Direct growth of single-chiral-angle tungsten disulfide nanotubes using gold nanoparticle catalysts.

Transition metal dichalcogenide (TMD) nanotubes offer a unique platform to explore the properties of TMD materials at the one-dimensional limit. Despite considerable efforts thus far, the direct growth of TMD nanotubes with controllable chirality remains challenging. Here we demonstrate the direct and facile growth of high-quality WS2 and WSe2 nanotubes on Si substrates using catalytic chemical vapour deposition with Au nanoparticles. The Au nanoparticles provide unique accommodation sites for the nucleation of WS2 or WSe2 shells on their surfaces and seed the subsequent growth of nanotubes. We find that the growth mode of nanotubes is sensitive to the temperature. With careful temperature control, we realize ~79% WS2 nanotubes with single chiral angles, with a preference of 30° (~37%) and 0° (~12%). Moreover, we demonstrate how the geometric, electronic and optical properties of the synthesized WS2 nanotubes can be modulated by the chirality. We anticipate that this approach using Au nanoparticles as catalysts will facilitate the growth of TMD nanotubes with controllable chirality and promote the study of their interesting properties and applications.

Nanoscale Optical Conductivity Imaging of Double-Moiré Twisted Bilayer Graphene.

A central paradigm of moiré materials relies on the formation of superlattices that yield enlarged effective crystal unit cells. While a critical consequence of this phenomenon is the celebrated flat electronic bands that foster strong interaction effects, the presence of superlattices has further implications. Here we explore the advantages of moiré superlattices in twisted bilayer graphene (TBG) aligned with hexagonal boron nitride (hBN) for passively enhancing optical conductivity in the low-energy regime. To probe the local optical response of TBG/hBN double-moiré lattices, we use infrared (IR) nano-imaging in conjunction with nanocurrent imaging to examine local optical conductivity over a wide range of TBG twist angles. We show that interband transitions associated with the multiple moiré flat and dispersive bands produce tunable transparent IR responses even at finite carrier densities, which is in stark contrast to the previously limited metallic near transparency observed only in undoped pristine graphene.

Dispersion-Selective Band Engineering in an Artificial Kagome Superlattice.

The relentless pursuit of band structure engineering continues to be a fundamental aspect in solid-state research. Here, we meticulously construct an artificial kagome potential to generate and control multiple Dirac bands of graphene. This unique high-order potential harbors natural multiperiodic components, enabling the reconstruction of band structures through different potential contributions. As a result, the band components, each characterized by distinct dispersions, shift in energy at different velocities in response to the variation of artificial potential. Thereby, we observe a significant spectral weight redistribution of the multiple Dirac peaks. Furthermore, the magnetic field can effectively weaken the superlattice effect and reactivate the intrinsic Dirac band. Overall, we achieve actively dispersion-selective band engineering, a functionality that would substantially increase the freedom in band design.

Real-Space Mapping of Local Subdegree Lattice Rotations in Low-Angle Twisted Bilayer Graphene.

In two-dimensional small-angle twisted bilayers, van der Waals (vdW) interlayer interaction introduces an atomic-scale reconstruction, which consists of a moiré-periodic network of local subdegree lattice rotations. However, real-space measurement of the subdegree lattice rotation requires extremely high spatial resolution, which is an outstanding challenge in an experiment. Here, a topmost small-period graphene moiré pattern is introduced as a magnifying lens to magnify sub-Angstrom lattice distortions in small-angle twisted bilayer graphene (TBG) by about 2 orders of magnitude. Local moiré periods of the topmost graphene moiré patterns and low-energy van Hove singularities of the system are spatially modified by the atomic-scale reconstruction of the underlying TBG, thus enabling real-space mapping of the networks of the subdegree lattice rotations both in structure and in electronic properties. Our results indicate that it is quite facile to study subdegree lattice rotation in vdW systems by measuring the periods of the topmost moiré superlattice.

Realizing One-Dimensional Electronic States in Graphene via Coupled Zeroth Pseudo-Landau Levels.

