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1.
Nature ; 582(7813): 511-514, 2020 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-32581381

RESUMO

Decrease in processing speed due to increased resistance and capacitance delay is a major obstacle for the down-scaling of electronics1-3. Minimizing the dimensions of interconnects (metal wires that connect different electronic components on a chip) is crucial for the miniaturization of devices. Interconnects are isolated from each other by non-conducting (dielectric) layers. So far, research has mostly focused on decreasing the resistance of scaled interconnects because integration of dielectrics using low-temperature deposition processes compatible with complementary metal-oxide-semiconductors is technically challenging. Interconnect isolation materials must have low relative dielectric constants (κ values), serve as diffusion barriers against the migration of metal into semiconductors, and be thermally, chemically and mechanically stable. Specifically, the International Roadmap for Devices and Systems recommends4 the development of dielectrics with κ values of less than 2 by 2028. Existing low-κ materials (such as silicon oxide derivatives, organic compounds and aerogels) have κ values greater than 2 and poor thermo-mechanical properties5. Here we report three-nanometre-thick amorphous boron nitride films with ultralow κ values of 1.78 and 1.16 (close to that of air, κ = 1) at operation frequencies of 100 kilohertz and 1 megahertz, respectively. The films are mechanically and electrically robust, with a breakdown strength of 7.3 megavolts per centimetre, which exceeds requirements. Cross-sectional imaging reveals that amorphous boron nitride prevents the diffusion of cobalt atoms into silicon under very harsh conditions, in contrast to reference barriers. Our results demonstrate that amorphous boron nitride has excellent low-κ dielectric characteristics for high-performance electronics.

2.
Nanoscale ; 2020 May 11.
Artigo em Inglês | MEDLINE | ID: mdl-32391820

RESUMO

Herein, we report for the first time the successful preparation of thiometallate-based precursors for use in a bottom-up synthetic process of supported Pt and PtNi nanoparticle catalyst. This precursor enabled the monodisperse synthesis of supported Pt nanoparticles and the in situ formation of S, which were caught directly in a collection system by the nanoparticle synthetic processes consisting of impregnation and thermal processes. S is proven to act as a capping agent in generating highly stable nanoparticles with the size ranging from 2 nm to 3 nm and further favors the formation of monodispersed particles by solid-state digestive ripening. The proposed synthetic methodology can be applied to high-quality PtNi alloy nanoparticle systems. The current route is readily scalable, and multi-gram quantities can be prepared. The prepared carbon-supported Pt and PtNi nanoparticles were characterized as electrocatalysts for the oxygen reduction reaction and exhibited superior performance and durability to commercial Pt/C.

3.
Nanoscale ; 2020 May 06.
Artigo em Inglês | MEDLINE | ID: mdl-32374331

RESUMO

Correction for 'Anomalous polarization dependence of Raman scattering and crystallographic orientation of black phosphorus' by Jungcheol Kim et al., Nanoscale, 2015, 7, 18708-18715, DOI: 10.1039/C5NR04349B.

4.
Nanoscale ; 2020 Apr 06.
Artigo em Inglês | MEDLINE | ID: mdl-32248214

RESUMO

Gallium selenide (GaSe) is one of the layered group-III metal monochalcogenides, which has an indirect bandgap in the monolayer and a direct bandgap in bulk unlike other conventional transition metal dichalcogenides (TMDs) such as MoX2 and WX2 (X = S and Se). Four polytypes of bulk GaSe, designated as ß-, ε-, γ-, and δ-GaSe, have been reported. Since different polytypes result in different optical and electrical properties even with the same thickness, identifying the polytype is essential in utilizing this material for various optoelectronic applications. We performed polarized Raman measurements on GaSe and found different ultra-low-frequency Raman spectra of inter-layer vibrational modes even with the same thickness due to different stacking sequences of the polytypes. By comparing the ultra-low-frequency Raman spectra with the theoretical calculations and high-resolution electron microscopy measurements, we established the correlation between the ultra-low-frequency Raman spectra and the stacking sequences of trilayer GaSe. We further found that the AB-type stacking is more stable than the AA'-type stacking in GaSe.

