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Twin boundaries (TBs) in transition metal dichalcogenides (TMDs) constitute distinctive one-dimensional electronic systems, exhibiting intriguing physical and chemical properties that have garnered significant attention in the fields of quantum physics and electrocatalysis. However, the controlled manipulation of TBs in terms of density and specific atomic configurations remains a formidable challenge. In this study, we present a non-epitaxial growth approach that enables the controlled and large-scale fabrication of homogeneous catalytically active TBs in monolayer TMDs on arbitrary substrates. Notably, the density achieved using this strategy is six times higher than that observed in convention chemical vapor deposition (CVD)-grown samples. Through rigorous experimental analysis and multigrain Wulff construction simulations, we elucidate the role of regulating the metal source diffusion process, which serves as the key factor for inducing the self-oriented growth of TMD grains and the formation of unified TBs. Furthermore, we demonstrate that this novel growth mode can be readily incorporated into the conventional CVD growth method by making a simple modification of the growth temperature profile, thereby offering a universal approach for engineering of grain boundaries in two-dimensional materials. Public summary: • Differences in diffusivity of metal sources trigger the non-epitaxial growth of twin boundaries. • The growth mechanism of high-density 1D twin boundaries on arbitrary substrates is revealed. • A possible universal strategy for grain boundary engineering in 2D materials is proposed. • Density-controllable twin boundaries provide a promising platform for exploring novel quantum states in 1D electronic systems.

Abstract Electron‐correlated materials have been drawing ever‐increasing attention due to their fascinating physical behaviors and extensive application scenarios. In this review, a new method for material research and design (R&D), named structural‐functional unit ordering (SFU ordering), which is presented, overcomes the shortcomings—for example, the limitation of finite chemical elements and long R&D circle‐of conventional strategy and thus provides guidance for the design of these high‐performance functional materials on demand. Meanwhile, with the development of material characterization technologies, SFUs of different scales and types can be directly observed, which, moreover, regulate the corresponding orderings. The review, starts with an introduction of the profile for SFU ordering and the synergistic effect between SFUs. Then, studies on several new high‐performance electronic‐correlated materials, for example, a ferromagnetic semiconductor with local spin, ferromagnetic metals with spin topologies, ferroelectric thin films with polar topologies, piezoelectric thin films with nanopillars enclosed by charged boundaries, thermoelectric materials with local ferromagnetic nanoparticles and topotactic phase transformation with conducting nanofilaments are stated in detail one by one. The vital aspect is the breaking of local symmetry, the construction, the structure, of SFUs and their orderings existing or theoretically existing, together with the enhanced/new performance. All in all, the main comments of the review tend to the remaining challenges, promising design approaches for the SFUs, and their orderings for high‐performance functional materials.

Defects are believed to always scatter carriers. Here, the authors find that the quantum gaps in GeTe-based materials do not scatter carriers, which decouple the carriers and phonons transport leading to high thermoelectric performance.

Maximizing the electromechanical response is crucial for developing piezoelectric devices. Here, the authors demonstrate a giant electric-field-induced strain and its origin in alkali niobate epitaxial thin films with self-assembled planar faults.

Abstract Combining isolated atomic active sites with those in nanoparticles for synergizing complex multistep catalysis is being actively pursued in the design of new electrocatalyst systems. However, these novel systems have been rarely studied due to the challenges with synthesis and analysis. Herein, a synergistically catalytic performance is demonstrated with a 0.89 V (vs reversible hydrogen electrode) onset potential in the four‐step oxygen reduction reaction (ORR) by localizing tungsten single atoms around tungsten nitride nanoparticles confined into nitrogen‐doped carbon (W SAs/WNNC). Through density functional theory calculations, it is shown that each of the active centers in the synergistic entity feature a specific potential‐determining step in their respective reaction pathway that can be merged to optimize the intermediate steps involving scaling relations on individual active centers. Impressively, the W SAs/WNNC as the air cathode in all‐solid‐state Zn‐air and Al‐air batteries demonstrate competitive durability and reversibility, despite the acknowledged low activity of W‐based catalyst toward the ORR.

Experimentally manipulating bubble domains remains elusive especially in the bulk form of ferroelectrics. Here, the authors achieve self-confined bubble domains with multiple polar topologies in bulk Bi0.5Na0.5TiO3 ferroelectrics, demonstrating reversible and donut-like domain morphology evolution.

Phase boundary engineering through chemical alloying and phase control is a traditional approach to enhancing piezoelectric properties. Here, the authors design a strategy in alkali niobate films, utilizing alkali vacancies without alloying to form nanopillars enclosed.

