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The disadvantages of layered double hydroxides (LDHs) such as easy stacking, poor inherent conductivity, and limited versatility hinder their application in splitting water and zinc-air batteries (ZABs). Interface engineering to regulate the electron distribution of LDHs by introducing another component is a way to compensate for the poor electron transport capacity of LDHs during catalysis. Herein, a hierarchical structure is synthesized by assembling CoFe-LDH nanosheets onto the surface of layered N-doped porous carbon (NPC), CoFe-LDH@NPC, by using an interface engineering strategy. CoFe-LDH@NPC has high catalytic activity for the oxygen/hydrogen evolution reaction (OER/HER) with overpotentials of 280/100 mV, respectively. The two-electrode water splitting catalyzed by CoFe-LDH@NPC only needs 1.61 V to drive a current density of 10 mA cm -2 for 60 h. The theoretical results show that there is an electron-deficient/electron-rich interface between the NPC substrate and the CoFe-LDH in CoFe-LDH@NPC. The electrons on the coupling interface are easily transferred, which results in a change of the adsorption behavior of the reaction intermediates and improves the catalytic activity for the OER and HER. In addition, CoFe-LDH@NPC-catalyzed rechargeable flexible ZABs have excellent performance with low charge-discharge polarization (0.87 V) and a long-term stability of 65 h.

Developing efficient electrocatalysts to realize the nitrate reduction reaction (eNO 3 - RR) for ammonia synthesis as an alternative to the traditional Haber-Bosch production process is of great significance. Herein, the heterostructured Bi 2 S 3 /MoS 2 nanoarrays were successfully synthesized by Bi 2 S 3 nanosheets. Owing to the interfacial coupling effect, both particular surface area and exposure active sites increase. Density functional theory further uncovered that the excellent activity originates from charge transfer of the interface and a low potential barrier of 0.58 eV for hydrogenation of *NO to *NOH on Bi 2 nanosheets. Owing to the interfacial coupling effect, both particular surface area and exposure active sites increase. Density functional theory further uncovered that the excellent activity originates from charge transfer of the interface and a low potential barrier of 0.58 eV for hydrogenation of *NO to *NOH on Bi 2 S 3 /MoS 2 . Compared with pure Bi 2 S 3 and MoS 2 catalysts, the heterostructured Bi 2 S 3 /MoS 2 nanoarrays exhibit a superior NH 3 yield of 15.04 × 10 -2 mmol·h -1 ·cm -2 and a Faraday efficiency of 88.4% at -0.8 V versus the reversible hydrogen electrode. This work provides a new avenue to explore advanced electrocatalysts, which is expected to shorten the distance from the practical application of the eNO 3 - RR technology.

The half-metallic manganite oxide La 2/3 Sr 1/3 MnO 3 (LSMO) has a very high spin polarization of ∼100%, making it ideal for ferromagnetic electrodes to realize tunneling magnetoresistance (TMR). Because of the in-plane magnetic anisotropy of the ferromagnetic LSMO electrode, which leads to the density limit of memory, realizing perpendicular tunneling in manganite-based magnetic tunnel junctions (MTJ) is critical for future applications. Here, we design and fabricate manganite-based MTJs composed of alternately stacked cobaltite and manganite layers that demonstrate strong perpendicular magnetic anisotropy (PMA) induced by interfacial coupling. Moreover, spin-dependent tunneling behaviors with an out-of-plane magnetic field were observed in the perpendicular MTJs. We found that the direct tunneling effect plays a dominant role in the low bias region during the transport behavior of devices, which is associated with thermionic emission of electrons or oxygen vacancies in the high bias region. Our works of realizing perpendicular tunneling in manganite-based MTJs lead to new approaches for designing and developing all-oxide spintronic devices.

In recent years, two-dimensional (2D) magnetic heterostructures have captured widespread interest as they provide a fertile ground for exploring the novel properties induced by interfacial magnetic coupling, modulating the intrinsic magnetism of the 2D magnet, and exploiting new spintronic device applications. In this Spotlight on Applications, dominating synthetic strategies employed to fabricate 2D magnetic heterostructures are introduced first. Notably, we then concentrate on two different kinds of magnetic interfaces, namely, the magnetic-nonmagnetic interface and the magnetic-magnetic interface. Specifically, various interface modulated magnetisms such as valley splitting and the anomalous Hall effect as well as their related device applications such as magnetic tunnel junctions have been further reviewed and discussed. Finally, we briefly summarize the recent progress of 2D magnetic heterostructures and outline the future development direction of this booming field.

It is of great importance to develop useful methods to evaluate interfacial coupling strength noninvasively for exploring and optimizing heterointerface functionality. Recently, organic-inorganic van der Waals (vdW) heterostructures (HSs) composed of organic semiconductors and transition-metal dichalcogenides (TMD) have shown great potential for developing next-generation flexible optical, electrical, and optoelectrical devices. Since vdW coupling dominates the property of such a vdW HS, it is crucial to develop a method to evaluate its interfacial coupling strength noninvasively. In this work, by combining electrical force microscopy (EFM) and Raman and photoluminescence spectroscopic measurements, we were able to directly probe the coupling strength between monolayer MoSe 2 and a copper phthalocyanine (CuPc) thin film. Especially, we also found a new Raman mode in HS due to the Davydov splitting of the CuPc thin film via strong interfacial coupling between the two materials. This new Raman mode was thus utilized as a probe to reveal the modulation of the coupling strength by changing post-treatment conditions. All of these results indicate that the method developed here is capable of evaluating the coupling strength of the MoSe 2 /CuPc HS effectively and innovatively, which aids in providing deep insights into such hybrid vdW HSs for future optical and optoelectrical applications.

