La fabrication d’aimants permanents nano-structurés est l’une des solutions envisagées pour remplacer les aimants actuels à base de terres rares, pour lesquelles se posent des problèmes géopolitiques et environnementaux. Dans le but d’élaborer de tels matériaux, nous avons suivi une approche bottom-up utilisant des méthodes chimiques.Nos travaux ont visé dans un premier temps à synthétiser des nanoparticules (NPs) magnétiques dures qui peuvent servir de briques élémentaires dans la fabrication d’aimants nano-structurés. Notre étude systématique sur des nanobâtonnets de cobalt (NBs Co) synthétisés par voie polyol, a montré que leur champ coercitif augmente de 3 à 7 kOe avec la diminution du diamètre et l’augmentation du rapport d’aspect structural. Des simulations micro-magnétiques ont montré qu’un mécanisme de retournement d’aimantation par nucléation-propagation de parois rendait compte des résultats expérimentaux. Des NPs bi-métalliques FePt et tri-métalliques FePtX (X = Ag, Cu, Sn, Sb) de structure CFC ont été obtenues par l’adaptation d’une synthèse organométallique ou par la réduction d’acétylacétonates métalliques. Les recuits à haute température (650°C pour FePt, 400°C pour FePtX) ont conduit à la transition de phase FePt CFC L10 et à des champs coercitifs élevés (>12 kOe). La maîtrise d’un procédé multi-étapes, impliquant la protection des NPs FePt CFC par une coquille MgO et un recuit à 850°C, a permis d’obtenir des NPs FePt L10 de taille moyenne 10 nm présentant des champs coercitifs jusqu’à 27 kOe.La seconde partie de nos travaux a porté sur l’assemblage de NPs présentant des anisotropies différentes. Deux systèmes ont été étudiés : FePt CFC+FeCo CC, FePt L10+NBs Co HCP. Dans les deux cas, le contact entre les deux types de NPs a été favorisé par l’utilisation d’un ligand bi-fonctionnel suivi d’un traitement thermique. Dans le système FePt+FeCo, le recuit à haute température (650°C), nécessaire pour obtenir la phase FePt L10, a entraîné l’inter-diffusion des phases et la quasi-disparition de la phase FeCo CC. Dans le second système FePt+Co, un comportement de spring magnet a clairement été identifié, les deux phases étant efficacement couplées. L’inter-diffusion des phases a été limitée par la température modérée du recuit (400°C). Un champ coercitif de 10 kOe a été mesuré pour une teneur en Pt de seulement 25%at., malgré la perte de la forme anisotrope des NBs Co. / The production of nano-structured permanent magnets is a promising alternative to rare earth magnets, which induced geopolitical and environmental issues. In order to elaborate such materials, we followed a bottom-up approach based on chemical methods. A first objective consisted in synthesizing hard magnetic nanoparticles (NPs) as building blocks for nano-structured magnets. The properties of cobalt nanorods (Co NRs) synthesized by the polyol process have been systematically studied. Coercive fields could be raised from 3 to 7 kOe by decreasing the diameter and improving the structural aspect ratio. Micro-magnetic simulations showed that a magnetization reversal following a nucleation and domain-wall propagation process could explain the experimental results. Bi-metallic FePt and tri-metallic FePtX (X = Ag, Cu, Sn, Sb) exhibiting the FCC structure were synthesized following two routes based on the reduction of an organometallic Fe precursor or of metallic acetylacetonates. Annealing at high temperatures (650°C for FePt, 400°C for FePtX) allowed the phase transition FCC  L10 to occur, leading to high coercive fields (>12 kOe). A multi-steps process, involving the protection of FePt NPs with an MgO shell and an annealing at 850°C, was optimized to produce L10 FePt NPs with a mean size of 10 nm and a coercivity up to 27 kOe. In the second part of our study, we worked on assemblies of NPs with different magnetic anisotropies. Two systems were studied : FCC FePt+BCC FeCo, L10 FePt+HCP Co NRs. In both cases, the contact between the two types of NPs was favored by the presence of a bi-functional ligand followed by an annealing step. Concerning the FePt+FeCo system, the high temperature annealing (650°C), required to get the L10 FePt phase, led to the inter-diffusion of the phases and to the dissolution of the BCC FeCo phase. For the FePt+Co system, a spring magnet behavior has been clearly evidenced, the two phases being efficiently coupled The inter-diffusion of the phases was limited thanks to the fairly low annealing temperature (400°C). A coercive field of 10 kOe was measured for a Pt content as low as 25%at., eventhough the Co NRs anisotropic morphology was lost

