Ultrahigh electromechanical response from competing ferroic orders.

Materials with electromechanical coupling are essential for transducers and acoustic devices as reversible converters between mechanical and electrical energy1-6. High electromechanical responses are typically found in materials with strong structural instabilities, conventionally achieved by two strategies-morphotropic phase boundaries7 and nanoscale structural heterogeneity8. Here we demonstrate a different strategy to accomplish ultrahigh electromechanical response by inducing extreme structural instability from competing antiferroelectric and ferroelectric orders. Guided by the phase diagram and theoretical calculations, we designed the coexistence of antiferroelectric orthorhombic and ferroelectric rhombohedral phases in sodium niobate thin films. These films show effective piezoelectric coefficients above 5,000 pm V-1 because of electric-field-induced antiferroelectric-ferroelectric phase transitions. Our results provide a general approach to design and exploit antiferroelectric materials for electromechanical devices.

Origin of a Topotactic Reduction Effect for Superconductivity in Infinite-Layer Nickelates.

Topotactic reduction utilizing metal hydrides as reagents has emerged as an effective approach to achieve exceptionally low oxidization states of metal ions and unconventional coordination networks. This method opens avenues to the development of entirely new functional materials, with one notable example being the infinite-layer nickelate superconductors. However, the reduction effect on the atomic reconstruction and electronic structures-crucial for superconductivity-remains largely unresolved. We designed two sets of control Nd_{0.8}Sr_{0.2}NiO_{2} thin films and used secondary ion mass spectroscopy to highlight the absence of reduction-induced hydrogen intercalation. X-ray absorption spectroscopy revealed a significant linear dichroism with dominant Ni 3d_{x2-y2} orbitals on superconducting samples, indicating a Ni single-band nature of infinite-layer nickelates. Consistent with the superconducting T_{c}, the Ni 3d orbitals asymmetry manifests a domelike dependence on the reduction duration. Our results unveil the critical role of reduction in modulating the Ni-3d orbital polarization and its impact on the superconducting properties.

Tunable Magnetic Properties in Sr2FeReO6 Double-Perovskite.

Double-perovskite oxides have attracted recent attention due to their attractive functionalities and application potential. In this paper, we demonstrate the effect of dual controls, i.e., the deposition pressure of oxygen (PO2) and lattice mismatch (ε), on tuning magnetic properties in epitaxial double-perovskite Sr2FeReO6 films. In a nearly lattice matched Sr2FeReO6/SrTiO3 film, the ferrimagnetic-to-paramagnetic phase transition occurs when PO2 is reduced to 30 mTorr, probably due to the formation of Re4+ ions that replace the stoichiometric Re5+ to cause disorders of B-site ions. On the other hand, a large compressive strain or tensile strain shifts this critical PO2 to below 1 mTorr or above 40 mTorr, respectively. The observations can be attributed to the modulation of B-site ordering by epitaxial strain through affecting elemental valence. Our results provide a feasible way to expand the functional tunability of magnetic double-perovskite oxides that hold great promise for spintronic devices.

Magnetic Anisotropy of a Quasi Two-Dimensional Canted Antiferromagnet.

We report the control of the interplane magnetic exchange coupling in CaIrO3 perovskite thin films and superlattices with SrTiO3. By analyzing the anisotropic magneto-transport data, we demonstrate that a semimetallic paramagnetic CaIrO3 turns into a canted antiferromagnetic Mott insulator at reduced dimensions. The emergence of a biaxial magneto-crystalline anisotropy indicates the canted moment responding to the cubic symmetry. Extending to superlattices and probing oxygen octahedral rotation by half-integer X-ray Braggs diffraction, a more complete picture about the canted moment evolution with interplane coupling can be understood. Remarkably, a rotation of the canted moments' easy axes by 45° is also observed by a sign reversal of the in-plane strain. These results demonstrate the robustness of anisotropic magnetoresistance in revealing quasi two-dimensional canted antiferromagnets, as well as valuable insights about quadrupolar magnetoelastic coupling, relevant for designing future antiferromagnetic spintronic devices.

Characteristic Lengths of Interlayer Charge Transfer in Correlated Oxide Heterostructures.

