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Two-dimensional topological materials have attracted intense research efforts owing to their promise in applications for low-energy, high-efficiency quantum computations. Group-VA elemental thin films with strong spin-orbit coupling have been predicted to host topologically nontrivial states as excellent two-dimensional topological materials. Herein, we experimentally demonstrated for the first time that the epitaxially grown high-quality antimonene monolayer islands with buckled configurations exhibit significantly robust one-dimensional topological edge states above the Fermi level. We further demonstrated that these topologically nontrivial edge states arise from a single p-orbital manifold as a general consequence of atomic spin-orbit coupling. Thus, our findings establish monolayer antimonene as a new class of topological monolayer materials hosting the topological edge states for future low-power electronic nanodevices and quantum computations.
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Group-V elemental monolayers were recently predicted to exhibit exotic physical properties such as nontrivial topological properties, or a quantum anomalous Hall effect, which would make them very suitable for applications in next-generation electronic devices. The free-standing group-V monolayer materials usually have a buckled honeycomb form, in contrast with the flat graphene monolayer. Here, we report epitaxial growth of atomically thin flat honeycomb monolayer of group-V element antimony on a Ag(111) substrate. Combined study of experiments and theoretical calculations verify the formation of a uniform and single-crystalline antimonene monolayer without atomic wrinkles, as a new honeycomb analogue of graphene monolayer. Directional bonding between adjacent Sb atoms and weak antimonene-substrate interaction are confirmed. The realization and investigation of flat antimonene honeycombs extends the scope of two-dimensional atomically-thick structures and provides a promising way to tune topological properties for future technological applications.
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As the thickness of a transition metal oxide thin film is reduced to several unit cells, dimensional and interfacial effects modulate its structure and properties, and initiate low-dimension quantum phase transitions different from its bulk counterparts. To check if a metal-insulator transition (MIT) occurs to a low-dimensional 4d2electron systems, we investigated SrMoO3thin films by characterizing and analyzing their lattice structures, electric transport properties and electronic states. Among various dimensional effects and interfacial effects, quantum confinement effect (QCE) was discerned as the dominating mechanism of the thickness-driven MIT. Surface/interface scattering contributes to the residual resistivity while the competition of several interactions modulated by QCE governs the temperature dependence of the resistivity of SrMoO3ultrathin films.
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Charge transfer dynamics across the lying-down 3,4,9,10-perylene-tetracarboxylic-dianhydride (PTCDA) organic semiconductor molecules on Au(111) interface has been investigated using the core-hole clock implementation of resonant photoemission spectroscopy. It is found that the charge transfer time scale at the PTCDA∕Au(111) interface is much larger than the C 1s core-hole lifetime of 6 fs, indicating weak electronic coupling between PTCDA and the gold substrate due to the absence of chemical reaction and∕or bonding.
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Metallofullerene Gd@C82 offers the opportunity to produce novel and advanced polymer-based nanocomposite materials. In this work, we reported the synthesis of novel Gd@C82-containing copolymers with the optimum condition found by changing the temperature, initiator and fullerene contents of C60-PS. The developed materials, based on polystyrene, displayed unique nanostructures which were confirmed by many measurements (GPC, AFM, SEM, TGA/DSC and NEXAFS analysis). The mechanism, stability and structure of Gd@C82-containing copolymer were discussed. This approach offers a new possibility of optimizing the polymer performance with metallofullerene.
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Fulerenos/química , Nanoestructuras/química , Nanoestructuras/ultraestructura , Polímeros/química , Cristalización/métodos , Sustancias Macromoleculares/química , Ensayo de Materiales , Conformación Molecular , Tamaño de la Partícula , Propiedades de SuperficieRESUMEN
Oxygen-vacancy-induced topotactic phase transformation between the ABO2.5brownmillerite structure and the ABO3perovskite structure attracts ever-increasing attention due to the perspective applications in catalysis, clean energy field, and memristors. However, a detailed investigation of the electronic-structure evolution during the topotactic phase transformation for understanding the underlying mechanism is highly desired. In this work, multiple analytical methods were used to explore evolution of the electronic structure of SrFeO3-xthin films during the topotactic phase transformation. The results indicate that the increase in oxygen content induces a new unoccupied state of O 2pcharacter near the Fermi energy, inducing the insulator-to-metal transition. More importantly, the hole states are more likely constrained to thedx2-y2orbital than to thed3z2-r2orbital. Our results reveal an unambiguous evolution of the electronic structure of SrFeO3-xfilms during topotactic phase transformation, which is crucial not only for fundamental understanding but also for perspective applications such as solid-state oxide fuel cells, catalysts, and memristor devices.
