Interface Design Beyond Epitaxy: Oxide Heterostructures Comprising Symmetry-forbidden Interfaces.

Epitaxial growth of thin-film heterostructures is generally considered the most successful procedure to obtain interfaces of excellent structural and electronic quality between three-dimensional materials. However, these interfaces can only join material systems with crystal lattices of matching symmetries and lattice constants. We present a novel category of interfaces, the fabrication of which is membrane-based and does not require epitaxial growth. These interfaces therefore overcome limitations imposed by epitaxy. Leveraging the additional degrees of freedom gained, we demonstrate atomically clean interfaces between three-fold symmetric sapphire and four-fold symmetric SrTiO3. Atomic-resolution imaging reveals structurally well-defined interfaces with a novel moiré-type reconstruction. This article is protected by copyright. All rights reserved.

Transport and Nonreciprocity in Monitored Quantum Devices: An Exact Study.

We study noninteracting fermionic systems undergoing continuous monitoring and driven by biased reservoirs. Averaging over the measurement outcomes, we derive exact formulas for the particle and heat flows in the system. We show that these currents feature competing elastic and inelastic components, which depend nontrivially on the monitoring strength γ. We highlight that monitor-induced inelastic processes lead to nonreciprocal currents, allowing one to extract work from measurements without active feedback control. We illustrate our formalism with two distinct monitoring schemes providing measurement-induced power or cooling. Optimal performances are found for values of the monitoring strength γ, which are hard to address with perturbative approaches.

Long-Range Atomic Order on Double-Stepped Al2O3(0001) Surfaces.

The deterministic preparation of highly ordered single-crystalline surfaces is a key step for studying and utilizing the physical properties of various advanced materials. This paper presents the fast and straightforward preparation of vicinal Al2O3(0001) surfaces with micrometer-scale atomic order. Crisp electron-diffraction spots up to at least 20th order evidence atomic coherence on terraces with widths exceeding 1 µm. The unique combination of three properties of Al2O3(0001) underlie this remarkable coherence: its high-temperature stability; the differences in the ionic bonding systems of the surface as compared to the bulk; and the fact that the terraces are non-polar whereas the step edges have a polar character. The step edges are furthermore found to have alternating configurations, which drive a step-doubling transition. On double-stepped surfaces, the Al-rich ( 31 × 31 ) R ± 9 $(\sqrt {31}\times \sqrt {31})\textrm {R}\pm 9$ ° surface reconstruction attains a singular in-plane orientation. These results set a benchmark for high-quality surface preparation and thus expand the scope for both fundamental studies on and the technological utilization of exciting material systems.

Self-Assembly of Nanocrystalline Structures from Freestanding Oxide Membranes.

The exploration of crystalline nanostructures enhances the understanding of quantum phenomena occurring in spatially confined quantum matter and may lead to functional materials with unforeseen applications. A novel route to fabricating nanocrystalline oxide structures of exceptional quality is presented. This is achieved by utilizing a self-assembly process of ultrathin membranes composed of the desired oxide. The thermally induced self-assembly of nanocrystalline structures is driven by dewetting the oxide membranes once they are lifted off and transferred onto sapphire surfaces. In three successive steps, the process provides nanovoids, nanowires, and nanocrystals. Regardless of substrate orientation, the nanostructures are highly anisotropic in shape due to material retraction favoring low-index crystalline lattice directions of the membranes. The orientation of the nanostructures is provided precisely by the crystal lattice of the transferred membrane. The microstructure of the nanocrystals exhibits exceptional quality, characterized by a pristine crystal structure and uniform stoichiometry, both maintained all the way down to the well-developed crystalline facets. The demonstrated self-assembly process holds the potential to improve the understanding of surface diffusion phenomena at the interface of materials, which is important for advancing epitaxial growth technology and paves the way to fabricating crystalline nanostructures by the transfer and self-assembly of membranes.

Inelastic Electron Tunneling Spectroscopy at High-Temperatures.

Ion conducting materials are critical components of batteries, fuel cells, and devices such as memristive switches. Analytical tools are therefore sought that allow the behavior of ions in solids to be monitored and analyzed with high spatial resolution and in real time. In principle, inelastic tunneling spectroscopy offers these capabilities. However, as its spectral resolution is limited by thermal softening of the Fermi-Dirac distribution, tunneling spectroscopy is usually constrained to cryogenic temperatures. This constraint would seem to render tunneling spectroscopy useless for studying ions in motion. Here, the first inelastic tunneling spectroscopy studies above room temperature are reported. For these measurements, high-temperature-stable tunnel junctions that incorporate within the tunnel barrier ultrathin layers for efficient proton conduction are developed. By analyzing the vibrational modes of OH bonds in BaZrO3 -based heterostructures, the detection of protons with a spectral resolution of 20 meV at 400 K (full-width-at-half maximum) is demonstrated. Overturning the hitherto existing prediction for the spectral resolution limit of 186 meV (5.4 kB T ) at 400 K, this resolution enables high-temperature tunneling spectroscopy of ion conductors. With these advances, inelastic tunneling spectroscopy constitutes a novel, valuable analytical tool for solid-state ionics.

