Local Density of States Modulated by Strain in Marginally Twisted Bilayer Graphene

In marginally twisted bilayer graphene,the Moirépattern consists of the maximized AB(BA)stacking regions,minimized AA stacking regions and triangular networks of domain walls.Here we realize the strain-modulated electronic structures of marginally twisted bilayer graphene by scanning tunneling microscopy/spectroscopy and density functional theory(DFT)calculations.The experimental data show four peaks near the Fermi energy at the AA regions.DFT calculations indicate that the two new peaks closer to the Fermi level may originate from the intrinsic heterostrain and the electric field implemented by back gate is likely to account for the observed shift of the four peaks.Furthermore,the d I/d V map across Moirépatterns with different strain strengths exhibits a distinct appearance of the helical edge states.

Intrinsic charge transport behaviors in graphene-black phosphorus van der Waals heterojunction devices

Heterostructures from mechanically-assembled stacks of two-dimensional materials allow for versatile electronic device applications. Here, we demonstrate the intrinsic charge transport behaviors in graphene-black phosphorus heterojunction devices under different charge carrier densities and temperature regimes. At high carder densities or in the ON state, tunneling through the Schottky barrier at the interface between graphene and black phosphorus dominates at low temperatures. With temperature increasing, the Schottky barrier at the interface is vanishing, and the channel current starts to decrease with increasing temperature, behaving like a metal. While at low carder densities or in the OFF state, thermal emission over the Schottky barrier at the interface dominates the carriers transport process. A barrier height of ～ 67.3 meV can be extracted from the thermal emission-diffusion theory.

Fabrication of large-scale graphene/2D-germanium heterostructure by intercalation

We report a large-scale, high-quality heterostructure composed of vertically-stacked graphene and two-dimensional(2D) germanium.The heterostructure is constructed by the intercalation-assisted technique.We first synthesize large-scale,single-crystalline graphene on Ir(111) surface and then intercalate germanium at the interface of graphene and Ir(111).The intercalated germanium forms a well-defined 2D layer with a 2 × 2 superstructure with respect to Ir(111).Theoretical calculations demonstrate that the 2D germanium has a double-layer structure.Raman characterizations show that the 2D germanium effectively weakens the interaction between graphene and Ir substrate, making graphene more like the intrinsic one.Further experiments of low-energy electron diffraction, scanning tunneling microscopy, and x-ray photoelectron spectroscopy(XPS) confirm the formation of large-scale and high-quality graphene/2D-germanium vertical heterostructure.The integration of graphene with a traditional 2D semiconductor provides a platform to explore new physical phenomena in the future.

Prediction of structured void-containing 1T-PtTe2 monolayer with potential catalytic activity for hydrogen evolution reaction

Two-dimensional(2D)transition metal dichalcogenides(TMDs)have attracted considerable attention because of their unique properties and great potential in nano-technology applications.Great efforts have been devoted to fabrication of novel structured TMD monolayers by modifying their pristine structures at the atomic level.Here we propose an intriguing structured 1T-PtTe2 monolayer as hydrogen evolution reaction(HER)catalyst,namely,Pt4Te7,using first-principles calculations.It is found that Pt4Te7 is a stable monolayer material verified by the calculation of formation energy,phonon dispersion,and ab initio molecular dynamics simulations.Remarkably,the novel structured void-containing monolayer exhibits superior catalytic activity toward HER compared with the pristine one,with a Gibbs free energy very close to zero(less than 0.07 eV).These features indicate that Pt4Te7 monolayer is a high-performance HER catalyst with a high platinum utilization.These findings open new perspectives for the functionalization of 2D TMD materials at an atomic level and its application in HER catalysis.