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This report establishes an in vitro model on glass surfaces for patterning multiple types of cells to simulate cell-cell interactions in vivo. The model employs a microfluidic system and poly(ethylene glycol)-terminated oxysilane (PEG-oxysilane) to modify glass surfaces in order to resist cell adhesion. The system allows the selective confinement of different types of cells to realize complete confinement, partial confinement, and no confinement of three types of cells on glass surfaces. The model was applied to study intercellular interactions among human umbilical vein endothelial cells (HUVEC), PLA 801 C and PLA801 D cells.
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Células Cultivadas , Vidrio , Animales , Técnicas de Cocultivo , Células Endoteliales/citología , Humanos , Ratones , Microfluídica , Microscopía Electrónica de Rastreo/métodos , Microscopía de Contraste de Fase/métodos , Células 3T3 NIH , Oxígeno/química , Polietilenglicoles/química , Silanos/química , Propiedades de SuperficieRESUMEN
The electronic properties of four metallofullerenol samples (La@C82(OH)32, La@C82(OH)24, La@C82(OH)18, La@C82(OH)12) and La@C82 were investigated by synchrotron radiation photoelectron emission spectra (PES). A new emission peak with binding energy of 13.9 eV, which is attributed to La 5d orbitals coupling with nanocage orbitals, is observed in PES of La@C82 for the first time. This suggestion is also supported by previous DFT calculations. Furthermore, the new emission peak disappears when the surface of La@C82 is modified with specific numbers of OH groups, which means the electron orbital coupling between inner metallic atoms and outer nanocage in metallofullerene could be shielded by surface modifications on the outer nanocage.
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Fulerenos/química , Lantano/química , Cromatografía Líquida de Alta Presión , Electrones , Espectroscopía de Fotoelectrones , Propiedades de SuperficieRESUMEN
X-ray absorption near-edge structure (XANES) spectroscopy has been applied to identify the modification process of single-walled carbon nanotubes (SWCNTs) treated by nitric acid. The carboxyl groups created by the nitric acid treatment have been found to be formed on both the carbonaceous fragments and the side walls of SWCNTs. The carbonaceous fragments could be removed by a following washing treatment with sodium hydroxide. XANES spectra indicate that carbonaceous fragments are the result of the synthesis process and/or of the nitric acid treatment. Tube walls of SWCNTs are weakly oxidized by the nitric acid treatment although, after removing carbonaceous fragments, a direct oxidation process of SWCNTs is observed. Experimental data address the removal of carbonaceous fragments on SWCNTs as an efficient method for side-wall modification of a SWCNT.
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Ensayo de Materiales/métodos , Nanotecnología/métodos , Nanotubos de Carbono/química , Nanotubos de Carbono/ultraestructura , Ácido Nítrico/química , Espectrometría por Rayos X/métodos , Propiedades de SuperficieRESUMEN
Nickel oxide (NiO) nanotubes were synthesized via a thermal oxidation process from Ni nanowires. The effects of oxidation temperature on the morphology, microstructures, and composition of nanowires were investigated using scanning electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy. The results show that the Ni nanowires convert initially to Ni/NiO core-shell nanowires with increasing annealing temperatures, and then to the nanotubes at the critical transition temperature of about 425 °C. Our findings provide useful information for the preparation of NiO nanotubes to meet the required applications.
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Using density functional theory calculations and photoemission measurements, we have studied the interaction between the non-fullerene small-molecule acceptor ITIC and K atoms (a representative of reactive metals). It is found that the acceptor-donor-acceptor-type geometric structure and the electronic structure of ITIC largely decide the interaction process. One ITIC molecule can combine with more than 20 K atoms. For stoichiometries K x≤6ITIC, the K atoms are attracted to the acceptor units of the molecule and donate their 4s electrons to the unoccupied molecular orbitals. K-ITIC organometallic complexes, characterized by the breaking of some S-C bonds in the donor unit of ITIC and the formation of K-S bonds, are formed for stoichiometries K x≥7ITIC. The complexes are still conjugated despite the breaking of some S-C bonds.
