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1.
Sci Adv ; 5(11): eaav4355, 2019 11.
Artigo em Inglês | MEDLINE | ID: mdl-31700996

RESUMO

Recently, several captivating topological structures of electric dipole moments (e.g., vortex, flux closure) have been reported in ferroelectrics with reduced size/dimensions. However, accurate polarization distribution of these topological ferroelectric structures has never been experimentally obtained. We precisely measure the polarization distribution of an individual ferroelectric vortex in PbTiO3/SrTiO3 superlattices at the subunit cell level by using the atomically resolved integrated differential phase contrast imaging in an aberration-corrected scanning transmission electron microscope. We find, in vortices, that out-of-plane polarization is larger than in-plane polarization, and that downward polarization is larger than upward polarization. The polarization magnitude is closely related to tetragonality. Moreover, the contribution of the Pb─O bond to total polarization is highly inhomogeneous in vortices. Our precise measurement at the subunit cell scale provides a sound foundation for mechanistic understanding of the structure and properties of a ferroelectric vortex and lattice-charge coupling phenomena in these topological ferroelectric structures.

2.
Nat Commun ; 10(1): 5013, 2019 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-31676774

RESUMO

For atomically thin two-dimensional materials, interfacial effects may dominate the entire response of devices, because most of the atoms are in the interface/surface. Graphene/sapphire has great application in electronic devices and semiconductor thin-film growth, but the nature of this interface is largely unknown. Here we find that the sapphire surface has a strong interaction with some of the carbon atoms in graphene to form a C-O-Al configuration, indicating that the interface interaction is no longer a simple van der Waals interaction. In addition, the structural relaxation of sapphire near the interface is significantly suppressed and very different from that of a bare sapphire surface. Such an interfacial C-O-Al bond is formed during graphene growth at high temperature. Our study provides valuable insights into understanding the electronic structures of graphene on sapphire and remote control of epitaxy growth of thin films by using a graphene-sapphire substrate.

3.
ACS Appl Mater Interfaces ; 11(40): 36800-36806, 2019 Oct 09.
Artigo em Inglês | MEDLINE | ID: mdl-31539219

RESUMO

The oxygen vacancy profile in LaCoO3 exhibits rich phases with distinct structures, symmetries, and magnetic properties. Exploration of the lattice degree of freedom of LaCoO3 in the transition between these different structural phases may provide a route to enable new functionality in oxide materials with potential applications. To date, the oxygen vacancy profile transition in LaCoO3 has mainly been induced by transition-metal doping or thermal treatment. Epitaxial strain was proposed to compete with the lattice degree of freedom but has not yet been rationalized. Here, the experimental findings of strain-inhibited structural transition from perovskite to brownmillerite during the electromigration of oxygen vacancies in epitaxial LaCoO3 thin films are demonstrated. The results indicate that the oxygen vacancy ordering phase induced by the electric field is suppressed locally by both epitaxial strain field and external loads shown by in situ aberration-corrected (scanning)/ transmission electron microscopy. The demonstrated complex interplay between the electric and strain fields in the structural transitions of LaCoO3 opens up prospects for manipulating new physical properties by external excitations and/or strain engineering of a substrate.

4.
Adv Mater ; 31(39): e1901964, 2019 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-31389096

RESUMO

Atomically thin oxychalcogenides have been attracting intensive attention for their fascinating fundamental properties and application prospects. Bi2 O2 Se, a representative of layered oxychalcogenides, has emerged as an air-stable high-mobility 2D semiconductor that holds great promise for next-generation electronics. The preparation and device fabrication of high-quality Bi2 O2 Se crystals down to a few atomic layers remains a great challenge at present. Here, molecular beam epitaxy (MBE) of atomically thin Bi2 O2 Se films down to monolayer on SrTiO3 (001) substrate is achieved by co-evaporating Bi and Se precursors in oxygen atmosphere. The interfacial atomic arrangements of MBE-grown Bi2 O2 Se/SrTiO3 are unambiguously revealed, showing an atomically sharp interface and atom-to-atom alignment. Importantly, the electronic band structures of one-unit-cell (1-UC) thick Bi2 O2 Se films are observed by angle-resolved photoemission spectroscopy (ARPES), showing low effective mass of ≈0.15 m0 and bandgap of ≈0.8 eV. These results may be constructive to the synthesis of other 2D oxychalcogenides and investigation of novel physical properties.