Strain-induced pseudomagnetic fields can mimic real magnetic fields to generate a zero-magnetic-field analog of the Landau levels (LLs), i.e., the pseudo-Landau levels (PLLs), in graphene. The distinct nature of the PLLs enables one to realize novel electronic states beyond what is feasible with real LLs. Here, we show that it is possible to realize exotic electronic states through the coupling of zeroth PLLs in strained graphene. In our experiment, nanoscale strained structures embedded with PLLs are generated along a one-dimensional (1D) channel of suspended graphene monolayer. Our results demonstrate that the zeroth PLLs of the strained structures are coupled together, exhibiting a serpentine pattern that snakes back and forth along the 1D suspended graphene monolayer. These results are verified theoretically by large-scale tight-binding calculations of the strained samples. Our result provides a new approach to realizing novel quantum states and to engineering the electronic properties of graphene by using localized PLLs as building blocks.

Tailoring Dirac Fermions by In-Situ Tunable High-Order Moiré Pattern in Graphene-Monolayer Xenon Heterostructure.

We report an experimental study of a high-order moiré pattern formed in graphene-monolayer xenon heterostructure. The moiré period is in situ tuned from few nanometers to +∞, by adjusting the lattice constant of the xenon monolayer through annealing. Using angle-resolved photoemission spectroscopy, we observe that Dirac node replicas move closer and finally overlap with a gap opening, as the moiré pattern expands to +∞ and evolves into a Kekulé distortion. A moiré Hamiltonian coupling Dirac fermions from different valleys explains experimental results and indicates narrow moiré band. Our Letter demonstrates a platform to study continuous evolution of the moiré pattern, and provides an unprecedented approach for tailoring Dirac fermions with tunable intervalley coupling.

2D GaN for Highly Reproducible Surface Enhanced Raman Scattering.

Surface-enhanced Raman scattering (SERS) based on 2D semiconductors has been rapidly developed due to their chemical stability and molecule-specific SERS activity. High signal reproducibility is urgently required towards practical SERS applications. 2D gallium nitride (GaN) with highly polar Ga-N bonds enables strong dipole-dipole interactions with the probe molecules, and abundant DOS (density of states) near its Fermi level increases the intermolecular charge transfer probability, making it a suitable SERS substrate. Herein, 2D micrometer-sized GaN crystals are demonstrated to be sensitive SERS platforms with excellent signal reproducibility and stability. Strong dipole-dipole interaction between the dye molecule and 2D GaN enhances the molecular polarizability. Furthermore, 2D GaN benefits its SERS enhancement by the combination of increased DOS and more efficient charge transfer resonances when compared with its bulk counterpart.

Strain induced spin-splitting and half-metallicity in antiferromagnetic bilayer silicene under bending.

Searching for half-metals in low dimensional materials is not only of scientific importance, but also has important implications for the realization of spintronic devices on a small scale. In this work, we show theoretically that simple bending can induce spin-splitting in bilayer silicene. For bilayer silicene with Bernal stacking, the monolayer has a long range ferromagnetic spin order and between the two monolayers, the spin orders are opposite, giving rise to an antiferromagnetic configuration for the ground state of the bilayer silicene. Under bending, the antiferromagnetic spin order is retained but the energetic degeneracy of opposite spin states is lifted. Due to the unusual deformation potentials of the conduction band minimum (CBM) and valence band maximum (VBM) as revealed by density-functional theory calculations and density-functional tight-binding calculations, this spin-splitting is nearly proportional to the degree of bending deformation. Consequently, the spin-splitting can be significant and the desired half-metallic state may emerge when the bending increases, which has been verified by direct simulation of the bent bilayer silicene using the generalized Bloch theorem. Our results hint that bilayer silicene may be an excellent candidate for half-metallicity.

Strain-tunable magnetic and electronic properties of monolayer CrI3.

Two-dimensional CrI3 has attracted much attention as it is reported to be a ferromagnetic semiconductor with a Curie temperature of around 45 K. By performing first-principles calculations, we find that the magnetic ground state of CrI3 is variable under biaxial strain. Our theoretical investigations show that the ground state of monolayer CrI3 is ferromagnetic under compression, but becomes antiferromagnetic under tension. Particularly, the transition occurs under a feasible in-plane strain of around 1.8%. Accompanied by the transition of the magnetic ground state, CrI3 undergoes a transition from magnetic-metal to half-metal to half-semiconductor to spin-relevant semiconductor when the strain varies from -15% to 10%. We attribute these transitions to the variation of the d-orbitals of Cr atoms and the p-orbitals of I atoms. Generally, we report a series of magnetic and electronic phase transitions in strained CrI3, which will help both theoretical and experimental researchers in further understanding the tunable electronic and magnetic properties of CrI3 and its analogs.

