High-Performance Ferroelectric Thin Film Transistors with Large Memory Window Using Epitaxial Yttrium-Doped Hafnium Zirconium Gate Oxide.

Preventing ferroelectric materials from losing their ferroelectricity over a low thickness of several nanometers is crucial in developing multifunctional nanoelectronics. Epitaxially grown 5 at. % yttrium-doped Hf0.5Zr0.5O2 (YHZO) thin films exhibit an atomically smooth surface, an ability to maintain ferroelectricity even at a thickness of 10 nm, and excellent insulating properties, making them suitable for use as gate oxides in ferroelectric thin film transistors (FeTFTs). Through the epitaxial growth of a YHZO/La0.67Sr0.33MnO3 (LSMO)/SrTiO3 (STO) heterostructure, YHZO effectively retains its ferroelectricity and orthorhombic single phase, leading to enhancing electron mobility (∼19.74 cm2 V-1 s-1) and memory window (3.7 V) in the amorphous InGaZnO4 (a-IGZO)/YHZO/LSMO/STO FeTFTs. These FeTFTs demonstrate a consistent memory function with remarkable endurance (∼106 cycles) and retention (∼104 s). Furthermore, they sustain a constant memory window even under ±6 V bias stress for 104 s and exhibit excellent stability even under ±6 V/1 ms pulse cycling for 107 cycles. For comparison, a transistor with the same structure was fabricated using epitaxial nonferroelectric LaAlO3 (LAO) and epitaxial undoped Hf0.5Zr0.5O2 (HZO) as alternatives to YHZO. This study presents a novel approach to exploit the potential of YHZO in FeTFTs, contributing to the development of next-generation logic-in-memory.

Spectral signatures of a unique charge density wave in Ta2NiSe7.

Charge Density Waves (CDW) are commonly associated with the presence of near-Fermi level states which are separated from others, or "nested", by a wavector of q. Here we use Angle-Resolved Photo Emission Spectroscopy (ARPES) on the CDW material Ta2NiSe7 and identify a total absence of any plausible nesting of states at the primary CDW wavevector q. Nevertheless we observe spectral intensity on replicas of the hole-like valence bands, shifted by a wavevector of q, which appears with the CDW transition. In contrast, we find that there is a possible nesting at 2q, and associate the characters of these bands with the reported atomic modulations at 2q. Our comprehensive electronic structure perspective shows that the CDW-like transition of Ta2NiSe7 is unique, with the primary wavevector q being unrelated to any low-energy states, but suggests that the reported modulation at 2q, which would plausibly connect low-energy states, might be more important for the overall energetics of the problem.

Atomically dispersed iridium catalysts on silicon photoanode for efficient photoelectrochemical water splitting.

Stabilizing atomically dispersed single atoms (SAs) on silicon photoanodes for photoelectrochemical-oxygen evolution reaction is still challenging due to the scarcity of anchoring sites. Here, we elaborately demonstrate the decoration of iridium SAs on silicon photoanodes and assess the role of SAs on the separation and transfer of photogenerated charge carriers. NiO/Ni thin film, an active and highly stable catalyst, is capable of embedding the iridium SAs in its lattices by locally modifying the electronic structure. The isolated iridium SAs enable the effective photogenerated charge transport by suppressing the charge recombination and lower the thermodynamic energy barrier in the potential-determining step. The Ir SAs/NiO/Ni/ZrO2/n-Si photoanode exhibits a benchmarking photoelectrochemical performance with a high photocurrent density of 27.7 mA cm-2 at 1.23 V vs. reversible hydrogen electrode and 130 h stability. This study proposes the rational design of SAs on silicon photoelectrodes and reveals the potential of the iridium SAs to boost photogenerated charge carrier kinetics.

High performance transition metal-based electrocatalysts for green hydrogen production.

Hydrogen energy is a promising energy source that is environmentally friendly due to its long-term, large-capacity storage and low greenhouse gas emissions. However, the mass production of hydrogen is still technically difficult due to limitations in efficiency, stability, and cost, even though it can satisfy all of the current energy demands. Water splitting using an electrocatalyst is an efficient method for environmentally friendly hydrogen production, and various catalyst-related studies are being conducted for this purpose. For the last decade, transition metal-based compositions have been at the center of water splitting catalyst research. Despite numerous studies and developments, studies on transition metal-based catalysts so far still have various problems to be solved. Although excellent review papers on transition metal-based catalysts have been reported, the overall scope of transition metal-based catalysts has rarely been covered in the reports. In this review, we present the research about overall transition metal-based electrocatalysts for hydrogen production from four different categories, namely, alloys, transition-metal dichalcogenides (TMDs), layered double hydroxides (LDHs), and single-atom catalysts (SACs). The fundamental roles of metal alloying and unique electrical properties of TMDs, LDHs, and SACs are mainly discussed. Furthermore, we present the recent advances in photovoltaic-electrochemical (PV-EC) systems for sustainable hydrogen production. Finally, perspectives on the issues to be addressed in the research on transition metal-based electrocatalysts are provided.

Toward Multicomponent Single-Atom Catalysis for Efficient Electrochemical Energy Conversion.

