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1.
Nat Nanotechnol ; 2020 Jul 13.
Artigo em Inglês | MEDLINE | ID: mdl-32661372

RESUMO

Lead halide perovskites have attracted increasing interest for their exciting potential in diverse optoelectronic devices. However, their charge transport properties remain elusive, plagued by the issues of excessive contact resistance and large hysteresis in ambient conditions. Here we report a van der Waals integration approach for creating high-performance contacts on monocrystalline halide perovskite thin films with minimum interfacial damage and an atomically clean interface. Compared to the deposited contacts, our van der Waals contacts exhibit two to three orders of magnitude lower contact resistance, enabling systematic transport studies in a wide temperature range. We report a Hall mobility exceeding 2,000 cm2 V-1 s-1 at around 80 K, an ultralow bimolecular recombination coefficient of 3.5 × 10-15 cm3 s-1 and a photocurrent gain >106 in the perovskite thin films. Furthermore, magnetotransport studies reveal a quantum-interference-induced weak localization behaviour with a phase coherence length up to 49 nm at 3.5 K. Our results lay the foundation for exploring new physics in this class of 'soft-lattice' materials.

2.
Nature ; 579(7799): 368-374, 2020 03.
Artigo em Inglês | MEDLINE | ID: mdl-32188941

RESUMO

Two-dimensional van der Waals heterostructures (vdWHs) have attracted considerable interest1-4. However, most vdWHs reported so far  are created by an arduous micromechanical exfoliation and manual restacking process5, which-although versatile for proof-of-concept demonstrations6-16 and fundamental studies17-30-is clearly not scalable for practical technologies. Here we report a general synthetic strategy for two-dimensional vdWH arrays between metallic transition-metal dichalcogenides (m-TMDs) and semiconducting TMDs (s-TMDs). By selectively patterning nucleation sites on monolayer or bilayer s-TMDs, we precisely control the nucleation and growth of diverse m-TMDs with designable periodic arrangements and tunable lateral dimensions at the predesignated spatial locations, producing a series of vdWH arrays, including VSe2/WSe2, NiTe2/WSe2, CoTe2/WSe2, NbTe2/WSe2, VS2/WSe2, VSe2/MoS2 and VSe2/WS2. Systematic scanning transmission electron microscopy studies reveal nearly ideal vdW interfaces with widely tunable moiré superlattices. With the atomically clean vdW interface, we further show that the m-TMDs function as highly reliable synthetic vdW contacts for the underlying WSe2 with excellent device performance and yield, delivering a high ON-current density of up to 900 microamperes per micrometre in bilayer WSe2 transistors. This general synthesis of diverse two-dimensional vdWH arrays provides a versatile material platform for exploring exotic physics and promises a scalable pathway to high-performance devices.

3.
Nat Commun ; 11(1): 659, 2020 Jan 31.
Artigo em Inglês | MEDLINE | ID: mdl-32005802

RESUMO

In atomically-thin two-dimensional (2D) semiconductors, the nonuniformity in current flow due to its edge states may alter and even dictate the charge transport properties of the entire device. However, the influence of the edge states on electrical transport in 2D materials has not been sufficiently explored to date. Here, we systematically quantify the edge state contribution to electrical transport in monolayer MoS2/WSe2 field-effect transistors, revealing that the charge transport at low temperature is dominated by the edge conduction with the nonlinear behavior. The metallic edge states are revealed by scanning probe microscopy, scanning Kelvin probe force microscopy and first-principle calculations. Further analyses demonstrate that the edge-state dominated nonlinear transport shows a universal power-law scaling relationship with both temperature and bias voltage, which can be well explained by the 1D Luttinger liquid theory. These findings demonstrate the Luttinger liquid behavior in 2D materials and offer important insights into designing 2D electronics.

