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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.
    
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   

4.
    
The performance of electronic/optoelectronic devices is governed by carrier injection through metal–semiconductor contact; therefore, it is crucial to employ low‐resistance source/drain contacts. However, unintentional introduction of extrinsic defects, such as substoichiometric oxidation states at the metal–semiconductor interface, can degrade carrier injection. In this report, controlling the unintentional extrinsic defect states in layered MoS2 is demonstrated using a two‐step chemical treatment, (NH4)2S(aq) treatment and vacuum annealing, to enhance the contact behavior of metal/MoS2 interfaces. The two‐step treatment induces changes in the contact of single layer MoS2 field effect transistors from nonlinear Schottky to Ohmic behavior, along with a reduction of contact resistance from 35.2 to 5.2 kΩ. Moreover, the enhancement of ION and electron field effect mobility of single layer MoS2 field effect transistors is nearly double for n‐branch operation. This enhanced contact behavior resulting from the two‐step treatment is likely due to the removal of oxidation defects, which can be unintentionally introduced during synthesis or fabrication processes. The removal of oxygen defects is confirmed by scanning tunneling microscopy and X‐ray photoelectron spectroscopy. This two‐step (NH4)2S(aq) chemical functionalization process provides a facile pathway to controlling the defect states in transition metal dichalcogenides (TMDs), to enhance the metal‐contact behavior of TMDs.  相似文献   

5.
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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 τr/τf 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.
    
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   

8.
    
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   

9.
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10.
    
Palladium diselenide (PdSe2), a thus far scarcely studied group‐10 transition metal dichalcogenide has exhibited promising potential in future optoelectronic and electronic devices due to unique structures and electrical properties. Here, the controllable synthesis of wafer‐scale and homogeneous 2D PdSe2 film is reported by a simple selenization approach. By choosing different thickness of precursor Pd layer, 2D PdSe2 with thickness of 1.2–20 nm can be readily synthesized. Interestingly, with the increase in thickness, obvious redshift in wavenumber is revealed by Raman spectroscopy. Moreover, in accordance with density functional theory (DFT) calculation, optical absorption and ultraviolet photoemission spectroscopy (UPS) analyses confirm that the PdSe2 exhibits an evolution from a semiconductor (monolayer) to semimetal (bulk). Further combination of the PdSe2 layer with Si leads to a highly sensitive, fast, and broadband photodetector with a high responsivity (300.2 mA W?1) and specific detectivity (≈1013 Jones). By decorating the device with black phosphorus quantum dots, the device performance can be further optimized. These results suggest the as‐selenized PdSe2 is a promising material for optoelectronic application.  相似文献   

11.
    
Charge density wave (CDW) systems have been widely studied and proposed to be potential candidates for next‐generation electronic devices. However, the lack of room‐temperature CDW materials has limited the development of CDW‐based electronic devices, and thus finding a way to manipulate the CDW transitions and orders toward room temperature will be of importance. Room‐temperature and above CDW transition in 1T‐VSe2 is reported. The CDW transition is found to shift to ≈114 K at 0.7 GPa, and further compression enhances the transition temperature dramatically, reaching ≈358 K at 14.6 GPa. High‐pressure Raman spectroscopy measurement confirms that room‐temperature CDW order is achieved and persists up to 15 GPa. Such significant enhancement in CDW can be attributed to the pressure enhanced out‐of‐plane Fermi surface nesting and CDW gap in 1T‐VSe2. The observation of room‐ and high‐temperature CDW transition in 1T‐VSe2 under pressure provides an engineering approach to optimizing the CDW as needed in applications, which does not only open up a new platform for searching and controlling novel states of two‐dimensional materials, but also promotes a practical development of CDW‐related technology and devices.  相似文献   

12.
    
Recently, germanium selenide (GeSe) has emerged as a promising van der Waals semiconductor for photovoltaics, solar light harvesting, and water photoelectrolysis cells. Contrary to previous reports claiming perfect ambient stability based on experiments with techniques without surface sensitivity, here, by means of surface-science investigations and density functional theory, it is demonstrated that actually both: i) the surface of bulk crystals; and ii) atomically thin flakes of GeSe are prone to oxidation, with the formation of self-assembled germanium-oxide skin with sub-nanometric thickness. Surface oxidation leads to the decrease of the bandgap of stoichiometric GeSe and GeSe1−x, while bandgap energy increases upon surface oxidation of Ge1−xSe. Remarkably, the formation of a surface oxide skin on GeSe crystals plays a key role in the physicochemical mechanisms ruling photoelectrocatalysis: the underlying van der Waals semiconductor provides electron–hole pairs, while the germanium-oxide skin formed upon oxidation affords the active sites for catalytic reactions. The self-assembled germanium-oxide/germanium-selenide heterostructure with different bandgaps enables the activation of photocatalytic processes by absorption of light of different wavelengths, with inherently superior activity. Finally, it is discovered that, depending on the specific solvent-GeSe interaction, the liquid phase exfoliation of bulk crystals can induce the formation of Se nanowires.  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.
    
