausches der Elektronen durch einfache bilineare Spin-Spin-Kopplungen beschrieben. Zur genaueren Approximation experimenteller Ergebnisse können, der jeweiligen Struktur des Moleküls entsprechend, verschiedene Erweiterungen des Heisenberg-Modells verwendet werden. Diese werden, explizit für das 4-Spin-System {Ni4Mo12}, in ihren Auswirkungen auf die Hochtemperatur-Nullfeldsuszeptibilität, die Nullfeldsuszeptibilität und die Hochfeldmagnetisierung betrachtet. Die wesentlichen Erweiterungen sind dabei die Einzelionen-Anisotropie, die Dzyaloshinskii-Moriya-Anisotropie und die allgemeinen Kopplungen zweiter Ordnung. Letztere stellen eine Verallgemeinerung der bekannten biquadratischen Kopplungen dar und werden im Rahmen eines magneto-elastischen Modells hergeleitet. Dabei ergeben sich unterschiedliche Einschränkungen der Kopplungsmatrix zweiter Ordnung für starre und flexible Molekülstrukturen. Speziell für {Ni4Mo12} entsprechen die Ergebnisse numerischer Simulationen von Messwerten einer Strukturänderung im externen Magnetfeld.

Comme nous le savons, les applications sont déterminées par des propriétés, qui sont essentiellement déterminées par la structure. L’interaction entre la forme (structure moléculaire) et la fonction (propriétés physiques) peut être exploitée par le ligand, l’ion métallique, l'approche métallacrown et ainsi de suite. Les travaux portent sur la synthèse et l’étude du comportement magnétique de complexes mononucléaires cobalt(II) de géométrie bipyramide trigonale et sur l’étude de complexes mononucléaires de lanthanides possédant une structure de type métallacrown.Pour les complexes de cobalt(II), l’objectif a été de modifier l’anisotropie magnétique en modifiant la nature du ligand organique tétradenté et du ligand terminal en gardant, autant que faire se peut, la géométrie et même la symétrie des complexes. Presque tous ces complexes se comportent comme des molécules-aimants avec une barrière énergétique à l’inversion de l’aimantation qui peut être liée à leur anisotropie magnétique et donc à la nature des ligands. Et les complexes métallacrown à base de lanthanides étant hautement symétriques, permet de les utiliser comme modèles pour effectuer une corrélation entre la nature de l’ion lanthanide et leurs propriétés d’aimants.La thèse est composée de 6 chapitres. Le chapitre 1 présente l’état de l’art du magnétisme, des molécules-aimants (SMMs et SIMs), et quelques exemples importants. Le chapitre 2 se concentre sur une famille de complexes de géométriebipyramide trigonale de formule générale [Co(Me6tren)X]Y avec le ligand axial (X) et le contre-ion (Y) induisant le comportement SMM.Dans cette série de composés, j’ai étudié l’influence du ligand axial X sur la nature et l’amplitude de l’anisotropie magnétique. J’ai montré que la série des halogénures, l’anisotropie la plus forte est obtenue pour le ligand axial fluorure (F–). J’ai aussi étudié l’effet du cation Y qui influence l’interaction entre les molécules qui affectent le comportement d’aimant moléculaire. Au chapitre 3, on étudie l’influence du changement du ligand tétradenté. Le remplacement des trois atomes d’azote qui se trouvent en position équatoriale dans la sphère de coordination de cobalt(II) par des atomes de soufre induit une augmentation des distances Co–L dans le plan équatorial qui conduit à une plus forte anisotropie. Les calculs théoriques effectués sur ces complexes permettent de rationaliser les résultats expérimentaux et surtout de prévoir les propriétés de nouveaux complexes. Les chapitres 4 et 5 concernent deux séries de SMM 12-MC-4 basées sur LnGa4 (Ln = TbIII, DyIII, HoIII, ErIII, YbIII) avec les ligands basés sur l’acide salicylhydroxamique (H3shi) et l’acide 3-hydroxy-2-naphtohydroxamique (H3nha). J’ai préparé plusieurs complexes et étudié leurs propriétés magnétiques. Les calculs théoriques permettent de rationaliser la différence entre les propriétés des magnétiques dues aux différents ions lanthanide. Enfin, une conclusion générale avec des perspectives sont récapitulées au chapitre 6. / As we know, the applications are determined by properties, which are essentially determined by structure. The interplay between form (molecular structure) and function (physical properties) can be exploited engineering by the ligand, the metal ion, the metallacrown approach and so on. The work focuses on the synthesis and the study of the magnetic behavior