4.
Chem Soc Rev ; 48(20): 5207-5241, 2019 Oct 14.
Artigo em Inglês | MEDLINE | ID: mdl-31573024

RESUMO

Electrocatalysis plays an essential role in diverse electrochemical energy conversion processes that are vital for improving energy utilization efficiency and mitigating the aggravating global warming challenge. The noble metals such as platinum are generally the most frequently used electrocatalysts to drive these reactions and facilitate the relevant energy conversion processes. The high cost and scarcity of these materials pose a serious challenge for the wide-spread adoption and the sustainability of these technologies in the long run, which have motivated considerable efforts in searching for alternative electrocatalysts with reduced loading of precious metals or based entirely on earth-abundant metals. Of particular interest are graphene-supported single atom catalysts (G-SACs) that integrate the merits of heterogeneous catalysts and homogeneous catalysts, such as high activity, selectivity, stability, maximized atom utilization efficiency and easy separation from reactants/products. The graphene support features a large surface area, high conductivity and excellent (electro)-chemical stability, making it a highly attractive substrate for supporting single atom electrocatalysts for various electrochemical energy conversion processes. In this review, we highlight the recent advancements in G-SACs for electrochemical energy conversion, from the synthetic strategies and identification of the atomistic structure to electrocatalytic applications in a variety of reactions, and finally conclude with a brief prospect on future challenges and opportunities.

5.
J Am Chem Soc ; 141(31): 12251-12257, 2019 Aug 07.
Artigo em Inglês | MEDLINE | ID: mdl-31361127

RESUMO

Silver nanowire (Ag-NW) thin films are of considerable interest for next-generation transparent conductors (TCs). However, their carrier transport properties are largely plagued by the residual polyvinylpyrrolidone (PVP) ligands on surface that were introduced during the synthesis of the Ag-NWs. Here we report a rapid electrochemical cleaning strategy to thoroughly remove the surface PVP ligands and greatly improve the carrier transport properties of the Ag-NW thin films while not affecting their transmittance. In particular, we show a negative electrochemical potential near the hydrogen adsorption/evolution regime can effectively displace all PVP ligands from the Ag-NW surface in 5-15 s, producing ultraclean interfaces between Ag-NW/Ag-NW junctions or Ag-NW film/active layer junction in a stacked optoelectronic device. We show that the removal of the PVP ligands can substantially reduce the sheet resistance of the Ag-NW thin film from 49 to 13 ohm/sq (with 90.91% transmittance at 550 nm) and reduce the interfacial resistance at the Ag-NW film/active layer interface by 94.3%. Such improved Ag-NW thin films can greatly enhance the sensitivity of the wearable strain sensor and the current collection efficiency of the vertically stacked devices constructed from the sandwiched thin films. These results demonstrate that the electrochemical cleaning approach is highly effective in removing surface ligands and improving both the in-plane and the out-of-plane carrier transport properties of the Ag-NW thin films, greatly facilitating their applications in electronic and optoelectronic devices.

6.
Adv Mater ; 31(33): e1900608, 2019 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-31183914

RESUMO

Energy devices such as rechargeable batteries, fuel cells, and solar cells are central to powering a renewable, mobile, and electrified future. To advance these devices requires a fundamental understanding of the complex chemical reactions, material transformations, and charge flow that are associated with energy conversion processes. Analytical in situ transmission electron microscopy (TEM) offers a powerful tool for directly visualizing these complex processes at the atomic scale in real time and in operando. Recent advancements in energy materials and devices that have been enabled by in situ TEM are reviewed. First, the evolutionary development of TEM nanocells from the open-cell configuration to the closed-cell, and finally the full-cell, is reviewed. Next, in situ TEM studies of rechargeable ion batteries in a practical operation environment are explored, followed by applications of in situ TEM for direct observation of electrocatalyst formation, evolution, and degradation in proton-exchange membrane fuel cells, and fundamental investigations of new energy materials such as perovskites for solar cells. Finally, recent advances in the use of environmental TEM and cryogenic electron microscopy in probing clean-energy materials are presented and emerging opportunities and challenges in in situ TEM research of energy materials and devices are discussed.

