The layered transition metal dichalcogenides host a rich collection of charge density wave phases in which both the conduction electrons and the atomic structure display translational symmetry breaking. Manipulating these complex states by purely electronic methods has been a long-sought scientific and technological goal. Here, we show how this can be achieved in 1T-TaS 2 in the 2D limit. We first demonstrate that the intrinsic properties of atomically thin flakes are preserved by encapsulation with hexagonal boron nitride in inert atmosphere. We use this facile assembly method together with transmission electron microscopy and transport measurements to probe the nature of the 2D state and show that its conductance is dominated by discommensurations. The discommensuration structure can be precisely tuned in few-layer samples by an in-plane electric current, allowing continuous electrical control over the discommensuration-melting transition in 2D.two-dimensional materials | strongly correlated systems | charge density waves L ayered 1T-TaS 2 exhibits a number of unique structural and electronic phases. At low temperature and ambient pressure, the ground state is a commensurate (C) charge density wave (CDW). On heating, it undergoes a sequence of first-order phase transitions to a nearly commensurate (NC) CDW at 225 K, to an incommensurate (IC) CDW at 355 K, and finally to a metallic phase at 545 K. Each transition involves both conduction electron and lattice degrees of freedom-large changes in electronic transport properties occur, concomitant with structural changes to the crystal. By either chemical doping or applying high pressures, it is possible to suppress the CDWs and induce superconductivity (1-3). For device applications, it is desirable to control these phases by electrical means, but this capability is difficult to achieve in bulk crystals due to the high conduction electron density. Recent efforts to produce thin samples by mechanical exfoliation provide a new avenue for manipulating the CDWs in 1T-TaS 2 (4-8). These studies have demonstrated the suppression of CDW phase transitions using polar electrolytes, as well as resistive switching between the different phases. As the material approaches the 2D limit, however, significant changes have been observed in the transport properties (4,5,8). However, the microscopic nature of the 2D state remains unclear. In this work, we use transmission electron microscopy (TEM) together with transport measurements to develop a systematic understanding of the CDW phases and phase transitions in ultrathin 1T-TaS 2 . We find that charge ordering disappears in flakes with few atomic layers due to surface oxidation. When samples are instead environmentally protected, the CDWs persist and their transitions can be carefully tuned by electric currents.Both the atomic and CDW structure of 1T-TaS 2 can be visualized in reciprocal space by TEM electron diffraction (9, 10). In Fig. 1A, we show diffraction images taken from a bulk-like, 50-nm-thick crystal at low and room tem...
In this work, we demonstrate abrupt, reversible switching of resistance in 1T-TaS2 using dc and pulsed sources, corresponding to an insulator-metal transition between the insulating Mott and equilibrium metallic states. This transition occurs at a constant critical resistivity of 7 mohm-cm regardless of temperature or bias conditions and the transition time is significantly smaller than abrupt transitions by avalanche breakdown in other small gap Mott insulating materials. Furthermore, this critical resistivity corresponds to a carrier density of 4.5 × 10(19) cm(-3), which compares well with the critical carrier density for the commensurate to nearly commensurate charge density wave transition. These results suggest that the transition is facilitated by a carrier driven collapse of the Mott gap in 1T-TaS2, which results in fast (3 ns) switching.
Two-dimensional (2D) van der Waals (vdW) materials show a range of profound physical properties that can be tailored through their incorporation in heterostructures and manipulated with external forces 1-5 . The recent discovery of long-range ferromagnetic order down to atomic layers provides an additional degree of freedom in engineering 2D materials and their heterostructure devices for spintronics, valleytronics and magnetic tunnel junction switches 6-9 . Here, using direct imaging by cryo-Lorentz transmission electron microscopy we show that topologically nontrivial magnetic-spin states, skyrmionic bubbles, can be realized in exfoliated insulating 2D vdW Cr2Ge2Te6. Due to the competition between dipolar interactions and uniaxial magnetic anisotropy, hexagonally-packed nanoscale bubble lattices emerge by field cooling with magnetic field applied along the out-of-plane direction. Despite a range of topological spin textures in stripe domains arising due to pair formation and annihilation of Bloch lines, bubble lattices with single chirality are prevalent. Our observation of topologically-nontrivial homochiral skyrmionic bubbles in exfoliated vdW materials provides a new avenue for novel quantum states in atomically-thin insulators for magneto-electronic and quantum devices.