The charge density wave (CDW) in transition metal dichalcogenides (TMDs) has drawn tremendous interest due to its potential for tailoring their surface electronic and chemical properties. Due to technical challenges, however, how the CDW could modulate the chemical behavior of TMDs is still not clear. Here, this work presents a study of applying the CDW of NbTe2, with a high transition temperature above room temperature, to generate the assembling adsorption of Sn adatoms on the surface. It is shown that highly ordered monatomic Sn adatoms with a quasi‐1D structure can be obtained under regulation by the single‐axis CDW of the substrate. In addition, the CDW modulated superlattices could in turn change the surface electronic properties from semimetallic to metallic. These results demonstrate an effective approach for tuning the surface chemical properties of TMDs by their CDWs, which could be applied in exploring them for various practical applications, such as heterogeneous catalysis, epitaxial growth of low‐dimensional materials, and future nanoelectronics.  相似文献   

15.
    
By means of density functional theory and experiments, surface chemical reactivity of single crystals of NbAs and TaAs Weyl semimetals is studied. Weyl semimetals exhibit outstanding reactivity toward simple molecules (oxygen, carbon monoxide, and water), with several active sites available for surface chemical reactions (adsorption, decomposition, formation of reaction products, recombination of decomposition fragments). When different chemical species are adsorbed on Weyl semimetals, strong lateral interactions between coadsorbed species occur, evidenced by CO‐promoted water decomposition at room temperature. The resulting ? OH groups react with CO to form HCOO, which is an intermediate species in water–gas shift reaction. These findings unambiguously demonstrate that Weyl semimetals could be effectively used in catalysis, whereas their employment in nanoelectronics or plasmonics is complicated by the poor ambient stability, due to the rapid surface oxidation, inevitably occurring unless protective capping layers are used.  相似文献   

16.
    
Monolayered transition metal dichalcogenides (TMDs) are one kind of hexagonal 2D semiconductors with a direct bandgap structure. Due to the property of natural broken inversion symmetry in the lattice, the strong spin–orbit coupling of electrons in TMDs can induce degenerate levels with antiparallel spins in K and K′ valleys, which selectively respond with external light excitations. Surface plasmon resonance with efficient electromagnetic enhancement and near-field coupling provides excellent potential opportunities to modulate valley emission of TMDs. Efforts have been devoted to investigating the interaction principles and applications of this research field. This review focuses on plasmonic modulation of valleytronic emission in TMDs with surface plasmon polaritons (SPP) and localized surface plasmons (LSP) based on different modulation principles, respectively, and discusses possible research directions for future device applications.  相似文献   

17.
    
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   

18.
    
Materials exhibiting nodal‐line fermions promise superb impact on technology for the prospect of dissipationless spintronic devices. Among nodal‐line semimetals, the ZrSiX (X = S, Se, Te) class is the most suitable candidate for such applications. However, the surface chemical reactivity of ZrSiS and ZrSiSe has not been explored yet. Here, by combining different surface‐science tools and density functional theory, it is demonstrated that the formation of ZrSiS and ZrSiSe surfaces by cleavage is accompanied by the washing up of the exotic topological bands, giving rise to the nodal line. Moreover, while the ZrSiS has a termination layer with both Zr and S atoms, in the ZrSiSe surface, reconstruction occurs with the appearance of Si surface atoms, which is particularly prone to oxidation. It is demonstrated that the chemical activity of ZrSiX compounds is mostly determined by the interaction of the Si layer with the ZrX sublayer. A suitable encapsulation for ZrSiX should not only preserve their surfaces from interaction with oxidative species, but also provide a saturation of dangling bonds with minimal distortion of the surface.  相似文献   

19.
    
2D transition metal dichalcogenide (TMD) materials have been recognized as active platforms for surface‐enhanced Raman spectroscopy (SERS). Here, the effect of crystal structure (phase) transition is shown, which leads to altered electronic structures of TMD materials, on the Raman enhancement. Using thermally evaporated copper phthalocyanine, solution soaked rhodamine 6G, and crystal violet as typical probe molecules, it is found that a phase transition from 2H‐ to 1T‐phase can significantly increase the Raman enhancement effect on MoX2 (X = S, Se) monolayers through a predominantly chemical mechanism. First‐principle density functional theory calculations indicate that the significant enhancement of the Raman signals on metallic 1T‐MoX2 can be attributed to the facilitated electron transfer from the Fermi energy level of metallic 1T‐MoX2 to the highest occupied molecular orbital level of the probe molecules, which is more efficient than the process from the top of valence band of semiconducting 2H‐MoX2. This study not only reveals the origin of the Raman enhancement and identifies 1T‐MoSe2 and 1T‐MoS2 as potential Raman enhancement substrates, but also paves the way for designing new 2D SERS substrates via phase‐transition engineering.  相似文献   

20.
    
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   

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