7.
Adv Mater ; 31(25): e1900901, 2019 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-31045286

RESUMO

Multiple structural phases in transition metal dichalcogenides have attracted considerable recent interest for their tunable chemical and electronic properties. Herein, a chemical vapor deposition route to ultrathin CoSe nanoplates with tunable structure phases is reported. By precisely tailoring the growth temperature, ultrathin 2D layered tetragonal CoSe nanoplates and nonlayered hexagonal CoSe nanoplates can be selectively prepared as square or hexagonal geometries, with thickness as thin as 2.3 and 3.7 nm, respectively. X-ray diffraction, transmission electron microscopy, and selected area electron diffraction studies show that both types of nanoplates are high-quality single crystals. Electrical transport studies reveal that both the tetragonal and hexagonal CoSe nanoplates show strong thickness-tunable electrical properties and excellent breakdown current density. The 2D hexagonal CoSe nanoplates display metallic behavior with an excellent conductivity up to 6.6 × 105 S m-1 and an extraordinary breakdown current density up to 3.9 × 107 A cm-2 , while the square tetragonal nanoplates show considerably lower conductivity up to 8.2 × 104 S m-1 with angle-dependent magnetoresistance and weak antilocalization effect at lower field. This study offers a tunable material system for exploring multiphase 2D materials and their potential applications for electronic and magnetoelectronic devices.

8.
J Am Chem Soc ; 140(43): 14217-14223, 2018 Oct 31.
Artigo em Inglês | MEDLINE | ID: mdl-30346160

RESUMO

Two-dimensional (2D) layered materials have stimulated extensive research interest for their unique thickness-dependent electronic and optical properties. However, the layer-number-dependent studies on 2D materials to date are largely limited to exfoliated flakes with relatively small lateral size and poor yield. The direct synthesis of 2D materials with a precise control of the number of atomic layers remains a substantial synthetic challenge. Here we report a systematic study of chemical vapor deposition synthesis of large-area atomically thin 2D nickel telluride (NiTe2) single crystals and investigate the thickness dependent electronic properties. By controlling the growth temperature, we show that the highly uniform NiTe2 single crystals can be synthesized with precisely tunable thickness varying from 1, 2, 3, . . . to multilayers with a standard deviation (∼0.3 nm) of less than the thickness of a monolayer layer NiTe2. Our studies further reveal a systematic evolution of single crystal domain size and nucleation density with the largest lateral domain size up to ∼440 µm. X-ray diffraction, transmission electron microscopy, and high resolution scanning transmission electron microscope studies demonstrate that the resulting 2D crystals are high quality single crystals and adopt hexagonal 1T phase. Electrical transport studies reveal that the 2D NiTe2 single crystals show a strong thickness-tunable electrical properties, with an excellent conductivity up to 7.8 × 105 S m-1 and extraordinary breakdown current density up to 4.7 × 107 A/cm2. The systematic study and robust synthesis of NiTe2 nanosheets defines a reliable chemical route to 2D single crystals with precisely tailored thickness and could enable the design of new device architectures based on thickness-tunable electrical properties.

