The correlated 4d transition metal oxide SrRuO3 (SRO) features an anomalous Hall effect that originates from momentum-space sources of Berry curvature and depends sensitively on the magnetization. Here, we exploit this sensitivity and realize an epitaxial extraordinary Hall balance device, consisting of two ultrathin layers of SRO, separated by an insulating SrTiO3 (STO) spacer. Our results highlight the potential of ultrathin SRO in the realization of oxide-based spintronic devices.@en

Complex oxide thin films and heterostructures exhibit a variety of electronic phases, often controlled by the mechanical coupling between film and substrate. Recently it has become possible to isolate epitaxially grown single-crystalline layers of these materials, enabling the study of their properties in the absence of interface effects. In this work, we use this technique to create nanomechanical resonators made out of SrTiO3 and SrRuO3. Using laser interferometry, we successfully actuate and measure the motion of the nanodrum resonators. By measuring the temperature-dependent mechanical response of the SrTiO3 resonators, we observe signatures of a structural phase transition, which affects both the strain and mechanical dissipation in the resonators. Here, we demonstrate the feasibility of integrating ultrathin complex oxide membranes for realizing nanoelectromechanical systems on arbitrary substrates and present a novel method of detecting structural phase transitions in these exotic materials.@en

Novel physical phenomena arising at the interface of complex oxide heterostructures offer exciting opportunities for the development of future electronic devices. Using the prototypical LaAlO3/SrTiO3 interface as a model system, we employ a single-step lithographic process to realize gate-tunable Josephson junctions through a combination of lateral confinement and local side gating. The action of the side gates is found to be comparable to that of a local back gate, constituting a robust and efficient way to control the properties of the interface at the nanoscale. We demonstrate that the side gates enable reliable tuning of both the normal-state resistance and the critical (Josephson) current of the constrictions. The conductance and Josephson current show mesoscopic fluctuations as a function of the applied side gate voltage, and the analysis of their amplitude enables the extraction of the phase coherence and thermal lengths. Finally, we realize a superconducting quantum interference device in which the critical currents of each of the constriction-type Josephson junctions can be controlled independently via the side gates.@en

In this work, we investigate electronic and magnetic phenomena in thin films and heterostructures of transition metal oxides with strong spin–orbit coupling. Ultrathin films are prepared by pulsed laser deposition, a technique which enables layer-by-layer growth of complex materials on atomically flat crystal surfaces. The properties of these heterostructures, which include materials such as strontium iridate (SrIrO3) and strontium ruthenate (SrRuO3), are probed by applying electric and magnetic fields. By varying parameters such as temperature, magnetic field strength and layer thickness, we obtain information about spin and charge transport in these atomically engineered crystals. Chapter 1 provides an introduction to the field of transition metal oxides, followed by a brief overview of the materials studied in this dissertation. Chapters 2 to 5 are dedicated to SrIrO3, a material that displays unexpected physical properties owing to the strong spin–orbit coupling of Ir. Chapter 2 starts with the growth and thermodynamic stability of SrIrO3, which is essential to obtain high-quality films and study their properties in the ultrathin limit. We develop a method to grow stoichiometric films by measuring their transport characteristics as a function of the target condition. We discover that the properties of SrIrO3 are sensitive to degradation in air and develop an encapsulation procedure to protect the filmsurface. SrIrO3 displays an exotic semimetallic state due to the interplay between electronic correlations, spin–orbit coupling, and octahedral rotations. In Chapter 3, we combine thermoelectric and magnetotransport measurements to quantitatively determine the transport coefficients of the different conduction channels. Despite their different dispersion relationships, electrons and holes are found to have strikingly similar transport coefficients. Chapters 4 and 5 focus on the electronic and magnetic properties of SrIrO3 in the two-dimensional limit. In Chapter 4, we discover a metal–insulator transition occurring at a critical thickness of 4 unit cells and an enhancement of spin fluctuations near the transition point. We investigate the magnetic state in Chapter 5, showing that a fourfold symmetric magnetoresistance component appears above a criticalmagnetic field. In Chapter 6, we interface ultrathin SrIrO3 with SrRuO3, an itinerant ferromagnet with an unconventional anomalous Hall conductivity. We discover that the presence of two dissimilar interfaces results in the emergence of two spin-polarized conduction channels. Having explored the influence of epitaxial interfaces, in Chapter 7 we develop a method to detach thin films fromtheir growth substrate using an epitaxial buffer layer. Using this approach, we prepare nanomechanical resonators of freestanding SrTiO3 and SrRuO3 films. By measuring the temperature dependence of theirmechanical response, we observe signatures of structural phase transitions in the SrTiO3, which affect the strain and mechanical dissipation of the resonators. Chapter 8 summarizes the findings of the previous chapters and provide perspectives for future work. We discuss ongoing experiments regarding Berry phase engineering and the manipulation of freestanding films. @en

