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1.
Palladium ditelluride (PdTe2) is a novel transition‐metal dichalcogenide exhibiting type‐II Dirac fermions and topological superconductivity. To assess its potential in technology, its chemical and thermal stability is investigated by means of surface‐science techniques, complemented by density functional theory, with successive implementation in electronics, specifically in a millimeter‐wave receiver. While water adsorption is energetically unfavorable at room temperature, due to a differential Gibbs free energy of ≈+12 kJ mol?1, the presence of Te vacancies makes PdTe2 surfaces unstable toward surface oxidation with the emergence of a TeO2 skin, whose thickness remains sub‐nanometric even after one year in air. Correspondingly, the measured photocurrent of PdTe2‐based optoelectronic devices shows negligible changes (below 4%) in a timescale of one month, thus excluding the need of encapsulation in the nanofabrication process. Remarkably, the responsivity of a PdTe2‐based millimeter‐wave receiver is 13 and 21 times higher than similar devices based on black phosphorus and graphene in the same operational conditions, respectively. It is also discovered that pristine PdTe2 is thermally stable in a temperature range extending even above 500 K, thus paving the way toward PdTe2‐based high‐temperature electronics. Finally, it is shown that the TeO2 skin, formed upon air exposure, can be removed by thermal reduction via heating in vacuum.  相似文献   

2.
PtTe2 is a novel transition‐metal dichalcogenide hosting type‐II Dirac fermions that displays application capabilities in optoelectronics and hydrogen evolution reaction. Here it is shown, by combining surface science experiments and density functional theory, that the pristine surface of PtTe2 is chemically inert toward the most common ambient gases (oxygen and water) and even in air. It is demonstrated that the creation of Te vacancies leads to the appearance of tellurium‐oxide phases upon exposing defected PtTe2 surfaces to oxygen or ambient atmosphere, which is detrimental for the ambient stability of uncapped PtTe2‐based devices. On the contrary, in PtTe2 surfaces modified by the joint presence of Te vacancies and substitutional carbon atoms, the stable adsorption of hydroxyl groups is observed, an essential step for water splitting and the water–gas shift reaction. These results thus pave the way toward the exploitation of this class of Dirac materials in catalysis.  相似文献   

3.
Emerging classes of 2D noble‐transition‐metal dichalcogenides (NTMDs) stand out for their unique structure and novel physical properties in recent years. With the nearly full occupation of the d orbitals, 2D NTMDs are expected to be more attractive due to the unique interlayer vibrational behaviors and largely tunable electronic structures compared to most transition metal dichalcogenide semiconductors. The novel properties of 2D NTMDs have stimulated various applications in electronics, optoelectronics, catalysis, and sensors. Here, the latest development of 2D NTMDs are reviewed from the perspective of structure characterization, preparation, and application. Based on the recent research, the conclusions and outlook for these rising 2D NTMDs are presented.  相似文献   

4.
Two‐dimensional (2D) transition metal dichalcogenides (TMDs) nanostructures have been widely applied in environmental and biological analysis, biomedicine, electronic devices, and hydrogen evolution catalysis. Meanwhile, this excitement in 2D TMDs has spilled over to their counterparts of different dimensionalities like one‐dimensional (1D) and zero‐dimensional (0D) TMDs nanostructures. Eventual physical and chemical properties of TMDs nanostructures still remain to be highly dependent on their dimensionalities and size scale, and recently creatively exploring these physical and chemical properties is extremely impactful for the sensing field of TMD nanomaterials. Herein, we review a wide range of sensing applications based on not only graphene‐like 2D TMDs nanostructures but also the rapidly emerging subclasses of 1D, and 0D TMDs nanostructures. Their unique and interesting structures, excellent properties, and valid preparation methods are also included and the analytical objectives, ranging from heavy metal ions to small molecules, from DNA to proteins, from liquids to even vapors, can be met with extremely high selectivity and sensitivity. We have also analyzed our current understanding of 0D and 1D TMDs nanostructures and learning from graphene with the goal of contributing fresh ideas to the overall development of more advanced future TMDs based sensors.  相似文献   