Using interlayer interaction to control functional heterostructures with atomic-scale designs has become one of the most effective interface-engineering strategies nowadays. Here, we demonstrate the effect of a crystalline LaFeO3 buffer layer on amorphous and crystalline LaAlO3/SrTiO3 heterostructures. The LaFeO3 buffer layer acts as an energetically favored electron acceptor in both LaAlO3/SrTiO3 systems, resulting in modulation of interfacial carrier density and hence metal-to-insulator transition. For amorphous and crystalline LaAlO3/SrTiO3 heterostructures, the metal-to-insulator transition is found when the LaFeO3 layer thickness crosses 3 and 6 unit cells, respectively. Such different critical LaFeO3 thicknesses are explained in terms of distinct characteristic lengths of the redox-reaction-mediated and polar-catastrophe-dominated charge transfer, controlled by the interfacial atomic contact and Thomas-Fermi screening effect, respectively. Our results not only shed light on the complex interlayer charge transfer across oxide heterostructures but also provide a new route to precisely tailor the charge-transfer process at a functional interface.

Emergent Topological Hall Effect at a Charge-Transfer Interface.

Exploring exotic interface magnetism due to charge transfer and strong spin-orbit coupling has profound application in the future development of spintronic memory. Here, the emergence and tuning of topological Hall effect (THE) from a CaMnO3 /CaIrO3 /CaMnO3 trilayer structure are studied in detail, which suggests the presence of magnetic Skyrmion-like bubbles. First, by tilting the magnetic field direction, the evolution of the Hall signal suggests a transformation of Skyrmions into topologically-trivial stripe domains, consistent with behaviors predicted by micromagnetic simulations. Second, by varying the thickness of CaMnO3 , the optimal thicknesses for the THE signal emergence are found, which allow identification of the source of Dzyaloshinskii-Moriya interaction (DMI) and its competition with antiferromagnetic superexchange. Employing high-resolution transmission electron microscopy, randomly distributed stacking faults are identified only at the bottom interface and may avoid mutual cancellation of DMI. Last, a spin-transfer torque experiment also reveals a low threshold current density of ≈109 A m-2 for initiating the bubbles' motion. This discovery sheds light on a possible strategy for integrating Skyrmions with antiferromagnetic spintronics.

Phase Diagram and Superconducting Dome of Infinite-Layer Nd_{1-x}Sr_{x}NiO_{2} Thin Films.

Infinite-layer Nd_{1-x}Sr_{x}NiO_{2} thin films with Sr doping level x from 0.08 to 0.3 are synthesized and investigated. We find a superconducting dome x between 0.12 and 0.235 accompanied by a weakly insulating behavior in both under- and overdoped regimes. The dome is akin to that in the electron-doped 214-type and infinite-layer cuprate superconductors. For x≥0.18, the normal state Hall coefficient (R_{H}) changes the sign from negative to positive as the temperature decreases. The temperature of the sign changes decreases monotonically with decreasing x from the overdoped side and approaches the superconducting dome at the midpoint, suggesting a reconstruction of the Fermi surface with the dopant concentration across the dome.

Revisiting the Ferroelectric Photovoltaic Properties of Vertical BiFeO3 Capacitors: A Comprehensive Study.

The ferroelectric photovoltaic effect has been extensively studied for possible applications in energy conversion and photo-electrics. The reversible spontaneous polarization gives rise to a switchable photovoltaic behavior. However, despite its long history, the origin of the ferroelectric photovoltaic effect still lacks a full understanding since multiple mechanisms such as bulk and Schottky-barrier-related interface effects are involved. Herein, we report a comprehensive study on the photovoltaic response of BiFeO3-based vertical heterostructures, using multiple strategies to clarify its origin. We found that, under white light illumination, polarization-modulated Schottky barrier at the interface is the dominating mechanism. By varying the top metal contacts, only the photovoltaic effect of the polarization downward state is strongly modulated, suggesting selective interface contribution in different polarization states. A Schottky-barrier-free device shows negligible photovoltaic effect, suggesting the lack of bulk photovoltaic effect in vertical heterostructures under white light illumination.

Scanning SQUID-on-tip microscope in a top-loading cryogen-free dilution refrigerator.