Interfaces between complex oxides constitute a unique playground for two-dimensional electron systems (2DESs), where superconductivity and magnetism can arise from combinations of bulk insulators. The 2DES at the LaAlO3/SrTiO3 interface is one of the most studied in this regard, and its origin is determined by the polar field in LaAlO3 as well as by the presence of point defects, like oxygen vacancies and intermixed cations. These defects usually reside in the conduction channel and are responsible for a decrease of the electronic mobility. In this work, we use an amorphous WO3 overlayer to obtain a high-mobility 2DES in WO3/LaAlO3/SrTiO3 heterostructures. The studied system shows a sharp insulator-to-metal transition as a function of both LaAlO3 and WO3 layer thickness. Low-temperature magnetotransport reveals a strong magnetoresistance reaching 900% at 10 T and 1.5 K, the presence of multiple conduction channels with carrier mobility up to 80 000 cm2 V-1 s-1, and quantum oscillations of conductance.@en

The combination of strain and electrostatic engineering in epitaxial heterostructures of ferroelectric oxides offers many possibilities for inducing new phases, complex polar topologies, and enhanced electrical properties. However, the dominant effect of substrate clamping can also limit the electromechanical response and often leaves electrostatics to play a secondary role. Releasing the mechanical constraint imposed by the substrate can not only dramatically alter the balance between elastic and electrostatic forces, enabling them to compete on par with each other, but also activates new mechanical degrees of freedom, such as the macroscopic curvature of the heterostructure. In this work, an electrostatically driven transition from a predominantly out-of-plane polarized to an in-plane polarized state is observed when a PbTiO3/SrTiO3 superlattice with a SrRuO3 bottom electrode is released from its substrate. In turn, this polarization rotation modifies the lattice parameter mismatch between the superlattice and the thin SrRuO3 layer, causing the heterostructure to curl up into microtubes. Through a combination of synchrotron-based scanning X-ray diffraction imaging, Raman scattering, piezoresponse force microscopy, and scanning transmission electron microscopy, the crystalline structure and domain patterns of the curved superlattices are investigated, revealing a strong anisotropy in the domain structure and a complex mechanism for strain accommodation.@en

In oxide heterostructures, different materials are integrated into a single artificial crystal, resulting in a breaking of inversion symmetry across the heterointerfaces. A notable example is the interface between polar and nonpolar materials, where valence discontinuities lead to otherwise inaccessible charge and spin states. This approach paved the way for the discovery of numerous unconventional properties absent in the bulk constituents. However, control of the geometric structure of the electronic wave functions in correlated oxides remains an open challenge. Here, we create heterostructures consisting of ultrathin SrRuO3, an itinerant ferromagnet hosting momentum-space sources of Berry curvature, and LaAlO3, a polar wide-band-gap insulator. Transmission electron microscopy reveals an atomically sharp LaO/RuO2/SrO interface configuration, leading to excess charge being pinned near the LaAlO3/SrRuO3 interface. We demonstrate through magneto-optical characterization, theoretical calculations and transport measurements that the real-space charge reconstruction drives a reorganization of the topological charges in the band structure, thereby modifying the momentum-space Berry curvature in SrRuO3. Our results illustrate how the topological and magnetic features of oxides can be manipulated by engineering charge discontinuities at oxide interfaces.@en

Obtaining high-quality thin films of 5d transition metal oxides is essential to explore the exotic semimetallic and topological phases predicted to arise from the combination of strong electron correlations and spin-orbit coupling. Here, we show that the transport properties of SrIrO3 thin films, grown by pulsed laser deposition, can be optimized by considering the effect of laser-induced modification of the SrIrO3 target surface. We further demonstrate that bare SrIrO3 thin films are subject to degradation in air and are highly sensitive to lithographic processing. A crystalline SrTiO3 cap layer deposited in-situ is effective in preserving the film quality, allowing us to measure metallic transport behavior in films with thicknesses down to 4 unit cells. In addition, the SrTiO3 encapsulation enables the fabrication of devices such as Hall bars without altering the film properties, allowing precise (magneto)transport measurements on micro- and nanoscale devices.@en