5.
Nano Lett ; 19(8): 5070-5076, 2019 Aug 14.
Artigo em Inglês | MEDLINE | ID: mdl-31322902

RESUMO

Phonon polaritons hold potential prospects of nanophotonic applications at the mid- and far-infrared wavelengths. However, their experimental investigation in the far-infrared range has long been a technical challenge due to the lack of suitable light sources and detectors. To obviate these difficulties, here we use an electron probe with sub-10 meV energy resolution and subnanometer spatial resolution to study far-infrared surface phonon polaritons (∼50-70 meV) in ZnO nanostructures. We observe ultraslow propagation and interference fringes of propagating surface phonon polaritons and obtain their dispersion relation through measurements in the coordinate space. By mapping localized modes in nanowires and flakes, we reveal their localized nature and investigate geometry and size effects. Associated with simulation, we show that surface phonon polariton behaviors can be well described by the local continuum dielectric model. Our work paves the way for spatial-resolved investigation of surface phonon polaritons by electron probes and forwards polaritonics in the far-infrared range.

6.
iScience ; 16: 368-377, 2019 Jun 28.
Artigo em Inglês | MEDLINE | ID: mdl-31220760

RESUMO

Oxide-based resistive switching devices, including ferroelectric tunnel junctions and resistance random access memory, are promising candidates for the next-generation non-volatile memory technology. In this work, we propose a ferroionic tunnel junction to realize a giant electroresistance. It functions as a ferroelectric tunnel junction at low resistance state and as a Schottky junction at high resistance state, due to interface engineering through the field-induced migration of oxygen vacancies. An extremely large electroresistance with ON/OFF ratios of 5.1×107 at room temperature and 2.1×109 at 10 K is achieved, using an ultrathin BaTiO3-δ layer as the ferroelectric barrier and a semiconducting Nb-doped SrTiO3 substrate as the bottom electrode. The results point toward an appealing way for the design of high-performance resistive switching devices based on ultrathin oxide heterostructures by ionic controlled interface engineering.

7.
Adv Mater ; 31(29): e1901624, 2019 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-31140651

RESUMO

For III-nitride-based devices, such as high-brightness light-emitting diodes (LEDs), the poor heat dissipation of the sapphire substrate is deleterious to the energy efficiency and restricts many of their applications. Herein, the role of vertically oriented graphene (VG) nanowalls as a buffer layer for improving the heat dissipation in AlN films on sapphire substrates is studied. It is found that VG nanowalls can effectively enhance the heat dissipation between an AlN film and a sapphire substrate in the longitudinal direction because of their unique vertical structure and good thermal conductivity. Thus, an LED fabricated on a VG-sapphire substrate shows a 37% improved light output power under a high injection current (350 mA) with an effective 3.8% temperature reduction. Moreover, the introduction of VG nanowalls does not degrade the quality of the AlN film, but instead promotes AlN nucleation and significantly reduces the epilayer strain that is generated during the cooling process. These findings suggest that the VG nanowalls can be a good buffer layer candidate in III-nitride semiconductor devices, especially for improving the heat dissipation in high-brightness LEDs.