An optimized TEM specimen preparation method of quantum nanostructures.

Electron transparent TEM lamella with unaltered microstructure and chemistry is the prerequisite for successful TEM explorations. Currently, TEM specimen preparation of quantum nanostructures, such as quantum dots (QDs), remains a challenge. In this work, we optimize the sample-preparation routine for achieving high-quality TEM specimens consisting of SrRuO3 (SRO) QDs grown on SrTiO3 (STO) substrates. We demonstrate that a combination of ion-beam-milling techniques can produce higher-quality specimens of quantum nanostructures compared to TEM specimens prepared by a combination of tripod polishing followed by Ar+ ion milling. In the proposed method, simultaneous imaging in a focused ion-beam device enables accurate positioning of the QD regions and assures the presence of dots in the thin lamella by cutting the sample inclined by 5° relative to the dots array. Furthermore, the preparation of TEM lamellae with several large electron-transparent regions that are separated by thicker walls effectively reduces the bending of the specimen and offers broad thin areas. The final use of a NanoMill efficiently removes the amorphous layer without introducing any additional damage.

Probing Charge Accumulation at SrMnO3/SrTiO3 Heterointerfaces via Advanced Electron Microscopy and Spectroscopy.

The last three decades have seen a growing trend toward studying the interfacial phenomena in complex oxide heterostructures. Of particular concern is the charge distribution at interfaces, which is a crucial factor in controlling the interface transport behavior. However, the study of the charge distribution is very challenging due to its small length scale and the intricate structure and chemistry at interfaces. Furthermore, the underlying origin of the interfacial charge distribution has been rarely studied in-depth and is still poorly understood. Here, by a combination of aberration-corrected scanning transmission electron microscopy (STEM) and spectroscopy techniques, we identify the charge accumulation in the SrMnO3 (SMO) side of SrMnO3/SrTiO3 heterointerfaces and find that the charge density attains the maximum of 0.13 ± 0.07 e-/unit cell (uc) at the first SMO monolayer. Based on quantitative atomic-scale STEM analyses and first-principle calculations, we explore the origin of interfacial charge accumulation in terms of epitaxial strain-favored oxygen vacancies, cationic interdiffusion, interfacial charge transfer, and space-charge effects. This study, therefore, provides a comprehensive description of the charge distribution and related mechanisms at the SMO/STO heterointerfaces, which is beneficial for the functionality manipulation via charge engineering at interfaces.

Direct Observation of Huge Flexoelectric Polarization around Crack Tips.

Flexoelectricity is especially relevant for nanoscale structures, and it is expected to be largest at the tip of cracks. We demonstrate the presence of a huge flexoelectric polarization at crack tips in SrTiO3 by direct observation with scanning transmission electron microscopy. We observe an averaged polarization of 62 ± 16 µC cm-2 in the three unit cells adjacent to the crack tip, which is one of the largest flexoelectric polarizations ever reported. The polarization is screened by an electron density of 0.7 ± 0.1 e-/uc localized within one unit cell. These findings reveal the relevance of flexoelectricity for the science of crack formation and propagation.

Magnetic Properties of Epitaxially Grown SrRuO3 Nanodots.

We present the fabrication and exploration of arrays of nanodots of SrRuO3 with dot sizes between 500 and 15 nm. Down to the smallest dot size explored, the samples were found to be magnetic with a maximum Curie temperature TC achieved by dots of 30 nm diameter. This peak in TC is associated with a dot-size-induced relief of the epitaxial strain, as evidenced by scanning transmission electron microscopy.

Integrated Circuits Comprising Patterned Functional Liquids.

Solid-state heterostructures are the cornerstone of modern electronics. To enhance the functionality and performance of integrated circuits, the spectrum of materials used in the heterostructures is being expanded by an increasing number of compounds and elements of the periodic table. While the integration of liquids and solid-liquid interfaces into such systems would allow unique and advanced functional properties and would enable integrated nanoionic circuits, solid-state heterostructures that incorporate liquids have not been considered thus far. Here solid-state heterostructures with integrated liquids are proposed, realized, and characterized, thereby opening a vast, new phase space of materials and interfaces for integrated circuits. Devices containing tens of microscopic capacitors and field-effect transistors are fabricated by using integrated patterned NaCl aqueous solutions. This work paves the way to integrated electronic circuits that include highly integrated liquids, thus yielding a wide array of novel research and application opportunities based on microscopic solid/liquid systems.

Single-Gap Superconductivity and Dome of Superfluid Density in Nb-Doped SrTiO_{3}.

