Extreme magnetoresistance at high-mobility oxide heterointerfaces with dynamic defect tunability.

Magnetic field-induced changes in the electrical resistance of materials reveal insights into the fundamental properties governing their electronic and magnetic behavior. Various classes of magnetoresistance have been realized, including giant, colossal, and extraordinary magnetoresistance, each with distinct physical origins. In recent years, extreme magnetoresistance (XMR) has been observed in topological and non-topological materials displaying a non-saturating magnetoresistance reaching 103-108% in magnetic fields up to 60 T. XMR is often intimately linked to a gapless band structure with steep bands and charge compensation. Here, we show that a linear XMR of 80,000% at 15 T and 2 K emerges at the high-mobility interface between the large band-gap oxides γ-Al2O3 and SrTiO3. Despite the chemically and electronically very dissimilar environment, the temperature/field phase diagrams of γ-Al2O3/SrTiO3 bear a striking resemblance to XMR semimetals. By comparing magnetotransport, microscopic current imaging, and momentum-resolved band structures, we conclude that the XMR in γ-Al2O3/SrTiO3 is not strongly linked to the band structure, but arises from weak disorder enforcing a squeezed guiding center motion of electrons. We also present a dynamic XMR self-enhancement through an autonomous redistribution of quasi-mobile oxygen vacancies. Our findings shed new light on XMR and introduce tunability using dynamic defect engineering.

Induced giant piezoelectricity in centrosymmetric oxides.

Piezoelectrics are materials that linearly deform in response to an applied electric field. As a fundamental prerequisite, piezoelectric materials must have a noncentrosymmetric crystal structure. For more than a century, this has remained a major obstacle for finding piezoelectric materials. We circumvented this limitation by breaking the crystallographic symmetry and inducing large and sustainable piezoelectric effects in centrosymmetric materials by the electric field-induced rearrangement of oxygen vacancies. Our results show the generation of extraordinarily large piezoelectric responses [with piezoelectric strain coefficients (d33) of ~200,000 picometers per volt at millihertz frequencies] in cubic fluorite gadolinium-doped CeO2-x films, which are two orders of magnitude larger than the responses observed in the presently best-known lead-based piezoelectric relaxor-ferroelectric oxide at kilohertz frequencies. These findings provide opportunities to design piezoelectric materials from environmentally friendly centrosymmetric ones.

The emergence of magnetic ordering at complex oxide interfaces tuned by defects.

Complex oxides show extreme sensitivity to structural distortions and defects, and the intricate balance of competing interactions which emerge at atomically defined interfaces may give rise to unexpected physics. In the interfaces of non-magnetic complex oxides, one of the most intriguing properties is the emergence of magnetism which is sensitive to chemical defects. Particularly, it is unclear which defects are responsible for the emergent magnetic interfaces. Here, we show direct and clear experimental evidence, supported by theoretical explanation, that the B-site cation stoichiometry is crucial for the creation and control of magnetism at the interface between non-magnetic ABO3-perovskite oxides, LaAlO3 and SrTiO3. We find that consecutive defect formation, driven by atomic charge compensation, establishes the formation of robust perpendicular magnetic moments at the interface. Our observations propose a route to tune these emerging magnetoelectric structures, which are strongly coupled at the polar-nonpolar complex oxide interfaces.

Thermodynamic Ground States of Complex Oxide Heterointerfaces.

The formation mechanism of 2-dimensional electron gases (2DEGs) at heterointerfaces between nominally insulating oxides is addressed with a thermodynamical approach. We provide a comprehensive analysis of the thermodynamic ground states of various 2DEG systems directly probed in high temperature equilibrium conductivity measurements. We unambiguously identify two distinct classes of oxide heterostructures: For epitaxial perovskite/perovskite heterointerfaces (LaAlO3/SrTiO3, NdGaO3/SrTiO3, and (La,Sr)(Al,Ta)O3/SrTiO3), we find the 2DEG formation being based on charge transfer into the interface, stabilized by the electric field in the space charge region. In contrast, for amorphous LaAlO3/SrTiO3 and epitaxial γ-Al2O3/SrTiO3 heterostructures, the 2DEG formation mainly relies on the formation and accumulation of oxygen vacancies. This class of 2DEG structures exhibits an unstable interface reconstruction associated with a quenched nonequilibrium state.

Evidence for lattice-polarization-enhanced field effects at the SrTiO3-based heterointerface.

Electrostatic gating provides a powerful approach to tune the conductivity of the two-dimensional electron liquid between two insulating oxides. For the LaAlO3/SrTiO3 (LAO/STO) interface, such gating effect could be further enhanced by a strong lattice polarization of STO caused by simultaneous application of gate field and illumination light. Herein, by monitoring the discharging process upon removing the gate field, we give firm evidence for the occurrence of this lattice polarization at the amorphous-LaAlO3/SrTiO3 interface. Moreover, we find that the lattice polarization is accompanied with a large expansion of the out-of-plane lattice of STO. Photo excitation affects the polarization process by accelerating the field-induced lattice expansion. The present work demonstrates the great potential of combined stimuli in exploring emergent phenomenon at complex oxide interfaces.

Extreme mobility enhancement of two-dimensional electron gases at oxide interfaces by charge-transfer-induced modulation doping.