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Structure determines material's functionality, and strain tunes the structure. Tuning the coherent epitaxial strain by varying the thickness of the films is a precise route to manipulate the functional properties in the low-dimensional oxide materials. Here, to explore the effects of the coherent epitaxial strain on the properties of SrCoO2.5 thin films, thickness-dependent evolutions of the structural properties and electronic structures were investigated by X-ray diffraction, Raman spectra, optical absorption spectra, scanning transmission electron microscopy (STEM), and first-principles calculations. By increasing the thickness of the SrCoO2.5 films, the c-axis lattice constant decreases, indicating the relaxation of the coherent epitaxial strain. The energy band gap increases and the Raman spectra undergo a substantial softening with the relaxation of the coherent epitaxial strain. From the STEM results, it can be concluded that the strain causes the variation of the oxygen content in the BM-SCO2.5 films, which results in the variation of band gaps with varying the strain. First-principles calculations show that strain-induced changes in bond lengths and angles of the octahedral CoO6 and tetrahedral CoO4 cannot explain the variation band gap. Our findings offer an alternative strategy to manipulate structural and electronic properties by tuning the coherent epitaxial strain in transition-metal oxide thin films.
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Recent experimental breakthroughs open up new opportunities for magnetism in few-atomic-layer two-dimensional (2D) materials, which makes fabrication of new magnetic 2D materials a fascinating issue. Here, we report the growth of monolayer VSe2 by molecular beam epitaxy (MBE) method. Electronic properties measurements by scanning tunneling spectroscopy (STS) method revealed that the as-grown monolayer VSe2 has magnetic characteristic peaks in its electronic density of states and a lower work-function at its edges. Moreover, air exposure experiments show air-stability of the monolayer VSe2. This high-quality monolayer VSe2, a very air-inert 2D material with magnetism and low edge work function, is promising for applications in developing next-generation low power-consumption, high efficiency spintronic devices and new electrocatalysts.
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The temperature-sensitive property of polyhydroxylated metallofullerene film of Gd@C82(OH)x with special hydroxyl number was studied using synchrotron radiation ultraviolet photoelectron spectroscopy (UPS) and TEM techniques. From room temperature (RT) to 4 degrees C the photoelectron onset energy of the spectra of Gd@C82(OH)12 shifted from 1.9 to 0.2 eV, indicating that Gd@C82(OH)12 automatically shifted from insulator at RT to semiconductor at 4 degrees C. However, this could not be observed for Gd@C82(OH)20. TEM experiments show that the variation of conductivity can be ascribed to formation of a microcrystal under low temperature. The dipole moment induced unique intermolecular interactions and self-assembled microcrystalline structures for Gd@C82(OH)12. This may cause reconstruction of the upper valence band formed by pi-like electrons as well as the density of states (DOS) around the Fermi level (EF) and reconstruct the deeper valence band formed by sigma-like electrons, eventually resulting in a shift to a semiconducting nature. These findings revealed a novel nature for polyhydroxylated Gd@C82(OH)x materials: Their insulating properties can be controllably tuned into semiconducting ones as a function of temperature.
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Conductividad Eléctrica , Fulerenos/química , Oro/química , Agua/química , Electrones , Microscopía Electrónica de Transmisión , Estructura Molecular , Fotoquímica , TemperaturaRESUMEN
Monolayer antimonene is fabricated on PdTe2 by an epitaxial method. Monolayer antimonene is theoretically predicted to have a large bandgap for nanoelectronic devices. Air-exposure experiments indicate amazing chemical stability, which is great for device fabrication. A method to fabricate high-quality monolayer antimonene with several great properties for novel electronic and optoelectronic applications is provided.
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The electronic state evolution of single bilayer (1BL) Bi(1 1 1) deposited on three-dimensional (3D) Bi2Se x Te3-x topological insulators at x = 0, 1.26, 2, 2.46, 3 is systematically investigated by angle-resolved photoemission spectroscopy (ARPES). Our results indicate that the electronic structures of epitaxial Bi films are strongly influenced by the substrate especially the topmost sublayer near the Bi films, manifesting in two main aspects. First, the Se atoms cause a stronger charge transfer effect, which induces a giant Rashba-spin splitting, while the low electronegativity of Te atoms induces a strong hybridization at the interface. Second, the lattice strain notably modifies the band dispersion of the surface bands. Furthermore, our experimental results are elucidated by first-principles band structure calculations.