5.
Artigo em Inglês | MEDLINE | ID: mdl-32298075

RESUMO

The electronic, catalytic, and optical properties of transition metal dichalcogenides (TMDs) are significantly affected by oxidation, and using oxidation to tune the properties of TMDs has been actively explored. In particular, because transition metal oxides (TMOs) are promising hole injection layers, a TMD-TMO heterostructure can be potentially applied as a p-type semiconductor. However, the oxidation of TMDs has not been clearly elucidated because of the structural instability and the extremely small quantity of oxides formed. Here, we reveal the phases and morphologies of oxides formed on two-dimensional molybdenum disulfide (MoS2) using transmission electron microscopy analysis. We find that MoS2 starts to oxidize around 400 °C to form orthorhombic-phase molybdenum trioxide (α-MoO3) nanosheets. The α-MoO3 nanosheets so formed are stacked layer-by-layer on the underlying MoS2 via van der Waals interaction and the nanosheets are aligned epitaxially with six possible orientations. Furthermore, the band gap of MoS2 is increased from 1.27 to 3.0 eV through oxidation. Our study can be extended to most TMDs to form TMO-TMD heterostructures, which are potentially interesting as p-type transistors, gas sensors, or photocatalysts.

6.
ACS Nano ; 14(1): 676-687, 2020 Jan 28.
Artigo em Inglês | MEDLINE | ID: mdl-31927973

RESUMO

Fine-tuning of the surface free energy (SFE) of a solid material facilitates its use in a wide range of applications requiring precise control of the ubiquitous presence of liquid on the surface. In this study, we found that the SFE of rare-earth oxide (REO) thin films deposited by atomic layer deposition (ALD) gradually decreased with increasing film thickness; however, these changes could not be understood by classical interaction models. Herein, the mechanism underlying the aforesaid decrease was systematically studied by measuring contact angles, surface potential, adhesion force, crystalline structures, chemical compositions, and morphologies of the REO films. A growth mode of the REO films was observed: layer-by-layer growth at the initial stage with an amorphous phase and subsequent crystalline island growth, accompanied by a change in the crystalline structure and orientation that affects the SFE. The portion of the surface crystalline facets terminated with (222) and (440) planes evolved with an increase in ALD cycles and film thickness, as an amorphous phase was transformed. Based on this information, we demonstrated an SFE-tuned liquid tweezer with selectivity to target liquid droplets. We believe that the results of this fundamental and practical study, with excellent selectivity to liquids, will have significant impacts on coating technology.

7.
Nat Nanotechnol ; 2020 Jan 20.
Artigo em Inglês | MEDLINE | ID: mdl-31959931

RESUMO

High-quality AB-stacked bilayer or multilayer graphene larger than a centimetre has not been reported. Here, we report the fabrication and use of single-crystal Cu/Ni(111) alloy foils with controllable concentrations of Ni for the growth of large-area, high-quality AB-stacked bilayer and ABA-stacked trilayer graphene films by chemical vapour deposition. The stacking order, coverage and uniformity of the graphene films were evaluated by Raman spectroscopy and transmission electron microscopy including selected area electron diffraction and atomic resolution imaging. Electrical transport (carrier mobility and band-gap tunability) and thermal conductivity (the bilayer graphene has a thermal conductivity value of about 2,300 W m-1 K-1) measurements indicated the superior quality of the films. The tensile loading response of centimetre-scale bilayer graphene films supported by a 260-nm thick polycarbonate film was measured and the average values of the Young's modulus (478 GPa) and fracture strength (3.31 GPa) were obtained.