Precisely regulating Pt catalytic sites is important and challenging. Herein the authors engineer the clustering of single atomic Te vacancies in atomically thin PtTe2 to optimize the electronic structure, adsorption energy, and catalytic performance of atomically defined Pt sites.

One major challenge for antiferromagnetic spintronics is how to control the antiferromagnetic state. Here Jani et al. demonstrate the reversible ionic control of the room-temperature magnetic anisotropy and spin reorientation transition in haematite, via the incorporation and removal of hydrogen.

The fabrication of singly dispersed metal cluster catalysts with atomic-level control of dopants is a long-standing challenge. Here, the authors report a strategy for the synthesis of a precisely doped single cluster catalyst which shows exceptional activity for electrochemical dinitrogen reduction.

Two-dimensional magnets with intrinsic ferromagnetic/antiferromagnetic ordering are highly desirable for future spintronic devices. Here, the authors demonstrate a chemical vapor deposition approach to controllably grow ultrathin FeTe crystals with antiferromagnetic tetragonal and ferromagnetic hexagonal phase, showing a thickness-dependent magnetic transition.

Abstract In recent years, two‐dimensional (2D) ternary materials have attracted wide attention due to their novel properties which can be achieved by regulating their chemical composition with a very great degree of freedom and adjustable space. However, as for the precise synthesis of 2D ternary materials, great challenges still lie ahead that hinder their further development. In this work, we demonstrated a simple and reliable approach to synthesize 2D ternary‐layered BiOCl crystals through a microwave‐assisted space‐confined process in a short time (

Abstract Atomically dispersed Pt species are advocated as a promising electrocatalyst for the oxygen reduction reaction (ORR) to boost noble metal utilization efficiency. However, when assembled on various substrates, isolated Pt single atoms are often demonstrated to proceed through the two‐electron ORR pathway due to the unfavorable O─O bond cleavage thermodynamics in the absence of catalytic ensemble sites. In addition, although their distinct local coordination environments at the exact single active sites are intensively explored, the interactions and synergy between closely neighboring single atom sites remain elusive. Herein, atomically dispersed Pt monomers strongly interacting on a Mo2C support is demonstrated as a model catalyst in the four‐electron ORR, and the beneficial interactions between two closely neighboring and yet non‐contiguous Pt single atom sites (named as quasi‐paired Pt single atoms) are shown. Compared to isolated Pt single atom sites, the quasi‐paired Pt single atoms deliver a superior mass activity of 0.224 A mg−1Pt and near‐100% selectivity toward four‐electron ORR due to the synergistic interaction from the two quasi‐paired Pt atom sites in modulating the binding mode of reaction intermediates. Our first‐principles calculations reveal a unique mechanism of such quasi‐paired configuration for promoting four‐electron ORR.

Abstract Enabled by the advances in aberration‐corrected scanning transmission electron microscopy (STEM), atomic‐resolution real space imaging of materials has allowed a direct structure‐property investigation. Traditional ways of quantitative data analysis suffer from low yield and poor accuracy. New ideas in the field of computer vision and machine learning have provided more momentum to harness the wealth of big data and sophisticated information in STEM data analytics, which has transformed STEM from a localized characterization technique to a macroscopic tool with intelligence. In this review article, we discuss the prime significance of defect topology and density in two‐dimensional (2D) materials, which have proved to be a powerful means to tune a wide range of properties. Subsequently, we systematically review advanced data analysis methods that have demonstrated promising prospects in analyzing STEM data, particularly for identifying structural defects, with high throughput and veracity. A unified framework for atomic structure identification is also summarized.

The two-dimensional electron gases that form at LaAlO3/SrTiO3 heterostructure interfaces feature strong spin-orbit interactions, leading to proposed spintronic applications. Lin et al. show that the design of asymmetric heterostructures enables the Rashba spin-orbit interaction to be tuned between two regimes.

Converting solar energy to hydrogen fuel requires light-absorbers that well-match the wavelengths of incoming sunlight. Here, authors prepare a broadband visible-light-absorbing molecular complex that efficiently produces hydrogen from water.

We report the synthesis of a spectrum of highly crystalline molybdenum sulphide/oxide-based materials such as MoS2 (2-H), MoO2 and unique hybrid MoS2/MoO2 nanostructures through chemical vapour deposition (CVD). The as-fabricated samples were scrutinized with materials characterization techniques. Our results reveal that, by tuning growth parameters, different samples demonstrate unique morphologies, which can be unequivocally tied to their chemical composition. We also explore their potential application as electrochemical catalysts, which we found that in addition to using large specific surface area and conductive substrate to improve interlayer conductivity,chemical heterogeneity and efficient charge transport are also essential for good catalytic activity.