Single-atom catalysts (SACs) have recently emerged as the ultimate solution for overcoming the limitations of traditional catalysts by bridging the gap between homogeneous and heterogeneous catalysts. Atomically dispersed identical active sites enable a maximal atom utilization efficiency, high activity, and selectivity toward the wide range of electrochemical reactions, superior structural robustness, and stability over nanoparticles due to strong atomic covalent bonding with supports. Mononuclear active sites of SACs can be further adjusted by engineering with multicomponent elements, such as introducing dual-metal active sites or additional neighbor atoms, and SACs can be regarded as multicomponent SACs if the surroundings of the active sites or the active sites themselves consist of multiple atomic elements. Multicomponent engineering offers an increased combinational diversity in SACs and unprecedented routes to exceed the theoretical catalytic performance limitations imposed by single-component scaling relationships for adsorption and transition state energies of reactions. The precisely designed structures of multicomponent SACs are expected to be responsible for the synergistic optimization of the overall electrocatalytic performance by beneficially modulating the electronic structure, the nature of orbital filling, the binding energy of reaction intermediates, the reaction pathways, and the local structural transformations. This Review demonstrates these synergistic effects of multicomponent SACs by highlighting representative breakthroughs on electrochemical conversion reactions, which might mitigate the global energy crisis of high dependency on fossil fuels. General synthesis methods and characterization techniques for SACs are also introduced. Then, the perspective on challenges and future directions in the research of SACs is briefly summarized. We believe that careful tailoring of multicomponent active sites is one of the most promising approaches to unleash the full potential of SACs and reach the superior catalytic activity, selectivity, and stability at the same time, which makes SACs promising candidates for electrocatalysts in various energy conversion reactions.

Tunable magnetization steps in mixed valent ferromagnet Eu2CoMnO6.

Magnetic properties can be manipulated to enhance certain functionalities by tuning different material processing parameters. Here, we present the controllable magnetization steps of hysteresis loops in double-perovskite single crystals of Eu2CoMnO6. Ferromagnetic order emerges below TC ≈ 122 K along the crystallographic c axis. The difficulty in altering Co2+ and Mn4+ ions naturally induces additional antiferromagnetic clusters in this system. Annealing the crystals in different gas environments modifies the mixed magnetic state, and results in the retardation (after O2-annealing) and bifurcation (after Ar-annealing) of the magnetization steps of isothermal magnetization. This remarkable variation offers an efficient approach for improving the magnetic properties of double-perovskite oxides.

Nanoscale electrodeposition: Dimension control and 3D conformality.

Electrodeposition with a long history has been considered one of the important synthesis techniques for applying various applications. It is a feasible route for fabricating nanostructures using diverse materials due to its simplicity, cost-effectiveness, flexibility, and ease of reaction control. Herein, we mainly focus on the nanoscale electrodeposition with respect to dimension control and three-dimensional (3D) conformality. The principles of electrodeposition, dimensional design of materials, and uniform coatings on various substrates are presented. We introduce that manipulating synthesis parameters such as precursors, applied current/voltage, and additives affect the synthesis reaction, resulting in not only dimensional control of materials from three-dimensional structures to zero-dimensional atomic-level but also conformal coatings on complicated substrates. Various cases regarding morphology control of metal (hydro)oxides, metals, and metal-organic frameworks according to electrodeposition conditions are summarized. Lastly, recent studies of applications such as batteries, photoelectrodes, and electrocatalysts using electrodeposited materials are summarized. This review represents significant advances in the nanoscale design of materials through methodological approaches, which are highly attractive from both academic and commercial aspects.

Highly nonlinear magnetoelectric effect in buckled-honeycomb antiferromagnetic Co4Ta2O9.

Strongly correlated materials with multiple order parameters provide unique insights into the fundamental interactions in condensed matter systems and present opportunities for innovative technological applications. A class of antiferromagnetic honeycomb lattices compounds, A4B2O9 (A = Co, Fe, Mn; B = Nb, Ta), have been explored owing to the occurrence of linear magnetoelectricity. From our investigation of magnetoelectricity on single crystalline Co4Ta2O9, we discovered strongly nonlinear and antisymmetric magnetoelectric behavior above the spin-flop transition for magnetic fields applied along two orthogonal in-plane directions. This observation suggests that two types of inequivalent Co2+ sublattices generate magnetic-field-dependent ferroelectric polarization with opposite signs. The results motivate fundamental and applied research on the intriguing magnetoelectric characteristics of these buckled-honeycomb lattice materials.

Realization of a three-dimensional spin-anisotropic harmonic honeycomb iridate.

Spin and orbital quantum numbers play a key role in the physics of Mott insulators, but in most systems they are connected only indirectly--via the Pauli exclusion principle and the Coulomb interaction. Iridium-based oxides (iridates) introduce strong spin-orbit coupling directly, such that these numbers become entwined together and the Mott physics attains a strong orbital character. In the layered honeycomb iridates this is thought to generate highly spin-anisotropic magnetic interactions, coupling the spin to a given spatial direction of exchange and leading to strongly frustrated magnetism. Here we report a new iridate structure that has the same local connectivity as the layered honeycomb and exhibits striking evidence for highly spin-anisotropic exchange. The basic structural units of this material suggest that a new family of three-dimensional structures could exist, the 'harmonic honeycomb' iridates, of which the present compound is the first example.