5.
2D semiconductors, especially 2D transition metal dichalcogenides (TMDCs), have attracted ever-growing attention toward extending Moore's law beyond silicon. Metal–organic chemical vapor deposition (MOCVD) has been widely considered as a scalable technique to achieve wafer-scale TMDC films for applications. However, current MOCVD process usually suffers from small domain size with only hundreds of nanometers, in which dense grain boundary defects degrade the crystalline quality of the films. Here, a periodical varying-temperature ripening (PVTR) process is demonstrated to grow wafer-scale high crystalline TMDC films by MOCVD. It is found that the high-temperature ripening significantly reduces the nucleation density and therefore enables single-crystal domain size over 20 µm. In this process, no additives or etchants are involved, which facilitates low impurity concentration in the grown films. Atom-resolved electron microscopy imaging, variable temperature photoluminescence (PL) spectroscopy, and electrical transport results further confirm comparable crystalline quality to those observed in mechanically exfoliated TMDC films. The research provides a scalable route to produce high-quality 2D semiconducting films for applications in electronics and optoelectronics.  相似文献   

6.
Group‐10 layered transitional metal dichalcogenides including PtS2, PtSe2, and PtTe2 are excellent potential candidates for optoelectronic devices due to their unique properties such as high carrier mobility, tunable bandgap, stability, and flexibility. Large‐area platinum diselenide (PtSe2) with semiconducting characteristics is far scarcely investigated. Here, the development of a high‐performance photodetector based on vertically aligned PtSe2‐GaAs heterojunction which exhibits a broadband sensitivity from deep ultraviolet to near‐infrared light, with peak sensitivity from 650 to 810 nm, is reported. The Ilight/Idark ratio and responsivity of photodetector are 3 × 104 and 262 mA W?1 measured at 808 nm under zero bias voltage. The response speed of τrf is 5.5/6.5 µs, which represents the best result achieved for Group‐10 TMDs based optoelectronic device thus far. According to first‐principle density functional theory, the broad photoresponse ranging from visible to near‐infrared region is associated with the semiconducting characteristics of PtSe2 which has interstitial Se atoms within the PtSe2 layers. It is also revealed that the PtSe2/GaAs photodetector does not exhibit performance degradation after six weeks in air. The generality of the above good results suggests that the vertically aligned PtSe2 is an ideal material for high‐performance optoelectronic systems in the future.  相似文献   

7.
8.
Presently, research in layered transition metal dichalcogenides (TMDs) for numerous electrochemical applications have largely focused on Group 6 TMDs, especially MoS2 and WS2, whereas TMDs belonging to other groups are relatively unexplored. This work unravels the electrochemistry of Group 10 TMDs: specifically PtS2, PtSe2, and PtTe2. Here, the inherent electroactivities of these Pt dichalcogenides and the effectiveness of electrochemical activation on their charge transfer and electrocatalytic properties are thoroughly examined. By performing density functional theory (DFT) calculations, the electrochemical and electrocatalytic behaviors of the Pt dichalcogenides are elucidated. The charge transfer and electrocatalytic attributes of the Pt dichalcogenides are strongly associated with their electronic structures. In terms of charge transfer, electrochemical activation has been successful for all Pt dichalcogenides as evident in the faster heterogeneous electron transfer (HET) rates observed in electrochemically reduced Pt dichalcogenides. Interestingly, the hydrogen evolution reaction (HER) performance of the Pt dichalcogenides adheres to a trend of PtTe2 > PtSe2 > PtS2 whereby the HER catalytic property increases down the chalcogen group. Importantly, the DFT study shows this correlation to their electronic property in which PtS2 is semiconducting, PtSe2is semimetallic, and PtTe2 is metallic. Furthermore, Pt dichalcogenides are effectively activated for HER. Distinct electronic structures of Pt dichalcogenides account for their different responses to electrochemical activation. Among all activated Pt dichalcogenides, PtS2 shows most accentuated improvement as a HER electrocatalyst with an exceptional 50% decline in HER overpotential. Knowledge on Pt dichalcogenides provides valuable insights in the field of TMD electrochemistry, in particular, for the currently underrepresented Group 10 TMDs.  相似文献   