Abstract Electrical control of material properties based on ionic liquids (IL) has seen great development and emerging applications in the field of functional oxides, mainly understood by the electrostatic and electrochemical gating mechanisms. Compared to the fast, flexible, and reproducible electrostatic gating, electrochemical gating is less controllable owing to the complex behaviors of ion migration. Here, the interface‐dependent oxygen migration by electrochemical gating is resolved at the atomic scale in the LaAlO3–SrTiO3 system through ex situ IL gating experiments and on‐site atomic‐resolution characterization. The difference between interface structures leads to the controllable electrochemical oxygen migration by filling oxygen vacancies. The findings not only provide an atomic‐scale insight into the origin of interface‐dependent electrochemical gating but also demonstrate an effective way of engineering interface structure to control the electrochemical gating.

Abstract Photothermal therapy (PTT) has emerged as a promising cancer therapeutic modality with high therapeutic specificity, however, its therapeutic effectiveness is limited by available high‐efficiency photothermal agents (PTAs), especially in the second near‐infrared (NIR‐II) biowindow. Here, based on facile liquid‐exfoliated FePS3 nanosheets, a highly efficient NIR‐II PTA with its photothermal conversion efficiency of up to 43.3% is demonstrated, which is among the highest reported levels in typical PTAs. More importantly, such Fe‐based 2D nanosheets also show superior Fenton catalytic activity facilitated by their ultrahigh specific surface area, simultaneously enabling cancer chemodynamic therapy (CDT). Impressively, the efficiency of CDT could be further remarkably enhanced by its photothermal effect, leading to cancer synergistic PTT/CDT. Both in vitro and in vivo studies reveal a highly efficient tumor ablation under NIR‐II light irradiation. This work provides a paradigm for cancer CDT and PTT in the NIR‐II biowindow via a single 2D nanoplatform with desired therapeutic effect. Furthermore, with additional possibilities for magnetic resonance imaging, photoacoustic tomography, as well as drug loading, this Fe‐based 2D material could potentially serve as a 2D “all‐in‐one” theranostic nanoplatform.

Interfacial magnetism at transition-metal oxide interfaces is of tremendous interest. The emergence of ferromagnetism and a matrix-dependent charge transfer between Co and Mn ions in the interdiffusion region of compressively strained LaMnO3–LaCoO3 superlattices (SLs) were studied. The SLs exhibit considerable ferromagnetism, which is negligible in both constituents. This is explained by the matrix-dependent charge transfer between Co and Mn ions. That is, the valence state of diffused Co ions into LaMnO3 shifts from 3+ to 2+ by adopting one electron from Mn3+, inducing the same amount of Mn4+, while the Mn ions that diffuses into LaCoO3 remains Mn3+.

Controllable synthesis of single atom catalysts with sufficiently high metal loading remains challenging due to the tendency of agglomeration. Here the authors synthesize a series of stable atomically dispersed cobalt atoms on graphene with high Co loadings via the regeneration of active sites by atomic layer deposition.

Magnetoresistance in ferromagnetic materials and heterostructures have been enabling advanced understanding of electron transport in solids, as well as new concepts for applications. Here the authors demonstrate a different type of magnetoresistance arising from anomalous Hall effect associated spin–charge mutual conversion.

Abstract Scanning transmission electron microscopy (STEM) has advanced rapidly in the last decade thanks to the ability to correct the major aberrations of the probe-forming lens. Now, atomic-sized beams are routine, even at accelerating voltages as low as 40 kV, allowing knock-on damage to be minimized in beam sensitive materials. The aberration-corrected probes can contain sufficient current for high-quality, simultaneous, imaging and analysis in multiple modes. Atomic positions can be mapped with picometer precision, revealing ferroelectric domain structures, composition can be mapped by energy-dispersive X-ray spectroscopy (EDX) and electron energy loss spectroscopy (EELS), and charge transfer can be tracked unit cell by unit cell using the EELS fine structure. Furthermore, dynamics of point defects can be investigated through rapid acquisition of multiple image scans. Today STEM has become an indispensable tool for analytical science at the atomic level, providing a whole new level of insights into the complex interplays that control material properties.

Quasicrystal precipitation in alloys should be favored at dislocations, which break crystal symmetry, but almost all precipitates at dislocations are periodic. Here, the authors show rare quasicrystal formation along dislocations in a magnesium zinc alloy with atomic resolution.

