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Different mechanisms driving a linear temperature dependence of the resistivity ρ â¼ T at van Hove singularities (VHSs) or metal-insulator transitions when doping a Mott insulator are being debated intensively with competing theoretical proposals. We experimentally investigate this using the exceptional tunability of twisted bilayer (TB) WSe2 by tracking the parameter regions where linear-in-T resistivity is found in dependency of displacement fields, filling, and magnetic fields. We find that even when the VHSs are tuned rather far away from the half-filling point and the Mott insulating transition is absent, the T-linear resistivity persists at the VHSs. When doping away from the VHSs, the T-linear behavior quickly transitions into a Fermi liquid behavior with a T2 relation. No apparent dependency of the linear-in-T resistivity, besides a rather strong change of prefactor, is found when applying displacement fields as long as the filling is tuned to the VHSs, including D â¼ 0.28 V/nm where a high-order VHS is expected. Intriguingly, such non-Fermi liquid linear-in-T resistivity persists even when magnetic fields break the spin-degeneracy of the VHSs at which point two linear in T regions emerge, for each of the split VHSs separately. This points to a mechanism of enhanced scattering at generic VHSs rather than only at high-order VHSs or by a quantum critical point during a Mott transition. Our findings provide insights into the many-body consequences arising out of VHSs, especially the non-Fermi liquid behavior found in moiré materials.
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Positive magnetoresistance (PMR) and negative magnetoresistance (NMR) describe two opposite responses of resistance induced by a magnetic field. Materials with giant PMR are usually distinct from those with giant NMR due to different physical natures. Here, we report the unusual photomagnetoresistance in the van der Waals heterojunctions of WSe2/quasi-two-dimensional electron gas, showing the coexistence of giant PMR and giant NMR. The PMR and NMR reach 1,007.5% at -9 T and -93.5% at 2.2 T in a single device, respectively. The magnetoresistance spans over two orders of magnitude on inversion of field direction, implying a giant unidirectional magnetoresistance (UMR). By adjusting the thickness of the WSe2 layer, we achieve the maxima of PMR and NMR, which are 4,900,000% and -99.8%, respectively. The unique magnetooptical transport shows the unity of giant UMR, PMR, and NMR, referred to as giant bipolar unidirectional photomagnetoresistance. These features originate from strong out-of-plane spin splitting, magnetic field-enhanced recombination of photocarriers, and the Zeeman effect through our experimental and theoretical investigations. This work offers directions for high-performance light-tunable spintronic devices.NMR).
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We engineered a two-dimensional Pt/WSe2/Ni avalanche photodetector (APD) optimized for ultraweak signal detection at room temperature. By fine-tuning the work functions, we achieved an ultralow dark current of 10-14 A under small bias, with a noise equivalent power (NEP) of 8.09 fW/Hz1/2. This performance is driven by effective dark barrier blocking and a record-long electron mean free path (123 nm) in intrinsic WSe2, minimizing dark carrier replenishment and suppressing noise under an ultralow electric field. Our APD exhibits a high gain of 5 × 105 at a modulation frequency of 20 kHz, effectively balancing gain and bandwidth, a common challenge in traditional photovoltaic-based APDs. By addressing the typical challenges of high noise and low gain and minimizing dependence on high electric fields, this work highlights the potential of 2D materials in developing efficient, low-power, and ultrasensitive photodetections.
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Semimetal electrodes for 2D semiconductors have been extensively studied; however, research on p-type semimetals has been limited due to the scarcity of materials that satisfy both high work functions and low resistances. In response, we investigated the behavior of NiSe2 as an electrode. Utilizing a novel co-evaporation method that suppresses oxidation and contamination, we synthesized NiSe2 demonstrating a high work function of 5.53 eV, a low resistance of 5.81 × 10-5 Ω cm, and a record hole concentration exceeding 1023 cm-3. We confirmed that when WSe2 comes into contact with NiSe2, the Fermi level of WSe2 falls below the work function of NiSe2, leading to complete hole degeneration of the channel. This unusual Fermi level alignment correlates with the high hole concentration in NiSe2 and the maximum energy level of its hole pockets. Our research provides new insights into how an electrode's hole concentration affects channel behavior.
