Ptychographic Nanoscale Imaging of the Magnetoelectric Coupling in Freestanding BiFeO3.

Understanding the magnetic and ferroelectric ordering of magnetoelectric multiferroic materials at the nanoscale necessitates a versatile imaging method with high spatial resolution. Here, soft X-ray ptychography is employed to simultaneously image the ferroelectric and antiferromagnetic domains in an 80 nm thin freestanding film of the room-temperature multiferroic BiFeO3 (BFO). The antiferromagnetic spin cycloid of period 64 nm is resolved by reconstructing the corresponding resonant elastic X-ray scattering in real space and visualized together with mosaic-like ferroelectric domains in a linear dichroic contrast image at the Fe L3 edge. The measurements reveal a near perfect coupling between the antiferromagnetic and ferroelectric ordering by which the propagation direction of the spin cycloid is locked orthogonally to the ferroelectric polarization. In addition, the study evinces both a preference for in-plane propagation of the spin cycloid and changes of the ferroelectric polarization by 71° between multiferroic domains in the epitaxial strain-free, freestanding BFO film. The results provide a direct visualization of the strong magnetoelectric coupling in BFO and of its fine multiferroic domain structure, emphasizing the potential of ptychographic imaging for the study of multiferroics and non-collinear magnetic materials with soft X-rays.

Self-Enhancement of Water Electrolysis by Electrolyte-Poled Ferroelectric Catalyst.

Efficient and durable electrocatalysts with superior activity are needed for the production of green hydrogen with a high yield and low energy consumption. Electrocatalysts based on transition metal oxides hold dominance due to their abundant natural resources, regulable physical properties, and good adaptation to a solution. In numerous oxide catalyst materials, ferroelectrics, possessing semiconducting characteristics and switchable spontaneous polarization, have been considered promising photoelectrodes for solar water splitting. However, few investigations noted their potential as electrocatalysts. In this study, we report an efficient electrocatalytic electrode made of a BiFeO3/nickel foam heterostructure, which displays a smaller overpotential and higher current density than the blank nickel foam electrode. Moreover, when in contact with an alkaline solution, the bond between hydroxyls and the BiFeO3 surface induces a large area of upward self-polarization, lowering the adsorption energy of subsequent adsorbates and facilitating oxygen and hydrogen evolution reaction. Our work demonstrates an infrequent pathway of using functional semiconducting materials for exploiting highly efficient electrocatalytic electrodes.

Engineering the Strain and Interlayer Excitons of 2D Materials via Lithographically Engraved Hexagonal Boron Nitride.

Strain engineering has quickly emerged as a viable option to modify the electronic, optical, and magnetic properties of 2D materials. However, it remains challenging to arbitrarily control the strain. Here we show that, by creating atomically flat surface nanostructures in hexagonal boron nitride, we achieve an arbitrary on-chip control of both the strain distribution and magnitude on high-quality molybdenum disulfide. The phonon and exciton emissions are shown to vary in accordance with our strain field designs, enabling us to write and draw any photoluminescence color image in a single chip. Moreover, our strain engineering offers a powerful means to significantly and controllably alter the strengths and energies of interlayer excitons at room temperature. This method can be easily extended to other material systems and offers promise for functional excitonic devices.

Twisted oxide lateral homostructures with conjunction tunability.

Epitaxial growth is of significant importance over the past decades, given it has been the key process of modern technology for delivering high-quality thin films. For conventional heteroepitaxy, the selection of proper single crystal substrates not only facilitates the integration of different materials but also fulfills interface and strain engineering upon a wide spectrum of functionalities. Nevertheless, the lattice structure, regularity and crystalline orientation are determined once a specific substrate is chosen. Here, we reveal the growth of twisted oxide lateral homostructure with controllable in-plane conjunctions. The twisted lateral homostructures with atomically sharp interfaces can be composed of epitaxial "blocks" with different crystalline orientations, ferroic orders and phases. We further demonstrate that this approach is universal for fabricating various complex systems, in which the unconventional physical properties can be artificially manipulated. Our results establish an efficient pathway towards twisted lateral homostructures, adding additional degrees of freedom to design epitaxial films.

Presence of Delocalized Ti 3d Electrons in Ultrathin Single-Crystal SrTiO3.

Strontium titanate (STO), with a wide spectrum of emergent properties such as ferroelectricity and superconductivity, has received significant attention in the community of strongly correlated materials. In the strain-free STO film grown on the SrRuO3 buffer layer, the existing polar nanoregions can facilitate room-temperature ferroelectricity when the STO film thickness approaches 10 nm. Here we show that around this thickness scale, the freestanding STO films without the influence of a substrate show the tetragonal structure at room temperature, contrasting with the cubic structure seen in bulk form. The spectroscopic measurements reveal the modified Ti-O orbital hybridization that causes the Ti ion to deviate from its nominal 4+ valency (3d0 configuration) with excess delocalized 3d electrons. Additionally, the Ti ion in TiO6 octahedron exhibits an off-center displacement. The inherent symmetry lowering in ultrathin freestanding films offers an alternative way to achieve tunable electronic structures that are of paramount importance for future technological applications.

Extremely Fast Optical and Nonvolatile Control of Mixed-Phase Multiferroic BiFeO3 via Instantaneous Strain Perturbation.

Multiferroics-materials that exhibit coupled ferroic orders-are considered to be one of the most promising candidate material systems for next-generation spintronics, memory, low-power nanoelectronics and so on. To advance potential applications, approaches that lead to persistent and extremely fast functional property changes are in demand. Herein, it is revealed that the phase transition and the correlated ferroic orders in multiferroic BiFeO3 (BFO) can be modulated via illumination of single short/ultrashort light pulses. Heat transport simulations and ultrafast optical pump-probe spectroscopy reveal that the transient strain induced by light pulses plays a key role in determining the persistent final states. Having identified the diffusionless phase transformation features via scanning transmission electron microscopy, sequential laser pulse illumination is further demonstrated to perform large-area phase and domain manipulation in a deterministic way. The work contributes to all-optical and rapid nonvolatile control of multiferroicity, offering different routes while designing novel optoelectronics.

Oxide Heteroepitaxy-Based Flexible Ferroelectric Transistor.

With the rise of Internet of Things, the presence of flexible devices has attracted significant attention owing to design flexibility. A ferroelectric field-effect transistor (FeFET), showing the advantages of high speed, nondestructive readout, and low-power consumption, plays a key role in next-generation technology. However, the performance of these devices is restricted since conventional flexible substrates show poor thermal stability to integrate traditional ferroelectric materials, limiting the compatibility of wearable devices. In this study, we adopt flexible muscovite mica as a substrate due to its good thermal properties and epitaxial integration ability. A flexible FeFET composed of oxide heteroepitaxy on muscovite is realized by combining an aluminum-doped zinc oxide film as the semiconductor channel layer and a Pb(Zr0.7Ti0.3)O3 film as the ferroelectric gate dielectric. The excellent characteristics of the transistor together with superior thermal stability and mechanical flexibility are demonstrated through various mechanical bending and temperature measurements. The on/off current ratio of the FeFET is higher than 103, which based on the field effect in the transfer curve. The smallest bending radius that can be achieved is 5 mm with a cyclability of 300 times and a retention of 100 h. This study opens an avenue to use oxide heteroepitaxy to construct a FeFET for next-generation flexible electronic systems.