The scanning superconducting quantum interference device (SQUID) fabricated on the tip of a sharp quartz pipette (SQUID-on-tip) has emerged as a versatile tool for the nanoscale imaging of magnetic, thermal, and transport properties of microscopic devices of quantum materials. We present the design and performance of a scanning SQUID-on-tip microscope in a top-loading probe of a cryogen-free dilution refrigerator. The microscope is enclosed in a custom-made vacuum-tight cell mounted at the bottom of the probe and is suspended by springs to suppress vibrations caused by the pulse tube cryocooler. Two capillaries allow for the in situ control of helium exchange gas pressure in the cell that is required for thermal imaging. A nanoscale heater is used to create local temperature gradients in the sample, which enables quantitative characterization of relative vibrations between the tip and the sample. The spectrum of the vibrations shows distinct resonant peaks with a maximal power density of about 27 nm/Hz1/2 in the in-plane direction. The performance of the SQUID-on-tip microscope is demonstrated by magnetic imaging of the MnBi2Te4 magnetic topological insulator, magnetization and current distribution imaging in a SrRuO3 ferromagnetic oxide thin film, and thermal imaging of dissipation in graphene.

Superconductivity in infinite-layer nickelate La1-xCaxNiO2 thin films.

We report the observation of superconductivity in infinite-layer Ca-doped LaNiO2 (La1-xCaxNiO2) thin films and construct their phase diagram. Unlike the metal-insulator transition in Nd- and Pr-based nickelates, the undoped and underdoped La1-xCaxNiO2 thin films are entirely insulating from 300 K down to 2 K. A superconducting dome is observed at 0.15 < x < 0.3 with weakly insulating behavior at the overdoped regime. Moreover, the sign of the Hall coefficient RH changes at low temperature for samples with a higher doping level. However, distinct from the Nd- and Pr-based nickelates, the RH-sign-change temperature remains at around 35 K as the doping increases, which begs further theoretical and experimental investigation to reveal the role of the 4f orbital to the (multi)band nature of the superconducting nickelates. Our results also emphasize a notable role of lattice correlation on the multiband structures of the infinite-layer nickelates.

CdS sensitized 3D hierarchical TiO2/ZnO heterostructure for efficient solar energy conversion.

For conventional dye or quantum dot sensitized solar cells, which are fabricated using mesoporous films, the inefficient electron transport due to defects such as grain boundaries and surface traps is a major drawback. To simultaneously increase the carrier transport efficiency as well as the surface area, optimal-assembling of hierarchical nanostructures is an attractive approach. Here, a three dimensional (3D) hierarchical heterostructure, consisting of CdS sensitized one dimensional (1D) ZnO nanorods deposited on two dimensional (2D) TiO2 (001) nanosheet, is prepared via a solution-process method. Such heterstructure exhibits significantly enhanced photoelectric and photocatalytic H2 evolution performance compared with CdS sensitized 1D ZnO nanorods/1D TiO2 nanorods photoanode, as a result of the more efficient light harvesting over the entire visible light spectrum and the effective electron transport through a highly connected 3D network.

General route to ZnO nanorod arrays on conducting substrates via galvanic-cell-based approach.

Wurtzite ZnO nanorod exhibits many unique properties, which make it promising for various optoelectronic applications. To grow well-aligned ZnO nanorod arrays on various substrates, a seed layer is usually required to improve the density and vertical alignment. The reported works about seedless hydrothermal synthesis either require special substrates, or require external electrical field to enhance the ZnO nucleation. Here, we report a general method for the one-pot synthesis of homogenous and well-aligned ZnO nanorods on common conducting substrates without a seed layer. This method, based on the galvanic-cell structure, makes use of the contact potential between different materials as the driving force for ZnO growth. It is applicable to different conducting substrates at low temperature. More importantly, the as-grown ZnO nanorods show enhanced photoelectric response. This unique large scale low-temperature processing method could be of great importance for the application of ZnO nanostructures.

Non-volatile memory based on the ferroelectric photovoltaic effect.

The quest for a solid state universal memory with high-storage density, high read/write speed, random access and non-volatility has triggered intense research into new materials and novel device architectures. Though the non-volatile memory market is dominated by flash memory now, it has very low operation speed with ~10 µs programming and ~10 ms erasing time. Furthermore, it can only withstand ~10(5) rewriting cycles, which prevents it from becoming the universal memory. Here we demonstrate that the significant photovoltaic effect of a ferroelectric material, such as BiFeO3 with a band gap in the visible range, can be used to sense the polarization direction non-destructively in a ferroelectric memory. A prototype 16-cell memory based on the cross-bar architecture has been prepared and tested, demonstrating the feasibility of this technique.