8.
Nat Nanotechnol ; 15(1): 59-66, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-31819243

RESUMO

Notwithstanding the numerous density functional studies on the chemically induced transformation of multilayer graphene into a diamond-like film carried out to date, a comprehensive convincing experimental proof of such a conversion is still lacking. We show that the fluorination of graphene sheets in Bernal (AB)-stacked bilayer graphene grown by chemical vapour deposition on a single-crystal CuNi(111) surface triggers the formation of interlayer carbon-carbon bonds, resulting in a fluorinated diamond monolayer ('F-diamane'). Induced by fluorine chemisorption, the phase transition from (AB)-stacked bilayer graphene to single-layer diamond was studied and verified by X-ray photoelectron, UV photoelectron, Raman, UV-Vis and electron energy loss spectroscopies, transmission electron microscopy and density functional theory calculations.

9.
Adv Mater ; 31(29): e1903039, 2019 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-31155773

RESUMO

A macroscopic film (2.5 cm × 2.5 cm) made by layer-by-layer assembly of 100 single-layer polycrystalline graphene films is reported. The graphene layers are transferred and stacked one by one using a wet process that leads to layer defects and interstitial contamination. Heat-treatment of the sample up to 2800 °C results in the removal of interstitial contaminants and the healing of graphene layer defects. The resulting stacked graphene sample is a freestanding film with near-perfect in-plane crystallinity but a mixed stacking order through the thickness, which separates it from all existing carbon materials. Macroscale tensile tests yields maximum values of 62 GPa for the Young's modulus and 0.70 GPa for the fracture strength, significantly higher than has been reported for any other macroscale carbon films; microscale tensile tests yield maximum values of 290 GPa for the Young's modulus and 5.8 GPa for the fracture strength. The measured in-plane thermal conductivity is exceptionally high, 2292 ± 159 W m-1 K-1 while in-plane electrical conductivity is 2.2 × 105 S m-1 . The high performance of these films is attributed to the combination of the high in-plane crystalline order and unique stacking configuration through the thickness.

10.
Adv Mater ; 31(29): e1901405, 2019 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-31157462

RESUMO

Despite many encouraging properties of transition metal dichalcogenides (TMDs), a central challenge in the realm of industrial applications based on TMD materials is to connect the large-scale synthesis and reproducible production of highly crystalline TMD materials. Here, the primary aim is to resolve simultaneously the two inversely related issues through the synthesis of MoS2(1- x ) Se2 x ternary alloys with customizable bichalcogen atomic (S and Se) ratio via atomic-level substitution combined with a solution-based large-area compatible approach. The relative concentration of bichalcogen atoms in the 2D alloy can be effectively modulated by altering the selenization temperature, resulting in 4 in. scale production of MoS1.62 Se0.38 , MoS1.37 Se0.63 , MoS1.15 Se0.85 , and MoS0.46 Se1.54 alloys, as well as MoS2 and MoSe2 . Comprehensive spectroscopic evaluations for vertical and lateral homogeneity in terms of heteroatom distribution in the large-scale 2D TMD alloys are implemented. Se-stimulated strain effects and a detailed mechanism for the Se substitution in the MoS2 crystal are further explored. Finally, the capability of the 2D alloy for industrial application in nanophotonic devices and hydrogen evolution reaction (HER) catalysts is validated. Substantial enhancements in the optoelectronic and HER performances of the 2D ternary alloy compared with those of its binary counterparts, including pure-phase MoS2 and MoSe2 , are unambiguously achieved.

11.
Nano Lett ; 19(7): 4229-4236, 2019 Jul 10.
Artigo em Inglês | MEDLINE | ID: mdl-30844285

RESUMO

Among the different growth mechanisms for two-dimensional (2D) hexagonal boron nitride (h-BN) synthesized using chemical vapor deposition, spiraling growth of h-BN has not been reported. Here we report the formation of intertwined double-spiral few-layer h-BN that is driven by screw dislocations located at the antiphase boundaries of monolayer domains. The microstructure and stacking configurations were studied using a combination of dark-field and atomic resolution transmission electron microscopy. Distinct from other 2D materials with single-spiral structures, the double-spiral structure enables the intertwined h-BN layers to preserve the most stable AA' stacking configuration. We also found that the occurrence of shear strains at the boundaries of merged spiral islands is dependent on the propagation directions of encountering screw dislocations and presented the strained features by density functional theory calculations and atomic image simulations. This study unveils the double-spiral growth of 2D h-BN multilayers and the creation of a shear strain band at the coalescence boundary of two h-BN spiral clusters.