of mononuclear cobalt(II) complexes with trigonal geometry and on the study of mononuclear lanthanide complexes that possess a metallacrown structure.For the cobalt(II) complexes, the aim was to tune the magnetic anisotropy by changing the nature of the tetradentate organic ligand and the terminal ligand. Almost all these complexes behave as Single Molecule Magnets with an energy barrier to the reversal of the magnetization that can be linked to their magnetic anisotropy and thus to the nature of the organic ligands. The lanthanide containing metallacrown complexes are highly symmetric, which allows performing a correlation between the nature of the lanthanide ion and their Single Molecule Magnet properties.The dissertation will be composed of 6 chapters. Chapter 1 introduces the background of the magnetism, Single Molecule Magnets, Single Ion Magnets, and some important SIMs. Chapter 2 focuses on a family of trigonal bipyramidal complexes [Co(Me6tren)X]Y. We show that the axial ligand affects the SMM behavior allowing us to prepare a complex with a magnetic bistability at T = 2 K. In Chapter 3, we examine the effect of changing the coordinated atoms (sulfur instead of nitrogen) in the equatorial coordination sphere of cobalt(II). We demonstrate that this slight change improves the SMM behavior. Chapter 4 and 5, which concern two series of 12-MC-4 SMMs based on LnGa4 (Ln = TbIII, DyIII, HoIII, ErIII, YbIII) with the ligands salicylhydroxamic acid (H3shi) and 3-hydroxy-2-naphthohydroxamic acid (H3nha), respectively, where we correlate the nature of the lanthanide ion to its magnetic behavior using ab initio calculations. At last, the understanding gained from this dissertation research, along with future research directions will be recapitulated in Chapter 6.

Dans le cadre d'un projet de transport automobile propre pour la mise en place de véhicules électriques décarbonés grand public, les aimants représentent un enjeu important au niveau des moteurs électriques. Il est alors nécessaire de se passer des aimants à base de terres rares, peu écologiques et dont un seul pays détient le monopole. Deux voies sont explorées ici : la nanostructuration des hexaferrites de type M par frittage flash de type SPS (Spark Plasma Sintering), et la synthèse d'alliages Mn-Al-C par la méthode de la trempe rapide sur roue. Concernant le premier matériau, l'optimisation du protocole de synthèse a permis d'augmenter le champ coercitif d'un facteur 2. Deux outils de caractérisation des aimants ont été mis en place : le premier évalue la texture du matériau (modèle de Stoner et Wohlfarth), le second étudie les processus d'aimantation (Preisach). Pour les alliages Mn-Al-C, nous avons pu démontrer la présence d'un couplage antiferromagnétique entre les atomes de Mn des sites 1a et 1d. La diffraction de neutrons à également pu montrer que le moment magnétique du Mn du site 1d est par ailleurs très supérieur à celui du site 1a. Un broyage cryogénique suivi d'un frittage SPS à haute pression (400 MPa) a permis d'augmenter la valeur du champ coercitif de 40 %. Les résultats obtenus sont très prometteurs quant à la faisabilité d'alternatives aux aimants à base de terres rares. / In the context of green car development for mass market, development of low cost rare-earth-free magnets is clearly a milestone, because the rare-earth are expensive and their production is not ecological and a monopoly of one country. Two routes are explored herein : nanostructuration of M-type hexaferrites by flash sintering (Spark Plasma Sintering), and the synthesis of Mn-Al-C alloys by melt spinning. Concerning the first material, the optimization of the synthesis protocol allowed to increase the coercive field by a factor of 2. Two characterization tools of the magnets were set-up : the first evaluates the texture of the material (Stoner and Wohlfarth model), the second, based on Preisach model, is used to infer the magnetization processes. For Mn-Al-C alloys, we have evidenced from Weiss plots the antiferromagnetic coupling between 1a and 1d-sites Mn atoms. Neutron diffraction confirmed this result and shown that the magnetic moment of the 1d-site Mn is also much larger than that of 1a-site. Cryogenic ball milling followed by high-pressure SPS (400 MPa) increased the coercive field by 40 %. The results obtained are very promising as to the feasibility of alternatives to rare-earth magnets.