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A monolayer semiconductor transferred on nanopillar arrays provides site-controlled, on-chip single photon emission, which is a scalable light source platform for quantum technologies. However, the brightness of these emitters reported to date often falls short of the perceived requirement for such applications. Also, the single photon purity usually degrades as the brightness increases. Hence, there is a need for a design methodology to achieve an enhanced emission rate while maintaining high single photon purity. By using WSe2 on high-aspect-ratio (â¼3, at least 2-fold higher than previous reports) nanopillar arrays, here we demonstrate >10 MHz single photon emission rate in the 770-800 nm band that is compatible with quantum memory and repeater networks (Rb-87-D1/D2 lines) and satellite quantum communication. The emitters exhibit excellent purity (even at high emission rates) and improved out-coupling due to the use of a gold back reflector that quenches the emission away from the nanopillar.
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Heterostrain is predicted to induce exceptionally rich physics in atomically thin two-dimensional structures by modifying the symmetry and optical selection rules. In this work, we introduce heterostrain into WSe2 bilayers by combining h-BN encapsulation and high-temperature vacuum annealing. Nonvolatile heterostrain gives rise to a Zeeman-like splitting associated with the elliptically polarized optical emission of interlayer K-K excitons. Further manipulation of the interlayer exciton emission in an external magnetic field reveals that the Zeeman-like splitting cannot be eliminated even in a magnetic field of up to ±6 T. We propose a microscopic picture with respect to the layer and valley pseudospin to interpret the results. Our findings imply an intriguing way to encode binary information with the layer pseudospin enabled by the heterostrain and open a venue for manipulating the layer pseudospin with heterostrain engineering, optical pseudospin injection, and an external magnetic field.
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Tuning the interfacial Schottky barrier with van der Waals (vdW) contacts is an important solution for two-dimensional (2D) electronics. Here we report that the interlayer dipoles of 2D vdW superlattices (vdWSLs) can be used to engineer vdW contacts to 2D semiconductors. A bipolar WSe2 with Ba6Ta11S28 (BTS) vdW contact was employed to exhibit this strategy. Strong interlayer dipoles can be formed due to charge transfer between the Ba3TaS5 and TaS2 layers. Mechanical exfoliation breaks the superlattice and produces two distinguished surfaces with TaS2 and Ba3TaS5 terminations. The surfaces thus have opposite surface dipoles and consequently different work functions. Therefore, all the devices fall into two categories in accordance with the rectifying direction, which were verified by electrical measurements and scanning photocurrent microscopy. The growing vdWSL family along with the addition surface dipoles enables prospective vdW contact designs and have practical application in nanoelectronics and nano optoelectronics.
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Monolayer transition metal dichalcogenides (TMDs) are considered promising building blocks for next-generation photonic and optoelectronic devices, owing to their fascinating optical properties. However, their inherent weak light absorption and low quantum yield severely hinder their practical applications. Here, we report up to 18000-fold photoluminescence (PL) enhancement in a monolayer WSe2-coupled plasmonic nanocavity. A spectroscopy-assisted nanomanipulation technique enables the assembly of a nanocavity with customizable resonances to simultaneously enhance the excitation and emission processes. In particular, precise control over the magnetic cavity mode facilitates spectral and spatial overlap with the exciton, resulting in plasmon-exciton intermediate coupling that approaches the maximum emission rate in the hybrid system. Meanwhile, the cavity mode exhibits high radiation directivity, which overwhelmingly directs surface-normal PL emission and leads to a 17-fold increase in the collection efficiency. Our approach opens up a new avenue to enhance the PL intensity of monolayer TMDs, facilitating their implementation in highly efficient optoelectronic devices.