We characterize the magnetic interfacial coupling of the Fe/FeGe heterostructure and its influence on the magnetic damping via ferromagnetic resonance in the temperature range of 200-300 K. When the temperature is below the critical temperature of FeGe, the interfacial coupling rises. The strength of the magnetic interfacial coupling is determined as a function of the temperature and reaches up to 0.194 erg/cm 2 at 200 K. Meanwhile, the Gilbert damping of the Fe layer is enhanced from 0.035 at 300 K to 0.050 at 200 K. The enhancement is linearly proportional to the strength of magnetic interfacial coupling. We attribute the enhancement to the interfacial coupling that transfers spin angular momentum from Fe to FeGe via the exchange interaction. Our results reveal that the interfacial coupling is an effective approach to inject spin current into the chiral spin texture.

The oxygen octahedral rotation around the out-of-plane axis is explored to study its effect on metastable status, magnetic cluster glass in manganite. The antiphase rotation around the out-of-plane axis (TiO 6 a 0 a 0 c - ) of SrTiO 3 substrate on material properties is obvious with a large irreversible MR effect for thin films, which fades away with the increase in film thickness. At 10 K, the irreversible MR is 0.91 for the 12 nm film and 0.22 for the 30 nm film. This work extends current understanding on interfacial coupling to metastable status and could help explore other systems in the perovskite structure with octahedral rotation.0.67 Sr 0.33 MnO 3 film on the (001) SrTiO 3 substrate, which together promote the formation of magnetic cluster-glassiness and enlarges the irreversible magnetoresistance (MR) effect with enhanced relaxation time of charge carriers. The effect of TiO 6 a 0 a 0 c - in the SrTiO 3 substrate on material properties is obvious with a large irreversible MR effect for thin films, which fades away with the increase in film thickness. At 10 K, the irreversible MR is 0.91 for the 12 nm film and 0.22 for the 30 nm film. This work extends current understanding on interfacial coupling to metastable status and could help explore other systems in the perovskite structure with octahedral rotation.

Highly efficient oxygen evolution driven by abundant sunlight is a key to realize overall water splitting for large-scale conversion of renewable energy. Here, we report a strategy for the interfacial atomic and electronic coupling of layered CoOOH and BiVO 4 to deactivate the surface trapping states and suppress the charge-carrier recombination for high photoelectrochemical (PEC) water oxidation activity. The successful synthesis of a 3D ultrathin-CoOOH-overlayer-coated coral-like BiVO 4 photoanode effectively tailors the migration route of photocarriers on the semiconductor/liquid interface to realize a great increase of ∼200% in the photovoltage relative to bare BiVO 4 , consequently decreasing the corresponding onset potential of PEC water splitting from 0.60 to 0.20 V RHE . As a result, the unique CoOOH/BiVO 4 photoanode could efficiently perform PEC water oxidation in a neutral aqueous solution (pH = 7) with a high photocurrent density of 4.0 mA/cm 2 at 1.23 V RHE and a prominent quantum efficiency of 65% at 450 nm. Electronic structural characterizations and theoretical calculations reveal that the combination of layered CoOOH and BiVO 4 forming interfacial oxo-bridge bonding could greatly eliminate surface trapping states and promote the direct transfer of photogenerated holes from the valence band to the surface water redox potential for water oxidation.

The magnetic properties of the all-oxide multiferroic heterostructures composed of orthorhombic YMnO3 (YMO) with E-type antiferromagnetic and double-exchange ferromagnetic (FM) La0.6Sr0.4MnO3 (LSMO) were studied. An orientation-modulated exchange bias effect, which is related to the interfacial Mn-O-Mn bond angle, was discovered. Because of the large bond angle in YMO/LSMO(100) heterostructures, a strong exchange coupling at the interface is formed. This strong exchange coupling sustains an FM phase in YMO at the interface region. The FM phase with strong magnetocrystalline anisotropy contributes to the vertical shift and exchange bias effect in (100) orientation heterostructures. When LSMO (110) and (111) were layered with YMO, the Mn-O-Mn bond angle was reduced, leading to a weakened exchange coupling at the interface, and only a relatively small exchange bias at low temperatures was visible.

The superlattice of energetically stable La2/3Sr1/3MnO3 and tetragonal BiFeO3 is investigated by means of density functional theory. The superlattice as a whole exhibits a half-metallic character, as is desired for spintronic devices. The interfacial electronic states and exchange coupling are analyzed in details. We demonstrate that the interfacial O atoms play a key role in controlling the coupling. The higher ferroelectricity of tetragonal BiFeO3 and stronger response to the magnetic moments in the La2/3Sr1/3MnO3/BiFeO3 superlattice show a strongly enhanced electric control of the magnetism as compared to the rhombohedral one. Therefore, it is particularly practical interest in the magnetoelectrically controlled spintronic devices.