Electronic structures and optical properties of partially and fully fluorinated graphene.

In this Letter, we study the electronic structures and optical properties of partially and fully fluorinated graphene by a combination of ab initio G0W0 calculations and large-scale multiorbital tight-binding simulations. We find that, for partially fluorinated graphene, the appearance of paired fluorine atoms is more favorable than unpaired atoms. We also show that different types of structural disorder, such as carbon vacancies, fluorine vacancies, fluorine vacancy clusters and fluorine armchair and zigzag clusters, will introduce different types of midgap states and extra excitations within the optical gap. Furthermore, we argue that the local formation of sp3 bonds upon fluorination can be distinguished from other disorder inducing mechanisms which do not destroy the sp2 hybrid orbitals by measuring the polarization rotation of passing polarized light.

Effect of Structural Relaxation on the Electronic Structure of Graphene on Hexagonal Boron Nitride.

We performed calculations of electronic, optical, and transport properties of graphene on hexagonal boron nitride with realistic moiré patterns. The latter are produced by structural relaxation using a fully atomistic model. This relaxation turns out to be crucially important for electronic properties. We describe experimentally observed features such as additional Dirac points and the "Hofstadter butterfly" structure of energy levels in a magnetic field. We find that the electronic structure is sensitive to many-body renormalization of the local energy gap.

Soil bacterial community characteristics and its effect on organic carbon under different fertilization treatments.

Introduction: By implementing small-scale and efficient fertilization techniques, it is possible to enhance the activity of microorganisms, thereby improving soil carbon sequestration and ecological value in agriculture. Methods: In this study, field experiments were conducted using various types of fertilizers: organic fertilizer, microbial fungal fertilizer, composite fertilizer, and an unfertilized control (CK). Additionally, different dosages of compound fertilizers were applied, including 0.5 times compound fertilizers, constant compound fertilizers, 1.5 times compound fertilizers and CK. Using advanced technologies such as Illumina MiSeq high-throughput sequencing, PICRUSt2 prediction, Anosim analysis, redundancy analysis, canonical correlation analysis, and correlation matrix, soil organic carbon (SOC) content and components, bacterial diversity, metabolic functions, and interaction mechanisms were examined in different fields. Results and Discussion: The results showed pronounced effects of various fertilization modes on SOC and the bacterial community, particularly in the topsoil layer (0-20 cm). Organic fertilizer treatments increased the richness and diversity of bacterial communities in the soil. However, conventional doses and excessive application of compound fertilizers reduced the diversity of soil bacterial communities and SOC content. Additionally, different fertilization treatments led to an increase in easily oxidizable organic carbon (EOC) contents. Interestingly, the relationship between SOC components and soil bacteria exhibited inconsistency. EOC was positively correlated with the bacterial diversity index. Additionally, Chloroflexi exhibited a negative correlation with both SOC and its components. The influence of metabolismon primary metabolic functions on the content of SOC components in the soil was more notable. It included seven types of tertiary functional metabolic pathways significantly correlated with SOC components (p < 0.05). Purpose and Significance: These findings enhance the understanding of the relative abundance of bacterial communities, particularly those related to the carbon cycle, by adjusting agricultural fertilization patterns. This adjustment serves as a reference for enhancing carbon sinks and reducing emissions in agricultural soils.

Optical properties and plasmons in moiré structures.

The discoveries of numerous exciting phenomena in twisted bilayer graphene (TBG) are stimulating significant investigations on moiré structures that possess a tunable moiré potential. Optical response can provide insights into the electronic structures and transport phenomena of non-twisted and twisted moiré structures. In this article, we review both experimental and theoretical studies of optical properties such as optical conductivity, dielectric function, non-linear optical response, and plasmons in moiré structures composed of graphene, hexagonal boron nitride (hBN), and/or transition metal dichalcogenides. Firstly, a comprehensive introduction to the widely employed methodology on optical properties is presented. After, moiré potential induced optical conductivity and plasmons in non-twisted structures are reviewed, such as single layer graphene-hBN, bilayer graphene-hBN and graphene-metal moiré heterostructures. Next, recent investigations of twist-angle dependent optical response and plasmons are addressed in twisted moiré structures. Additionally, we discuss how optical properties and plasmons could contribute to the understanding of the many-body effects and superconductivity observed in moiré structures.