Les travaux présentés dans cette thèse portent sur la modélisation et l’optimisation de machines électriques pour des applications à entraînement direct. Ils s’inscrivent dans un contexte de réduction de l’utilisation des aimants en terres rares et d’amélioration du rendement énergétique. Un état de l’art des machines électriques est réalisé et l’accent est mis sur les machines à flux radial et axial pour les applications à fort couple et basse vitesse. Une classification est établie visant à identifier les structures intéressantes et innovantes. L’étude de la machine radiale est d’abord réalisée. Une étude comparative de différentes machines issues de l’étude bibliographique est effectuée. Cette étude a permis de choisir une structure originale à bobinage concentré sur dents et aimants en multi-V. Dans le but de calculer les performances du moteur avec un temps de calcul réduit, une modélisation analytique multi-physique de la structure est réalisée. Un premier dimensionnement de la machine a conduit à la définition d’un prototype qui a servi à la validation expérimentale du modèle multi-physique. Une approche de conception par optimisation multi-objectifs est adoptée pour obtenir les machines optimales répondant à un cahier des charges industriel. La suite de l’étude concerne une machine à flux axial à structure innovante. Il s’agit d’une machine à double rotor et simple stator avec plusieurs barrières de flux par pôle. Une étude par éléments finis est d’abord réalisée afin de valider le passage d’un modèle tridimensionnel à modèle bidimensionnel. L’analyse des pertes fer a permis de choisir les matériaux utilisés au stator et aux rotors. L’étape suivante consiste à établir un modèle analytique multiphysique de la machine à flux axial et de l’optimiser selon le même cahier des charges que celui de la machine radiale. Finalement, une comparaison entre les deux structures radiale et axiale est effectuée pour évaluer les avantages en termes de densité de couple. / The work presented in this thesis deals with the modeling and optimization of electrical machines for direct drive applications. The objective is to reduce the use of rare earth permanent magnets along with the improvement of the motor’s efficiency. A state of the art of electrical machines is realized. It focused on radial and axial flow structures for high torque and low speed applications. A classification is established to identify interesting and innovative structures. Firstly, the radial machine is studied. The choice of the structure is made after a finite element comparison of different machines resulting from the literature. This led to an original structure with concentrated winding and multi-V shape barriers. Then, a multi-physics analytical modeling of the structure is detailed in order to calculate the performances with a reduced calculation time. A preliminary design led to the definition of a prototype which was used to experimentally validate the multi-physics model. An optimization design approach is adopted to obtain optimal machines meeting industrial specifications. Secondly, a novel axial flux structure is studied. It is a machine with double rotor and single stator with several barriers per pole. A finite element study is carried out in order to validate the transition from a three dimensional to a two-dimensional model. The analysis of iron losses made it possible to choose the materials used in the stator and the rotors. Then, the development of a multi-physics analytical model for the axial machine is proposed. It is used to optimize the structure according to the same specifications defined for the radial machine. Finally, a comparison between the radial and axial structures is performed in order to evaluate the advantages in terms of torque density.