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We study monolayer WSe2 using ultrafast electron diffraction. We introduce an approach to quantitatively extract atomic-site-specific information, providing an element-specific view of incoherent atomic vibrations following femtosecond excitation. Via differences between W and Se vibrations, we identify stages in the nonthermal evolution of the phonon population. Combined with a calculated phonon dispersion, this element specificity enables us to identify a long-lasting overpopulation of specific optical phonons and to interpret the stages as energy transfer processes between specific phonon groups. These results demonstrate the appeal of resolving element-specific vibrational information in the ultrafast time domain.
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The experimental demonstration of a p-type 2D WSe2 transistor with a ferroelectric perovskite BaTiO3 gate oxide is presented. The 30 nm thick BaTiO3 gate stack shows a robust ferroelectric hysteresis with a remanent polarization of 20 µC/cm2 and further enables a capacitance equivalent thickness of 0.5 nm in the hybrid WSe2/BaTiO3 stack due to its high dielectric constant of 323. We demonstrate one of the best ON currents for perovskite gate 2D transistors in the literature. This is enabled by high-quality epitaxial growth of BaTiO3 and a single 2D layer transfer based fabrication method that is shown to be amenable to silicon platforms. This demonstration is an important milestone toward the integration of crystalline complex oxides with 2D channel materials for scaled CMOS and low-voltage ferroelectric logic applications.
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Advanced microelectronics in the future may require semiconducting channel materials beyond silicon. Two-dimensional (2D) semiconductors, with their atomically thin thickness, hold great promise for future electronic devices. One challenge to achieving high-performance 2D semiconductor field effect transistors (FET) is the high contact resistance at the metal-semiconductor interface. In this study, we develop a charge-transfer doping strategy with WSe2/α-RuCl3 heterostructures to achieve low-resistance ohmic contact for p-type monolayer WSe2 transistors. We show that hole doping as high as 3 × 1013 cm-2 can be achieved in the WSe2/α-RuCl3 heterostructure due to its type-III band alignment, resulting in an ohmic contact with resistance of 4 kΩ µm. Based on that, we demonstrate p-type WSe2 transistors with an on-current of 35 µA·µm-1 and an ION/IOFF ratio exceeding 109 at room temperature.
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Interlayer excitons, with prolonged lifetimes and tunability, hold potential for advanced optoelectronics. Previous research on the interlayer excitons has been dominated by two-dimensional heterostructures. Here, we construct WSe2/GaN composite heterostructures, in which the doping concentration of GaN and the twist angle of bilayer WSe2 are employed as two ingredients for the manipulation of exciton behaviors and polarizations. The exciton energies in monolayer WSe2/GaN can be regulated continuously by the doping levels of the GaN substrate, and a remarkable increase in the valley polarizations is achieved. Especially in a heterostructure with 4°-twisted bilayer WSe2, a maximum polarization of 38.9% with a long lifetime is achieved for the interlayer exciton. Theoretical calculations reveal that the large polarization and long lifetime are attributed to the high exciton binding energy and large spin flipping energy during depolarization in bilayer WSe2/GaN. This work introduces a distinctive member of the interlayer exciton with a high degree of polarization and a long lifetime.
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Two-dimensional transition metal dichalcogenide (2D TMD) semiconductors allow facile integration of p- and n-type materials without a lattice mismatch. Here, we demonstrate gate-tunable n- and p-type junctions based on vertical heterostructures of MoS2 and WSe2 using van der Waals (vdW) contacts. The p-n junction shows negative differential resistance (NDR) due to Fowler-Nordheim (F-N) tunneling through the triangular barrier formed by applying a global back-gate bias (VGS). We also show that the integration of hexagonal boron nitride (h-BN) as an insulating tunnel barrier between MoS2 and WSe2 leads to the formation of sharp band edges and unintentional inelastic tunnelling current. The devices based on vdW contacts, global VGS, and h-BN tunnel barriers exhibit NDR with a peak current (Ipeak) of 315 µA, suggesting that the approach may be useful for applications.
