Most studied two-dimensional (2D) materials exhibit isotropic behavior due to high lattice symmetry; however, lower-symmetry 2D materials such as phosphorene and other elemental 2D materials exhibit very interesting anisotropic properties. In this work, we report the atomic structure, electronic properties, and vibrational modes of few-layered PdSe exfoliated from bulk crystals, a pentagonal 2D layered noble transition metal dichalcogenide with a puckered morphology that is air-stable. Micro-absorption optical spectroscopy and first-principles calculations reveal a wide band gap variation in this material from 0 (bulk) to 1.3 eV (monolayer). The Raman-active vibrational modes of PdSe were identified using polarized Raman spectroscopy, and a strong interlayer interaction was revealed from large, thickness-dependent Raman peak shifts, agreeing with first-principles Raman simulations. Field-effect transistors made from the few-layer PdSe display tunable ambipolar charge carrier conduction with a high electron field-effect mobility of ∼158 cm V s, indicating the promise of this anisotropic, air-stable, pentagonal 2D material for 2D electronics.
Large-area and high-quality 2D transition metal tellurides are synthesized by the chemical vapor deposition method. The as-grown WTe maintains two different stacking sequences in the bilayer, where the atomic structure of the stacking boundary is revealed by scanning transmission electron microscopy. The low-temperature transport measurements reveal a novel semimetal-to-insulator transition in WTe layers and an enhanced superconductivity in few-layer MoTe .
The experimental manifestation of topological effects in bulk materials under ambient conditions, especially those with practical applications, has attracted enormous research interest. Recent discovery of Weyl semimetal provides an ideal material platform for such endeavors. The Berry curvature in a Weyl semimetal becomes singular at the Weyl node, creating an effective magnetic monopole in the k-space. A pair of Weyl nodes carry quantized effective magnetic charges with opposite signs, and therefore, opposite chirality. Although Weyl-point-related signatures such as chiral anomaly and non-closing surface Fermi arcs have been detected through transport and ARPES measurements, direct experimental evidence of the effective k-space monopole of the Weyl nodes has so far been lacking. In this work, signatures of the singular topology in a type-II Weyl semimetal TaIrTe4 is revealed in the photo responses, which are shown to be directly related to the divergence of Berry curvature. As a result of the divergence of Berry curvature at the Weyl nodes, TaIrTe4 exhibits unusually large photo responsivity of 130.2 mA/W with 4-m excitation in an unbiased field effect transistor at room temperature arising from the third-order nonlinear optical response.The room temperature mid-IR responsivity is approaching the performance of commercial HgCdTe detector operating at low temperature, making Type-II Weyl semimetal TaIrTe4 of practical importance in terms of photo sensing and solar energy harvesting. Furthermore, the circularly polarized galvanic response is also enhanced at 4-m, possibly due to the same Berry curvature singularity enhancement as the shift current. Considering the optical selection rule of Weyl cones with opposite chirality, it may open new experimental possibilities for studying and controlling the chiral polarization of Weyl Fermions through an in-plane DC electric field in addition to the optical helicities.
The semiconductor-electrolyte interface dominates the behaviors of semiconductor electrocatalysis, which has been modeled as a Schottky-analog junction according to the classic electron transfer theories. However, this model cannot be used to explain the extremely high carrier accumulations in ultrathin semiconductor catalysis observed in our work. Inspired by the recently developed ion-controlled electronics, we revisited the semiconductor-electrolyte interface and unraveled a universal self-gating phenomenon through micro-cell based in-situ electronic/electrochemical measurements to clarify the electronic-conduction modulation of semiconductors during electrocatalytic reaction. Then we demonstrate that the type of semiconductor catalysts strongly correlates their electrocatalysis, i.e., n-type semiconductor catalysts favor cathodic reactions such as hydrogen evolution reaction (HER), p-type ones prefer anodic reactions such as oxygen evolution reaction (OER), and bipolar ones tend to perform both anodic and cathodic reactions.Our study provides a new insight into the electronic origin of semiconductor-electrolyte interface during electrocatalysis, paving the way for designing high-performance semiconductor catalysts.
High-yield preparation of ultrathin two-dimensional (2D) nanosheets is of great importance for the further exploration of their unique properties and promising applications. Herein, for the first time, the high-yield and scalable production of ultrathin 2D ternary chalcogenide nanosheets, including Ta2NiS5 and Ta2NiSe5, in solution is achieved by exfoliating their layered microflakes. The size of resulting Ta2NiS5 and Ta2NiS5 nanosheets ranges from tens of nanometers to few micrometers. Importantly, the production yield of single-layer Ta2NiS5 nanosheets is very high, ca. 86%. As a proof-of-concept application, the single-layer Ta2NiS5 is used as a novel fluorescence sensing platform for the detection of DNA with excellent selectivity and high sensitivity (with detection limit of 50 pM). These solution-processable, high-yield, large-amount ternary chalcogenide nanosheets may also have potential applications in electrocatalysis, supercapacitors, and electronic devices.
The layered ternary compound TaIrTe is an important candidate to host the recently predicted type-II Weyl Fermions that break Lorentz invariance. Photodetectors based on Weyl semimetal promise extreme performance in terms of highly sensitive, broadband, and self-powered operation owing to its topologically protected band structures. In this work, we report the realization of a broadband self-powered photodetector based on TaIrTe. The photocurrent generation mechanisms are investigated with power- and temperature-dependent photoresponse measurements. The prototype metal-TaIrTe-metal photodetector exhibits a responsivity of 20 μA W or a specific detectivity of 1.8 × 10 Jones with 27 μs response time at 10.6 μm. Broadband responses from 532 nm to 10.6 μm are experimentally tested with potential detection range extendable to far-infrared and terahertz. Furthermore, anisotropic response of the TaIrTe photodetector is identified using polarization-angle-dependent measurement with linearly polarized light. The anisotropy is found to be wavelength dependent, and the degree of anisotropy increases as the excitation wavelength gets closer to the Weyl nodes. Our results suggest this emerging class of materials can be harnessed for broadband, polarization angle-sensitive, self-powered photodetection with reasonable responsivities.
The recent discovery of a Weyl semimetal in TaAs offers the first Weyl fermion observed in nature and dramatically broadens the classification of topological phases. However, in TaAs it has proven challenging to study the rich transport phenomena arising from emergent Weyl fermions. The series MoxW1−xTe2 are inversion-breaking, layered, tunable semimetals already under study as a promising platform for new electronics and recently proposed to host Type II, or strongly Lorentz-violating, Weyl fermions. Here we report the discovery of a Weyl semimetal in MoxW1−xTe2 at x=25%. We use pump-probe angle-resolved photoemission spectroscopy (pump-probe ARPES) to directly observe a topological Fermi arc above the Fermi level, demonstrating a Weyl semimetal. The excellent agreement with calculation suggests that MoxW1−xTe2 is a Type II Weyl semimetal. We also find that certain Weyl points are at the Fermi level, making MoxW1−xTe2 a promising platform for transport and optics experiments on Weyl semimetals.
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