8.
Nat Nanotechnol ; 14(7): 691-697, 2019 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-31011219

RESUMO

Spin waves may constitute key components of low-power spintronic devices. Antiferromagnetic-type spin waves are innately high-speed, stable and dual-polarized. So far, it has remained challenging to excite and manipulate antiferromagnetic-type propagating spin waves. Here, we investigate spin waves in periodic 100-nm-wide stripe domains with alternating upward and downward magnetization in La0.67Sr0.33MnO3 thin films. In addition to ordinary low-frequency modes, a high-frequency mode around 10 GHz is observed and propagates along the stripe domains with a spin-wave dispersion different from the low-frequency mode. Based on a theoretical model that considers two oppositely oriented coupled domains, this high-frequency mode is accounted for as an effective antiferromagnetic spin-wave mode. The spin waves exhibit group velocities of 2.6 km s-1 and propagate even at zero magnetic bias field. An electric current pulse with a density of only 105 A cm-2 can controllably modify the orientation of the stripe domains, which opens up perspectives for reconfigurable magnonic devices.

9.
ACS Nano ; 12(12): 12869-12878, 2018 Dec 26.
Artigo em Inglês | MEDLINE | ID: mdl-30452226

RESUMO

Sodium ion batteries are one of most promising alternatives to lithium ion batteries for large-scale energy storage, due to the high abundance and low cost of sodium in the earth. However, the lack of advanced electrode materials greatly affects their applications. Here, layered-structure SbPO4 is explored as an anode material for sodium ion batteries in terms of SbPO4 nanorods on reduced graphene oxide (SbPO4/rGO). In situ transmission electron microscopy images reveal the preferential expansion along the transverse direction of the nanorods upon the first discharging, which arises from the reduction of SbPO4 to Sb and the subsequent alloying of Sb as supported by in situ X-ray diffraction and selected area electron diffraction patterns. SbPO4/rGO exhibits a capacity retention of 99% after 100 cycles at 0.5 A g-1 both in half cells and in full cells. Its specific capacity at 5 A g-1 is 214 mA h g-1 in half cells or 134 mA h g-1 in full cells. Moreover, the energy density of the full cells at 1.2 kW kg-1total is still 99.8 W h kg-1total, very promising as an advanced electrode material.

10.
ACS Appl Mater Interfaces ; 8(51): 35163-35171, 2016 Dec 28.
Artigo em Inglês | MEDLINE | ID: mdl-27977117

RESUMO

The commercial applications of Mn3O4 in lithium ion batteries (LIBs) are greatly restricted because of the low electrical conductivity and poor cycling stability at high current density. To overcome these drawbacks, mesoporous Mn3O4@C networks were designed and synthesized via an improved bake-in-salt method using NaCl as the assistant salt, and without the protection of inert gas. The added NaCl plays a versatile role during the synthetic process, including the heat conducting medium, removable hard template and protective layer. Because of the homogeneous distribution of Mn3O4 nanoparticles within the carbon matrix, the as-prepared Mn3O4@C networks show excellent cycling stability in LIBs. After cycling for 950 times at a current density of 1 A g-1, the discharge capacity of the as-prepared Mn3O4@C networks is determined to be 754.4 mA h g-1, showing superior cycling stability as compared to its counterparts. The valuable and promising method, simple synthetic procedure and excellent cycling stability of the as-prepared Mn3O4@C networks makes it a promising candidate as the potential anode material for LIBs.

11.
Nanoscale Res Lett ; 11(1): 444, 2016 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-27699715

RESUMO

MnS has been attracting more and more attentions in the fields of lithium ion batteries (LIBs) because of its high energy density and low voltage potential. In this paper, we present a simple method for the preparation of urchin-like γ-MnS microstructures using L-cysteine and MnCl2 · 4H2O as the starting materials. The urchin-like γ-MnS microstructures exhibit excellent cycling stability (823.4 mA h g-1 at a current density of 500 mA g-1, after 1000 cycles). And the discharge voltage is about 0.75 V, making it a good candidate for the application as the anode material in LIBs. SEM, TEM, and XRD were employed to inspect the changes of the active materials during the electrochemical process, which clearly indicate that the structural pulverization and reformation of the γ-MnS microstructures play important roles for the maintenance of the electrochemical performance during the charge/discharge process.

