The electronic properties of heterostructures of atomically thin van der Waals crystals can be modified substantially by moiré superlattice potentials from an interlayer twist between crystals
. ...Moiré tuning of the band structure has led to the recent discovery of superconductivity
and correlated insulating phases
in twisted bilayer graphene (TBG) near the 'magic angle' of twist of about 1.1 degrees, with a phase diagram reminiscent of high-transition-temperature superconductors. Here we directly map the atomic-scale structural and electronic properties of TBG near the magic angle using scanning tunnelling microscopy and spectroscopy. We observe two distinct van Hove singularities (VHSs) in the local density of states around the magic angle, with an energy separation of 57 millielectronvolts that drops to 40 millielectronvolts with high electron/hole doping. Unexpectedly, the VHS energy separation continues to decrease with decreasing twist angle, with a lowest value of 7 to 13 millielectronvolts at a magic angle of 0.79 degrees. More crucial to the correlated behaviour of this material, we find that at the magic angle, the ratio of the Coulomb interaction to the bandwidth of each individual VHS (U/t) is maximized, which is optimal for electronic Cooper pairing mechanisms. When doped near the half-moiré-band filling, a correlation-induced gap splits the conduction VHS with a maximum size of 6.5 millielectronvolts at 1.15 degrees, dropping to 4 millielectronvolts at 0.79 degrees. We capture the doping-dependent and angle-dependent spectroscopy results using a Hartree-Fock model, which allows us to extract the on-site and nearest-neighbour Coulomb interactions. This analysis yields a U/t of order unity indicating that magic-angle TBG is moderately correlated. In addition, scanning tunnelling spectroscopy maps reveal an energy- and doping-dependent three-fold rotational-symmetry breaking of the local density of states in TBG, with the strongest symmetry breaking near the Fermi level and further enhanced when doped to the correlated gap regime. This indicates the presence of a strong electronic nematic susceptibility or even nematic order in TBG in regions of the phase diagram where superconductivity is observed.
The emerging field of twistronics, which harnesses the twist angle between two-dimensional materials, represents a promising route for the design of quantum materials, as the twist-angle-induced ...superlattices offer means to control topology and strong correlations. At the small twist limit, and particularly under strain, as atomic relaxation prevails, the emergent moiré superlattice encodes elusive insights into the local interlayer interaction. Here we introduce moiré metrology as a combined experiment-theory framework to probe the stacking energy landscape of bilayer structures at the 0.1 meV/atom scale, outperforming the gold-standard of quantum chemistry. Through studying the shapes of moiré domains with numerous nano-imaging techniques, and correlating with multi-scale modelling, we assess and refine first-principle models for the interlayer interaction. We document the prowess of moiré metrology for three representative twisted systems: bilayer graphene, double bilayer graphene and H-stacked MoSe
/WSe
. Moiré metrology establishes sought after experimental benchmarks for interlayer interaction, thus enabling accurate modelling of twisted multilayers.
Visualization of moiré superlattices McGilly, Leo J; Kerelsky, Alexander; Finney, Nathan R ...
Nature nanotechnology,
07/2020, Letnik:
15, Številka:
7
Journal Article
Recenzirano
Moiré superlattices in van der Waals heterostructures have given rise to a number of emergent electronic phenomena due to the interplay between atomic structure and electron correlations. Indeed, ...electrons in these structures have been recently found to exhibit a number of emergent properties that the individual layers themselves do not exhibit. This includes superconductivity
, magnetism
, topological edge states
, exciton trapping
and correlated insulator phases
. However, the lack of a straightforward technique to characterize the local structure of moiré superlattices has thus far impeded progress in the field. In this work we describe a simple, room-temperature, ambient method to visualize real-space moiré superlattices with sub-5-nm spatial resolution in a variety of twisted van der Waals heterostructures including, but not limited to, conducting graphene, insulating boron nitride and semiconducting transition metal dichalcogenides. Our method uses piezoresponse force microscopy, an atomic force microscope modality that locally measures electromechanical surface deformation. We find that all moiré superlattices, regardless of whether the constituent layers have inversion symmetry, exhibit a mechanical response to out-of-plane electric fields. This response is closely tied to flexoelectricity wherein electric polarization and electromechanical response is induced through strain gradients present within moiré superlattices. Therefore, moiré superlattices of two-dimensional materials manifest themselves as an interlinked network of polarized domain walls in a non-polar background matrix.