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2D materials with heterolayered structures beyond graphene are explored. A theoretically predicted superconductor-topological insulator-normal metal heterolayered structure is realized experimentally. The generated hybrid structure HfTe3 /HfTe5 /Hf has potential applications in both quantum-spin Hall effect-based and Majorana-based devices.
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The possibility of modulating the electronic configurations of the innermost atoms inside a nanospace, nano sheath with chemical modification was investigated using synchrotron X-ray photoelectron spectroscopy. Systems of definite nanostructures were chosen for this study. Systematic variations in energy, intensity, and width of pi and sigma O 1s core level spectra, in absorption characteristics of C 1s-->pi transition, in photoabsorption of pre-edge and resonance regions of the Gd 4d-->4f transition, were observed for Gd@C(82) (an isolated nanospace for Gd), Gd@C(82)(OH)(12) (a modified nanospace for Gd), and Gd@C(82)(OH)(22) (a differently modified nanospace for Gd), and the reference materials Gd-DTPA (a semi-closed space for Gd) and Gd(2)O(3). A sandwich-type electronic interaction along [outer modification group]-[nano sheaths]-[inner metallic atom] was observed in the molecules of modifications. This makes it possible to control electron-donation directions, either from the innermost metallic atom toward the outer nano sheaths or the reverse. The results suggest that one may effectively tune the fine structures of electronic configurations of such a metallic atom being astricted into nanostructures through changing the number or category of outer groups of chemical modifications. This may open a door to realizing the desired designs for electronic and magnetic properties of functionalized nanomaterials.
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Metales/química , Nanotecnología , Gadolinio/química , Espectrometría de Masa por Láser de Matriz Asistida de Ionización DesorciónRESUMEN
Preparation of heterogeneous catalysts with active ferrous centers is of great significance for industrial and environmental catalytic processes. Nanostructured carbon materials (NCM), which possess free-flowing π electrons, can coordinate with transition metals, provide a confinement environment for catalysis, and act as potential supports or ligands to construct analogous complexes. However, designing such catalysts using NCM is still seldom studied to date. Herein, we synthesized a sandwich structured ternary complex via the coordination of Fe-loaded humic acid (HA) with C=C bonds in the aromatic rings of carbon nanotubes (CNTs), in which the O/N-Fe-C interface configuration provides the confinement environment for the ferrous sites. The experimental and theoretical results revealed octahedrally/tetrahedrally coordinated geometry at Fe centers, and the strong hybridization between CNT C π* and Fe 3d orbitals induces discretization of the atomic charges on aromatic rings of CNTs, which facilitates O2 adsorption and electron transfer from carbon to O2, which enhances O2 activation. The O2 activation by the novel HA/Fe-CNT complex can be applied in the oxidative degradation of phenol red (PR) and bisphenol A (BPA) in aqueous media.
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Sustancias Húmicas , Nanotubos de Carbono/química , Adsorción , Compuestos de Bencidrilo/química , Carbono/química , Catálisis , Espectroscopía de Resonancia por Spin del Electrón , Electrones , Peróxido de Hidrógeno/química , Iones , Hierro/química , Ligandos , Metales/química , Distribución Normal , Oxígeno/química , Fenoles/química , Fenolsulfonftaleína/química , Agua/químicaRESUMEN
Hydrogen-related defects play crucial roles in determining physical properties of their host oxides. In this work, we report our systematic experimental and theoretical (based on density functional theory) studies of the defect states formed in hydrogenated-rutile TiO2 in gaseous H2 and atomic H. In gas-hydrogenated TiO2, the incorporated hydrogen tends to occupy the oxygen vacancy site and negatively charged. The incorporated hydrogen takes the interstitial position in atom-hydrogenated TiO2, forming a weak O-H bond with the closest oxygen ion, and becomes positive. Both states of hydrogen affect the electronic structure of TiO2 mainly through changes of Ti 3d and O 2p states instead of the direct contributions of hydrogen. The resulted electronic structures of the hydrogenated TiO2 are manifested in modifications of the electrical and optical properties that will be useful for the design of new materials capable for green energy economy.