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1.
Nature ; 605(7908): 57-62, 2022 05.
Artigo em Inglês | MEDLINE | ID: mdl-35508779

RESUMO

The Luttinger liquid (LL) model of one-dimensional (1D) electronic systems provides a powerful tool for understanding strongly correlated physics, including phenomena such as spin-charge separation1. Substantial theoretical efforts have attempted to extend the LL phenomenology to two dimensions, especially in models of closely packed arrays of 1D quantum wires2-13, each being described as a LL. Such coupled-wire models have been successfully used to construct two-dimensional (2D) anisotropic non-Fermi liquids2-6, quantum Hall states7-9, topological phases10,11 and quantum spin liquids12,13. However, an experimental demonstration of high-quality arrays of 1D LLs suitable for realizing these models remains absent. Here we report the experimental realization of 2D arrays of 1D LLs with crystalline quality in a moiré superlattice made of twisted bilayer tungsten ditelluride (tWTe2). Originating from the anisotropic lattice of the monolayer, the moiré pattern of tWTe2 hosts identical, parallel 1D electronic channels, separated by a fixed nanoscale distance, which is tuneable by the interlayer twist angle. At a twist angle of approximately 5 degrees, we find that hole-doped tWTe2 exhibits exceptionally large transport anisotropy with a resistance ratio of around 1,000 between two orthogonal in-plane directions. The across-wire conductance exhibits power-law scaling behaviours, consistent with the formation of a 2D anisotropic phase that resembles an array of LLs. Our results open the door for realizing a variety of correlated and topological quantum phases based on coupled-wire models and LL physics.

3.
Angew Chem Int Ed Engl ; 60(37): 20094-20100, 2021 Sep 06.
Artigo em Inglês | MEDLINE | ID: mdl-34235841

RESUMO

In view of rising ecological awareness, materials development is primarily aimed at improving the performance and efficiency of innovative and more elaborate materials. However, a materials performance figure of merit should include essential aspects of materials: environmental impact, economic constraints, technical feasibility, etc. Thus, we promote the inclusion of sustainability criteria already during the materials design process. With such a holistic design approach, new products may be more likely to meet the circular economy requirements than when traditional development strategies are pursued. Using catalysts for water electrolysis as an example, we present a modelling method based on experimental data to holistically evaluate processes.

5.
Nature ; 589(7841): 225-229, 2021 01.
Artigo em Inglês | MEDLINE | ID: mdl-33398136

RESUMO

In strongly correlated materials, quasiparticle excitations can carry fractional quantum numbers. An intriguing possibility is the formation of fractionalized, charge-neutral fermions-for example, spinons1 and fermionic excitons2,3-that result in neutral Fermi surfaces and Landau quantization4,5 in an insulator. Although previous experiments in quantum spin liquids1, topological Kondo insulators6-8 and quantum Hall systems3,9 have hinted at charge-neutral Fermi surfaces, evidence for their existence remains inconclusive. Here we report experimental observation of Landau quantization in a two-dimensional insulator, monolayer tungsten ditelluride (WTe2), a large-gap topological insulator10-13. Using a detection scheme that avoids edge contributions, we find large quantum oscillations in the material's magnetoresistance, with an onset field as small as about 0.5 tesla. Despite the huge resistance, the oscillation profile, which exhibits many periods, mimics the Shubnikov-de Haas oscillations in metals. At ultralow temperatures, the observed oscillations evolve into discrete peaks near 1.6 tesla, above which the Landau quantized regime is fully developed. Such a low onset field of quantization is comparable to the behaviour of high-mobility conventional two-dimensional electron gases. Our experiments call for further investigation of the unusual ground state of the WTe2 monolayer, including the influence of device components and the possible existence of mobile fermions and charge-neutral Fermi surfaces inside its insulating gap.

6.
Sci Adv ; 6(51)2020 12.
Artigo em Inglês | MEDLINE | ID: mdl-33355138

RESUMO

Magnetic Weyl semimetals are a newly discovered class of topological materials that may serve as a platform for exotic phenomena, such as axion insulators or the quantum anomalous Hall effect. Here, we use angle-resolved photoelectron spectroscopy and ab initio calculations to discover Weyl cones in CoS2, a ferromagnet with pyrite structure that has been long studied as a candidate for half-metallicity, which makes it an attractive material for spintronic devices. We directly observe the topological Fermi arc surface states that link the Weyl nodes, which will influence the performance of CoS2 as a spin injector by modifying its spin polarization at interfaces. In addition, we directly observe a minority-spin bulk electron pocket in the corner of the Brillouin zone, which proves that CoS2 cannot be a true half-metal.