Helicity-Resolved Vibrational Coupling in Twist WS2/WSe2 Heterostructures.

Helicity-resolved Raman spectra can provide an intricate view into lattice structural details. Through the analysis of peak positions, intensities, and circular polarized Raman signals, a wealth of information about chiral structure arrangement within the moiré superlattice, interlayer interaction strength, polarizability change in chemical bond, and beyond can be unveiled. However, the relationship between the circular polarization of high-frequency Raman and twist angle is still not clear. Here, we utilize helicity-resolved Raman spectroscopy to explore the interlayer interactions and the effect of the moiré superlattice in WS2/WSe2 heterostructures. For the out-of-plane Raman mode A1g of WS2 (A1g and 1E2g of WSe2), its intensity is significantly enhanced (suppressed) in WS2/WSe2 heterostructures when θ is less than 10° or greater than 50°. This observation could be attributed to the large polarizability changes in both W-S and W-Se covalent bonds. The circular polarization of 2LA(M) in WSe2 of the WS2/WSe2 heterostructure (θ < 10° or θ > 50°) is significantly enhanced compared to that of 2LA(M) in the monolayer WSe2. We deduce that the circular polarization of the Raman mode correlates with the proportion of high-symmetry area within a supercell of the moiré lattice. Our findings improve the understanding of twist-angle-modulated Raman modes in TMD heterostructures.

Catalytic selectivity of nanorippled graphene.

Experiments have shown that nanoscale ripples in a graphene membrane exhibit unexpectedly high catalytic activity with respect to hydrogen dissociation. Nonetheless, the catalytic selectivity of nanorippled graphene remains unknown, which is an equally important property for assessing a catalyst's potential and its fit-for-purpose applications. Herein, we examine the catalytic selectivity of nanorippled graphene using a model reaction of molecular hydrogen with another simple but double-bonded molecule, oxygen, and comparing the measurement results with those from splitting of hydrogen molecules. We show that although nanorippled graphene exhibits a high catalytic activity toward hydrogen dissociation, the activity for catalyzing the hydrogen-oxygen reaction is quite low, translating into a strong catalytic selectivity. The latter reaction involves the reduction of oxygen molecules by the dissociated hydrogen adatoms, which requires additional energy cost and practically determines the selectivity. In this sense, the well-established information about reactions in general of atomic hydrogen with many other species in the literature could potentially predict the selectivity of nanorippled graphene as a catalyst. Our work provides implications for the catalytic properties of nanorippled graphene, especially its selectivity. The results would be important for its extension to a wider range of reactions and for designer technologies involving hydrogen.

Constructing Ultra-Shallow Near-Edge States for Efficient and Stable Perovskite Solar Cells.

Electronic band structure engineering of metal-halide perovskites (MHP) lies at the core of fundamental materials research and photovoltaic applications. However, reconfiguring the band structures in MHP for optimized electronic properties remains challenging. This article reports a generic strategy for constructing near-edge states to improve carrier properties, leading to enhanced device performances. The near-edge states are designed around the valence band edge using theoretical prediction and constructed through tailored material engineering. These states are experimentally revealed with activation energies of around 23 milli-electron volts by temperature-dependent time-resolved spectroscopy. Such small activation energies enable prolonged carrier lifetime with efficient carrier transition dynamics and low non-radiative recombination losses, as corroborated by the millisecond lifetimes of microwave conductivity. By constructing near-edge states in positive-intrinsic-negative inverted cells, a champion efficiency of 25.4% (25.0% certified) for a 0.07-cm2 cell and 23.6% (22.7% certified) for a 1-cm2 cell is achieved. The most stable encapsulated cell retains 90% of its initial efficiency after 1100 h of maximum power point tracking under one sun illumination (100 mW cm-2) at 65 °C in ambient air.

Ferrielectricity controlled widely-tunable magnetoelectric coupling in van der Waals multiferroics.

