Magnetic van der Waals (vdW) materials have been heavily pursued for fundamental physics as well as for device design. Despite the rapid advances, so far magnetic vdW materials are mainly insulating or semiconducting, and none of them possesses a high electronic mobilitya property that is rare in layered vdW materials in general. The realization of a magnetic high-mobility vdW material would open the possibility for novel magnetic twistronic or spintronic devices.Here we report very high carrier mobility in the layered vdW antiferromagnet GdTe 3. The electron mobility is beyond 60,000 cm 2 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 GdTe 3 is comparable to that of black phosphorus, and is only surpassed by graphite. By mechanical exfoliation, we further demonstrate that GdTe 3 can be exfoliated to ultrathin flakes of three monolayers, and that the magnetic order and relatively high mobility is retained in ~20-nm-thin flakes.VdW materials are the parent compounds of two-dimensional (2D) materials, which are currently actively studied for new device fabrications (1) involving the creation of heterostructure stacks (2) or twisted bilayers (3) of 2D building blocks. Magnetic vdW materials have recently led to the observation of intrinsic magnetic order in atomically thin layers (4-12), which was followed by exciting discoveries of giant tunneling magnetoresistance (13-16) and tunable magnetism (17)(18)(19) in such materials.So far, the known magnetic vdW materials (ferro-or antiferromagnetic) that can be exfoliated are limited to a few examples, such as: CrI3 (4), Cr2Ge2Te6 (5), FePS3 (6,7), CrBr3 (8, 9), CrCl3 (10-12), Fe3GeTe2 (17,20), and RuCl3 (21-23). Out of these, only Fe3GeTe2 is a metallic ferromagnet and there is no known vdW-based 2D antiferromagnetic metal. Moreover, no evidence of high carrier mobilities has been reported in any of these exfoliated thin materials or even in their bulk vdW crystals. In general, high mobility is limited to very few vdW materials, such as graphite (24) and black phosphorus (25). A material with high electronic mobility and a corresponding high mean-free-path (MFP), might be critical for potential magnetic "twistronic" devices (3) where a large MFP could enable interesting phenomena in a Moiré-supercell induced flat band. In addition, conducting antiferromagnetic materials are the prime candidates for high-speed antiferromagnetic spintronic devices (26). Here we report the realization of a very high electronic mobility in a vdW layered antiferromagnet, GdTe3, both in bulk and exfoliated thin flakes.We chose to study GdTe3, since rare-earth tritellurides (RTe3, R = La-Nd, Sm, and Gd-Tm) are structurally related to topological semimetal ZrSiS (27,28), while being known to exhibit an incommensurate charge density wave (CDW) (29-31), rich magnetic properties (32), and becoming superconducting under high-pressure (R = Gd, Tb and Dy) (33). Combined, these properties ...
High-performance piezoelectrics are lead-based solid solutions that exhibit a so-called morphotropic phase boundary, which separates two competing phases as a function of chemical composition; as a consequence, an intermediate low-symmetry phase with a strong piezoelectric effect arises. In search for environmentally sustainable lead-free alternatives that exhibit analogous characteristics, we use a network of competing domains to create similar conditions across thermal inter-ferroelectric transitions in simple, lead-free ferroelectrics such as BaTiO 3 and KNbO 3 . Here we report the experimental observation of thermotropic phase boundaries in these classic ferroelectrics, through direct imaging of low-symmetry intermediate phases that exhibit large enhancements in the existing nonlinear optical and piezoelectric property coefficients. Furthermore, the symmetry lowering in these phases allows for new property coefficients that exceed all the existing coefficients in both parent phases. Discovering the thermotropic nature of thermal phase transitions in simple ferroelectrics thus presents unique opportunities for the design of 'green' high-performance materials.
Many materials crystallize in structure types that feature a square-net of atoms. While these compounds can exhibit many different properties, some members of this family are topological materials. Within the square-net-based topological materials, the observed properties are rich, ranging for example from nodal-line semimetals to a bulk halfinteger quantum Hall effect. Hence, the potential for guided design of topological properties is enormous. Here we provide an overview of the crystallographic and electronic properties of these phases and show how they are linked, with the goal of understanding which square-net materials can be topological, and to predict additional examples. We close the review by discussing the experimentally observed electronic properties in this family. 2 Schoop et al. 6 Schoop et al.
Oxynitrides have been explored extensively in the past decade because of their interesting properties, such as visible-light absorption, photocatalytic activity and high dielectric permittivity. Their synthesis typically requires high-temperature NH3 treatment (800-1,300 °C) of precursors, such as oxides, but the highly reducing conditions and the low mobility of N(3-) species in the lattice place significant constraints on the composition and structure-and hence the properties-of the resulting oxynitrides. Here we show a topochemical route that enables the preparation of an oxynitride at low temperatures (<500 °C), using a perovskite oxyhydride as a host. The lability of H(-) in BaTiO3-xHx (x ≤ 0.6) allows H(-)/N(3-) exchange to occur, and yields a room-temperature ferroelectric BaTiO3-xN2x/3. This anion exchange is accompanied by a metal-to-insulator crossover via mixed O-H-N intermediates. These findings suggest that this 'labile hydride' strategy can be used to explore various oxynitrides, and perhaps other mixed anionic compounds.
Polar domains arise in insulating ferroelectrics when free carriers are unable to fully screen surface-bound charges. Recently discovered binary and ternary polar metals exhibit broken inversion symmetry coexisting with free electrons that might be expected to suppress the electrostatic driving force for domain formation. Contrary to this expectation, we report the first direct observation of polar domains in single crystals of the polar metal CaRuO. By a combination of mesoscale optical second-harmonic imaging and atomic-resolution scanning transmission electron microscopy, the polar domains are found to possess a quasi-two-dimensional slab geometry with a lateral size of ∼100 μm and thickness of ∼10 nm. Electronic structure calculations show that the coexistence of electronic and parity-lifting orders arise from anharmonic lattice interactions, which support 90° and 180° polar domains in a metal. Using in situ transmission electron microscopy, we also demonstrate a strain-tuning route to achieve ferroelastic switching of polar metal domains.
We report a new H x CrS 2 -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 NaCrS 2 . 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.
The interplay between topology and correlations can generate a variety of unusual quantum phases, many of which remain to be explored. Recent advances have identified monolayer WTe2 as a promising material for exploring such interplay in a highly tunable fashion. The ground state of this two-dimensional (2D) crystal can be electrostatically tuned from a quantum spin Hall insulator (QSHI) to a superconductor. However, much remains unknown about the nature of these ground states, including the gap-opening mechanism of the insulating state. Here we report systematic studies of the insulating phase in WTe2 monolayer and uncover evidence supporting that the QSHI is also an excitonic insulator (EI). An EI, arising from the spontaneous formation of electron-hole bound states (excitons), is a largely unexplored quantum phase to date, especially when it is topological. Our experiments on high-quality transport devices reveal the presence of an intrinsic insulating state at the charge neutrality point (CNP) in clean samples. The state exhibits both a strong sensitivity to the electric displacement field and a Hall anomaly that are consistent with the excitonic pairing. We further confirm the correlated nature of this charge-neutral insulator by tunneling spectroscopy. Our results support the existence of an EI phase in the clean limit and rule out alternative scenarios of a band insulator or a localized insulator. These observations lay the foundation for understanding a new class of correlated insulators with nontrivial topology and identify monolayer WTe2 as a promising candidate for exploring quantum phases of ground-state excitons.
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