Abstract 2D transition metal dichalcogenides (2D‐TMDs) and their unique polymorphic features such as the semiconducting 1H and quasi‐metallic 1T′ phases exhibit intriguing optical and electronic properties, which can be used in novel electronic and photonic device applications. With the favorable quasi‐metallic nature of 1T′‐phase 2D‐TMDs, the 1H‐to‐1T′ phase engineering processes are an immensely vital discipline exploited for novel device applications. Here, a high‐yield 1H‐to‐1T′ phase transition of monolayer‐MoS2 on Cu and monolayer‐WSe2 on Au via an annealing‐based process is reported. A comprehensive experimental and first‐principles study is performed to unravel the underlying mechanism and derive the general trends for the high‐yield phase transition process of 2D‐TMDs on metallic substrates. While each 2D‐TMD possesses different intrinsic 1H‐1T′ energy barriers, the option of metallic substrates with higher chemical reactivity plays a significantly pivotal role in enhancing the 1H‐1T′ phase transition yield. The yield increase is achieved via the enhancement of the interfacial hybridizations by the means of increased interfacial binding energy, larger charge transfer, shorter interfacial spacing, and weaker bond strength. Fundamentally, this study opens up the field of 2D‐TMD/metal‐like systems to further scientific investigation and research, thereby creating new possibilities for 2D‐TMDs‐based device applications.

Atom probe tomography (APT) data acquired from a CAMECA LEAP 4000 XHR for the CdS/CdTe interface for a non-CdCl2 treated CdTe solar cell as well as the mass spectrum of an APT data set including a GB in a CdCl2-treated CdTe solar cell are presented. Scanning electron microscopy (SEM) data showing the evolution of sample preparation for APT and scanning transmission electron microscopy (STEM) electron beam induced current (EBIC) are also presented. These data show mass spectrometry peak decomposition of Cu and Te within an APT dataset, the CdS/CdTe interface of an untreated CdTe solar cell, preparation of APT needles from the CdS/CdTe interface in superstrate grown CdTe solar cells, and the preparation of a cross-sectional STEM EBIC sample. Keywords: Scanning electron microscopy, Atom probe tomography, Mass spectroscopy, Solar cells

Single and few-layers MoS2 were uniformly grown on the surface of chemically reduced graphene oxide (r-GO), via a facile liquid phase approach. The method is based on a simple functionalization of r-GO with oleyl amine which seems to affect significantly the MoS2 way of growth. Scanning-transmission-electron microscopy (STEM) analysis revealed the presence of single-layer MoS2 on the surface of a few-layers r-GO. This result was also confirmed by atomic-force microscopy (AFM) images. X-ray photoemission spectroscopy (XPS) and Raman spectroscopy were used for in-depth structural characterization. Furthermore, we have successfully applied the method to synthesize MoS2 nanocomposites with multi wall carbon nanotubes (CN) and carbon nanofibers (CNF). The results demonstrate clearly the selective MoS2 growth on both carbon-based supports.

A wide range of advanced technology for existing and emerging products based on high temperature metal-ceramic composites used in aircrafts, cutting tools, lithium-ion based rechargeable batteries, superconductors, field emission based flat-panel displays, etc. employ micron to submicron sized (0.1-10 microns) particulate precursors in their manufacturing process. Although there has been a significant emphasis given to control of the particle characteristics (shape, size, surface chemistry, adsorption, etc.), relatively little or no attention has been paid to concomitant designing desirable surface and bulk properties at the particulate level, which can ultimately lead to enhanced properties of the product. By attaching atomic to nano-sized inorganic, multi-elemental clusters either in discrete or continuous from onto the surface of the core particles, i.e. nano-functionalization of the particulate surface, materials and products with significantly enhanced properties can be obtained. In this paper, we demonstrate for the first time the synthesis of artificially structured, nano-functionalized particulate materials with unique optical, cathodoluminescent, superconducting and electrical properties. In this paper, we show the feasibility of the pulsed laser ablation technique to make very thin, uniformly distributed and discrete coatings in particulate systems so that the properties of the core particles can be suitably modified. Experiments were conducted for laser deposition of Ag nano particles on Al2O3 and SiO2 core particles by pulsed excimer laser (wavelength =248 nm and pulse duration =25 nanosecond) irradiation of a Ag, Y2O3:Eu3+, and TaSi2 sputtering targets. Analytical techniques using scanning electron microscopy (SEM), wavelength dispersive x-ray mapping (WDX) , transmission electron microscopy (TEM) , scanning transmission electron microscopy with z contrast (STEMZ), and photoluminesence (PL) were utilized to examine the structural, chemical, and morphological characteristics of the nanometric coatings. Qualitative surface uniformity measurements by WDX mapping techniques showed a high degree of coating uniformity on the core particulate. Structural TEM and STEMZ imaging showed both continuous and discrete polycrystalline, multiply twinned nano particle coatings ranging from 5-40 nm in thickness.