9.
The intrinsic spin‐dependent transport properties of two types of lateral VS2|MoS2 heterojunctions are systematically investigated using first‐principles calculations, and their various nanodevices with novel properties are designed. The lateral VS2|MoS2 heterojunction diodes show a perfect rectifying effect and are promising for the applications of Schottky diodes. A large spin‐polarization ratio is observed for the A‐type device and pure spin‐mediated current is then realized. The gate voltage significantly tunes the current and rectification ratio of their field‐effect transistors. In addition, they all demonstrate a sensitive photoresponse to blue light, and could be used as photodetector and photovoltaic device. Moreover, they generate an effective thermally driven current when a temperature gratitude appears between the two terminals, suggesting them as potential thermoelectric materials. Hence, the lateral VS2|MoS2 heterojunctions show a multifunctional nature and have various potential applications in spintronics, optoelectronics, and spin caloritronics.  相似文献   

10.
The synthesis of high‐quality 2D MoTe2 with a desired phase on SiO2/Si substrate is crucial to its diverse applications. A side reaction of Te with the substrate Si leading to SiTe and Si2Te3 tends to happen during growth, resulting in the failure to obtain MoTe2. It has been found that molecular sieves can adsorb the silicon telluride byproducts and eliminate the influence of the side reaction during the chemical vapor deposition synthesis of MoTe2. With the help of molecular sieves, few‐layer 1T′ MoTe2 can be grown from the MoOx precursor. Pure 1T′ MoTe2 and 2H MoTe2 regions in centimeter‐sized areas synthesized on the same piece of SiO2/Si substrate can be obtained by using an overlapped geometry. The strategy provides a new method to controllably synthesize MoTe2 with desired phases and can be generalizable to the synthesis of other tellurium‐based layered materials.  相似文献   

11.
Mono‐ and few‐layer transition metal dichalcogenides (TMDCs) have been widely used as saturable absorbers for ultrashort laser pulse generation, but their preparation is complicated and requires much expertise. The possible use of bulk‐structured TMDCs as saturable absorbers is therefore a very intriguing and technically important issue in laser technology. Here, for the first time, it is demonstrated that defective, bulk‐structured WTe2 microflakes can serve as a base saturable absorption material for fast mode‐lockers that can produce femtosecond pulses from fiber laser cavities. They have a modulation depth of 2.85%, from which stable laser pulses with a duration of 770 fs are readily obtained at a repetition rate of 13.98 MHz and a wavelength of 1556.2 nm, which is comparable to the performance achieved using mono‐ and few‐layer TMDCs. Density functional theory calculations show that the oxidative and defective surfaces of WTe2 microflakes do not degrade their saturable absorption performance in the near‐infrared range, allowing for a broad range of operative bandwidth. This study suggests that saturable absorption is an intrinsic property of TMDCs without relying on their structural dimensionality, providing a new direction for the development of TMDC‐based saturable absorbers.  相似文献   

12.
2D transition metal dichalcogenide (TMD) nanosheets, including MoS2, WS2, and TaS2, are used as hole injection layers (HILs) in organic light‐emitting diodes (OLEDs). MoS2, WS2, and TaS2 nanosheets are prepared using an exfoliation by ultrasonication method. The thicknesses and sizes of the TMD nanosheets are measured to be 3.1–4.3 nm and more than 100 nm, respectively. The work functions of the TMD nanosheets increase from 4.4–4.9 to 4.9–5.1 eV following ultraviolet/ozone (UVO) treatment. The turn‐on voltages at 10 cd m?2 for UVO‐treated TMD‐based devices decrease from 7.3–12.8 to 4.3–4.4 V and maximum luminance efficiencies increase from 5.74–9.04 to 12.01–12.66 cd A?1. In addition, this study confirms that the stabilities of the devices in air can be prolonged by using UVO‐treated TMDs as HILs in OLEDs. These results demonstrate the great potential of liquid‐exfoliated TMD nanosheets for use as HILs in OLEDs.  相似文献   

13.
Three new heteroleptic iridium complexes that combine two approaches, one leading to a high stability and the other yielding a high luminescence efficiency, are presented. All complexes contain a phenyl group at the 6‐position of the neutral bpy ligand, which holds an additional, increasingly bulky substituent on the 4‐position. The phenyl group allows for intramolecular π–π stacking, which renders the complex more stable and yields long‐living light‐emitting electrochemical cells (LECs). The additional substituent increases the intersite distance between the cations in the film, reducing the quenching of the excitons, and should improve the efficiency of the LECs. Density functional theory calculations indicate that the three complexes have the desired π–π intramolecular interactions between the pendant phenyl ring of the bpy ligand and the phenyl ring of one of the ppy ligands in the ground and the excited states. The photoluminescence quantum efficiency of concentrated films of the complexes improves with the increasing size of the bulky groups indicating that the adopted strategy for improving the efficiency is successful. Indeed, LEC devices employing these complexes as the primary active component show shorter turn‐on times, higher efficiencies and luminances, and, surprisingly, also demonstrate longer device stabilities.  相似文献   