12.
Nanoscale Res Lett ; 11(1): 126, 2016 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-26951126

RESUMO

In this report, a novel photocatalyst based on Bi2WO6/Ag2S heterostructures was prepared by a 3-mercaptopropionic acid (MPA)-assisted route at room temperature. Compared to bare Bi2WO6 and Ag2S nanoparticles, the as-formed Bi2WO6/Ag2S heterostructures exhibit enhanced photocatalytic activity for the degradation of rhodamine B (Rh B) under visible-light irradiation. This kind of enhancement in the photocatalytic activity is considered to be the synergistic effects of both the effective electron-hole separation and expansion of the light-absorption range. The pH of the solution is of vital importance to the photocatalytic activity of the as-formed Bi2WO6/Ag2S heterostructures. Under low pH value, the photosensitization process is suppressed, while under higher pH value, the photosensitization process is favored. The mechanism of the photocatalytic process was proposed by the active-species-trapping experiments, indicating that the photogenerated holes (h(+)) play a crucial role in the degradation of Rh B under visible light. The enhanced photocatalytic performance of this heterostructure makes it a promising material for the treatment of dye-containing wastewater.

13.
J Colloid Interface Sci ; 466: 388-99, 2016 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-26752434

RESUMO

Highly-efficient photocatalyst based on Bi2WO6/SnS heterostructure was prepared via a surface functionalization method using 3-mercaptopropionic (MPA) as the surface functionalizing agent. Compared to bare Bi2WO6 and SnS nanoparticles, the as-formed Bi2WO6/SnS heterostructure exhibits enhanced photocatalytic activity for the degradation of Rhodamine B (Rh B). Photoluminescence and photocurrent measurements demonstrate that the enhanced photocatalytic activity during the photocatalytic process is closely related to the enhanced electron-hole separation efficiency. The photocatalytic activity of the as-formed Bi2WO6/SnS heterostructure can be perfectly remained even after being used for five times, showing excellent durability during the photocatalytic process. The influence of pH and inorganic ions are systematically investigated. And the optimum pH for the photocatalytic process is determined to be 6. The addition of chloride ion will exert negative effect on the photodegradation process of Rh B. The mechanism of photodegradation process was investigated by exploring the quenching effects of different scavengers and the results suggest that the reactive holes play the major role in the photodegradation process of Rh B.

14.
Spectrochim Acta A Mol Biomol Spectrosc ; 133: 514-20, 2014 Dec 10.
Artigo em Inglês | MEDLINE | ID: mdl-24983919

RESUMO

Alkyne bridged porphyrin sensitizers have attracted great attention in the field of dye-sensitized solar cells (DSSCs) because of their excellent photo-to-electric conversion efficiencies, among which YD2 has reached 11% while YD2-o-C8 has reached 11.9% solely and 12.3% co-sensitized with other sensitizers. Design and screening of porphyrin sensitizer candidates with wider electronic absorption spectra to further improve the photo-to-electric conversion efficiencies of corresponding solar cells is still very important. Twenty novel alkyne bridged zinc porphyrin sensitizer candidates composed of the donors diarylamino-, tri-4-methylphenyl-, tri-hydroxyl- and tri-amino-substituted zinc porphyrins as well as the selected acceptors E, M, Q, R and S have been designed and calculated at the density functional B3LYP level. YD2 and YD2-o-C8 are also calculated at the same level for comparison. The result shows that the sensitizer candidates all have smaller HOMO-LUMO gaps as well as wider and red-shifted absorption bands than those of YD2 and YD2-o-C8. Most of the sensitizer candidates have appropriate HOMO and LUMO energy levels relative to the redox potential of the mediator and the TiO2 conduction band, showing that they are promising to provide comparable or even higher photo-to-electric conversion efficiencies than 11% of YD-2 or 11.9% of YD2-o-C8.


Assuntos
Alquinos/química , Corantes/química , Metaloporfirinas/química , Fontes de Energia Elétrica , Elétrons , Teoria Quântica , Energia Solar
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