Nanokristalline Permanentmagnete zeigen ungewöhnliche magnetische Eigenschaften aufgrund von Oberflächen- und Grenzflächeneffekten, die verschieden von denen massiver oder mikrokristalliner Materialien sind. Diese Arbeit zeigt Ergebnisse einer systematischen Untersuchung der Beziehung zwischen Mikrostruktur und magnetischen Eigenschaften von isotropen nanokristallinen (Nd,Pr)(Fe,Co)B-Permanentmagneten. Hochkoerzitive Magnete vom Typ (Nd,Pr)FeB wurden durch hochenergetisches Mahlen in der Kugelmühle oder Rascherstarrung hergestellt. Der Einfluss geringer Mengen von Zusätzen wie Dy und Zr und die Substitution von Nd durch Pr auf die magnetischen Eigenschaften wird dargestellt. Weiterhin wurde eine Einschätzung des Warmumformverhaltens dieser Materialien durchgeführt. Hochenergetisches Kugelmahlen einer Legierung mit der Anfangszusammensetzung Pr9Nd3Dy1Fe72Co8B6.9Zr0.1 führte, nach Glühbehandlung, zu fast einphasigem Magnetpulver mit einem maximalen Energieprodukt von (BH)max~140 kJm-3. Das hochenergetische Kugelmahlen wurde zu einer sehr vielseitigen Technik zur Herstellung hochleistungsfähiger Nanokompositmagnete weiterentwickelt. Das Zulegieren unterschiedlicher Anteile von weichmagnetischem alpha-Fe ist damit sehr effektiv möglich. Der Zusatz von 25 Gew.-% alpha-Fe führt zu einem hohen (BH)max=178kJm-3. Dies wird auf eine sehr effektive Austauschkopplung zwischen den hart- und weichmagnetischen Phasen zurückgeführt. Die Natur der intergranularen Wechselwirkungen kann durch die Wohlfarth´sche Remanenzanalyse (?deltaJ-plot¡§) beschrieben werden. Im speziellen wurden deltaJ-Diagramme für verschiedene (i) alpha-Fe Gehalte, (ii) Korngrößen und (iii) Austauschlängen erstellt. Es konnte gezeigt werden, dass in den Nanokompositmagneten auf Pr-Basis keine Spinumorientierung auftritt. Abschließend zeigt die Arbeit die Möglichkeit der Nutzung einer mechanisch aktivierten Gas-Festkörper-Reaktion auf, mit der eine sehr feinkörnige Mikrostruktur erhalten wird. Die Untersuchungen wurden mit stöchiometrischen Nd2(Fe1-xCox)14B-Legierungen begonnen (x=0-1). Die Verbindungen wurden unter höheren Wasserstoffdrücken und Temperaturen gemahlen, wodurch sie zu NdH2+delta und krz-(Fe,Co) (x=0-0.75) oder kfz-Co (x=1) entmischt wurden. Die Korngrößen des rekombinierten Nd2(Co,Fe)14B-Materials liegen im Bereich von 40-50 nm. / Nanocrystalline permanent magnets present unusual magnetic properties because of surface/interface effects different from those of bulk or microcrystalline materials. This work presents results of a systematic investigation of the relationship between microstructure and magnetic properties in isotropic nanocrystalline (Nd,Pr)(Fe,Co)B permanent magnets. Highly coercive (Nd,Pr)FeB-type magnets have been produced using high energy ball milling and melt-spinning. The influence of small amounts of additives, Dy and Zr, and the substitution of Nd by Pr on the microstructural and magnetic properties are shown. An assessment of the hot deformation behaviour has been carried out. Intensive milling of an alloy with starting composition Pr9Nd3Dy1Fe72Co8B6.9Zr0.1 yields, after annealing treatment, nearly single-phase magnet powders with a maximum energy product (BH)max?î140kJm-3. Co has a beneficial effect on the intrinsic magnetic properties but also on the microstructure, with a mean grain size of 20nm. Intensive milling is used to produce high-performance nanocomposite magnets by blending this latter alloy with different fractions of soft magnetic alfa-Fe. Addition of 25wt.% alfa-Fe leads to a high (BH)max=178 kJm-3 due to an effective exchange-coupling between the hard and the soft magnetic phases. The intergrain interactions between the crystallites of the nanocomposite structure are analysed. Demagnetisation recoil loops of the nanocomposite magnets show relatively open minor loops due to the exchange-spring mechanism. Information about the intergrain interactions during demagnetisation are obtained by plotting the deviation of the demagnetising remanence from the Wohlfarth-model (¡§deltaJ-plot¡¨). Exchange-coupling phenomena are studied by analysing the evolution of the corresponding deltaJ values when varying (i) the alfa-Fe content, (ii) the annealing temperature, i.e. the grain size and (iii) the measurement temperature. Low temperature measurements do not reveal any sign of spin reorientation for these Pr-based nanocomposite magnets. The work concludes showing the possibility of using a mechanically activated gas-solid reaction to obtain an effective grain refined microstructure starting from stoichiometric Nd2(Fe1-xCox)14B alloys (x=0-1). These compounds were milled under enhanced hydrogen pressure and temperature leading to their disproportionation into NdH2+delta and bcc-(Fe,Co) (x=0-0.75) or fcc-Co (x=1). Grain sizes of recombined Nd2(Fe,Co)14B materials were found to be 40-50nm.

