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Register a new userEmergence of a Metal-Insulator Transition and High Temperature Charge Density Waves in VSe2 at the Monolayer Limit
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Emergent phenomena driven by electronic reconstructions in oxide heterostructures have been intensively discussed. However, the role of these phenomena in shaping the electronic properties in van der Waals heterointerfaces has hitherto not been established. By reducing the material thickness and forming a heterointerface, we find two types of charge-ordering transitions in monolayer VSe2 on graphene substrates. Angle-resolved photoemission spectroscopy (ARPES) uncovers that Fermi-surface nesting becomes perfect in ML VSe2. Renormalization group analysis confirms that imperfect nesting in three dimensions universally flows into perfect nesting in two dimensions. As a result, the charge density wave transition temperature is dramatically enhanced to a value of 350 K compared to the 105 K in bulk VSe2. More interestingly, ARPES and scanning tunneling microscopy measurements confirm an unexpected metal-insulator transition at 135 K, driven by lattice distortions. The heterointerface plays an important role in driving this novel metal-insulator transition in the family of monolayered transition metal dichalcogenides.
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The correlation-driven Mott transition is commonly characterized by a drop in resistivity across the insulator-metal phase boundary; yet, the complex permittivity provides a deeper insight into the microscopic nature. We investigate the frequency- and temperature-dependent dielectric response of the Mott insulator $kappa$-(BEDT-TTF)$_{2}$-Cu$_2$(CN)$_3$ when tuning from a quantum spin liquid into the Fermi-liquid state by applying external pressure and chemical substitution of the donor molecules. At low temperatures the coexistence region at the first-order transition leads to a strong enhancement of the quasi-static dielectric constant $epsilon_1$ when the effective correlations are tuned through the critical value. Several dynamical regimes are identified around the Mott point and vividly mapped through pronounced permittivity crossovers. All experimental trends are captured by dynamical mean-field theory of the single-band Hubbard model supplemented by percolation theory.
Vanadium disulfide (VS_{2}) attracts elevated interests for its charge-density wave (CDW) phase transition, ferromagnetism, and catalytic reactivity, but the electronic structure of monolayer has not been well understood yet. Here we report synthesis of epitaxial 1T VS_{2} monolayer on bilayer graphene grown by molecular-beam epitaxy (MBE). Angle-resolved photoemission spectroscopy (ARPES) measurements reveal that Fermi surface with six elliptical pockets centered at the M points shows gap opening at low temperature. Temperature-dependence of the gap size suggests existence of CDW phase transition above room temperature. Our observations provide important evidence to understand the strongly correlated electron physics and the related surface catalytic properties in two-dimensional transition-metal dichalcogenides (TMDCs).
We report pressure evolution of charge density wave (CDW) order and emergence of superconductivity (SC) in 1T-VSe2 single crystal by studying resistance and magnetoresistance behavior under high pressure. With increasing quasi-hydrostatic pressure the CDW order enhances with increase ofthe ordering temperature up to 240K at 12 GPa. Upon further increase of pressure, the resistance anomaly due to CDW order gets suppressed drastically and superconductivity emerges at ~15 GPa, with the onset critical temperature (Tc) ~ 4K. The pressure dependence of Tc is found negligible, different from the significant increase or a dome-shape seen in iso-structural layered diselenide superconductors. The high pressure magnetoresistance and Hall measurements suggest successive electronic structural changes with Fermi surface modifications at 6 GPa and 12GPa. From the observed negative magnetoresistance in this pressure range and absence of coexisting CDW and SC phases, we propose that intra-layer spin-fluctuation can play a role in the emergence of superconductivity in the high pressure phase.
Low-dimensional electron systems, as realized naturally in graphene or created artificially at the interfaces of heterostructures, exhibit a variety of fascinating quantum phenomena with great prospects for future applications. Once electrons are confined to low dimensions, they also tend to spontaneously break the symmetry of the underlying nuclear lattice by forming so-called density waves; a state of matter that currently attracts enormous attention because of its relation to various unconventional electronic properties. In this study we reveal a remarkable and surprising feature of charge density waves (CDWs), namely their intimate relation to orbital order. For the prototypical material 1T-TaS2 we not only show that the CDW within the two-dimensional TaS2-layers involves previously unidentified orbital textures of great complexity. We also demonstrate that two metastable stackings of the orbitally ordered layers allow to manipulate salient features of the electronic structure. Indeed, these orbital effects enable to switch the properties of 1T-TaS2 nanostructures from metallic to semiconducting with technologically pertinent gaps of the order of 200 meV. This new type of orbitronics is especially relevant for the ongoing development of novel, miniaturized and ultra-fast devices based on layered transition metal dichalcogenides.
First-order phase transitions in solids are notoriously challenging to study. The combination of change in unit cell shape, long range of elastic distortion, and flow of latent heat leads to large energy barriers resulting in domain structure, hysteresis, and cracking. The situation is still worse near a triple point where more than two phases are involved. The famous metal-insulator transition (MIT) in vanadium dioxide, a popular candidate for ultrafast optical and electrical switching applications, is a case in point. Even though VO2 is one of the simplest strongly correlated materials, experimental difficulties posed by the first-order nature of the MIT as well as the involvement of at least two competing insulating phases have led to persistent controversy about its nature. Here, we show that studying single-crystal VO2 nanobeams in a purpose-built nanomechanical strain apparatus allows investigation of this prototypical phase transition with unprecedented control and precision. Our results include the striking finding that the triple point of the metallic and two insulating phases is at the transition temperature, T_tr = T_c, which we determine to be 65.0 +- 0.1 C. The findings have profound implications for the mechanism of the MIT in VO2, but in addition they demonstrate the importance of such an approach for mastering phase transitions in many other strongly correlated materials, such as manganites and iron-based superconductors.
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