High quality PdTe_2 thin films grown by molecular beam epitaxy

PdTe2, a member of layered transition metal dichalcogenides （TMDs）, has aroused significant research interest due to the coexistence of superconductivity and type-II Dirac fermions. It provides a promising platform to explore the inter- play between superconducting quasiparticles and Dirac fermions. Moreover, PdTe2 has also been used as a substrate for monolayer antimonene growth. Here in this paper, we report the epitaxial growth of high quality PdTe2 films on bilayer graphene/SiC（0001） by molecular beam epitaxy （MBE）. Atomically thin films are characterized by scanning tunneling microscopy （STM）, X-ray photoemission spectroscopy （XPS）, low-energy electron diffraction （LEED）, and Raman spec- troscopy. The band structure of 6-layer PdTe2 film is measured by angle-resolved photoemission spectroscopy （ARPES）. Moreover, our air exposure experiments show excellent chemical stability of epitaxial PdTe2 film. High-quality PdTe2 films provide opportunities to build antimonene/PdTe2 heterostructure in ultrahigh vacuum for future applications in electronic and optoelectronic nanodevices.

Real-space observation on standing configurations of phenylacetylene on Cu(111) by scanning probe microscopy

The adsorption configurations of molecules adsorbed on substrates can significantly affect their physical and chemical properties. A standing configuration can be difficult to determine by traditional techniques, such as scanning tunneling microscopy(STM) due to the superposition of electronic states. In this paper, we report the real-space observation of the standing adsorption configuration of phenylacetylene on Cu(111) by non-contact atomic force microscopy(nc-AFM).Deposition of phenylacetylene at 25 K shows featureless bright spots in STM images. Using nc-AFM, the line features representing the C–H and C–C bonds in benzene rings are evident, which implies a standing adsorption configuration. Further density functional theory(DFT) calculations reveal multiple optimized adsorption configurations with phenylacetylene breaking its acetylenic bond and forming C–Cu bond(s) with the underlying copper atoms, and hence stand on the substrate.By comparing the nc-AFM simulations with the experimental observation, we identify the standing adsorption configuration of phenylacetylene on Cu(111). Our work demonstrates an application of combining nc-AFM measurements and DFT calculations to the study of standing molecules on substrates, which enriches our knowledge of the adsorption behaviors of small molecules on solid surfaces at low temperatures.

Band engineering of B_2H_2 nanoribbons

Freestanding honeycomb borophene is unstable due to the electron-deficiency of boron atoms. B_2H_2 monolayer, a typical borophene hydride, has been predicted to be structurally stable and attracts great attention. Here, we investigate the electronic structures of B_2H_2 nanoribbons. Based on first-principles calculations, we have found that all narrow armchair nanoribbons with and without mirror symmetry(ANR-s and ANR-as, respectively) are semiconducting. The energy gap has a relation with the width of the ribbon. When the ribbon is getting wider, the gap disappears. The zigzag ribbons without mirror symmetry(ZNR-as) have the same trend. But the zigzag ribbons with mirror symmetry(ZNR-s) are always metallic. We have also found that the metallic ANR-as and ZNR-s can be switched to semiconducting by applying a tensile strain along the nanoribbon. A gap of 1.10 eV is opened under 16% strain for the 11.0-■ ANR-as. Structural stability under such a large strain has also been confirmed. The flexible band tunability of B_2H_2 nanoribbon increases its possibility of potential applications in nanodevices.

Interaction of two symmetric monovacancy defects in graphene

We investigate the interactions between two symmetric monovacancy defects in graphene grown on Ru(0001) after silicon intercalation by combining first-principles calculations with scanning tunneling microscopy(STM). First-principles calculations based on free-standing graphene show that the interaction is weak and no scattering pattern is observed when the two vacancies are located in the same sublattice of graphene, no matter how close they are, except that they are next to each other. For the two vacancies in different sublattices of graphene, the interaction strongly influences the scattering and new patterns' emerge, which are determined by the distance between two vacancies. Further experiments on silicon intercalated graphene epitaxially grown on Ru(0001) shows that the experiment results are consistent with the simulated STM images based on free-standing graphene, suggesting that a single layer of silicon is good enough to decouple the strong interaction between graphene and the Ru(0001) substrate.

