Coherent Bragg nanodiffraction at the hard X-ray Nanoprobe beamline.

Bragg coherent diffraction with nanofocused hard X-ray beams provides unique opportunities for quantitative in situ studies of crystalline structure in nanoscale regions of complex materials and devices by a variety of diffraction-based techniques. In the case of coherent diffraction imaging, a major experimental challenge in using nanoscale coherent beams is maintaining a constant scattering volume such that coherent fringe visibility is maximized and maintained over the course of an exposure lasting several seconds. Here, we present coherent Bragg diffraction patterns measured from different nanostructured thin films at the Sector 26 Nanoprobe beamline at the Advanced Photon Source and demonstrate that with nanoscale positional control, coherent diffraction patterns can be measured with source-limited fringe visibilities more than 50% suitable for imaging by coherent Bragg ptychography techniques.

Imaging local polarization in ferroelectric thin films by coherent x-ray Bragg projection ptychography.

We used x-ray Bragg projection ptychography (BPP) to map spatial variations of ferroelectric polarization in thin film PbTiO3, which exhibited a striped nanoscale domain pattern on a high-miscut (001) SrTiO3 substrate. By converting the reconstructed BPP phase image to picometer-scale ionic displacements in the polar unit cell, a quantitative polarization map was made that was consistent with other characterization. The spatial resolution of 5.7 nm demonstrated here establishes BPP as an important tool for nanoscale ferroelectric domain imaging, especially in complex environments accessible with hard x rays.

Artificially engineered superlattices of pnictide superconductors.

Significant progress has been achieved in fabricating high-quality bulk and thin-film iron-based superconductors. In particular, artificial layered pnictide superlattices offer the possibility of tailoring the superconducting properties and understanding the mechanism of the superconductivity itself. For high-field applications, large critical current densities (J(c)) and irreversibility fields (H(irr)) are indispensable along all crystal directions. On the other hand, the development of superconducting devices such as tunnel junctions requires multilayered heterostructures. Here we show that artificially engineered undoped Ba-122/Co-doped Ba-122 compositionally modulated superlattices produce ab-aligned nanoparticle arrays. These layer and self-assemble along c-axis-aligned defects, and combine to produce very large J(c) and H(irr) enhancements over a wide angular range. We also demonstrate a structurally modulated SrTiO3(STO)/Co-doped Ba-122 superlattice with sharp interfaces. Success in superlattice fabrication involving pnictides will aid the progress of heterostructured systems exhibiting new interfacial phenomena and device applications.

Modular instrument mounting system for variable environment in operando X-ray experiments.

In the growing field of in operando and in situ X-ray experiments, there exists a large disparity in the types of environments and equipment to control them. This situation makes it challenging to conduct multiple experiments with a single mechanical interface to the diffractometer. Here, we describe the design and implementation of a modular instrument mounting system that can be installed on a standard six-circle diffractometer (e.g., 5021 Huber GmbH). This new system allows for the rapid changeover of different chambers and sample heaters and permits accurate sample positioning (x, y, z, and azimuthal rotation) without rigid coupling to the chamber body. Isolation of the sample motion from the chamber enclosure is accomplished through a combination of custom rotary seals and bellows. Control of the pressure and temperature has been demonstrated in the ranges of 10(-6)-10(3) Torr and 25°C-900°C, respectively. We have utilized the system with several different modular instruments. As an example, we provide in situ sputtering results, where the growth dynamics of epitaxial LaGaO3 thin films on (001) SrTiO3 substrates were investigated.

Evidence for charge-vortex duality at the LaAlO3/SrTiO3 interface.

The concept of duality has proved extremely powerful in extending our understanding in many areas of physics. Charge-vortex duality has been proposed as a model to understand the superconductor to insulator transition in disordered thin films and Josephson junction arrays. In this model, on the superconducting side, one has delocalized Cooper pairs but localized vortices; while on the insulating side, one has localized Cooper pairs but mobile vortices. Here we show a new experimental manifestation of this duality in the electron gas that forms at the interface between LaAlO(3) and SrTiO(3). The effect is due to the motion of vortices generated by the magnetization dynamics of the ferromagnet that also forms at the same interface, which results in an increase in resistance on the superconducting side of the transition, but an increase in conductance on the insulating side.

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.

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.

Giant piezoelectricity on Si for hyperactive MEMS.