12.
Adv Mater ; 31(15): e1807486, 2019 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-30785234

RESUMO

Van der Waals (vdW) epitaxy allows the fabrication of various heterostructures with dramatically released lattice matching conditions. This study demonstrates interface-driven stacking boundaries in WS2 using epitaxially grown tungsten disulfide (WS2 ) on wrinkled graphene. Graphene wrinkles function as highly reactive nucleation sites on WS2 epilayers; however, they impede lateral growth and induce additional stress in the epilayer due to anisotropic friction. Moreover, partial dislocation-driven in-plane strain facilitates out-of-plane buckling with a height of 1 nm to release in-plane strain. Remarkably, in-plane strain relaxation at partial dislocations restores the bandgap to that of monolayer WS2 due to reduced interlayer interaction. These findings clarify significant substrate morphology effects even in vdW epitaxy and are potentially useful for various applications involving modifying optical and electronic properties by manipulating extended 1D defects via substrate morphology control.

13.
Adv Sci (Weinh) ; 6(3): 1801370, 2019 Feb 06.
Artigo em Inglês | MEDLINE | ID: mdl-30775229

RESUMO

As the elements of integrated circuits are downsized to the nanoscale, the current Cu-based interconnects are facing limitations due to increased resistivity and decreased current-carrying capacity because of scaling. Here, the bottom-up synthesis of single-crystalline WTe2 nanobelts and low- and high-field electrical characterization of nanoscale interconnect test structures in various ambient conditions are reported. Unlike exfoliated flakes obtained by the top-down approach, the bottom-up growth mode of WTe2 nanobelts allows systemic characterization of the electrical properties of WTe2 single crystals as a function of channel dimensions. Using a 1D heat transport model and a power law, it is determined that the breakdown of WTe2 devices under vacuum and with AlO x capping layer follows an ideal pattern for Joule heating, far from edge scattering. High-field electrical measurements and self-heating modeling demonstrate that the WTe2 nanobelts have a breakdown current density approaching ≈100 MA cm-2, remarkably higher than those of conventional metals and other transition-metal chalcogenides, and sustain the highest electrical power per channel length (≈16.4 W cm-1) among the interconnect candidates. The results suggest superior robustness of WTe2 against high-bias sweep and its possible applicability in future nanoelectronics.

14.
Nanoscale ; 10(46): 21978-21984, 2018 Nov 29.
Artigo em Inglês | MEDLINE | ID: mdl-30451270

RESUMO

Molybdenum ditellurides (MoTe2) have recently attracted attention owing to their excellent structurally tunable nature between 1T'(metallic)- and 2H(semiconducting)-phases; thus, the controllable fabrication and critical identification of MoTe2 are highly desired. Here, we semi-controllably synthesized 1T'- and 2H-MoTe2 crystals using the atmospheric pressure chemical vapor deposition (APCVD) technique and studied their grain-orientation dependency using polarization-sensitive optical microscopy, Raman scattering, and second-harmonic generation (SHG) microspectroscopy. The polycrystalline 1T'-MoTe2 phase with quasi-1D "Mo-Mo" zigzag chains showed anisotropic optical absorption, leading to a clear visualization of the lattice domains. On the other hand, 2H-MoTe2 lattice grains did not exhibit any discernible difference under polarized light illumination. The combined aforementioned microscopy techniques could be used as an easy-to-access and non-destructive tool for a quick and solid identification of intended lattice orientation development in industry-scale MoTe2 crystal manufacturing.