Two-dimensional electron gases (2DEGs) formed at the interface of insulating complex oxides promise the development of all-oxide electronic devices. These 2DEGs involve many-body interactions that give rise to a variety of physical phenomena such as superconductivity, magnetism, tunable metal-insulator transitions and phase separation. Increasing the mobility of the 2DEG, however, remains a major challenge. Here, we show that the electron mobility is enhanced by more than two orders of magnitude by inserting a single-unit-cell insulating layer of polar La(1-x)Sr(x)MnO3 (x = 0, 1/8, and 1/3) at the interface between disordered LaAlO3 and crystalline SrTiO3 produced at room temperature. Resonant X-ray spectroscopy and transmission electron microscopy show that the manganite layer undergoes unambiguous electronic reconstruction, leading to modulation doping of such atomically engineered complex oxide heterointerfaces. At low temperatures, the modulation-doped 2DEG exhibits Shubnikov-de Haas oscillations and fingerprints of the quantum Hall effect, demonstrating unprecedented high mobility and low electron density.

Visible-light-enhanced gating effect at the LaAlO3/SrTiO3 interface.

Electrostatic gating field and light illumination are two widely used stimuli for semiconductor devices. Via capacitive effect, a gate field modifies the carrier density of the devices, while illumination generates extra carriers by exciting trapped electrons. Here we report an unusual illumination-enhanced gating effect in a two-dimensional electron gas at the LaAlO3/SrTiO3 interface, which has been the focus of emergent phenomena exploration. We find that light illumination decreases, rather than increases, the carrier density of the gas when the interface is negatively gated through the SrTiO3 layer, and the density drop can be 20 times as large as that caused by the conventional capacitive effect. This effect is further found to stem from an illumination-accelerated interface polarization, an originally extremely slow process. This unusual effect provides a promising controlling of the correlated oxide electronics in which a much larger gating capacity is demanding due to their intrinsic larger carrier density.

Room temperature formation of high-mobility two-dimensional electron gases at crystalline complex oxide interfaces.

Well-controlled sub-unit-cell layer-bylayer epitaxial growth of spinel alumina is achieved at room temperature on a TiO2 -terminated SrTiO3 single-crystalline substrate. By tailoring the interface redox reaction, 2D electron gases with mobilities exceeding 3000 cm 2 V(-1) s(-1) are achieved at this novel oxide interface.

A high-mobility two-dimensional electron gas at the spinel/perovskite interface of γ-Al2O3/SrTiO3.

The discovery of two-dimensional electron gases at the heterointerface between two insulating perovskite-type oxides, such as LaAlO(3) and SrTiO(3), provides opportunities for a new generation of all-oxide electronic devices. Key challenges remain for achieving interfacial electron mobilities much beyond the current value of approximately 1,000 cm(2) V(-1) s(-1) (at low temperatures). Here we create a new type of two-dimensional electron gas at the heterointerface between SrTiO(3) and a spinel γ-Al(2)O(3) epitaxial film with compatible oxygen ions sublattices. Electron mobilities more than one order of magnitude higher than those of hitherto-investigated perovskite-type interfaces are obtained. The spinel/perovskite two-dimensional electron gas, where the two-dimensional conduction character is revealed by quantum magnetoresistance oscillations, is found to result from interface-stabilized oxygen vacancies confined within a layer of 0.9 nm in proximity to the interface. Our findings pave the way for studies of mesoscopic physics with complex oxides and design of high-mobility all-oxide electronic devices.

Large anisotropy in colossal magnetoresistance of charge orbital ordered epitaxial Sm(0.5)Ca(0.5)MnO(3) films.

We investigated the structure and magnetotransport properties of Sm(0.5)Ca(0.5)MnO(3) (SCMO) films epitaxially grown on (011)-oriented SrTiO(3) substrates, which exhibited clear charge/orbital ordering transition. A significant anisotropy of ∼1000 in the colossal magnetoresistance (CMR) effect was observed in the films with a thickness between 50 and 80 nm, which was distinctly different from the basically isotropic CMR effect in bulk SCMO. The large anisotropy in the CMR can be ascribed to the intrinsic asymmetric strain in the film, which plays an important role in tuning the spin-orbit coupling in manganite films. The origin of the peculiar CMR effect is discussed.

Indirect measurement of the magnetocaloric effect using a novel differential scanning calorimeter with magnetic field.

A simple and high-sensitivity differential scanning calorimeter (DSC) unit operating under magnetic field has been built for indirect determination of the magnetocaloric effect. The principle of the measuring unit in the calorimeter is based on Peltier elements as heat flow sensors. The high sensitivity of the apparatus combined with a suitable calibration procedure allows very fast and accurate heat capacity measurements under magnetic field to be made. The device was validated from heat capacity measurements for the typical DSC reference material gallium (Ga) and a La(0.67)Ca(0.33)MnO(3) manganite system and the results were highly consistent with previous reported data for these materials. The DSC has a working range from 200 to 340 K and has been tested in magnetic fields reaching 1.8 T. The signal-to-noise ratio is in the range of 10(2)-10(3) for the described experiments. Finally the results have been compared to results from a Quantum Design(R) physical properties measuring system. The configuration of the system also has the advantage of being able to operate with other types of magnets, e.g., permanent magnets or superconducting coils, as well as the ability to be expanded to a wider temperature range.

A versatile magnetic refrigeration test device.

A magnetic refrigeration test device has been built and tested. The device allows variation and control of many important experimental parameters, such as the type of heat transfer fluid, the movement of the heat transfer fluid, the timing of the refrigeration cycle, and the magnitude of the applied magnetic field. An advanced two-dimensional numerical model has previously been implemented in order to help in the optimization of the design of a refrigeration test device. Qualitative agreement between the results from model and the experimental results is demonstrated for each of the four different parameter variations mentioned above.