7.
J Phys Chem Lett ; 11(15): 6105-6111, 2020 Aug 06.
Artigo em Inglês | MEDLINE | ID: mdl-32657592

RESUMO

The ultrafast optical response of nodal-line semimetals ZrSiS and ZrSiSe was studied in the near-infrared using transient reflectivity. The materials exhibit similar responses, characterized by two features, well-resolved in time and energy; the first decays after hundreds of femtoseconds, and the second lasts for nanoseconds. Using Drude-Lorentz fits of the materials' equilibrium reflectance, we show that these are well-represented by a sudden change of the electronic properties (increase of screening or reduction of the plasma frequency) followed by an increase of the Drude scattering rate. This directly connects the transient data to a physical picture in which carriers, after excitation into the conduction band, return to the valence band by sharing excess energy with the phonon bath, resulting in a hot lattice that relaxes through slow diffusive processes. The emerging picture reveals that the sudden electronic reorganization instantaneously modifies the materials' electronic properties on a time scale not compatible with electron-phonon thermalization.

8.
J Am Chem Soc ; 142(13): 6350-6359, 2020 04 01.
Artigo em Inglês | MEDLINE | ID: mdl-32142261

RESUMO

Principles that predict reactions or properties of materials define the discipline of chemistry. In this work, we derive chemical rules, based on atomic distances and chemical bond character, which predict topological materials in compounds that feature the structural motif of a square-net. Using these rules, we identify over 300 potential new topological materials. We show that simple chemical heuristics can be a powerful tool to characterize topological matter. In contrast to previous database-driven materials' categorization, our approach allows us to identify candidates that are alloys, solid-solutions, or compounds with statistical vacancies. While previous material searches relied on density functional theory, our approach is not limited by this method and could also be used to discover magnetic and statistically disordered topological semimetals.

9.
Sci Adv ; 6(6): eaay6407, 2020 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-32083184

RESUMO

Van der Waals (vdW) materials with magnetic order have been heavily pursued for fundamental physics as well as for device design. Despite the rapid advances, so far, they are mainly insulating or semiconducting, and none of them has a high electronic mobility-a property that is rare in layered vdW materials in general. The realization of a high-mobility vdW material that also exhibits magnetic order would open the possibility for novel magnetic twistronic or spintronic devices. Here, we report very high carrier mobility in the layered vdW antiferromagnet GdTe3. The electron mobility is beyond 60,000 cm2 V-1 s-1, which is the highest among all known layered magnetic materials, to the best of our knowledge. Among all known vdW materials, the mobility of bulk GdTe3 is comparable to that of black phosphorus. By mechanical exfoliation, we further demonstrate that GdTe3 can be exfoliated to ultrathin flakes of three monolayers.

10.
Inorg Chem ; 59(2): 1176-1182, 2020 Jan 21.
Artigo em Inglês | MEDLINE | ID: mdl-31880436

RESUMO

The development of novel, intrinsic two-dimensional (2D) antiferromagnets presents the opportunity to vastly improve the efficiency of spintronic devices and sensors. The strong intrinsic antiferromagnetism and van der Waals layered structure exhibited by the bulk transition-metal oxychlorides provide a convenient system for the synthesis of such materials. In this work, we report the exfoliation of bulk FeOCl into and subsequent characterization of intrinsically antiferromagnetic thin-layer FeOCl nanosheets. The magnetic properties of bulk FeOCl, its lithium intercalate, and its nanosheet pellet are measured to determine the evolution of magnetic properties from the three-dimensional to the quasi-two-dimensional system. This work establishes FeOCl and isostructural compounds as a source for the development of two-dimensional intrinsic antiferromagnets.

11.
J Am Chem Soc ; 141(39): 15634-15640, 2019 Oct 02.
Artigo em Inglês | MEDLINE | ID: mdl-31479248

RESUMO

We report a new HxCrS2-based crystalline/amorphous layered material synthesized by soft chemical methods. We study the structural nature and composition of this material with atomic resolution scanning transmission electron microscopy (STEM), revealing a complex structure consisting of alternating layers of amorphous and crystalline lamellae. Furthermore, the magnetic properties show evidence for increased magnetic frustration compared to the parent compound NaCrS2. Finally, we show that this material can be exfoliated, thus providing a facile synthesis method for chromium-sulfide-based ultrathin layers. The material reported herein can not only be a source of new thin TMD-related sheets for potential application in catalysis but also be of interest for realizing new 2D magnetic materials.

