M. S. Rzchowski

Tunneling electroresistance effect in ferroelectric tunnel junctions at the nanoscale.

Using a set of scanning probe microscopy techniques, we demonstrate the reproducible tunneling electroresistance effect on nanometer-thick epitaxial BaTiO(3) single-crystalline thin films on SrRuO(3) bottom electrodes. Correlation between ferroelectric and electronic transport properties is established by direct nanoscale visualization and control of polarization and tunneling current. The obtained results show a change in resistance by about 2 orders of magnitude upon polarization reversal on a lateral scale of 20 nm at room temperature. These results are promising for employing ferroelectric tunnel junctions in nonvolatile memory and logic devices.

Ferroelastic switching for nanoscale non-volatile magnetoelectric devices

Multiferroics, where (anti-) ferromagnetic, ferroelectric and ferroelastic order parameters coexist, enable manipulation of magnetic ordering by an electric field through switching of the electric polarization. It has been shown that realization of magnetoelectric coupling in a single-phase multiferroic such as BiFeO(3) requires ferroelastic (71 degrees, 109 degrees) rather than ferroelectric (180 degrees) domain switching. However, the control of such ferroelastic switching in a single-phase system has been a significant challenge as elastic interactions tend to destabilize small switched volumes, resulting in subsequent ferroelastic back-switching at zero electric field, and thus the disappearance of non-volatile information storage. Guided by our phase-field simulations, here we report an approach to stabilize ferroelastic switching by eliminating the stress-induced instability responsible for back-switching using isolated monodomain BiFeO(3) islands. This work demonstrates a critical step to control and use non-volatile magnetoelectric coupling at the nanoscale. Beyond magnetoelectric coupling, it provides a framework for exploring a route to control multiple order parameters coupled to ferroelastic order in other low-symmetry materials.

Tailoring a two-dimensional electron gas at the LaAlO3/SrTiO3 (001) interface by epitaxial strain

Recently a metallic state was discovered at the interface between insulating oxides, most notably LaAlO3 and SrTiO3. Properties of this two-dimensional electron gas (2DEG) have attracted significant interest due to its potential applications in nanoelectronics. Control over this carrier density and mobility of the 2DEG is essential for applications of these unique systems, and may be achieved by epitaxial strain. However, despite the rich nature of strain effects on oxide materials properties, such as ferroelectricity, magnetism, and superconductivity, the relationship between the strain and electrical properties of the 2DEG at the LaAlO3/SrTiO3 heterointerface remains largely unexplored. Here, we use different lattice constant single-crystal substrates to produce LaAlO3/SrTiO3 interfaces with controlled levels of biaxial epitaxial strain. We have found that tensile-strained SrTiO3 destroys the conducting 2DEG, while compressively strained SrTiO3 retains the 2DEG, but with a carrier concentration reduced in comparison to the unstrained LaAlO3/SrTiO3 interface. We have also found that the critical LaAlO3 overlayer thickness for 2DEG formation increases with SrTiO3 compressive strain. Our first-principles calculations suggest that a strain-induced electric polarization in the SrTiO3 layer is responsible for this behavior. The polarization is directed away from the interface and hence creates a negative polarization charge opposing that of the polar LaAlO3 layer. This behavior both increases the critical thickness of the LaAlO3 layer, and reduces carrier concentration above the critical thickness, in agreement with our experimental results. Our findings suggest that epitaxial strain can be used to tailor 2DEGs properties of the LaAlO3/SrTiO3 heterointerface.

Metallic and Insulating Oxide Interfaces Controlled by Electronic Correlations

The strength of electronic correlations dictates the transport properties of oxide interfaces. The formation of two-dimensional electron gases (2DEGs) at complex oxide interfaces is directly influenced by the oxide electronic properties. We investigated how local electron correlations control the 2DEG by inserting a single atomic layer of a rare-earth oxide (RO) [(R is lanthanum (La), praseodymium (Pr), neodymium (Nd), samarium (Sm), or yttrium (Y)] into an epitaxial strontium titanate oxide (SrTiO3) matrix using pulsed-laser deposition with atomic layer control. We find that structures with La, Pr, and Nd ions result in conducting 2DEGs at the inserted layer, whereas the structures with Sm or Y ions are insulating. Our local spectroscopic and theoretical results indicate that the interfacial conductivity is dependent on electronic correlations that decay spatially into the SrTiO3 matrix. Such correlation effects can lead to new functionalities in designed heterostructures.