<p>Critical materials are crucial to the wide deployment of clean energy technologies and advanced technology such as electric vehicles (EVs), smartphones, high-efficiency lighting, and wind turbines. Particularly, rare earth elements (REEs) and lithium are key elements for clean energy and EVs. However, higher REEs and lithium demand for clean energy transformation, extreme supply reliance on certain area exports, and severe environmental issues during mining and processing cause uncertainty for future clean energy and transportation development. Our study aims to develop dynamic LCA with scenario analysis to simulate the future possible sustainability pathways for critical materials for stakeholders and apply life cycle assessment (LCA) to evaluate the latest REEs and lithium extraction and recycling technologies. Dynamic LCA (DLCA) integrates the temporal datasets to predict the future environmental impact of a product. The databases are mainly from Ecoinvent and Critical Materials Life Cycle Assessment Tool (CMLCAT). Python package Brightway2 and Temporalis are used to simulate the DLCA.</p> <p>The study of DLCA on the REEs industry reveals the future predictive REEs environmental impact trend, providing a clear policy strategy to reach sustainability goals for stakeholders. The results show that shifting REEs resources from China to Australia and increasing the recycling rate are key factors in reducing environmental impact in the future. Considering the degradation of rare earths ore and storage depletion in China, such as the decreased production of heavy REEs from Ion adsorption clay in southern China, exploration, and inclusion of potential REEs production projects will be the possible sustainable way in the following decade. </p> <p>LCA of RE recovery from room temperature ionic liquid (RTIL) electrochemical process helps us explore the benefits of recycling RE from the e-waste. Although RTIL contributes a higher impact on ozone depletion and global warming, close-loop recycling RTIL could reduce substantial environmental impact. Lithium recovery from geothermal brine provides the great source for fulfilling the domestic demand of the U.S. Compared to the conventional Li compounds production, this method is efficient and has 25-41% lower global warming potential. The government, researchers, and industry could benefit from this study for exploring advantage and drawback strategies for the future environmental footprint of NdFeB magnet production and identifying environmental hotspots of the latest recycling and extraction process of REEs and lithium.</p>

<p dir="ltr">Since the discovery of graphene in 2004, numerous other materials with intriguing electronic, optical, and magnetic properties have been found to be layered and exfoliatable down to atomic thickness. Owing to their weak interlayer coupling, mediated only by van der Waals forces, this new class of 2-dimensional materials, also known as van der Waals (vdW) materials, allows layer-by-layer stacking, overcoming some of the limitations of growth techniques. In particular, the growing inventory of vdW materials has expanded to include magnetic materials, further broadening the possibilities of novel devices based on stacked heterostructures. These magnetic heterostructures can find applications in spintronics and memory devices and may be combined with other vdW materials with optical properties for applications in optoelectronics. In this thesis, we assembled heterostructures via mechanical transfer or growth to modify the magnetism in these vdW materials. We used various optical and electrical techniques to probe the modified magnetism or its effects on the novel heterostructure. Thus, we observed the emergence of the magnetic proximity effect on the topological insulator BiSbTeSe₂ after dry transferring a thin flake of Cr₂Ge₂Te₆ on top, taking steps towards the observation of novel topological phases, such as the quantum Hall insulator. Additionally, we demonstrated an increased Curie temperature and magnetic anisotropy, effectively enhancing the magnetism, in thin flakes of Cr₂Ge₂Te₆ and Cr₂Si₂Te₆ after sputtering NiO or MgO. Finally, noting that the effect of modified magnetism in Cr2Ge2Te6 after sputtering NiO or MgO is induced due to wrinkle formation and strain, we further reproduce similar wrinkle formation on other 2D materials such as hBN, graphite, and 2D antiferromagnets (XPS₃, (X= Mn, Fe, Ni), CrSBr, RuCl₃). We used polarized Raman spectroscopy to characterize the induced biaxial strain in hBN and showed that such wrinkle formation can lead to moderately (up to 1.4% strain) spatially inhomogeneous and anisotropic strain profiles. These efforts demonstrate the versatility of tailoring the properties of these vdW materials.</p>

The spin-lattice relaxation rates are calculated for a rigid magnetic spin cluster in an elastic medium in the presence of a magnetic eld using the latticerame method. This rate is then compared with both the rate calculated using the quantum mechanical densitymatrix method and with the Glauber dynamics. These calculation results are used in the contribution of various heat baths, such as a phonon bath in various dimensions or a fermionic bath, to transition rates that enter into dynamic Monte Carlo simulations of molecular magnets and nanomagnets.