14.
Chemical vapor deposition (CVD) has been developed as the most promising method for the growth of transition metal dichalcogenides (TMDs). In this work, the key factor determining the growth of TMDs is ascertained. A straightforward method is devised to directly achieve a holistic control of thickness, shape, and size of WS2 flakes via a single parameter control, namely, the status of the S‐precursor. The thickness‐dependent growth of WS2 flakes from mono‐ to quad‐layers is achieved by precise control of the feeding rate of elemental S‐precursor. Moreover, the explicit control over amount and exposure time of S‐precursor determines the most optimum combination of these parameters to tune the shape of the crystals from triangular to hexagonal with appropriate size. Hence, the experimental findings provide a promising strategy to engineer the growth evolution of WS2 atomic layers by fine tuning of the sulfur supply, paving a pathway to scalable electronic and photonic devices.  相似文献   

15.
A molten lithium infusion strategy has been proposed to prepare stable Li‐metal anodes to overcome the serious issues associated with dendrite formation and infinite volume change during cycling of lithium‐metal batteries. Stable host materials with superior wettability of molten Li are the prerequisite. Here, it is demonstrated that a series of strong oxidizing metal oxides, including MnO2, Co3O4, and SnO2, show superior lithiophilicity due to their high chemical reactivity with Li. Composite lithium‐metal anodes fabricated via melt infusion of lithium into graphene foams decorated by these metal oxide nanoflake arrays successfully control the formation and growth of Li dendrites and alleviate volume change during cycling. A resulting Li‐Mn/graphene composite anode demonstrates a super‐long and stable lifetime for repeated Li plating/stripping of 800 cycles at 1 mA cm?2 without voltage fluctuation, which is eight times longer than the normal lifespan of a bare Li foil under the same conditions. Furthermore, excellent rate capability and cyclability are realized in full‐cell batteries with Li‐Mn/graphene composite anodes and LiCoO2 cathodes. These results show a major advancement in developing a stable Li anode for lithium‐metal batteries.  相似文献   

16.
Rechargeable batteries with a Li metal anode and Ni‐rich Li[NixCoyMn1?x?y]O2 cathode (Li/Ni‐rich NCM battery) have been emerging as promising energy storage devices because of their high‐energy density. However, Li/Ni‐rich NCM batteries have been plagued by the issue of the thermodynamic instability of the Li metal anode and aggressive surface chemistry of the Ni‐rich cathode against electrolyte solution. In this study, a bi‐functional additive, adiponitrile (C6H8N2), is proposed which can effectively stabilize both the Li metal anode and Ni‐rich NCM cathode interfaces. In the Li/Ni‐rich NCM battery, the addition of 1 wt% adiponitrile in 0.8 m LiTFSI + 0.2 M LiDFOB + 0.05 M LiPF6 dissolved in EMC/FEC = 3:1 electrolyte helps to produce a conductive and robust Li anode/electrolyte interface, while strong coordination between Ni4+ on the delithiated Ni‐rich cathode and nitrile group in adiponitrile reduces parasitic reactions between the electrolyte and Ni‐rich cathode surface. Therefore, upon using 1 wt% adiponitrile, the Li/full concentration gradient Li[Ni0.73Co0.10Mn0.15Al0.02]O2 battery achieves an unprecedented cycle retention of 75% over 830 cycles under high‐capacity loading of 1.8 mAh cm?2 and fast charge–discharge time of 2 h. This work marks an important step in the development of high‐performance Li/Ni‐rich NCM batteries with efficient electrolyte additives.  相似文献   