Layered 1T-TaS2–xSex (0≤x≤2) single crystals have been systematically fabricated by a chemical vapor transport technique. Surprisingly, the superconductivity is induced by the Se doping. We demonstrate the appearance of a series of electronic states: the Mott phase melts into a nearly commensurate charge-density-wave (CDW) phase, superconductivity in a wide x range develops within the nearly commensurate CDW state, and finally commensurate CDW phase reproduces for heavy Se content. The rich phase diagram provides an ideal platform to investigate the interplay between electron correlation, CDW, and superconductivity, as well as the potential applications in electronic devices.
Identifying material parameters affecting properties of ferromagnets is key to optimize materials better suited for spintronics. Magnetic anisotropy is of particular importance in van der Waals magnets, since it not only influences magnetic and spin transport properties, but also is essential to stabilizing magnetic order in the two dimensional limit. Here, we report that a hole doping effectively modulates the magnetic anisotropy of a van der Waals ferromagnet, and explore the physical origin of this effect. Fe3-xGeTe2 nanoflakes show a significant suppression of the magnetic anisotropy with hole doping. Electronic structure measurements and calculations reveal that the chemical potential shift associated with hole doping is responsible for the reduced magnetic anisotropy by decreasing the energy gain from the spin-orbit induced band splitting. Our findings provide an understanding of the intricate connection between electronic structures and magnetic properties in two-dimensional magnets and propose a method to engineer magnetic properties through doping.
We report on the strain-induced switch between ferromagnetic (FM) and antiferromagnetic (AFM) orderings in 1T -CrX2 (X = Se, Te) monolayers based on the first-principles calculations. The CrSe2 and CrTe2 monolayers without strains are found to be AFM and FM, respectively. Under the biaxial tensile strain, the CrSe2 monolayer tends to be FM when the strain is larger than 2%. The FM state is further stabilized when the strain is increased. Moreover, the CrSe2 monolayer changes to be halfmetallic when the tensile strain is larger than 10%. While for the CrTe2 monolayer, the critical strain at which the transition between the FM and AFM states occurs is compressive, of −1%. Relatively small tensile strains of 4% and 2%, respectively, can enhance the Curie temperature of CrSe2 and CrTe2 monolayers above the room temperature. The strain-induced switch between the FM and AFM states in CrSe2 (CrTe2) monolayer can be understood by the competition between the AFM Cr-Cr direct exchange interaction and FM Cr-Se(Te)-Cr superexchange interaction. The tunable and attractive magnetic and electronic properties controlled by the flexible strain are desirable for the future nanoelectronic applications.
CrI3 is a promising candidate for the van der Waals bonded ferromagnetic devices since its ferromagnetism can be maintained upon exfoliating of bulk crystals down to single layer. In this work we studied critical properties of bulk CrI3 single crystals around the paramagnetic to ferromagnetic phase transition. Critical exponents β = 0.260(4) with a critical temperature Tc = 60.05(13) K and γ = 1.136(6) with Tc = 60.43(4) K are obtained by the Kouvel-Fisher method, whereas δ = 5.32(2) is obtained by a critical isotherm analysis at Tc = 60 K. The critical exponents determined in bulk CrI3 single crystals suggest a three-dimensional long-range magnetic coupling with the exchange distance decaying as J(r) ≈ r −4.69 .
The electronic structure of WTe2 bulk and layers are investigated by using the first principles calculations. The perfect electron-hole (n-p) charge compensation and high carrier mobilities are found in WTe2 bulk, which may result in the large and non-saturating magnetoresistance (MR) observed very recently in the experiment [Ali et al., Nature 514, 205 (2014)]. The monolayer and bilayer of WTe2 preserve the semimetallic property, with the equal hole and electron carrier concentrations. Moreover, the very high carrier mobilities are also found in WTe2 monolayer, indicating that the WTe2 monolayer would have the same extraordinary MR effect as the bulk, which could have promising applications in nanostructured magnetic devices.
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