Graphene produced by chemical vapor deposition (CVD) is polycrystalline, and scattering of charge carriers at grain boundaries (GBs) could degrade its performance relative to exfoliated, single-crystal graphene. However, the electrical properties of GBs have so far been addressed indirectly without simultaneous knowledge of their locations and structures. We present electrical measurements on individual GBs in CVD graphene first imaged by transmission electron microscopy. Unexpectedly, the electrical conductance improves by one order of magnitude for GBs with better interdomain connectivity. Our study suggests that polycrystalline graphene with good stitching may allow for uniformly high electrical performance rivaling that of exfoliated samples, which we demonstrate using optimized growth conditions and device geometry.
2 Control of the interlayer twist angle in two-dimensional (2D) van der Waals (vdW)heterostructures enables one to engineer a quasiperiodic moiré superlattice of tunable length scale 1-7 . In twisted bilayer graphene (TBG), the simple moiré superlattice band description suggests that the electronic band width can be tuned to be comparable to the vdW interlayer interaction at a 'magic angle' 8 , exhibiting strongly correlated behavior. However, the vdW interlayer interaction can also cause significant structural reconstruction at the interface by favoring interlayer commensurability, which competes with the intralayer lattice distortion 9-15 . Here we report the atomic scale reconstruction in TBG and its effect on the electronic structure. We find a gradual transition from incommensurate moiré structure to an array of commensurate domain structures as we decrease the twist angle across the characteristic crossover angle, θc ~1°. In the twist regime smaller than θc where the atomic and electronic reconstruction become significant, a simple moiré band description breaks down. Upon applying a transverse electric field, we observe electronic transport along the network of onedimensional (1D) topological channels that surround the alternating triangular gapped domains, providing a new pathway to engineer the system with continuous tunability.In the absence of atomic scale reconstruction, a small rigid rotation of the vdW layers relative to each other results in a moiré pattern, whose long wavelength periodicity is determined by the twist angle. For unreconstructed TBG, atomic registry varies continuously across the moiré period between three distinct types of symmetric stacking configurations: energetically favorable AB and BA Bernal stacking and unfavorable AA stacking (Fig. 1a). This quasiperiodic moiré superlattice, associated with the incommensurability of the twisted layers, modifies the band structure significantly. In the small twist regime, low-energy flat bands appear at a series of magic angles ( ≤ 1.1°) where the diverging density of states (DOS) and vanishing Fermi velocity, associated with strong electronic correlation, are predicted 8 . The recent experiment demonstrated the presence of the first magic angle near ~1.1° where Mott insulator and unconventional superconductivity were observed 6,7 . The TBG moiré band calculation, however, assumes a rigid rotation of layers ignoring atomic scale reconstruction. Despite the weak nature of vdW interaction and the absence of dangling bonds, recent experimental works on similar material systems suggestthere is substantial lattice reconstruction at vdW interfaces, especially at small twist angle close to global commensuration between two adjacent layers 9,10 . Atomic scale reconstruction at vdW B 92, 155438 (2015).