15.
Nanoscale ; 10(40): 19212-19219, 2018 Oct 18.
Artigo em Inglês | MEDLINE | ID: mdl-30303224

RESUMO

The recent emergence of vertically stacked van der Waals (vdW) heterostructures provides new opportunities for these materials to be employed in a wide range of novel applications. Understanding the interlayer coupling in the stacking geometries of the heterostructures and its effect on the resultant material properties is particularly important for obtaining materials with desirable properties. Here, we report that the atomic bonding between stacked layers and thereby the interlayer properties of the vdW heterostructures can be well tuned by the substrate surface defects using WS2 flakes directly grown on graphene. We show that the defects of graphene have no significant effect on the crystal structure or the quality of the grown WS2 flakes; however, they have a strong influence on the interlayer interactions between stacked layers, thus affecting the layer deformability, thermal stability, and physical and electrical properties. Our experimental and computational investigations also reveal that WS2 flakes grown on graphene defects form covalent bonds with the underlying graphene via W atomic bridges (i.e., formation of larger overlapping hybrid orbitals), enabling these flakes to exhibit different intrinsic properties, such as higher conductivity and improved contact characteristics than heterostructures that have vdW interactions with graphene. This result emphasizes the importance of understanding the interlayer coupling in the stacking geometries and its correlation effect for designing desirable properties.

16.
ACS Appl Mater Interfaces ; 10(40): 34163-34171, 2018 Oct 10.
Artigo em Inglês | MEDLINE | ID: mdl-30222310

RESUMO

Two-dimensional (2D) transition-metal dichalcogenides (TMDCs) have attracted considerable attention as promising building blocks for a new generation of gas-sensing devices because of their excellent electrical properties, superior response, flexibility, and low-power consumption. Owing to their large surface-to-volume ratio, various 2D TMDCs, such as MoS2, MoSe2, WS2, and WSe2, have exhibited excellent gas-sensing characteristics. However, exploration toward the enhancement of TMDC gas-sensing performance has not yet been intensively addressed. Here, we synthesized large-area uniform WS2 xSe2-2 x alloys for room-temperature gas sensors. As-synthesized WS2 xSe2-2 x alloys exhibit an elaborative composition control owing to their thermodynamically stable sulfurization process. Further, utilizing uniform WS2 xSe2-2 x alloys over a large area, we demonstrated improved NO2-sensing performance compared to WSe2 on the basis of an electronic sensitization mechanism. The WS0.96Se1.04 alloy gas sensor exhibits 2.4 times enhanced response for NO2 exposure. Further, we demonstrated a low-power wearable NO2-detecting wristband that operates at room temperature. Our results show that the proposed method is a promising strategy to improve 2D TMDC gas sensors and has a potential for applications in advanced gas-sensing devices.

17.
Nanotechnology ; 29(43): 435705, 2018 Oct 26.
Artigo em Inglês | MEDLINE | ID: mdl-30101755

RESUMO

With the acceleration of the scaling down of integrated circuits, it has become very challenging to fabricate a metal-insulator-metal (MIM) capacitor with a high capacitance density and low leakage current for nanoscale dynamic random access memory. Yttria-stabilized-zirconia (YSZ) thin films, one of the insulators in the constitution of MIM capacitors, have been reported to have various crystal structures from the monoclinic phase to the cubic phase according to different Y doping levels. The electrical characteristics depend on the crystal structure of the YSZ thin film. Here, we report the local crystallization of YSZ thin films via Joule heating and the leakage current induced during in situ transmission electron microscopy biasing tests. We studied the crystallization process and the increase in the leakage current using experimental and simulation results. It is important to understand the relationship between the crystallinity and electrical properties of YSZ thin films in MIM capacitors.