Microelectromechanical systems (MEMS) incorporating active piezoelectric layers offer integrated actuation, sensing, and transduction. The broad implementation of such active MEMS has long been constrained by the inability to integrate materials with giant piezoelectric response, such as Pb(Mg(1/3)Nb(2/3))O(3)-PbTiO(3) (PMN-PT). We synthesized high-quality PMN-PT epitaxial thin films on vicinal (001) Si wafers with the use of an epitaxial (001) SrTiO(3) template layer with superior piezoelectric coefficients (e(31,f) = -27 ± 3 coulombs per square meter) and figures of merit for piezoelectric energy-harvesting systems. We have incorporated these heterostructures into microcantilevers that are actuated with extremely low drive voltage due to thin-film piezoelectric properties that rival bulk PMN-PT single crystals. These epitaxial heterostructures exhibit very large electromechanical coupling for ultrasound medical imaging, microfluidic control, mechanical sensing, and energy harvesting.

Coexistence of superconductivity and ferromagnetism in two dimensions.

Ferromagnetism is usually considered to be incompatible with conventional superconductivity, as it destroys the singlet correlations responsible for the pairing interaction. Superconductivity and ferromagnetism are known to coexist in only a few bulk rare-earth materials. Here we report evidence for their coexistence in a two-dimensional system: the interface between two bulk insulators, LaAlO(3) (LAO) and SrTiO(3) (STO), a system that has been studied intensively recently. Magnetoresistance, Hall, and electric-field dependence measurements suggest that there are two distinct bands of charge carriers that contribute to the interface conductivity. The sensitivity of properties of the interface to an electric field makes this a fascinating system for the study of the interplay between superconductivity and magnetism.

Metallic and insulating oxide interfaces controlled by electronic correlations.

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 (SrTiO(3)) 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 SrTiO(3) 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.

Ferroelectricity in strain-free SrTiO3 thin films.

Biaxial strain is known to induce ferroelectricity in thin films of nominally nonferroelectric materials such as SrTiO3. By a direct comparison of the strained and strain-free SrTiO3 films using dielectric, ferroelectric, Raman, nonlinear optical and nanoscale piezoelectric property measurements, we conclude that all SrTiO3 films and bulk crystals are relaxor ferroelectrics, and the role of strain is to stabilize longer-range correlation of preexisting nanopolar regions, likely originating from minute amounts of unintentional Sr deficiency in nominally stoichiometric samples. These findings highlight the sensitive role of stoichiometry when exploring strain and epitaxy-induced electronic phenomena in oxide films, heterostructures, and interfaces.

Template engineering of Co-doped BaFe2As2 single-crystal thin films.

Understanding new superconductors requires high-quality epitaxial thin films to explore intrinsic electromagnetic properties and evaluate device applications. So far, superconducting properties of ferropnictide thin films seem compromised by imperfect epitaxial growth and poor connectivity of the superconducting phase. Here we report new template engineering using single-crystal intermediate layers of (001) SrTiO(3) and BaTiO(3) grown on various perovskite substrates that enables genuine epitaxial films of Co-doped BaFe(2)As(2) with a high transition temperature (T(c,rho=0) of 21.5 K, where rho=resistivity), a small transition width (DeltaT(c)=1.3 K), a superior critical current density J(c) of 4.5 MA cm(-2) (4.2 K) and strong c-axis flux pinning. Implementing SrTiO(3) or BaTiO(3) templates to match the alkaline-earth layer in the Ba-122 with the alkaline-earth/oxygen layer in the templates opens new avenues for epitaxial growth of ferropnictides on multifunctional single-crystal substrates. Beyond superconductors, it provides a framework for growing heteroepitaxial intermetallic compounds on various substrates by matching interfacial layers between templates and thin-film overlayers.

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.

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.

Strain-induced polarization rotation in epitaxial (001) BiFeO3 thin films.

Direct measurement of the remanent polarization of high quality (001)-oriented epitaxial BiFeO3 thin films shows a strong strain dependence, even larger than conventional (001)-oriented PbTiO3 films. Thermodynamic analysis reveals that a strain-induced polarization rotation mechanism is responsible for the large change in the out-of-plane polarization of (001) BiFeO3 with biaxial strain while the spontaneous polarization itself remains almost constant.

Magnetic color symmetry of lattice rotations in a diamagnetic material.

Oxygen octahedral rotations are the most common phase transitions in perovskite crystal structures. Here we show that the color symmetry of such pure elastic distortions is isomorphic to magnetic point groups, which allows their probing through distinguishing polar versus magnetic symmetry. We demonstrate this isomorphism using nonlinear optical probing of the octahedral rotational transition in a compressively strained SrTiO3 thin film that exhibits ferroelectric (4mm) and antiferrodistortive (4{'}mm{'}) phases evolving through independent phase transitions. The approach has broader applicability for probing materials with lattice rotations that can be mapped to color groups.