MoTe2 is an exfoliable transition metal dichalcogenide (TMD) which crystallizes in three symmetries; the semiconducting trigonal-prismatic 2H−phase, the semimetallic 1T ′ monoclinic phase, and the semimetallic orthorhombic T d structure 1-4 . The 2H−phase displays a band gap of ∼ 1 eV 5 making it appealing for flexible and transparent optoelectronics. The T d−phase is predicted to possess unique topological properties 6-9 which might lead to topologically protected non-dissipative transport channels 9 . Recently, it was argued that it is possible to locally induce phasetransformations in TMDs 3,10,11,14 , through chemical doping 12 , local heating 13 , or electric-field 14,15 to achieve ohmic contacts or to induce useful functionalities such as electronic phase-change memory elements 11 . The combination of semiconducting and topological elements based upon the same compound, might produce a new generation of high performance, low dissipation optoelectronic elements. Here, we show that it is possible to engineer the phases of MoTe2 through W substitution by unveiling the phase-diagram of the Mo1−xWxTe2 solid solution which displays a semiconducting to semimetallic transition as a function of x. We find that only ∼ 8 % of W stabilizes the T d−phase at room temperature. Photoemission spectroscopy, indicates that this phase possesses a Fermi surface akin to that of WTe2 16 .The properties of semiconducting and of semimetallic MoTe 2 are of fundamental interest in their own right, but are also for their potential technological relevance. In the mono-or few-layer limit it is a direct-gap semiconductor, while the bulk has an indirect bandgap 5,17,18 of ∼ 1 eV. The size of the gap is similar to that of Si, making 2H−MoTe 2 particularly appealing for both purely electronic devices 19,20 and optoelectronic applications 21 . Moreover, the existence of different phases opens up the possibility for many novel devices and architectures. For example, controlled conversion of the 1T ′ −MoTe 2 phase to the 2H−phase, as recently reported 22 , could
Permanent WRAP URL:http://wrap.warwick.ac.uk/93409 Copyright and reuse:The Warwick Research Archive Portal (WRAP) makes this work by researchers of the University of Warwick available open access under the following conditions. Copyright © and all moral rights to the version of the paper presented here belong to the individual author(s) and/or other copyright owners. To the extent reasonable and practicable the material made available in WRAP has been checked for eligibility before being made available.Copies of full items can be used for personal research or study, educational, or not-for-profit purposes without prior permission or charge. Provided that the authors, title and full bibliographic details are credited, a hyperlink and/or URL is given for the original metadata page and the content is not changed in any way. A note on versions:The version presented here may differ from the published version or, version of record, if you wish to cite this item you are advised to consult the publisher's version. Please see the 'permanent WRAP url' above for details on accessing the published version and note that access may require a subscription. The electronic structure of semi-metallic transition-metal dichalcogenides, such as WTe2 and orthorhombic γ−MoTe2, are claimed to contain pairs of Weyl points or linearly touching electron and hole pockets associated with a non-trivial Chern number. For this reason, these compounds were recently claimed to conform to a new class, deemed type-II, of Weyl semi-metallic systems. A series of angle resolved photoemission experiments (ARPES) claim a broad agreement with these predictions detecting, for example, topological Fermi arcs at the surface of these crystals. We synthesized singlecrystals of semi-metallic MoTe2 through a Te flux method to validate these predictions through measurements of its bulk Fermi surface (FS) via quantum oscillatory phenomena. We find that the superconducting transition temperature of γ−MoTe2 depends on disorder as quantified by the ratio between the room-and low-temperature resistivities, suggesting the possibility of an unconventional superconducting pairing symmetry. Similarly to WTe2, the magnetoresistivity of γ−MoTe2 does not saturate at high magnetic fields and can easily surpass 10 6 %. Remarkably, the analysis of the de Haas-van Alphen (dHvA) signal superimposed onto the magnetic torque, indicates that the geometry of its FS is markedly distinct from the calculated one. The dHvA signal also reveals that the FS is affected by the Zeeman-effect precluding the extraction of the Berry-phase. A direct comparison between the previous ARPES studies and density-functional-theory (DFT) calculations reveals a disagreement in the position of the valence bands relative to the Fermi level εF . Here, we show that a shift of the DFT valence bands relative to εF , in order to match the ARPES observations, and of the DFT electron bands to explain some of the observed dHvA frequencies, leads to a good agreement between the calculations and the angular depend...
We present a detailed quantum oscillatory study on the Dirac type-II semimetallic candidates PdTe2 and PtTe2 via the temperature and the angular dependence of the de Haas-van Alphen (dHvA) and Shubnikov-de Haas (SdH) effects. In high quality single crystals of both compounds, i.e. displaying carrier mobilities between 10 3 and 10 4 cm 2 /Vs, we observed a large non-saturating magnetoresistivity (MR) which in PtTe2 at a temperature T = 1.3 K, leads to an increase in the resistivity up to 5 × 10 4 % under a magnetic field µ0H = 62 T. These high mobilities correlate with their light effective masses in the range of 0.04 to 1 bare electron mass according to our measurements. For PdTe2 the experimentally determined Fermi surface cross-sectional areas show an excellent agreement with those resulting from band-structure calculations. Surprisingly, this is not the case for PtTe2 whose agreement between calculations and experiments is relatively poor even when electronic correlations are included in the calculations. Therefore, our study provides a strong support for the existence of a Dirac type-II node in PdTe2 and probably also for PtTe2. Band structure calculations indicate that the topologically non-trivial bands of PtTe2 do not cross the Fermi-level (εF). In contrast, for PdTe2 the Dirac type-II cone does intersect εF , although our calculations also indicate that the associated cyclotron orbit on the Fermi surface is located in a distinct kz plane with respect to the one of the Dirac type-II node. Therefore it should yield a trivial Berry-phase.
