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Register a new userMeasuring Chern numbers above the Fermi level in the Type II Weyl semimetal Mo$_x$W$_{1-x}$Te$_2$
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It has recently been proposed that electronic band structures in crystals give rise to a previously overlooked type of Weyl fermion, which violates Lorentz invariance and, consequently, is forbidden in particle physics. It was further predicted that Mo$_x$W$_{1-x}$Te$_2$ may realize such a Type II Weyl fermion. One crucial challenge is that the Weyl points in Mo$_x$W$_{1-x}$Te$_2$ are predicted to lie above the Fermi level. Here, by studying a simple model for a Type II Weyl cone, we clarify the importance of accessing the unoccupied band structure to demonstrate that Mo$_x$W$_{1-x}$Te$_2$ is a Weyl semimetal. Then, we use pump-probe angle-resolved photoemission spectroscopy (pump-probe ARPES) to directly observe the unoccupied band structure of Mo$_x$W$_{1-x}$Te$_2$. For the first time, we directly access states $> 0.2$ eV above the Fermi level. By comparing our results with $textit{ab initio}$ calculations, we conclude that we directly observe the surface state containing the topological Fermi arc. Our work opens the way to studying the unoccupied band structure as well as the time-domain relaxation dynamics of Mo$_x$W$_{1-x}$Te$_2$ and related transition metal dichalcogenides.
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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 Mo$_x$W$_{1-x}$Te$_2$ 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 Mo$_x$W$_{1-x}$Te$_2$ 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 Mo$_x$W$_{1-x}$Te$_2$ is the first Type II Weyl semimetal. We also find that certain Weyl points are at the Fermi level, making Mo$_x$W$_{1-x}$Te$_2$ a promising platform for transport and optics experiments on Weyl semimetals.
Weyl semimetals have sparked intense research interest, but experimental work has been limited to the TaAs family of compounds. Recently, a number of theoretical works have predicted that compounds in the Mo$_x$W$_{1-x}$Te$_2$ series are Weyl semimetals. Such proposals are particularly exciting because Mo$_x$W$_{1-x}$Te$_2$ has a quasi two-dimensional crystal structure well-suited to many transport experiments, while WTe$_2$ and MoTe$_2$ have already been the subject of numerous proposals for device applications. However, with available ARPES techniques it is challenging to demonstrate a Weyl semimetal in Mo$_x$W$_{1-x}$Te$_2$. According to the predictions, the Weyl points are above the Fermi level, the system approaches two critical points as a function of doping, there are many irrelevant bulk bands, the Fermi arcs are nearly degenerate with bulk bands and the bulk band gap is small. Here, we study Mo$_x$W$_{1-x}$Te$_2$ for $x = 0.07$ and 0.45 using pump-probe ARPES. The system exhibits a dramatic response to the pump laser and we successfully access states $> 0.2$eV above the Fermi level. For the first time, we observe direct, experimental signatures of Fermi arcs in Mo$_x$W$_{1-x}$Te$_2$, which agree well with theoretical calculations of the surface states. However, we caution that the interpretation of these features depends sensitively on free parameters in the surface state calculation. We comment on the prospect of conclusively demonstrating a Weyl semimetal in Mo$_x$W$_{1-x}$Te$_2$.
Weyl nodes and Fermi arcs in type-II Weyl semimetals (WSMs) have led to lots of exotic transport phenomena. Recently, Mo$_{0.25}$W$_{0.75}$Te$_{2}$ has been established as a type-II WSM with Weyl points located near Fermi level, which offers an opportunity to study its intriguing band structure by electrical transport measurements. Here, by selecting a special sample with the thickness gradient across two- (2D) and three-dimensional (3D) regime, we show strong evidences that Mo$_{0.25}$W$_{0.75}$Te$_{2}$ is a type-II Weyl semimetal by observing the following two dimensionality-dependent transport features: 1) A chiral-anomaly-induced anisotropic magneto-conductivity enhancement, proportional to the square of in-plane magnetic field (B$_{in}$$^{2}$); 2) An additional quantum oscillation with thickness-dependent phase shift. Our theoretical calculations show that the observed quantum oscillation originates from a Weyl-orbit-like scenario due to the unique band structure of Mo$_{0.25}$W$_{0.75}$Te$_{2}$. The in situ dimensionality-tuned transport experiment offers a new strategy to search for type-II WSMs.
The recently discovered type-II Weyl points appear at the boundary between electron and hole pockets. Type-II Weyl semimetals that host such points are predicted to exhibit a new type of chiral anomaly and possess thermodynamic properties very different from their type-I counterparts. In this Letter, we describe the prediction of a type-II Weyl semimetal phase in the transition metal diphosphides MoP$_2$ and WP$_2$. These materials are characterized by relatively simple band structures with four pairs of type-II Weyl points. Neighboring Weyl points have the same chirality, which makes the predicted topological phase robust with respect to small perturbations of the crystalline lattice. In addition, this peculiar arrangement of the Weyl points results in long topological Fermi arcs, thus making them readily accessible in angle-resolved photoemission spectroscopy.
The structural polymorphism in transition metal dichalcogenides (TMDs) provides exciting opportunities for developing advanced electronics. For example, MoTe$_2$ crystallizes in the 2H semiconducting phase at ambient temperature and pressure, but transitions into the 1T$^prime$ semimetallic phase at high temperatures. Alloying MoTe$_2$ with WTe$_2$ reduces the energy barrier between these two phases, while also allowing access to the T$_d$ Weyl semimetal phase. The MoWTe$_2$ alloy system is therefore promising for developing phase change memory technology. However, achieving this goal necessitates a detailed understanding of the phase composition in the MoTe$_2$-WTe$_2$ system. We combine polarization-resolved Raman spectroscopy with X-ray diffraction (XRD) and scanning transmission electron microscopy (STEM) to study MoWTe$_2$ alloys over the full compositional range x from 0 to 1. We identify Raman and XRD signatures characteristic of the 2H, 1T$^prime$, and T$_d$ structural phases that agree with density-functional theory (DFT) calculations, and use them to identify phase fields in the MoTe$_2$-WTe$_2$ system, including single-phase 2H, 1T$^prime$, and T$_d$ regions, as well as a two-phase 1T$^prime$ + T$_d$ region. Disorder arising from compositional fluctuations in MoWTe$_2$ alloys breaks inversion and translational symmetry, leading to the activation of an infrared 1T$^prime$-MoTe$_2$ mode and the enhancement of a double-resonance Raman process in 2H-MoWTe$_2$ alloys. Compositional fluctuations limit the phonon correlation length, which we estimate by fitting the observed asymmetric Raman lineshapes with a phonon confinement model. These observations reveal the important role of disorder in MoWTe$_2$ alloys, clarify the structural phase boundaries, and provide a foundation for future explorations of phase transitions and electronic phenomena in this system.
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