In this dissertation, we utilized a wide range of complementary synchrotron-based X-ray spectroscopic and scattering techniques, notably X-ray absorption spectroscopy (XAS), hard X-ray photoelectron spectroscopy (HAXPES), standing-wave X-ray photoelectron spectroscopy (SW-XPS), and X-ray resonant magnetic reflectometry (XRMR), to understand and control the phenomenon of emergent interfacial ferromagnetism in strongly-correlated oxide heterostructures. This field holds great promise for the development of next-generation spintronic devices. In the heterostructures we investigated, neither of the parent oxide layers exhibits inherent ferromagnetism. Yet, when these layers are combined in an epitaxial film stack, charge-transfer phenomena give rise to an emergent ferromagnetic state at the interface. Throughout my graduate studies, I focused on studying such charge-transfer phenomena as the driving force for stabilizing interfacial ferromagnetism. This dissertation is structured around two main projects. The first project delves into the intriguing possibility of tuning the emergent interfacial ferromagnetism. More specifically, we investigated the mechanisms for suppressing interfacial charge transfer to gain control over and manipulate this magnetic phenomenon. In our second project, we explored a different facet of interfacial ferromagnetism, focusing on the origins of the imbalance in the magnitudes of the magnetic moment between the top and bottom interfaces in the same layer. Our investigation aimed to uncover the possible causes of this imbalance, ultimately leading us to scrutinize the role of defect states in this magnetic asymmetry. In the first part of this dissertation, we investigated the thickness-dependent metal-insulator transition within LaNiO3 and how it impacts the electronic and magnetic states at the interface between LaNiO3 and CaMnO3. We present a direct observation of a reduced effective valence state in the interfacial Mn cations. This reduction is most pronounced in the metallic LaNiO3/CaMnO3 superlattice, where the above-critical LaNiO3 thickness of 6-unit cells triggers this phenomenon, facilitated by the charge transfer of the itinerant Ni 3d eg electrons into the interfacial CaMnO3 layer. In contrast, when we examine the insulating superlattice with a LaNiO3 thickness below the critical value (2-unit cells), we observe a homogeneous effective valence state of Mn throughout the CaMnO3 layers. This homogeneity is attributed to the suppression of charge transfer across the interface. The second part of this dissertation delves deeply into the complexities of interfacial magnetism within the CaMnO3/CaRuO3 superlattices. Our experimental investigation unveiled an unexpected asymmetry in the strength of magnetism at these interfaces. Our findings suggest that within the superlattice CaMnO3/CaRuO3, the lower interface (CaRuO3/CaMnO3) exhibits a weaker magnetic moment when compared to the upper interface (CaMnO3/CaRuO3). This observation, supported by XRMR and XAS experimental data, was further clarified by first-principles density functional theory (DFT) calculations. Our calculations suggest that the observed magnetic asymmetry may be linked to the presence of oxygen vacancies at the interfaces. Our study significantly contributes to our understanding of interfacial ferromagnetism, potentially paving the way for controlling and manipulating this emergent property. This may be achieved by utilizing engineered defect states, offering exciting prospects for applications in the field of spintronics devices. / Physics

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We have embarked on a systematic study of novel charge states at oxide interfaces. We have performed pulsed laser deposition (PLD) growth of epitaxial oxide thin films on single crystal oxide substrates. We studied the effects of epitaxial strain and rare-earth composition of the metal oxide thin films. We have successfully created TiO₂ terminated SrTiO₃ (STO) substrates and have grown epitaxial thin films of LaAlO₃ (LAO), LaGaO₃ (LGO), and RAlO₃ on STO using a KrF pulsed excimer laser. Current work emphasizes the importance of understanding the effect of both epitaxial strain and R³+ magnetism on the interface between RAlO₃ and STO. We have demonstrated that the interfaces between LAO/STO and LGO/STO are metallic with carrier concentrations of 1.1 x 10¹⁴ cm[superscript -2] and 4.5 x 10¹⁴ cm[superscript −2], respectively. Rare-earth aluminate films, RAlO₃, with R = Ce, Pr, Nd, Sm, Eu, Gd, and Tb, were also grown on STO. Conducting interfaces were found for R = Pr, Nd and Gd, and the results indicate that for R [does not equal] La the magnetic nature of the R³+ ion causes increased scattering with decreasing temperature that is modeled by the Kondo effect. Epitaxial strain between the polar RAlO₃ films and STO appears to play a crucial role in the transport properties of the metallic interface, where a decrease in the R³+ ion size causes an increase in sheet resistance and an increase in the onset temperatures for increased scattering. / text