Crystalline two-dimensional (2D) superconductors (SCs) with low carrier density are an exciting new class of materials in which electrostatic gating can tune superconductivity, electronic interactions play a prominent role, and electrical transport properties may directly reflect the topology of the Fermi surface. Here, we report the dramatic enhancement of superconductivity with decreasing thickness in semimetallic T d-MoTe2, with critical temperature (T c) increasing up to 7.6 K for monolayers, a 60-fold increase with respect to the bulk T c. We show that monolayers possess a similar electronic structure and density of states (DOS) as the bulk, implying that electronic interactions play a strong role in the enhanced superconductivity. Reflecting the low carrier density, the critical temperature, magnetic field, and current density are all tunable by an applied gate voltage. The response to high in-plane magnetic fields is distinct from that of other 2D SCs and reflects the canted spin texture of the electron pockets.
Asymmetric three-dimensional (3D) nanoarchitectures that cannot coincide with their mirrored-symmetric counterparts are known as chiral objects. Numerous studies have focused on chiral plasmonic nanoarchitectures created intentionally with 3D asymmetric configurations, whose plasmonic chirality is promising for various nanoplasmonic and nanophotonic applications. Here, we show that gold nanorod (AuNR) plasmonic nanoarchitectures assembled on a soft 2D DNA origami template, which was often simplified to be a rigid rectangle, can exhibit strong chiroptical activities. The slight flexibility of the origami templates was found to play a critical role in inducing the plasmonic chirality of the assembled nanoarchitectures. Our study set a new example of reflecting the native conformation of nanostructures using chiral spectroscopy and can inspire the exploration of the softness of DNA templates for the future design of assembled chiral nanoarchitectures.
Weyl type-II fermions are massless quasiparticles that obey the Weyl equation and which are predicted to occur at the boundary between electron-and hole-pockets in certain semi-metals, i.e. the (W,Mo)(Te,P)2 compounds. Here, we present a study of the Fermi-surface of WP2 via the Shubnikov-de Haas (SdH) effect. Compared to other semi-metals WP2 exhibits a very low residual resistivity, i.e. ρ0 ≃ 10 nΩcm, which leads to perhaps the largest non-saturating magneto-resistivity (ρ(H)) reported for any compound. For the samples displaying the smallest ρ0, ρ(H) is observed to increase by a factor of 2.5 × 10 7 % under µ0H = 35 T at T = 0.35 K. The angular dependence of the SdH frequencies is found to be in very good agreement with the first-principle calculations when the electron-and hole-bands are slightly shifted with respect to the Fermi level, thus supporting the existence of underlying Weyl type-II points in WP2.
Recently, a new group of layered transition-metal tetra-chalcogenides was proposed via first principles calculations to correspond to a new family of Weyl type-II semimetals with promising topological properties in the bulk as well as in the monolayer limit. In this article, we present measurements of the Shubnikov-de Haas (SdH) and de Haas-van Alphen effects under high magnetic fields for the type-II Weyl semimetallic candidate NbIrTe4. We find that the angular dependence of the observed Fermi surface extremal cross-sectional areas agree well with our DFT calculations supporting the existence of Weyl type-II points in this material. Although we observe a large and non-saturating magnetoresistivity in NbIrTe4 under fields all the way up to 35 T, Hall-effect measurements indicate that NbIrTe4 is not a compensated semimetal. The transverse magnetoresistivity displays a fourfold angular dependence akin to the so-called butterfly magnetoresistivity observed in nodal line semimetals. We conclude that the field and this unconventional angular-dependence are governed by the topography of the Fermi-surface and the resulting anisotropy in effective masses and in carrier mobilities.
Organic-inorganic hybrid perovskites have shown great potential as building blocks for low-cost optoelectronics for their exceptional optical and electrical properties. Despite the remarkable progress in device demonstration, fundamental understanding of the physical processes in halide perovskites remains limited, especially the unusual electronic behaviors such as the current-voltage hysteresis and the switchable photovoltaic effect. These phenomena are of particular interests for being closely related to device functionalities and performance. In this work, a microscopic picture of electric fields in halide perovskite thin films was obtained using scanning laser microscopy. Unlike conventional semiconductors, distribution of the built-in electric fields in the halide perovskite evolves dynamically under the stimulation of external biases. The observations can be well explained using a model based on field-assisted ion migration, indicating that the mechanism responsible for the evolving charge transport observed in this material is not purely electronic. The anomalous dynamic responses to the applied bias are found to be effectively suppressed by operating the devices at reduced temperature or processing the materials at elevated temperature, which provide potential strategies for designing and creating halide perovskites with more stable charge transport properties in the development of viable perovskite-based optoelectronics.
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