9.
Nature ; 562(7726): 254-258, 2018 10.
Artigo em Inglês | MEDLINE | ID: mdl-30283139

RESUMO

Two-dimensional (2D) materials, consisting of atomically thin crystal layers bound by the van der Waals force, have attracted much interest because of their potential in diverse technologies, including electronics, optoelectronics and catalysis1-10. In particular, solution-processable 2D semiconductor (such as MoS2) nanosheets are attractive building blocks for large-area thin-film electronics. In contrast to conventional zero- and one-dimensional nanostructures (quantum dots and nanowires, respectively), which are typically plagued by surface dangling bonds and associated trapping states, 2D nanosheets have dangling-bond-free surfaces. Thin films created by stacking multiple nanosheets have atomically clean van der Waals interfaces and thus promise excellent charge transport11-15. However, preparing high-quality solution-processable 2D semiconductor nanosheets remains a challenge. For example, MoS2 nanosheets and thin films produced using lithium intercalation and exfoliation are plagued by the presence of the metallic 1T phase and poor electrical performance (mobilities of about 0.3 square centimetres per volt per second and on/off ratios of less than 10)2,12, and materials produced by liquid exfoliation exhibit an intrinsically broad thickness distribution, which leads to poor film quality and unsatisfactory thin-film electrical performance (mobilities of about 0.4 square centimetres per volt per second and on/off ratios of about 100)14,16,17. Here we report a general approach to preparing highly uniform, solution-processable, phase-pure semiconducting nanosheets, which involves the electrochemical intercalation of quaternary ammonium molecules (such as tetraheptylammonium bromide) into 2D crystals, followed by a mild sonication and exfoliation process. By precisely controlling the intercalation chemistry, we obtained phase-pure, semiconducting 2H-MoS2 nanosheets with a narrow thickness distribution. These nanosheets were then further processed into high-performance thin-film transistors, with room-temperature mobilities of about 10 square centimetres per volt per second and on/off ratios of 106 that greatly exceed those obtained for previous solution-processed MoS2 thin-film transistors. The scalable fabrication of large-area arrays of thin-film transistors enabled the construction of functional logic gates and computational circuits, including an inverter, NAND, NOR, AND and XOR gates, and a logic half-adder. We also applied our approach to other 2D materials, including WSe2, Bi2Se3, NbSe2, In2Se3, Sb2Te3 and black phosphorus, demonstrating its potential for generating versatile solution-processable 2D materials.

10.
Nanotechnology ; 29(47): 474002, 2018 Nov 23.
Artigo em Inglês | MEDLINE | ID: mdl-30188325

RESUMO

Doping can effectively regulate the electrical and optical properties of two-dimensional semiconductors. Here, we present high-quality Pb-doped SnSe2 monolayer exfoliated using a micromechanical cleavage method. X-ray photoelectron spectroscopy measurement demonstrates that Pb content of the doped sample is ∼3.6% and doping induces the downward shift of the Fermi level with respect to the pure SnSe2. Transmission electron microscopy characterization exhibits that Pb0.036Sn0.964Se2 nanosheets have a high-quality hexagonal symmetry structure and Pb element is uniformly distributed in the nanosheets. The current of the SnSe2 field effect transistors (FETs) was found to be very difficult to turn off due to the high electron density. The FETs based on the Pb0.036Sn0.964Se2 monolayer show n-type behavior with a high on/off ratio of 106 which is higher than any values of SnSe2 FETs reported at the moment. The estimated carrier concentration of Pb0.036Sn0.964Se2 is approximately six times lower than that of SnSe2. The results suggest that the method of reducing carrier concentration by doping to achieve high on/off ratio is effective, and Pb-doped SnSe2 monolayer has significant potential in future nanoelectronic and optoelectronic applications.

11.
Chem Soc Rev ; 47(16): 6388-6409, 2018 Aug 13.
Artigo em Inglês | MEDLINE | ID: mdl-30079920

RESUMO

Two-dimensional semiconductors (2DSCs) have attracted considerable attention as atomically thin channel materials for field-effect transistors. Each layer in 2DSCs consists of a single- or few-atom-thick, covalently bonded lattice, in which all carriers are confined in their atomically thin channel with superior gate controllability and greatly suppressed OFF-state current, in contrast to typical bulk semiconductors plagued by short channel effects and heat generation from static power. Additionally, 2DSCs are free of surface dangling bonds that plague traditional semiconductors, and hence exhibit excellent electronic properties at the limit of single atom thickness. Therefore, 2DSCs can offer significant potential for the ultimate transistor scaling to single atomic body thickness. Earlier studies of graphene transistors have been limited by the zero bandgap and low ON-OFF ratio of graphene, and transition metal dichalcogenide (TMDC) devices are typically plagued by insufficient carrier mobility. To this end, considerable efforts have been devoted towards searching for new 2DSCs with optimum electronic properties. Within a relatively short period of time, a large number of 2DSCs have been demonstrated to exhibit unprecedented characteristics or unique functionalities. Here we review the recent efforts and progress in exploring novel 2DSCs beyond graphene and TMDCs for ultra-thin body transistors, discussing the merits, limits and prospects of each material.