17.
Structural distortions in the oxygen octahedral network in transition‐metal oxides play crucial roles in yielding a broad spectrum of functional properties, and precise control of such distortions is a key for developing future oxide‐based electronics. Here, it is shown that the displacement of apical oxygen atom shared between the octahedra at the heterointerface is a determining parameter for these distortions and consequently for control of structural and electronic phases of a strained oxide film. The present analysis by complementary annular dark‐ and bright‐field imaging in aberration‐corrected scanning transmission electron microscopy reveals that structural phase differences in strained monoclinic and tetragonal SrRuO3 films grown on GdScO3 substrates result from relaxation of the octahedral tilt, associated with changes in the in‐plane displacement of the apical oxygen atom at the heterointerface. It is further demonstrated that octahedral distortions and magnetrotransport properties of the SrRuO3 films can be controlled by interface engineering of the oxygen displacement. This provides a further degree of freedom for manipulating structural and electronic properties in strained films, allowing the design of novel oxide‐based heterostructures.  相似文献   

18.
Transition metal dichalcogenides (TMDs) display a rich variety of instabilities such as spin and charge orders, Ising superconductivity, and topological properties. Their physical properties can be controlled by doping in electric double-layer field-effect transistors (FET). However, for the case of single layer NbSe2, FET doping is limited to ≈ 1 × 1014 cm−2, while a somewhat larger charge injection can be obtained via deposition of K atoms. Here, by performing angle-resolved photoemission spectroscopy, scanning tunneling microscopy, quasiparticle interference measurements, and first-principles calculations it is shown that a misfit compound formed by sandwiching NbSe2 and LaSe layers behaves as a NbSe2 single layer with a rigid doping of 0.55–0.6 electrons per Nb atom or ≈ 6 × 1014 cm−2. Due to this huge doping, the 3 × 3 charge density wave is replaced by a 2 × 2 order with very short coherence length. As a tremendous number of different misfit compounds can be obtained by sandwiching TMDs layers with rock salt or other layers, this work paves the way to the exploration of heavily doped 2D TMDs over an unprecedented wide range of doping.  相似文献   

19.
Edges of 2D transition metal dichalcogenides (TMDs) are well known as highly reactive sites, thus researchers have attempted to maximize the edge site density of 2D TMDs. In this work, metal‐organic framework (MOF) templates are introduced to synthesize few‐layered WS2 nanoplates (a lateral dimension of ≈10 nm) confined in Co, N‐doped hollow carbon nanocages (WS2_Co‐N‐HCNCs), for highly sensitive NO2 gas sensors. WS2 precursors are assembled in the surface cavity of Co‐based zeolite imidazole framework (ZIF‐67) and subsequent pyrolysis produced WS2_Co‐N‐HCNCs. During the pyrolysis, the carbonized ZIF‐67 are doped by Co and N elements, and the growth of WS2 is effectively suppressed, creating few‐layered WS2 nanoplates functionalized Co‐N‐HCNCs. The WS2_Co‐N‐HCNCs exhibit outstanding NO2 sensing characteristics at room temperature, in terms of response (48.2% to 5 ppm), selectivity, response and recovery speed, and detection limit (100 ppb). These results are attributed to the enhanced adsorption and desorption kinetics of NO2 on abundant WS2 edges, confined in the gas permeable HCNCs. This work opens up an efficient way for the facile synthesis of edge abundant few‐layered TMDs combined with porous carbon matrix via MOF templating route, for applications relying on highly active sites.  相似文献   

20.
2D H‐phase vanadium disulfide (VS2) is expected to exhibit tunable semiconductor properties as compared with its metallic T‐phase structure, and thus is of promise for future electronic applications. However, to date such 2D H‐phase VS2 nanostructures have not been realized in experiment likely due to the polymorphs of vanadium sulfides and thermodynamic instability of H‐phase VS2. Preparation of H‐phase VS2 monolayer with lateral size up to 250 µm, as a new member in the 2D transition metal dichalcogenides (TMDs) family, is reported. A unique growth environment is built by introducing the molten salt‐mediated precursor system as well as the epitaxial mica growth platform, which successfully overcomes the aforementioned growth challenges and enables the evolution of 2D H‐phase structure of VS2. The honeycomb‐like structure of H‐phase VS2 with broken inversion symmetry is confirmed by spherical aberration‐corrected scanning transmission electron microscopy and second harmonic generation characterization. The phase structure is found to be ultra‐stable up to 500 K. The field‐effect device study further demonstrates the p‐type semiconducting nature of the 2D H‐phase VS2. The study introduces a new phase‐stable 2D TMDs materials with potential features for future electronic devices.  相似文献   

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