Bilayer graphene has been a subject of intense study in recent years. The interlayer registry between the layers can have dramatic effects on the electronic properties: for example, in the presence of a perpendicular electric field, a band gap appears in the electronic spectrum of so-called Bernal-stacked graphene [Oostinga JB, et al. (2007) Nature Materials 7:151-157]. This band gap is intimately tied to a structural spontaneous symmetry breaking in bilayer graphene, where one of the graphene layers shifts by an atomic spacing with respect to the other. This shift can happen in multiple directions, resulting in multiple stacking domains with soliton-like structural boundaries between them. Theorists have recently proposed that novel electronic states exist at these boundaries [Vaezi A, et al. (2013) arXiv:1301.1690Zhang F, et al. (2013) arXiv:1301], but very little is known about their structural properties. Here we use electron microscopy to measure with nanoscale and atomic resolution the widths, motion, and topological structure of soliton boundaries and related topological defects in bilayer graphene. We find that each soliton consists of an atomic-scale registry shift between the two graphene layers occurring over 6-11 nm. We infer the minimal energy barrier to interlayer translation and observe soliton motion during in situ heating above 1,000°C. The abundance of these structures across a variety of samples, as well as their unusual properties, suggests that they will have substantial effects on the electronic and mechanical properties of bilayer graphene.domain wall | TEM | stacking faults | STEM S pontaneous symmetry breaking, where the ground state of a system has lower symmetry than the underlying Hamiltonian, occurs in systems ranging from magnetism in solids to the Higgs mechanism in high-energy physics. It leads to multiply degenerate ground states, each with a different "broken" symmetry labeled by an order parameter. In the case of a magnet, the spins locally align, creating a magnetization that plays the role of the order parameter. However, the global orientation of the magnetization can be in one of many directions, determined, for example, by the crystal axes. Locally, the system "spontaneously" chooses one such direction based on external constraints or history. Different local regions can have different orientations, and the boundary between adjacent regions is called a domain wall. Mathematically, this boundary takes the form of a soliton that is finite in width but free to move. Other, more complex topological structures are also possible.The stacking of two graphene sheets exhibits analogous physics. Fig. 1A shows the energy of bilayer graphene as a function of the relative in-plane displacement u between the two graphene sheets, which we will use as a continuous-order parameter (1). The energy as a function of u is maximal in the high-symmetry state (u = 0) where one layer is directly on top of the other, called AA stacking (Fig. 1 A, center and B, edges). Away from u = 0 are six ener...
Two-dimensional (2D) materials are not expected to be metals at low temperature due to electron localization [1]. Consistent with this, pioneering studies on thin films reported only superconducting and insulating ground states, with a direct transition between the two as a function of disorder or magnetic field [2][3][4][5][6]. However, more recent works have revealed the presence of an intermediate quantum metallic state occupying a substantial region of the phase diagram [7-10] whose nature is intensely debated [11][12][13][14][15][16][17]. Here, we observe such a state in the disorder-free limit of a crystalline 2D superconductor, produced by mechanical co-lamination of NbSe 2 in inert atmosphere. Under a small perpendicular magnetic field, we induce a transition from superconductor to the quantum metal. We find a unique power law scaling with field in this phase, which is consistent with the Bose metal model where metallic behavior arises from strong phase fluctuations caused by the magnetic field [11][12][13][14].Global superconductivity emerges in a sample when conduction electrons form Cooper pairs and condense into a macroscopic, phase-coherent quantum state. In two dimensions, the phase coherence can be disrupted even at zero temperature by increasing disorder, either by degrading crystal quality or applying magnetic fields to create vortices [2]. Granular or amorphous superconducting thin films, for which disorder levels can be controlled during growth, have thus provided an established platform for the study of quantum phase transitions in 2D superconductors. Within the conventional theoretical framework, increasing disorder or magnetic field perpendicular to a strongly disordered film at T = 0 induces a direct transition to an insulating state as the normal state sheet resistance approaches the pair quantum resistance h/(2e) 2 = 6.4 kΩ [2,4]. As film quality has improved over time, however, an intervening metallic phase with resistance much lower than the normal state resistance has been observed in several systems with generally less disorder [7][8][9][10]. Its origin is not well understood, and the various theoretical treatments can be generally divided between purely bosonic-based models, in which Cooper pairing persists in the metallic phase but phase coherence is lost [11][12][13][14], and models that also incorporate other fermionic degrees of freedom [15][16][17].Recently, mechanical exfoliation has emerged as a technique to produce ultra-clean, crystalline 2D materials, with graphene being a well-known example [18]. Like amorphous films, the thickness of these samples can be easily controlled down to the level of individual atomic layers. In contrast to amorphous films, a 2D superconductor exfoliated from a lay- Figure 1. Environmentally controlled device fabrication. a) Schematic of heterostructure assembly process. Boron nitride (BN)/graphite (G) on a polymer stamp (PDMS) is used to electrically contact and encapsulate NbSe2 in inert atmosphere. The heterostructure is lithographically patte...
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...
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