Low-temperature growth of large-scale,single-crystalline graphene on Ir(111)

Iridium is a promising substrate for self-limiting growth of graphene. However, single-crystalline graphene can only be fabricated over 1120 K. The weak interaction between graphene and Ir makes it challenging to grow graphene with a single orientation at a relatively low temperature. Here, we report the growth of large-scale, single-crystalline graphene on Ir(111) substrate at a temperature as low as 800 K using an oxygen-etching assisted epitaxial growth method. We firstly grow polycrystalline graphene on Ir. The subsequent exposure of oxygen leads to etching of the misaligned domains.Additional growth cycle, in which the leftover aligned domain serves as a nucleation center, results in a large-scale and single-crystalline graphene layer on Ir(111). Low-energy electron diffraction, scanning tunneling microscopy, and Raman spectroscopy experiments confirm the successful growth of large-scale and single-crystalline graphene. In addition, the fabricated single-crystalline graphene is transferred onto a SiO_2/Si substrate. Transport measurements on the transferred graphene show a carrier mobility of about 3300 cm^2·V^(-1)·s^(-1). This work provides a way for the synthesis of large-scale,high-quality graphene on weak-coupled metal substrates.

Structural and thermal stabilities of Au@Ag core-shell nanoparticles and their arrays:A molecular dynamics simulation

Thermal stability of core-shell nanoparticles(CSNPs)is crucial to their fabrication processes,chemical and physical properties,and applications.Here we systematically investigate the structural and thermal stabilities of single Au@Ag CSNPs with different sizes and their arrays by means of all-atom molecular dynamics simulations.The formation energies of all Au@Ag CSNPs we reported are all negative,indicating that Au@Ag CSNPs are energetically favorable to be formed.For Au@Ag CSNPs with the same core size,their melting points increase with increasing shell thickness.If we keep the shell thickness unchanged,the melting points increase as the core sizes increase except for the CSNP with the smallest core size and a bilayer Ag shell.The melting points of Au@Ag CSNPs show a feature of non-monotonicity with increasing core size at a fixed NP size.Further simulations on the Au@Ag CSNP arrays with 923 atoms reveal that their melting points decrease dramatically compared with single Au@Ag CSNPs.We find that the premelting processes start from the surface region for both the single NPs and their arrays.

Dirac states from p_(x,y)orbitals in the buckled honeycomb structures:A tight-binding model and first-principles combined study

Dirac states composed of Px,y orbitals have been reported in many two-dimensional （2D） systems with honeycomb lattices recently. Their potential importance has aroused strong interest in a comprehensive understanding of such states. Here, we construct a four-band tight-binding model for the Px,y-orbital Dirac states considering both the nearest neighbor hopping interactions and the lattice-buckling effect. We find that Px,y-orbital Dirac states are accompanied with two addi- tional narrow bands that are flat in the limit of vanishing n bonding, which is in agreement with previous studies. Most importantly, we analytically obtain the linear dispersion relationship between energy and momentum vector near the Dirac cone. We find that the Fermi velocity is determined not only by the hopping through n bonding but also by the hopping through ~ bonding of Px,y orbitals, which is in contrast to the case of pz-orbital Dirac states. Consequently, Px,y-orbital Dirac states offer more flexible engineering, with the Fermi velocity being more sensitive to the changes of lattice constants and buckling angles, if strain is exerted. We further validate our tight-binding scheme by direct first-principles calcula- tions of model-materials including hydrogenated monolayer Bi and Sb honeycomb lattices. Our work provides a more in-depth understanding of Px,y-orbital Dirac states in honeycomb lattices, which is useful for the applications of this family of materials in nanoelectronics.

Experimental Synthesis of Strained Monolayer Silver Arsenide on Ag(111)Substrates

Two-dimensional(2 D)materials are playing more and more important roles in both basic sciences and industrial applications.For 2 D materials,strain could tune the properties and enlarge applications.Since the growth of 2 D materials on substrates is often accompanied by strain,the interaction between 2 D materials and substrates is worthy of careful attention.Here we demonstrate the fabrication of strained monolayer silver arsenide(AgAs)on Ag(111)by molecular beam epitaxy,which shows one-dimensional stripe structures arising from uniaxial strain.The atomic geometric structure and electronic band structure are investigated by low energy electron diffraction,scanning tunneling microscopy,x-ray photoelectron spectroscopy,angle-resolved photoemission spectroscopy and first-principle calculations.Monolayer AgAs synthesized on Ag(111)provides a platform to study the physical properties of strained 2 D materials.