We report on the discovery and transport study of the superconducting ground state present at the (111)LaAlO3/SrTiO3 (LAO/STO) interface. The superconducting transition is consistent with a Berezinskii-Kosterlitz-Thouless transition and its two-dimensional nature is further corroborated by the anisotropy of the critical magnetic field, as calculated by Tinkham. The estimated superconducting layer thickness and coherence length are 10 and 60nm, respectively. The results of this work provide insight to clarify the microscopic details of superconductivity in LAO/STO interfaces, in particular in what concerns the link with orbital symmetry.@en

Three-dimensional strontium ruthenate (SrRuO3) is an itinerant ferromagnet that features Weyl points acting as sources of emergent magnetic fields, anomalous Hall conductivity, and unconventional spin dynamics. Integrating SrRuO3 in oxide heterostructures is potentially a novel route to engineer emergent electrodynamics, but its electronic band topology in the two-dimensional limit remains unknown. Here we show that ultrathin SrRuO3 exhibits spin-polarized topologically nontrivial bands at the Fermi energy. Their band anticrossings show an enhanced Berry curvature and act as competing sources of emergent magnetic fields. We control their balance by designing heterostructures with symmetric (SrTiO3/SrRuO3/SrTiO3 and SrIrO3/SrRuO3/SrIrO3) and asymmetric interfaces (SrTiO3/SrRuO3/SrIrO3). Symmetric structures exhibit an interface-tunable single-channel anomalous Hall effect, while ultrathin SrRuO3 embedded in asymmetric structures shows humplike features consistent with multiple Hall contributions. The band topology of two-dimensional SrRuO3 proposed here naturally accounts for these observations and harmonizes a large body of experimental results.@en

SrIrO 3, the three-dimensional member of the Ruddlesden–Popper iridates, is a paramagnetic semimetal characterised by a the delicate interplay between spin–orbit coupling and Coulomb repulsion. In this work, we study the anisotropic magnetoresistance (AMR) of SrIrO 3 thin films, which is closely linked to spin–orbit coupling and probes correlations between electronic transport, magnetic order and orbital states. We show that the low-temperature negative magnetoresistance is anisotropic with respect to the magnetic field orientation, and its angular dependence reveals the appearance of a fourfold symmetric component above a critical magnetic field. We show that this AMR component is of magnetocrystalline origin, and attribute the observed transition to a field-induced magnetic state in SrIrO 3.@en

We investigate the thickness-dependent electronic properties of ultrathin SrIrO3 and discover a transition from a semimetallic to a correlated insulating state below 4 unit cells. Low-temperature magnetoconductance measurements show that spin fluctuations in the semimetallic state are significantly enhanced while approaching the transition point. The electronic properties are further studied by scanning tunneling spectroscopy, showing that 4 unit cell SrIrO3 is on the verge of a gap opening. Our density functional theory calculations reproduce the critical thickness of the transition and show that the opening of a gap in ultrathin SrIrO3 requires antiferromagnetic order.@en

Quantum confinement at complex oxide interfaces establishes an intricate hierarchy of the strongly correlated d orbitals which is widely recognized as a source of emergent physics. The most prominent example is the (001) LaAlO3/SrTiO3 (LAO/STO) interface, which features a dome-shaped phase diagram of superconducting critical temperature and spin-orbit coupling (SOC) as a function of electrostatic doping, arising from a selective occupancy of t2g orbitals of different character. Here we study (111)-oriented LAO/STO interfaces, where the three t2g orbitals contribute equally to the subband states caused by confinement, and investigate the impact of this unique feature on electronic transport. We show that transport occurs through two sets of electronlike subbands, and the carrier density of one of the sets shows a nonmonotonic dependence on the sample conductance. Using tight-binding modeling, we demonstrate that this behavior stems from a band inversion driven by on-site Coulomb interactions. The balanced contribution of all t2g orbitals to electronic transport is shown to result in strong SOC with reduced electrostatic modulation.@en