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Herein, the structure of integrated M3D inverters are successfully demonstrated where a chemical vapor deposition (CVD) synthesized monolayer WSe2 p-type nanosheet FET is vertically integrated on top of CVD synthesized monolayer MoS2 n-type film FET arrays (2.5 × 2.5 cm) by semiconductor industry techniques, such as transfer, e-beam evaporation (EBV), and plasma etching processes. A low temperature (below 250 °C) is employed to protect the WSe2 and MoS2 channel materials from thermal decomposition during the whole fabrication process. The MoS2 NMOS and WSe2 PMOS device fabricated show an on/off current ratio exceeding 106 and the integrated M3D inverters indicate an average voltage gain of ≈9 at VDD = 2 V. In addition, the integrated M3D inverter demonstrates an ultra-low power consumption of 0.112 nW at a VDD of 1 V. Statistical analysis of the fabricated inverters devices shows their high reliability, rendering them suitable for large-area applications. The successful demonstration of M3D inverters based on large-scale 2D monolayer TMDs indicate their high potential for advancing the application of 2D TMDs in future integrated circuits.
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The intrinsic low-symmetry crystal structures or external geometries of low-dimensional materials are crucial for polarization-sensitive photodetection. However, these inherently anisotropic materials are limited in variety, and their anisotropy is confined to specific crystal directions. Transforming 2D semiconductors, such as WSe2, from isotropic 2D nanosheets into anisotropic 1D nanoscrolls expands their application in polarization photodetection. Despite this considerable potential, research on polarization photodetection based on nanoscrolls remains scarce. Here, the uniform crystalline orientation of WSe2 nanoscrolls is achieved conveniently and efficiently by applying ethanol droplets to vapor deposition-grown bilayer WSe2 nanosheets. Angle-resolved polarized Raman spectroscopy of WSe2 nanoscrolls demonstrates vibrational anisotropy. Photodetectors based on these nanoscrolls show competitive overall performance with a broadband detection range from 405 to 808 nm, a competitive on/off ratio of ≈900, a high detectivity of 3.4 × 108 Jones, and a fast response speed of ≈30 ms. Additionally, WSe2 nanoscroll-based photodetectors exhibit strong polarization-sensitive detection with a maximum dichroic ratio of 1.5. More interestingly, due to high photosensitivity, the WSe2 nanoscroll detectors can easily record sequential puppy images. This work reveals the potential of WSe2 nanoscrolls as excellent polarization-sensitive photodetectors and provides new insights into the development of high-performance optoelectronic devices.
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Electrochemiluminescence (ECL) is a powerful tool for clinical diagnosis due to its exceptional sensitivity. However, the standard tripropylamine (TPrA) coreactant for Ru(bpy)3Cl2, the most widely studied and used ECL system, is highly toxic. Despite extensive research on alternative coreactants, they often fall short in poor efficiency. From a reaction kinetics perspective, accelerating electrooxidation rate of Ru(bpy)3Cl2 is an essential way to compensate the efficiency limitation of coreactants, but is rarely reported. Here, a hybrid electrocatalyst@coreactant dots for the ECL of Ru(bpy)3Cl2 is reported. The as-prepared WSe2@bovine serum albumin (WSe2@BSA) dots is biocompatible, and demonstrate dual functions, i.e., the BSA shell works as a coreactant, meanwhile, the WSe2 core effectively catalyzes Ru(bpy)3Cl2 oxidation. As a result, WSe2@BSA dots exhibit an exceptionally high efficiency comparable to TPrA for the ECL of Ru(bpy)3Cl2. In addition, the procedure for synthesizing WSe2@BSA dots is facile (room temperature, atmospheric conditions), rapid (5 min), and scalable (for millions of bioassays). A biosensor utilizing WSe2@BSA dots shows promise for highly sensitive detecting glypican-3 in clinical liver cancer serum samples, especially for alpha-fetoprotein-negative patients. This work opens a new avenue for developing a highly efficient ECL system for biosensing and clinical diagnosis.
