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 ...
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.
The interaction between electrons in graphene under high magnetic fields drives the formation of a rich set of quantum Hall ferromagnetic (QHFM) phases with broken spin or valley symmetry. Visualizing atomic-scale electronic wave functions with scanning tunneling spectroscopy (STS), we resolved microscopic signatures of valley ordering in QHFM phases and spectral features of fractional quantum Hall phases of graphene. At charge neutrality, we observed a field-tuned continuous quantum phase transition from a valley-polarized state to an intervalley coherent state, with a Kekulé distortion of its electronic density. Mapping the valley texture extracted from STS measurements of the Kekulé phase, we could visualize valley skyrmion excitations localized near charged defects. Our techniques can be applied to examine valley-ordered phases and their topological excitations in a wide range of materials.
Moiré superlattices created by the twisted stacking of two-dimensional crystals can host electronic bands with flat energy dispersion in which enhanced interactions promote correlated electron states. The twisted double bilayer graphene (TDBG), where two Bernal bilayer graphene are stacked with a twist angle, is such a moiré system with tunable flat bands. Here, we use gate-tuned scanning tunneling spectroscopy to directly demonstrate the tunability of the band structure of TDBG with an electric field and to show spectroscopic signatures of electronic correlations and topology for its flat band. Our spectroscopic experiments are in agreement with a continuum model of TDBG band structure and reveal signatures of a correlated insulator gap at partial filling of its isolated flat band. The topological properties of this flat band are probed with the application of a magnetic field, which leads to valley polarization and the splitting of Chern bands with a large effective g-factor.
Supramolecular chemistry protocols applied on surfaces offer compelling avenues for atomic-scale control over organic-inorganic interface structures. In this approach, adsorbate-surface interactions and two-dimensional confinement can lead to morphologies and properties that differ dramatically from those achieved via conventional synthetic approaches. Here, we describe the bottom-up, on-surface synthesis of one-dimensional coordination nanostructures based on an iron (Fe)-terpyridine (tpy) interaction borrowed from functional metal-organic complexes used in photovoltaic and catalytic applications. Thermally activated diffusion of sequentially deposited ligands and metal atoms and intraligand conformational changes lead to Fe-tpy coordination and formation of these nanochains. We used low-temperature scanning tunneling microscopy and density functional theory to elucidate the atomic-scale morphology of the system, suggesting a linear tri-Fe linkage between facing, coplanar tpy groups. Scanning tunneling spectroscopy reveals the highest occupied orbitals, with dominant contributions from states located at the Fe node, and ligand states that mostly contribute to the lowest unoccupied orbitals. This electronic structure yields potential for hosting photoinduced metal-to-ligand charge transfer in the visible/near-infrared. The formation of this unusual tpy/tri-Fe/tpy coordination motif has not been observed for wet chemistry synthetic methods and is mediated by the bottom-up on-surface approach used here, offering pathways to engineer the optoelectronic properties and reactivity of metal-organic nanostructures.
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