12.
Adv Mater ; : e1801043, 2018 Jul 31.
Artigo em Inglês | MEDLINE | ID: mdl-30063088

RESUMO

Two-dimensional materials with intrinsic magnetism have recently drawn intense interest for both the fundamental studies and potential technological applications. However, the studies to date have been largely limited to mechanically exfoliated materials. Herein, an atmospheric pressure chemical vapor deposition route to ultrathin group VB metal telluride MTe2 (M = V, Nb, Ta) nanoplates with thickness as thin as 3 nm is reported. It is shown that the resulting nanoplates can be systematically evolved from mostly thicker hexagonal domains to thinner triangular domains with an increasing flow rate of the carrier gas. X-ray diffraction and transmission electron microscopy studies reveal MTe2 (M = V, Nb, Ta) nanoplates are high-quality single crystals. High-resolution scanning transmission electron microscope imaging reveals the VTe2 and NbTe2 nanoplates adopt the hexagonal 1T phase and the TaTe2 nanoplates show a monoclinic distorted 1T phase. Electronic transport studies show that MTe2 single crystals exhibit metallic behavior. Magnetic measurements show that VTe2 and NbTe2 exhibit ferromagnetism and TaTe2 shows paramagnetic behavior. The preparation of ultrathin few-layered MTe2 nanoplates will open up exciting opportunities for the burgeoning field of spintronics, sensors, and magneto-optoelectronics.

13.
Nano Lett ; 18(6): 3523-3529, 2018 06 13.
Artigo em Inglês | MEDLINE | ID: mdl-29786447

RESUMO

The recent discovery of topological semimetals has stimulated extensive research interest due to their unique electronic properties and novel transport properties related to a chiral anomaly. However, the studies to date are largely limited to bulk crystals and exfoliated flakes. Here, we report the controllable synthesis of ultrathin two-dimensional (2D) platinum telluride (PtTe2) nanosheets with tunable thickness and investigate the thickness-dependent electronic properties. We show that PtTe2 nanosheets can be readily grown, using a chemical vapor deposition approach, with a hexagonal or triangular geometry and a lateral dimension of up to 80 µm, and the thickness of the nanosheets can be systematically tailored from over 20 to 1.8 nm by reducing the growth temperature or increasing the flow rate of the carrier gas. X-ray-diffraction, transmission-electron microscopy, and electron-diffraction studies confirm that the resulting 2D nanosheets are high-quality single crystals. Raman spectroscopic studies show characteristics Eg and A1g vibration modes at ∼109 and ∼155 cm-1, with a systematic red shift with increasing nanosheet thickness. Electrical transport studies show the 2D PtTe2 nanosheets display an excellent conductivity up to 2.5 × 106 S m-1 and show strong thickness-tunable electrical properties, with both the conductivity and its temperature dependence varying considerably with the thickness. Moreover, 2D PtTe2 nanosheets show an extraordinary breakdown current density up to 5.7 × 107 A/cm2, the highest breakdown current density achieved in 2D metallic transition-metal dichalcogenides to date.

14.
Chem Soc Rev ; 47(9): 3129-3151, 2018 May 08.
Artigo em Inglês | MEDLINE | ID: mdl-29528342

RESUMO

Two-dimensional atomic crystals (2DACs) have attracted intense recent interest. With a nearly perfect crystalline structure and dangling-bond free surface, these atomically thin materials have emerged as a new material platform for fundamental materials science and diverse technology opportunities at the limit of single atom thickness. Over the past decade, a wide range of 2DACs has been prepared by mechanically exfoliating bulk layered crystals, which has fueled the rapid progress of the entire field in terms of fundamental physics and basic device demonstrations. However, studies to date are largely limited to mechanically exfoliated flakes, which are clearly not scalable for practical applications. The chemical synthesis of these materials has been lagging far behind fundamental property investigations or novel device demonstrations, which limits further progress of the field. To explore the full potential of 2DACs requires a robust synthesis of these atomically thin materials and scalable construction of complex heterostructures with designed spatial modulation of chemical compositions and electronic structures. The extreme aspect ratio and highly delicate nature of the atomically thin crystals pose a significant synthetic challenge beyond traditional bulk crystals and have motivated considerable efforts worldwide. Here we will review the recent advances, challenges and future perspective of the chemical synthesis of 2DACs, heterostructures and superlattices.