Ultrafast photodoping of the Mott insulators, possessing strong correlation between electronic and magnetic degrees of freedom, holds promise for launching an ultrafast dynamics of spins which cannot be described in terms of conventional models of ultrafast magnetism. Here we study the ultrafast laser-induced dynamics of the magnetic order in a novel spin-orbit Mott insulator Sr2IrO4 featuring an uncompensated pattern of antiferromagnetic spin ordering. Using the transient magneto-optical Kerr effect sensitive to the net magnetization, we reveal that photodoping by femtosecond laser pulses with photon energy above the Mott gap launches melting of the antiferromagnetic order seen as ultrafast demagnetization with a characteristic time of 300 fs followed by a sub-10-ps recovery. Nonequilibrium dynamical mean-field theory calculations based on the single-band Hubbard model confirm that ultrafast demagnetization is primarily governed by the laser-induced generation of electron-hole pairs, although the precise simulated time dependencies are rather different from the experimentally observed ones. To describe the experimental results, here we suggest a phenomenological model which is based on Onsager's formalism and accounts for the photogenerated electron-hole pairs using the concepts of holons and doublons.@en

Relating the band structure of correlated semimetals to their transport properties is a complex and often open issue. The partial occupation of numerous electron and hole bands can result in properties that are seemingly in contrast with one another, complicating the extraction of the transport coefficients of different bands. The 5d oxide SrIrO3 hosts parabolic bands of heavy holes and light electrons in gapped Dirac cones due to the interplay between electron-electron interactions and spin-orbit coupling. We present a multifold approach relying on different experimental techniques and theoretical calculations to disentangle its complex electronic properties. By combining magnetotransport and thermoelectric measurements in a field-effect geometry with first-principles calculations, we quantitatively determine the transport coefficients of different conduction channels. Despite their different dispersion relationships, electrons and holes are found to have strikingly similar transport coefficients, yielding a holelike response under field-effect and thermoelectric measurements and a linear electronlike Hall effect up to 33 T.@en

Isolation and characterization of mechanically exfoliated black phosphorus flakes with a thickness down to two single-layers is presented. A modification of the mechanical exfoliation method, which provides higher yield of atomically thin flakes than conventional mechanical exfoliation, has been developed. We present general guidelines to determine the number of layers using optical microscopy, Raman spectroscopy and transmission electron microscopy (TEM) in a fast and reliable way. Moreover, we demonstrate that the exfoliated flakes are highly crystalline and that they are stable even in free-standing form through Raman spectroscopy and TEM measurements. A strong thickness dependence of the band structure is found by density functional theory (DFT) calculations. The exciton binding energy, within an effective mass approximation, is also calculated for different number of layers. Our computational results for the optical gap are consistent with preliminary photoluminescence results on thin flakes. Finally, we study the environmental stability of black phosphorus flakes finding that the flakes are very hydrophilic and that long term exposure to air moisture etches black phosphorus away. Nonetheless, we demonstrate that the aging of the flakes is slow enough to allow fabrication of field-effect transistors with strong ambipolar behavior. DFT calculations also give us insight into the water-induced changes of the structural and electronic properties of black phosphorus.@en

Isolation and characterization of mechanically exfoliated black phosphorus flakes with a thickness down to two single-layers is presented. A modification of the mechanical exfoliation method, which provides higher yield of atomically thin flakes than conventional mechanical exfoliation, has been developed. We present general guidelines to determine the number of layers using optical microscopy, Raman spectroscopy and transmission electron microscopy (TEM) in a fast and reliable way. Moreover, we demonstrate that the exfoliated flakes are highly crystalline and that they are stable even in free-standing form through Raman spectroscopy and TEM measurements. A strong thickness dependence of the band structure is found by density functional theory (DFT) calculations. The exciton binding energy, within an effective mass approximation, is also calculated for different number of layers. Our computational results for the optical gap are consistent with preliminary photoluminescence results on thin flakes. Finally, we study the environmental stability of black phosphorus flakes finding that the flakes are very hydrophilic and that long term exposure to air moisture etches black phosphorus away. Nonetheless, we demonstrate that the aging of the flakes is slow enough to allow fabrication of field-effect transistors with strong ambipolar behavior. DFT calculations also give us insight into the water-induced changes of the structural and electronic properties of black phosphorus.@en