Thickness-dependent magnetic order and phase transition in V5S8

V5S8 is an ideal candidate to explore the magnetism at the two-dimensional(2D)limit.A recent experiment has shown that the V5S8 thin films exhibit an antiferromagnetic(AFM)to ferromagnetic(FM)phase transition with reducing thickness.Here,for the first time,using density functional theory calculations,we report the antiferromagnetic order of bulk V5S8,which is consistent with the previous experiments.The specific antiferromagnetic order is reproduced when Ueff=2 eV is applied on the intercalated vanadium atoms within LDA.We find that the origin of the magnetic ordering is from superexchange interaction.We also investigate the thickness-dependent magnetic order in V5S8 thin films.It is found that there is an antiferromagnetic to ferromagnetic phase transition when V5S8 is thinned down to 2.2 nm.The main magnetic moments of the antiferromagnetic and ferromagnetic states of the thin films are located on the interlayered vanadium atoms,which is the same as that in the bulk.Meanwhile,the strain in the thin films also influences the AFM-FM phase transition.Our results not only reveal the magnetic order and origin in bulk V5S8 and thin films,but also provide a set of parameters which can be used in future calculations.

“小分子机器”量子结构的构造及其物性

低维量子结构的构筑及调控是物理学向小尺度研究方向延伸的核心问题之一.本文重点围绕高鸿钧及合作者在"小分子机器"量子结构的构造及其物性方面开展的研究,系统地介绍了他们在单原子层次上设计、构造和调控的若干小分子机器量子结构.代表性工作有:(1)构筑了四叔丁基酞菁锌((t-Bu)4-Zn Pc)分子在Au(111)表面上"抛锚"的、带有固定偏心轴的单分子转子及其有序阵列,证实了转动行为的可调控性;(2)实现了单个小分子极限尺度(0.6 nm)的可逆电导转变,进而实现了稳定、重复、可逆的超高密度信息存储中的原理性应用;(3)首次直接证实代表性的"分子机器"轮烷(Rotaxane)分子的构型及其电导的可逆转变,澄清了当时化学界的一个争论热点,该热点也是2016年诺贝尔化学奖的主要成果;(4)通过单个H原子的吸脱附实现了酞菁锰(Mn Pc)分子在Au(111)表面Kondo效应的调控,这种单个自旋量子态的可逆控制,实现了极高密度信息存储(>40 TB/cm^2)的原理性应用;(5)在通过"原子手术"Mn Pc分子所创制的一种新"功能体系"上发现了朗德g因子在原子尺度上具有的空间分布不均匀性,这是长期以来一直未解决的问题.这些系统工作为单分子发电机/无线电辐射器及纳米电子器件等的构造组装与应用奠定了基础.

MgO intercalation and crystallization between epitaxial graphene and Ru(0001)

Graphene on insulator is the foundation of its practical applications in electronic information technology.However,fabrication of graphene on insulating substrates suffers from small size and limited quality by direct growth of graphene on dielectric substrates,and the method of transferring graphene onto insulating substrates is not so compatible with the large-scale production in industry.Here,we report the fabrication of high-quality,large-area,single-crystal graphene on crystalline magnesium oxide(MgO),which has a dielectric constant of 7–10.Magnesium and oxygen are intercalated at the interface of epitaxial graphene/Ru(0001)and form crystalline structure after high-temperature annealing.The graphene/MgO/Ru(0001)sample was characterized by low energy electron diffraction(LEED),scanning tunneling microscopy(STM),X-ray photoelectron spectroscopy(XPS),and scanning transmission electron microscopy(STEM).LEED pattern shows that the magnesium oxide displays crystalline structure,and STM studies show clearly that the top layer is graphene.STEM characterization of as-intercalated sample demonstrates that the MgO intercalation layer,with a thickness of up to 2.3 nm,has a crystal structure of rock salt MgO,and the out-of-plane crystal orientation is[001].Our work provides a new route for fabrication of graphene on high dielectric constant insulators,which may have potential applications in future electronics.