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The advancement of rechargeable Mg-metal batteries (RMBs) is severely impeded by the lack of suitable cathode materials. Despite the good cyclic stability of intercalation-type compounds, their specific capacity is relatively low. Conversely, the conversion-type cathodes can deliver a higher capacity but often suffer from poor cycling reversibility and stability. Herein, a WSe2/Se intercalation-conversion hybrid material with elemental Se uniformly distributed into WSe2 nanosheets is fabricated via a simple solvothermal method for high-performance RMBs. The uniformly introduced Se confined in WSe2 nanosheets can not only efficiently improve the conductivity of the hybrid cathodes, facilitating the fast electron transport and ion diffusion, but also provide additional specific capacity. Besides, the WSe2 can effectively inhibit the detrimental Se dissolution and polyselenide shuttle, thereby activating the activity of Se and improving its utilization. Consequently, the synergy of intercalation and conversion mechanisms endows WSe2/Se hybrids with superior reversible capacity of 252 mAh g-1 at 0.1 A g-1 and ultra-long cyclability of up to 5000 cycles at 2.0 A g-1 with capacity retention of 78.1%. This work demonstrates the feasibility of the strategy by integrating intercalation and conversion mechanisms for developing high-performance cathode materials for RMBs.
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Most properties of solid materials are defined by their internal electric field and charge density distributions which so far are difficult to measure with high spatial resolution. Especially for 2D materials, the atomic electric fields influence the optoelectronic properties. In this study, the atomic-scale electric field and charge density distribution of WSe2 bi- and trilayers are revealed using an emerging microscopy technique, differential phase contrast (DPC) imaging in scanning transmission electron microscopy (STEM). For pristine material, a higher positive charge density located at the selenium atomic columns compared to the tungsten atomic columns is obtained and tentatively explained by a coherent scattering effect. Furthermore, the change in the electric field distribution induced by a missing selenium atomic column is investigated. A characteristic electric field distribution in the vicinity of the defect with locally reduced magnitudes compared to the pristine lattice is observed. This effect is accompanied by a considerable inward relaxation of the surrounding lattice, which according to first principles DFT calculation is fully compatible with a missing column of Se atoms. This shows that DPC imaging, as an electric field sensitive technique, provides additional and remarkable information to the otherwise only structural analysis obtained with conventional STEM imaging.
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Two-dimensional transition metal dichalcogenide (TMDC) semiconductors are emerging as strong contenders for electronic devices that can be used in highly radioactive environments such as outer space where conventional silicon-based devices exhibit nonideal characteristics for such applications. To address the radiation-induced interface effects of TMDC-based electronic devices, we studied high-energy proton beam irradiation effects on the electrical properties of field-effect transistors (FETs) made with tungsten diselenide (WSe2) channels and hexagonal boron-nitride (hBN)/SiO2gate dielectrics. The electrical characteristics of WSe2FETs were measured before and after the irradiation at various proton beam doses of 1013, 1014, and 1015cm-2. In particular, we demonstrated the dependence of proton irradiation-induced effects on hBN layer thickness in WSe2FETs. We observed that the hBN layer reduces the WSe2/dielectric interface effect which would shift the transfer curve of the FET toward the positive direction of the gate voltage. Also, this interface effect was significantly suppressed when a thicker hBN layer was used. This phenomenon can be explained by the fact that the physical separation of the WSe2channel and SiO2dielectric by the hBN interlayer prevents the interface effects originating from the irradiation-induced positive trapped charges in SiO2reaching the interface. This work will help improve our understanding of the interface effect of high-energy irradiation on TMDC-based nanoelectronic devices.
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Transition metal dichalcogenides (TMDs) with a two-dimensional (2D) structure and semiconducting features are highly favorable for the production of NH3gas sensors. Among the TMD family, WS2, WSe2, MoS2, and MoSe2exhibit high conductivity and a high surface area, along with high availability, reasons for which they are favored in gas-sensing studies. In this review, we have discussed the structure, synthesis, and NH3sensing characteristics of pristine, decorated, doped, and composite-based WS2, WSe2, MoS2, and MoSe2gas sensors. Both experimental and theoretical studies are considered. Furthermore, both room temperature and higher temperature gas sensors are discussed. We also emphasized the gas-sensing mechanism. Thus, this review provides a reference for researchers working in the field of 2D TMD gas sensors.