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Register a new userStacking transition in rhombohedral graphite
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Added by
Tatiana Latychevskaia
Publication date
2019
fields
Physics
and research's language is
English
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Few layer graphene (FLG) has been recently intensively investigated for its variable electronic properties defined by a local atomic arrangement. While the most natural layers arrangement in FLG is ABA (Bernal) stacking, a metastable ABC (rhombohedral) stacking characterized by a relatively high energy barrier can also occur. When both stacking occur in the same FLG device this results in in-plane heterostructure with a domain wall (DW). We show that ABC stacking in FLG can be controllably and locally turned into ABA stacking by two following approaches. In the first approach, Joule heating was introduced and the transition was characterized by 2D-peak Raman spectra at a submicron spatial resolution. The observed transition was initiated at a small region and then the DW controllably shifted until the entire device became ABA stacked. In the second approach, the transition was achieved by illuminating the ABC region with a train of laser pulses of 790 nm wavelength, while the transition was visualized by transmission electron microscopy in both diffraction and dark field modes. Also, with this approach, a DW was visualized in the dark-field imaging mode, at a nanoscale spatial resolution.
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Van der Waals (vdW) materials have greatly expanded our design space of heterostructures by allowing individual layers to be stacked at non-equilibrium configurations, for example via control of the twist angle. Such heterostructures not only combine characteristics of the individual building blocks, but can also exhibit emergent physical properties absent in the parent compounds through interlayer interactions. Here we report on a new family of emergent, nanometer-thick, semiconductor 2D ferroelectrics, where the individual constituents are well-studied non-ferroelectric monolayer transition metal dichalcogenides (TMDs), namely WSe2, MoSe2, WS2, and MoS2. By stacking two identical monolayer TMDs in parallel, we obtain electrically switchable rhombohedral-stacking configurations, with out-of-plane polarization that is flipped by in-plane sliding motion. Fabricating nearly-parallel stacked bilayers enables the visualization of moire ferroelectric domains as well as electric-field-induced domain wall motion with piezoelectric force microscopy (PFM). Furthermore, by using a nearby graphene electronic sensor in a ferroelectric field transistor geometry, we quantify the ferroelectric built-in interlayer potential, in good agreement with first-principles calculations. The novel semiconducting ferroelectric properties of these four new TMDs opens up the possibility of studying the interplay between ferroelectricity and their rich electric and optical properties.
Of the two stable forms of graphite, hexagonal (HG) and rhombohedral (RG), the former is more common and has been studied extensively. RG is less stable, which so far precluded its detailed investigation, despite many theoretical predictions about the abundance of exotic interaction-induced physics. Advances in van der Waals heterostructure technology have now allowed us to make high-quality RG films up to 50 graphene layers thick and study their transport properties. We find that the bulk electronic states in such RG are gapped and, at low temperatures, electron transport is dominated by surface states. Because of topological protection, the surface states are robust and of high quality, allowing the observation of the quantum Hall effect, where RG exhibits phase transitions between gapless semimetallic phase and gapped quantum spin Hall phase with giant Berry curvature. An energy gap can also be opened in the surface states by breaking their inversion symmetry via applying a perpendicular electric field. Moreover, in RG films thinner than 4 nm, a gap is present even without an external electric field. This spontaneous gap opening shows pronounced hysteresis and other signatures characteristic of electronic phase separation, which we attribute to emergence of strongly-correlated electronic surface states.
There has been a lot of excitement around the observation of superconductivity in twisted bilayer graphene, associated to flat bands close to the Fermi level. Such correlated electronic states also occur in multilayer rhombohedral stacked graphene (RG), which has been receiving increasing attention in the last years. In both natural and artificial samples however, multilayer stacked Bernal graphene (BG) occurs more frequently, making it desirable to determine what is their relative stability and under which conditions RG might be favored. Here, we study the energetics of BG and RG in bulk and also multilayer stacked graphene using first-principles calculations. It is shown that the electronic temperature, not accounted for in previous studies, plays a crucial role in determining which phase is preferred. We also show that the low energy states at room temperature consist of BG, RG and mixed BG-RG systems with a particular type of interface. Energies of all stacking sequences (SSs) are calculated for N = 12 layers, and an Ising model is used to fit them, which can be used for larger N as well. In this way, the ordering of low energy SSs can be determined and analyzed in terms of a few parameters. Our work clarifies inconsistent results in the literature, and sets the basis to studying the effect of external factors on the stability of multilayer graphene systems in first principles calculations.
In rhombohedral-stacked few-layer graphene, the very flat energy bands near the charge neutrality point are unstable to electronic interactions, giving rise to states with spontaneous broken symmetries. Using transport measurements on suspended rhombohedral-stacked tetralayer graphene, we observe an insulating ground state with a large interaction-induced gap up to 80 meV. This gapped state can be enhanced by a perpendicular magnetic field, and suppressed by an interlayer potential, carrier density, or a critical temperature of ~ 40 K.
Multi-layer graphene with rhombohedral stacking is a promising carbon phase possibly displaying correlated states like magnetism or superconductivity due to the occurrence of a flat surface band at the Fermi level. Recently, flakes of thickness up to 17 layers were tentatively attributed ABC sequences although the Raman fingerprint of rhombohedral multilayer graphene is currently unknown and the 2D resonant Raman spectrum of Bernal graphite not understood. We provide a first principles description of the 2D Raman peak in three and four layers graphene (all stackings) as well as in Bernal, rhombohedral and an alternation of Bernal and rhombohedral graphite. We give practical prescriptions to identify long range sequences of ABC multi-layer graphene. Our work is a prerequisite to experimental non-destructive identification and synthesis of rhombohedral graphite.
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