Materials research has driven the development of modern nano-electronic devices. In particular, research in magnetic thin films has revolutionized the development of spintronic devices1,2 because identifying new magnetic materials is key to better device performance and design. Van der Waals crystals retain their chemical stability and structural integrity down to the monolayer and, being atomically thin, are readily tuned by various kinds of gate modulation3,4. Recent experiments have demonstrated that it is possible to obtain two-dimensional ferromagnetic order in insulating Cr2Ge2Te6 (ref. 5) and CrI3 (ref. 6) at low temperatures. Here we develop a device fabrication technique and isolate monolayers from the layered metallic magnet Fe3GeTe2 to study magnetotransport. We find that the itinerant ferromagnetism persists in Fe3GeTe2 down to the monolayer with an out-of-plane magnetocrystalline anisotropy. The ferromagnetic transition temperature, Tc, is suppressed relative to the bulk Tc of 205 kelvin in pristine Fe3GeTe2 thin flakes. An ionic gate, however, raises Tc to room temperature, much higher than the bulk Tc. The gate-tunable room-temperature ferromagnetism in two-dimensional Fe3GeTe2 opens up opportunities for potential voltage-controlled magnetoelectronics7-11 based on atomically thin van der Waals crystals.

Gate-tunable room-temperature ferromagnetism in two-dimensional Fe 3 GeTe 2 .

Gate-tunable Room-temperature Ferromagnetism in Two-dimensional Fe 3 GeTe 2

https://absimage.aps.org/image/MAR14/MWS_MAR14-2014-020819.pdf

Van der Waals heterostructures

Monolayers of transition-metal dichalcogenides (TMDs) exhibit numerous crystal phases with distinct structures, symmetries and physical properties. Exploring the physics of transitions between these different structural phases in two dimensions may provide a means of switching material properties, with implications for potential applications. Structural phase transitions in TMDs have so far been induced by thermal or chemical means; purely electrostatic control over crystal phases through electrostatic doping was recently proposed as a theoretical possibility, but has not yet been realized. Here we report the experimental demonstration of an electrostatic-doping-driven phase transition between the hexagonal and monoclinic phases of monolayer molybdenum ditelluride (MoTe2). We find that the phase transition shows a hysteretic loop in Raman spectra, and can be reversed by increasing or decreasing the gate voltage. We also combine second-harmonic generation spectroscopy with polarization-resolved Raman spectroscopy to show that the induced monoclinic phase preserves the crystal orientation of the original hexagonal phase. Moreover, this structural phase transition occurs simultaneously across the whole sample. This electrostatic-doping control of structural phase transition opens up new possibilities for developing phase-change devices based on atomically thin membranes.

Structural phase transition in monolayer MoTe 2 driven by electrostatic doping

The ability to tune material properties using gating by electric fields is at the heart of modern electronic technology. It is also a driving force behind recent advances in two-dimensional systems, such as the observation of gate electric-field-induced superconductivity and metal-insulator transitions. Here, we describe an ionic field-effect transistor (termed an iFET), in which gate-controlled Li ion intercalation modulates the material properties of layered crystals of 1T-TaS2. The strong charge doping induced by the tunable ion intercalation alters the energetics of various charge-ordered states in 1T-TaS2 and produces a series of phase transitions in thin-flake samples with reduced dimensionality. We find that the charge-density wave states in 1T-TaS2 collapse in the two-dimensional limit at critical thicknesses. Meanwhile, at low temperatures, the ionic gating induces multiple phase transitions from Mott-insulator to metal in 1T-TaS2 thin flakes, with five orders of magnitude modulation in resistance, and superconductivity emerges in a textured charge-density wave state induced by ionic gating. Our method of gate-controlled intercalation opens up possibilities in searching for novel states of matter in the extreme charge-carrier-concentration limit.

http://absimage.aps.org/image/MAR15/MWS_MAR15-2014-020259.pdf

Gate-tunable phase transitions in thin flakes of 1T-TaS$_{2}$

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-TaS2 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.

https://www.pnas.org/content/pnas/112/49/15054.full.pdf

Yu Liu

Papers

Structure and control of charge density waves in two-dimensional 1T-TaS2