18.
Adv Mater ; 30(30): e1707260, 2018 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-29882243

RESUMO

Following the celebrated discovery of graphene, considerable attention has been directed toward the rich spectrum of properties offered by van der Waals crystals. However, studies have been largely limited to their 2D properties due to lack of 1D structures. Here, the growth of high-yield, single-crystalline 1D nanobelts composed of transition metal ditellurides at low temperatures (T ≤ 500 °C) and in short reaction times (t ≤ 10 min) via the use of tellurium-rich eutectic metal alloys is reported. The synthesized semimetallic 1D products are highly pure, stoichiometric, structurally uniform, and free of defects, resulting in high electrical performances. Furthermore, complete compositional tuning of the ternary ditelluride nanobelts is achieved with suppressed phase separation, applicable to the creation of unprecedented low-dimensional materials/devices. This approach may inspire new growth/fabrication strategies of 1D layered nanostructures, which may offer unique properties that are not available in other materials.

19.
Adv Mater ; 30(30): e1800022, 2018 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-29889331

RESUMO

Graphene has recently attracted particular interest as a flexible barrier film preventing permeation of gases and moistures. However, it has been proved to be exceptionally challenging to develop large-scale graphene films with little oxygen and moisture permeation suitable for industrial uses, mainly due to the presence of nanometer-sized defects of obscure origins. Here, the origins of water permeable routes on graphene-coated Cu foils are investigated by observing the micrometer-sized rusts in the underlying Cu substrates, and a site-selective passivation method of the nanometer-sized routes is devised. It is revealed that nanometer-sized holes or cracks are primarily concentrated on graphene wrinkles rather than on other structural imperfections, resulting in severe degradation of its water impermeability. They are found to be predominantly induced by the delamination of graphene bound to Cu as a release of thermal stress during the cooling stage after graphene growth, especially at the intersection of the Cu step edges and wrinkles owing to their higher adhesion energy. Furthermore, the investigated routes are site-selectively passivated by an electron-beam-induced amorphous carbon layer, thus a substantial improvement in water impermeability is achieved. This approach is likely to be extended for offering novel barrier properties in flexible films based on graphene and on other atomic crystals.

20.
ACS Nano ; 12(6): 6117-6127, 2018 Jun 26.
Artigo em Inglês | MEDLINE | ID: mdl-29790339

RESUMO

Fast-growth of single crystal monolayer graphene by CVD using methane and hydrogen has been achieved on "homemade" single crystal Cu/Ni(111) alloy foils over large area. Full coverage was achieved in 5 min or less for a particular range of composition (1.3 at.% to 8.6 at.% Ni), as compared to 60 min for a pure Cu(111) foil under identical growth conditions. These are the bulk atomic percentages of Ni, as a superstructure at the surface of these foils with stoichiometry Cu6Ni1 (for 1.3 to 7.8 bulk at.% Ni in the Cu/Ni(111) foil) was discovered by low energy electron diffraction (LEED). Complete large area monolayer graphene films are either single crystal or close to single crystal, and include folded regions that are essentially parallel and that were likely wrinkles that "fell over" to bind to the surface; these folds are separated by large, wrinkle-free regions. The folds occur due to the buildup of interfacial compressive stress (and its release) during cooling of the foils from 1075 °C to room temperature. The fold heights measured by atomic force microscopy (AFM) and scanning tunneling microscopy (STM) prove them to all be 3 layers thick, and scanning electron microscopy (SEM) imaging shows them to be around 10 to 300 nm wide and separated by roughly 20 µm. These folds are always essentially perpendicular to the steps in this Cu/Ni(111) substrate. Joining of well-aligned graphene islands (in growths that were terminated prior to full film coverage) was investigated with high magnification SEM and aberration-corrected high-resolution transmission electron microscopy (TEM) as well as AFM, STM, and optical microscopy. These methods show that many of the "join regions" have folds, and these arise from interfacial adhesion mechanics (they are due to the buildup of compressive stress during cool-down, but these folds are different than for the continuous graphene films-they occur due to "weak links" in terms of the interface mechanics). Such Cu/Ni(111) alloy foils are promising substrates for the large-scale synthesis of single-crystal graphene film.

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