The discovery of various primary ferroic phases in atomically-thin van der Waals crystals have created a new two-dimensional wonderland for exploring and manipulating exotic quantum phases. It may also bring technical breakthroughs in device applications, as evident by prototypical functionalities of giant tunneling magnetoresistance, gate-tunable ferromagnetism and non-volatile ferroelectric memory etc. However, two-dimensional multiferroics with effective magnetoelectric coupling, which ultimately decides the future of multiferroic-based information technology, has not been realized yet. Here, we show that an unconventional magnetoelectric coupling mechanism interlocked with heterogeneous ferrielectric transitions emerges at the two-dimensional limit in van der Waals multiferroic CuCrP2S6 with inherent antiferromagnetism and antiferroelectricity. Distinct from the homogeneous antiferroelectric bulk, thin-layer CuCrP2S6 under external electric field makes layer-dependent heterogeneous ferrielectric transitions, minimizing the depolarization effect introduced by the rearrangements of Cu+ ions within the ferromagnetic van der Waals cages of CrS6 and P2S6 octahedrons. The resulting ferrielectric phases are characterized by substantially reduced interlayer magnetic coupling energy of nearly 50% with a moderate electric field of 0.3 V nm-1, producing widely-tunable magnetoelectric coupling which can be further engineered by asymmetrical electrode work functions.

Bonding iron chalcogenides in a hierarchical structure for high-stability sodium storage.

Owing to price-boom and low-reserve of Lithium ion batteries (LIBs), cost-cutting and well-stocked sodium ion batteries (SIBs) attract a lot of attention, aiming to develop an effective energy storage and conversion equipment. As a typical anode for SIBs, Iron sulfide (FeS) is difficult to maintain the high theoretical capacity. Structural instability and inherent low conductivity limit the cyclic and rate performance of FeS. Herein, hierarchical architecture of FeS-FeSe2 coated with nitrogen-doped carbon (NC) is obtained by single-step solvothermal method and two-stage high-temperature treatments. Specifically, lattice imperfections provided by heterogeneous interfaces increase the Na+ storage sites and fasten ion/electron transfer. Synergistic effect induced by the hierarchical architecture effectively enhances the electrochemical activity and reduces the resistance, which contributes to the transfer kinetics of Na+. In addition, the phenomenon that heterogeneous interfaces provide more active site and extra migration Na+ path is also proved by density functional theory (DFT). As an anode for SIBs, FeS-FeSe2/NC (FSSe/C) delivers highly reversible capacity (704.5 mAh·g-1 after 120 cycles at 0.2 A·g-1), excellent rate performance (326.3 mAh·g-1 at 12 A·g-1) and long-lasting durability (492.3 mAh·g-1 after 1000 cycles at 4 A·g-1 with 100 % capacity retention). Notably, the full battery, assembled with FSSe/C and Na3V2(PO4)3/C (NVP/C), delivers reversible capacity of 252.1 mAh·g-1 after 300 cycles at 1 A·g-1. This work provides a facile method to construct a hierarchical architecture anode for high-performance SIBs.

Observation of Rydberg moiré excitons.

Rydberg excitons, the solid-state counterparts of Rydberg atoms, have sparked considerable interest with regard to the harnessing of their quantum application potentials, but realizing their spatial confinement and manipulation poses a major challenge. Lately, the rise of two-dimensional moiré superlattices with highly tunable periodic potentials provides a possible pathway. Here, we experimentally demonstrate this capability through the spectroscopic evidence of Rydberg moiré excitons (XRM), which are moiré-trapped Rydberg excitons in monolayer semiconductor tungsten diselenide adjacent to twisted bilayer graphene. In the strong coupling regime, the XRM manifest as multiple energy splittings, pronounced red shift, and narrowed linewidth in the reflectance spectra, highlighting their charge-transfer character wherein electron-hole separation is enforced by strongly asymmetric interlayer Coulomb interactions. Our findings establish the excitonic Rydberg states as candidates for exploitation in quantum technologies.

Enhanced screening in chemically functionalized graphene.

Resonant scatterers such as hydrogen adatoms can strongly enhance the low-energy density of states in graphene. Here, we study the impact of these impurities on electronic screening. We find a two-faced behavior: Kubo formula calculations reveal an increased dielectric function ε upon creation of midgap states but no metallic divergence of the static ε at small momentum transfer q→0. This bad metal behavior manifests also in the dynamic polarization function and can be directly measured by means of electron energy loss spectroscopy. A new length scale l(c) beyond which screening is suppressed emerges, which we identify with the Anderson localization length.