SrTiO_{3} exhibits a superconducting dome upon doping with Nb, with a maximum critical temperature T_{c}≈0.4 K. Using microwave stripline resonators at frequencies from 2 to 23 GHz and temperatures down to 0.02 K, we probe the low-energy optical response of superconducting SrTiO_{3} with a charge carrier concentration from 0.3 to 2.2×10^{20} cm^{-3}, covering the majority of the superconducting dome. We find single-gap electrodynamics even though several electronic bands are superconducting. This is explained by a single energy gap 2Δ due to gap homogenization over the Fermi surface consistent with the low level of defect scattering in Nb-doped SrTiO_{3}. Furthermore, we determine T_{c}, 2Δ, and the superfluid density as a function of charge carrier concentration, and all three quantities exhibit the characteristic dome shape.

Electron-phonon Coupling and the Superconducting Phase Diagram of the LaAlO3-SrTiO3 Interface.

The superconductor at the LaAlO3-SrTiO3 interface provides a model system for the study of two-dimensional superconductivity in the dilute carrier density limit. Here we experimentally address the pairing mechanism in this superconductor. We extract the electron-phonon spectral function from tunneling spectra and conclude, without ruling out contributions of further pairing channels, that electron-phonon mediated pairing is strong enough to account for the superconducting critical temperatures. Furthermore, we discuss the electron-phonon coupling in relation to the superconducting phase diagram. The electron-phonon spectral function is independent of the carrier density, except for a small part of the phase diagram in the underdoped region. The tunneling measurements reveal that the increase of the chemical potential with increasing carrier density levels off and is zero in the overdoped region of the phase diagram. This indicates that the additionally induced carriers do not populate the band that hosts the superconducting state and that the superconducting order parameter therefore is weakened by the presence of charge carriers in another band.

Ultrafast optical tuning of ferromagnetism via the carrier density.

Interest in manipulating the magnetic order by ultrashort laser pulses has thrived since it was observed that such pulses can be used to alter the magnetization on a sub-picosecond timescale. Usually this involves demagnetization by laser heating or, in rare cases, a transient increase of magnetization. Here we demonstrate a mechanism that allows the magnetic order of a material to be enhanced or attenuated at will. This is possible in systems simultaneously possessing a low, tunable density of conduction band carriers and a high density of magnetic moments. In such systems, the thermalization time can be set such that adiabatic processes dominate the photoinduced change of the magnetic order--the three-temperature model for interacting thermalized electron, spin and lattice reservoirs is bypassed. In ferromagnetic Eu(1-x)Gd(x)O, we thereby demonstrate the strengthening as well as the weakening of the magnetic order by ~10% and within ≤3 ps by optically controlling the magnetic exchange interaction.

Locally enhanced conductivity due to the tetragonal domain structure in LaAlO3/SrTiO3 heterointerfaces.

The ability to control materials properties through interface engineering is demonstrated by the appearance of conductivity at the interface of certain insulators, most famously the {001} interface of the band insulators LaAlO3 and TiO2-terminated SrTiO3 (STO; refs 1, 2). Transport and other measurements in this system show a plethora of diverse physical phenomena. To better understand the interface conductivity, we used scanning superconducting quantum interference device microscopy to image the magnetic field locally generated by current in an interface. At low temperature, we found that the current flowed in conductive narrow paths oriented along the crystallographic axes, embedded in a less conductive background. The configuration of these paths changed on thermal cycling above the STO cubic-to-tetragonal structural transition temperature, implying that the local conductivity is strongly modified by the STO tetragonal domain structure. The interplay between substrate domains and the interface provides an additional mechanism for understanding and controlling the behaviour of heterostructures.

Oxide nanoelectronics on demand.

Electronic confinement at nanoscale dimensions remains a central means of science and technology. We demonstrate nanoscale lateral confinement of a quasi-two-dimensional electron gas at a lanthanum aluminate-strontium titanate interface. Control of this confinement using an atomic force microscope lithography technique enabled us to create tunnel junctions and field-effect transistors with characteristic dimensions as small as 2 nanometers. These electronic devices can be modified or erased without the need for complex lithographic procedures. Our on-demand nanoelectronics fabrication platform has the potential for widespread technological application.

Epitaxial integration of the highly spin-polarized ferromagnetic semiconductor EuO with silicon and GaN.

Doped EuO is an attractive material for the fabrication of proof-of-concept spintronic devices. Yet for decades its use has been hindered by its instability in air and the difficulty of preparing and patterning high-quality thin films. Here, we establish EuO as the pre-eminent material for the direct integration of a carrier-concentration-matched half-metal with the long-spin-lifetime semiconductors silicon and GaN, using methods that transcend these difficulties. Andreev reflection measurements reveal that the spin polarization in doped epitaxial EuO films exceeds 90%, demonstrating that EuO is a half-metal even when highly doped. Furthermore, EuO is epitaxially integrated with silicon and GaN. These results demonstrate the high potential of EuO for spintronic devices.