12.
J Phys Chem Lett ; 9(23): 6833-6840, 2018 Dec 06.
Artigo em Inglês | MEDLINE | ID: mdl-30433790

RESUMO

Transition-metal chalcogenides are a promising family of materials for applications as photocathodes in photoelectrochemical (PEC) H2 generation. A long-standing challenge for chalcopyrite semiconductors is characterizing their electronic structure, both experimentally and theoretically, because of their relatively high-energy band gaps and spin-orbit coupling (SOC), respectively. In this work, we present single crystals of CuInTe2, whose relatively small optically measured band gap of 0.9 ± 0.03 eV enables electronic structure characterization by angle-resolved photoelectron spectroscopy (ARPES) in conjunction with first-principles calculations incorporating SOC. ARPES measurements reveal bands that are steeply dispersed in energy with a band velocity of 2.5-5.4 × 105 m/s, almost 50% of the extremely conductive material graphene. Additionally, CuInTe2 single crystals are fabricated into electrodes to experimentally determine the valence band edge energy and confirm the thermodynamic suitability of CuInTe2 for water redox chemistry. The electronic structure characterization and band edge position presented in this work provide kinetic and thermodynamic factors that support CuInTe2 as a strong candidate for water reduction.

13.
ChemSusChem ; 11(18): 3150-3156, 2018 Sep 21.
Artigo em Inglês | MEDLINE | ID: mdl-30047577

RESUMO

High-performance catalysts for the oxygen-evolution reaction in water electrolysis are usually based on expensive and rare elements. Herein, mixed-metal borides are shown to be competitive with established electrocatalysts like noble metal oxides and other transition-metal(oxide)-based catalysts. Iron incorporation into nanoscale dicobalt boride results in excellent activity and stability in alkaline solutions. (Co0.7 Fe0.3 )2 B shows an overpotential of η=0.33 V (1.56 V vs. RHE) at 10 mA cm-2 in 1 m KOH with a very low onset potential of ≈1.5 V vs. RHE, comparable to the performance of IrO2 and RuO2 . XPS shows that the original catalyst is modified under the reaction conditions and indicates that CoOOH and Co(OH)2 are formed as active surface species, whereas the Fe remains in the catalyst, contributing to an improved catalyst performance. The nanoscale borides are obtained by a one-step solution synthesis, calcined, and characterized by XRD, energy-dispersive X-ray spectroscopy, and SEM. Single crystals of (Co1-x Fex )2 B grown under chemical transport conditions were used for an unambiguous specification of the nanostructured particles by relating the cobalt/iron ratio to the lattice parameters.

14.
ACS Appl Mater Interfaces ; 9(30): 25184-25193, 2017 Aug 02.
Artigo em Inglês | MEDLINE | ID: mdl-28653526

RESUMO

In this work, we present a comprehensive study on the role of metal species in MOF-based Me-N-C (mono- and bimetallic) catalysts for the hydrogen evolution reaction (HER). The catalysts are investigated with respect to HER activity and stability in alkaline electrolyte. On the basis of the structural analysis by X-ray diffraction, X-ray-induced photoelectron spectroscopy, and transmission electron microscopy, it is concluded that MeN4 sites seem to dominate the HER activity of these catalysts. There is a strong relation between the amount of MeN4 sites that are formed and the energy of formation related to these sites integrated at the edge of a graphene layer, as obtained from density functional theory (DFT) calculations. Our results show, for the first time, that the combination of two metals (Co and Mo) in a bimetallic (Co,Mo)-N-C catalyst allows hydrogen production with a significantly improved overpotential in comparison to its monometallic counterparts and other Me-N-C catalysts. By the combination of experimental results with DFT calculations, we show that the origin of the enhanced performance of our (Co,Mo)-N-C catalyst seems to be provided by an improved hydrogen binding energy on one MeN4 site because of the presence of a second MeN4 site in its close vicinity, as investigated in detail for our most active (Co,Mo)-N-C catalyst. The outstanding stability and good activity make especially the bimetallic Me-N-C catalysts interesting candidates for solar fuel applications.

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