15.
Nature ; 555(7695): 231-236, 2018 03 07.
Artigo em Inglês | MEDLINE | ID: mdl-29517002

RESUMO

Artificial superlattices, based on van der Waals heterostructures of two-dimensional atomic crystals such as graphene or molybdenum disulfide, offer technological opportunities beyond the reach of existing materials. Typical strategies for creating such artificial superlattices rely on arduous layer-by-layer exfoliation and restacking, with limited yield and reproducibility. The bottom-up approach of using chemical-vapour deposition produces high-quality heterostructures but becomes increasingly difficult for high-order superlattices. The intercalation of selected two-dimensional atomic crystals with alkali metal ions offers an alternative way to superlattice structures, but these usually have poor stability and seriously altered electronic properties. Here we report an electrochemical molecular intercalation approach to a new class of stable superlattices in which monolayer atomic crystals alternate with molecular layers. Using black phosphorus as a model system, we show that intercalation with cetyl-trimethylammonium bromide produces monolayer phosphorene molecular superlattices in which the interlayer distance is more than double that in black phosphorus, effectively isolating the phosphorene monolayers. Electrical transport studies of transistors fabricated from the monolayer phosphorene molecular superlattice show an on/off current ratio exceeding 107, along with excellent mobility and superior stability. We further show that several different two-dimensional atomic crystals, such as molybdenum disulfide and tungsten diselenide, can be intercalated with quaternary ammonium molecules of varying sizes and symmetries to produce a broad class of superlattices with tailored molecular structures, interlayer distances, phase compositions, electronic and optical properties. These studies define a versatile material platform for fundamental studies and potential technological applications.

16.
J Am Chem Soc ; 140(1): 193-199, 2018 01 10.
Artigo em Inglês | MEDLINE | ID: mdl-29185776

RESUMO

Silver nanowire (Ag-NW) thin films have emerged as a promising next-generation transparent electrode. However, the current Ag-NW thin films are often plagued by high NW-NW contact resistance and poor long-term stability, which can be largely attributed to the ill-defined polyvinylpyrrolidone (PVP) surface ligands and nonideal Ag-PVP-Ag contact at NW-NW junctions. Herein, we report a room temperature direct welding and chemical protection strategy to greatly improve the conductivity and stability of the Ag-NW thin films. Specifically, we use a sodium borohydride (NaBH4) treatment process to thoroughly remove the PVP ligands and produce a clean Ag-Ag interface that allows direct welding of NW-NW junctions at room temperature, thus greatly improving the conductivity of the Ag-NW films, outperforming those obtained by thermal or plasmonic thermal treatment. We further show that, by decorating the as-formed Ag-NW thin film with a dense, hydrophobic dodecanethiol layer, the stability of the Ag-NW film can be greatly improved by 150-times compared with that of PVP-wrapped ones. Our studies demonstrate that a proper surface ligand design can effectively improve the conductivity and stability of Ag-NW thin films, marking an important step toward their applications in electronic and optoelectronic devices.

17.
Science ; 357(6353): 788-792, 2017 08 25.
Artigo em Inglês | MEDLINE | ID: mdl-28775210

RESUMO

We report a general synthetic strategy for highly robust growth of diverse lateral heterostructures, multiheterostructures, and superlattices from two-dimensional (2D) atomic crystals. A reverse flow during the temperature-swing stage in the sequential vapor deposition growth process allowed us to cool the existing 2D crystals to prevent undesired thermal degradation and uncontrolled homogeneous nucleation, thus enabling highly robust block-by-block epitaxial growth. Raman and photoluminescence mapping studies showed that a wide range of 2D heterostructures (such as WS2-WSe2 and WS2-MoSe2), multiheterostructures (such as WS2-WSe2-MoS2 and WS2-MoSe2-WSe2), and superlattices (such as WS2-WSe2-WS2-WSe2-WS2) were readily prepared with precisely controlled spatial modulation. Transmission electron microscope studies showed clear chemical modulation with atomically sharp interfaces. Electrical transport studies of WSe2-WS2 lateral junctions showed well-defined diode characteristics with a rectification ratio up to 105.