Creation of a two-dimensional electron gas at an oxide interface on silicon

In recent years, reversible control over metal-insulator transition has been shown, at the nanoscale, in a two-dimensional electron gas (2DEG) formed at the interface between two complex oxides. These materials have thus been suggested as possible platforms for developing ultrahigh-density oxide nanoelectronics. A prerequisite for the development of these new technologies is the integration with existing semiconductor electronics platforms. Here, we demonstrate room-temperature conductivity switching of 2DEG nanowires formed at atomically sharp LaAlO(3)/SrTiO(3) (LAO/STO) heterointerfaces grown directly on (001) Silicon (Si) substrates. The room-temperature electrical transport properties of LAO/STO heterointerfaces on Si are comparable with those formed from a SrTiO(3) bulk single crystal. The ability to form reversible conducting nanostructures directly on Si wafers opens new opportunities to incorporate ultrahigh-density oxide nanoelectronic memory and logic elements into well-established Si-based platforms.

Switchable induced polarization in LaAlO3/SrTiO3 heterostructures.

Demonstration of a tunable conductivity of the LaAlO(3)/SrTiO(3) interfaces drew significant attention to the development of oxide electronic structures where electronic confinement can be reduced to the nanometer range. While the mechanisms for the conductivity modulation are quite different and include metal-insulator phase transition and surface charge writing, generally it is implied that this effect is a result of electrical modification of the LaAlO(3) surface (either due to electrochemical dissociation of surface adsorbates or free charge deposition) leading to the change in the two-dimensional electron gas (2DEG) density at the LaAlO(3)/SrTiO(3) (LAO/STO) interface. In this paper, using piezoresponse force microscopy we demonstrate a switchable electromechanical response of the LAO overlayer, which we attribute to the motion of oxygen vacancies through the LAO layer thickness. These electrically induced reversible changes in bulk stoichiometry of the LAO layer are a signature of a possible additional mechanism for nanoscale oxide 2DEG control on LAO/STO interfaces.

Anisotropic magnetoresistance in tetragonal La1-xCaxMnOδ thin films

We have fabricated thin films of La1−xCaxMnOδ with tetragonal symmetry. For low temperatures and magnetic fields the measured magnetoresistance is anisotropic: initially positive for applied magnetic field perpendicular to the film plane and negative for field applied parallel to the film plane. At high temperatures the magnetoresistance is negative for all fields and field orientations. We also observe an in‐plane magnetoresistance anisotropy with an angular dependence corresponding to that observed in transition metal ferromagnets. We suggest an interpretation requiring a substantial spin‐orbit interaction in the material.

Positive exchange bias in ferromagnetic La0.67Sr0.33MnO3∕SrRuO3 bilayers

Epitaxial La0.67Sr0.33MnO3(LSMO)∕SrRuO3(SRO) ferromagnetic bilayers have been grown on (001)SrTiO3(STO) substrates by pulsed laser deposition with atomic layer control. We observe a shift in the magnetic hysteresis loop of the LSMO layer in the same direction as the applied biasing field (positive exchange bias). The effect is not present above the Curie temperature of the SRO layer (TcSRO), and its magnitude increases rapidly as the temperature is lowered below TcSRO. The direction of the shift is consistent with an antiferromagnetic exchange coupling between the ferromagnetic LSMO layer and the ferromagnetic SRO layer. We propose that atomic layer charge transfer modifies the electronic state at the interface, resulting in the observed antiferromagnetic interfacial exchange coupling.

Enhancement of Ferroelectric Polarization Stability by Interface Engineering

By using theoretical predictions based on first-principle calculations, we explore an interface engineering approach to stabilize polarization states in ferroelectric heterostructures with a thickness of just several nanometers.

Polar metals by geometric design

Gauss’s law dictates that the net electric field inside a conductor in electrostatic equilibrium is zero by effective charge screening; free carriers within a metal eliminate internal dipoles that may arise owing to asymmetric charge distributions. Quantum physics supports this view, demonstrating that delocalized electrons make a static macroscopic polarization, an ill-defined quantity in metals—it is exceedingly unusual to find a polar metal that exhibits long-range ordered dipoles owing to cooperative atomic displacements aligned from dipolar interactions as in insulating phases. Here we describe the quantum mechanical design and experimental realization of room-temperature polar metals in thin-film ANiO3 perovskite nickelates using a strategy based on atomic-scale control of inversion-preserving (centric) displacements. We predict with ab initio calculations that cooperative polar A cation displacements are geometrically stabilized with a non-equilibrium amplitude and tilt pattern of the corner-connected NiO6 octahedra—the structural signatures of perovskites—owing to geometric constraints imposed by the underlying substrate. Heteroepitaxial thin-films grown on LaAlO3 (111) substrates fulfil the design principles. We achieve both a conducting polar monoclinic oxide that is inaccessible in compositionally identical films grown on (001) substrates, and observe a hidden, previously unreported, non-equilibrium structure in thin-film geometries. We expect that the geometric stabilization approach will provide novel avenues for realizing new multifunctional materials with unusual coexisting properties.