When a permanent magnet is considered for an application, the quantity that quantifies the usability of that material is the magnetic energy product (BH)max. In today’s world, rare earth transition metal permanent magnets like Nd-Fe-B, Sm-Co possesses the maximum magnetic energy product. But still for the industrial application, the ferrite permanent magnets are the primary choice over these rare transition metal magnets. Thus, in the present context, the magnetic energy product of the low cost ferrite system makes it unsuitable for the high magnetic energy application. In this regard, exchange spring magnets which combine the magnetization of the soft phase and coercivity of the hard magnetic phases become important in enhancing the magnetic energy product of the system. In this thesis, the exchange spring behaviour is reported for the first time in hard/soft oxide nanocomposites by microstructural tailoring of hard Barium Ferrite and soft Nickel Zinc Ferrite particles. We have analyzed the magnetization reversal and its correlation with the coercivity mechanism in the Ni0.8Zn0.2Fe2O4/BaFe12O19 exchange spring systems. Using this exchange spring concept, we could enhance the magnetic energy product in Iron Oxide/ Barium Calcium Ferrite nanocomposites compared to the bare hard ferrite by ~13%. The presence of the exchange interaction in this nanocomposite is confirmed by the Henkel plot. Moreover, a detailed Reitveld study, magnetization loop and corresponding variation of the magnetic energy product, Henkel plot analysis and First Order Reversal Curve analysis are performed on nanocomposites of hard Strontium Ferrite and soft Cobalt Ferrite. We have proved the exchange spring behaviour in this composite. In addition, we could successfully tailor the magnetization behaviour of the soft Cobalt Ferrite- hard Strontium Ferrite nanocomposite from non exchange spring behaviour to exchange spring behaviour, by tuning the size of the soft Cobalt Ferrite in the Cobalt Ferrite/Strontium Ferrite nanocomposite. The relative strength of the interaction governing the magnetization process in the composites has been studied using Henkel plot and First Order Reversal Curve method. The FORC method has been utilized to understand the magnetization reversal behaviour as well as the extent of the irreversible magnetization present in both the nanocomposites, having smaller and larger particle size of the Cobalt Ferrite. It has been found that for the all the studied composites, the pinning is the dominant process for magnetization reversal. The detailed structural analysis using thin film XRD, angle dependent magnetic hysteresis and remanent coercivity measurement, coercivity mechanism by micromagnetic analysis and First Order Reversal Curve analysis are performed for thin films of Strontium Ferrite which are grown on c-plane alumina using Pulsed Laser Deposition (PLD) at two different oxygen partial pressures. The magnetic easy directions of both the films lie in the out of plane direction where as the in plane direction corresponds to the magnetic hard direction. Depending on the oxygen partial pressure during deposition, the magnetization reversal changes from S-W type reversal to Kondorsky kind of reversal. Thus, the growth parameter for the Strontium Ferrite single layer which will be used further as a hard layer for realizing oxide exchange spring in oxide multilayer, is optimized. The details of the magnetic and structural properties are analyzed for Nickel Zinc Ferrite thin film grown on (100) MgAl2O4. We have obtained an epitaxial growth of Nickel Zinc Ferrite by tuning the growth parameters of PLD deposition. The ferromagnetic resonance and the angle dependent hysteresis loop suggest that, the magnetic easy direction for the soft Nickel Zinc Ferrite lie in the film plane whereas the out of plane direction is the magnetic hard direction. Using the growth condition of respective Nickel Zinc Ferrite and Strontium Ferrite, we have realized the exchange spring behaviour for the first time in the trilayer structure of SrFe12O19 (20 nm)/Ni0.8Zn0.2Fe2O4(20 nm)/ SrFe12O19 (20 nm) grown on c-plane alumina (Al2O3) using PLD. The FORC distribution for this trilayer structure shows the single switching behaviour, corresponding to the exchange spring behaviour. The reversible ridge measurement shows that the reversible and the irreversible part of the magnetizations are not coupled with each other.