18.
Adv Mater ; 29(39)2017 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-28833598

RESUMO

Van der Waals (vdW) heterostructures have received intense attention for their efficient stacking methodology with 2D nanomaterials in vertical dimension. However, it is still a challenge to scale down the lateral size of vdW heterostructures to the nanometer and make proper contacts to achieve optimized performances. Here, a carbon-nanotube-confined vertical heterostructure (CCVH) is employed to address this challenge, in which 2D semiconductors are asymmetrically sandwiched by an individual metallic single-walled carbon nanotube (SWCNT) and a metal electrode. By using WSe2 and MoS2 , the CCVH can be made into p-type and n-type field effect transistors with high on/off ratios even when the channel length is 3.3 nm. A complementary inverter was further built with them, indicating their potential in logic circuits with a high integration level. Furthermore, the Fermi level of SWCNTs can be efficiently modulated by the gate voltage, making it competent for both electron and hole injection in the CCVHs. This unique property is shown by the transition of WSe2 CCVH from unipolar to bipolar, and the transition of WSe2 /MoS2 from p-n junction to n-n junction under proper source-drain biases and gate voltages. Therefore, the CCVH, as a member of 1D/2D mixed heterostructures, shows great potentials in future nanoelectronics and nano-optoelectronics.

19.
Small ; 13(38)2017 10.
Artigo em Inglês | MEDLINE | ID: mdl-28791794

RESUMO

Two-dimensional layered materials (2DLMs) have attracted considerable recent interest as a new material platform for fundamental materials science and potential new technologies. Here we report the growth of layered metal halide materials and their optoelectronic properties. BiI3 nanoplates can be readily grown on SiO2 /Si substrates with a hexagonal geometry, with a thickness in the range of 10-120 nm and a lateral dimension of 3-10 µm. Transmission electron microscopy and electron diffraction studies demonstrate that the individual nanoplates are high quality single crystals. Micro-Raman studies show characteristic Ag band at ≈115 cm-1 with slight red-shift with decreasing thickness, and micro-photoluminescence studies show uniform emission around 690 nm with blue-shift with decreasing thickness. Electrical transport studies of individual nanoplates show n-type semiconductor characteristics with clear photoresponse. Further, the BiI3 can be readily grown on other 2DLMs (e.g., WSe2 ) to form van der Waals heterostructures. Electrical transport measurements of BiI3 /WSe2 vertical heterojunctions demonstrate p-n diode characteristics with gate-tunable rectification behavior and distinct photovoltaic effect. The synthesis of the BiI3 nanoplates can expand the library of 2DLMs and enable a wider range of van der Waals heterostructures.

20.
Angew Chem Int Ed Engl ; 56(26): 7610-7614, 2017 06 19.
Artigo em Inglês | MEDLINE | ID: mdl-28464460

RESUMO

The metallic 1T-MoS2 has attracted considerable attention as an effective catalyst for hydrogen evolution reactions (HERs). However, the fundamental mechanism about the catalytic activity of 1T-MoS2 and the associated phase evolution remain elusive and controversial. Herein, we prepared the most stable 1T-MoS2 by hydrothermal exfoliation of MoS2 nanosheets vertically rooted into rigid one-dimensional TiO2 nanofibers. The 1T-MoS2 can keep highly stable over one year, presenting an ideal model system for investigating the HER catalytic activities as a function of the phase evolution. Both experimental studies and theoretical calculations suggest that 1T phase can be irreversibly transformed into a more active 1T' phase as true active sites in photocatalytic HERs, resulting in a "catalytic site self-optimization". Hydrogen atom adsorption is the major driving force for this phase transition.

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