Two dimensional (2D) transition-metal dichalcogenide (TMD) based semiconductors have generated intense recent interest due to their novel optical and electronic properties and potential for ...applications. In this work, we characterize the atomic and electronic nature of intrinsic point defects found in single crystals of these materials synthesized by two different methods, chemical vapor transport and self-flux growth. Using a combination of scanning tunneling microscopy (STM) and scanning transmission electron microscopy (STEM), we show that the two major intrinsic defects in these materials are metal vacancies and chalcogen antisites. We show that by control of the synthetic conditions, we can reduce the defect concentration from above 1013/cm2 to below 1011/cm2. Because these point defects act as centers for nonradiative recombination of excitons, this improvement in material quality leads to a hundred-fold increase in the radiative recombination efficiency
Protein phosphorylation is one of the most widespread post-translational modifications in biology
. With advances in mass-spectrometry-based phosphoproteomics, 90,000 sites of serine and threonine ...phosphorylation have so far been identified, and several thousand have been associated with human diseases and biological processes
. For the vast majority of phosphorylation events, it is not yet known which of the more than 300 protein serine/threonine (Ser/Thr) kinases encoded in the human genome are responsible
. Here we used synthetic peptide libraries to profile the substrate sequence specificity of 303 Ser/Thr kinases, comprising more than 84% of those predicted to be active in humans. Viewed in its entirety, the substrate specificity of the kinome was substantially more diverse than expected and was driven extensively by negative selectivity. We used our kinome-wide dataset to computationally annotate and identify the kinases capable of phosphorylating every reported phosphorylation site in the human Ser/Thr phosphoproteome. For the small minority of phosphosites for which the putative protein kinases involved have been previously reported, our predictions were in excellent agreement. When this approach was applied to examine the signalling response of tissues and cell lines to hormones, growth factors, targeted inhibitors and environmental or genetic perturbations, it revealed unexpected insights into pathway complexity and compensation. Overall, these studies reveal the intrinsic substrate specificity of the human Ser/Thr kinome, illuminate cellular signalling responses and provide a resource to link phosphorylation events to biological pathways.
Conductive bridge random access memory (CBRAM) is a leading candidate to supersede flash memory, but poor understanding of its switching process impedes widespread implementation. The underlying ...physics and basic, unresolved issues such as the connecting filament’s growth direction can be revealed with direct imaging, but the nanoscale target region is completely encased and thus difficult to access with real-time, high-resolution probes. In Pt/Al2O3/Cu CBRAM devices with a realistic topology, we find that the filament grows backward toward the source metal electrode. This observation, consistent over many cycles in different devices, corroborates the standard electrochemical metallization model of CBRAM operation. Time-resolved scanning transmission electron microscopy (STEM) reveals distinct nucleation-limited and potential-limited no-growth periods occurring before and after a connection is made, respectively. The subfemtoampere ionic currents visualized move some thousands of atoms during a switch and lag the nanoampere electronic currents.
High quality electrical contact to semiconducting transition metal dichalcogenides (TMDCs) such as MoS2 is key to unlocking their unique electronic and optoelectronic properties for fundamental ...research and device applications. Despite extensive experimental and theoretical efforts reliable ohmic contact to doped TMDCs remains elusive and would benefit from a better understanding of the underlying physics of the metal–TMDC interface. Here we present measurements of the atomic-scale energy band diagram of junctions between various metals and heavily doped monolayer MoS2 using ultrahigh vacuum scanning tunneling microscopy (UHV-STM). Our measurements reveal that the electronic properties of these junctions are dominated by two-dimensional metal-induced gap states (MIGS). These MIGS are characterized by a spatially growing measured gap in the local density of states (L-DOS) of the MoS2 within 2 nm of the metal–semiconductor interface. Their decay lengths extend from a minimum of ∼0.55 nm near midgap to as long as 2 nm near the band edges and are nearly identical for Au, Pd, and graphite contacts, indicating that it is a universal property of the monolayer semiconductor. Our findings indicate that even in heavily doped semiconductors, the presence of MIGS sets the ultimate limit for electrical contact.
Abstract
The topology of Weyl semimetals requires the existence of unique surface states. Surface states have been visualized in spectroscopy measurements, but their connection to the topological ...character of the material remains largely unexplored. 1T'-MoTe
2
, presents a unique opportunity to study this connection. This material undergoes a phase transition at 240 K that changes the structure from orthorhombic (putative Weyl semimetal) to monoclinic (trivial metal), while largely maintaining its bulk electronic structure. Here, we show from temperature-dependent quasiparticle interference measurements that this structural transition also acts as a topological switch for surface states in 1T'-MoTe
2
. At low temperature, we observe strong quasiparticle scattering, consistent with theoretical predictions and photoemission measurements for the surface states in this material. In contrast, measurements performed at room temperature show the complete absence of the scattering wavevectors associated with the trivial surface states. These distinct quasiparticle scattering behaviors show that 1T'-MoTe
2
is ideal for separating topological and trivial electronic phenomena via temperature-dependent measurements.
Moiréless correlations in ABCA graphene Kerelsky, Alexander; Rubio-Verdú, Carmen; Xian, Lede ...
Proceedings of the National Academy of Sciences - PNAS,
01/2021, Letnik:
118, Številka:
4
Journal Article
Recenzirano
Odprti dostop
Atomically thin van der Waals materials stacked with an interlayer twist have proven to be an excellent platform toward achieving gate-tunable correlated phenomena linked to the formation of flat ...electronic bands. In this work we demonstrate the formation of emergent correlated phases in multilayer rhombohedral graphene--a simple material that also exhibits a flat electronic band edge but without the need of having a moiré superlattice induced by twisted van der Waals layers. We show that two layers of bilayer graphene that are twisted by an arbitrary tiny angle host large (micrometer-scale) regions of uniform rhombohedral four-layer (ABCA) graphene that can be independently studied. Scanning tunneling spectroscopy reveals that ABCA graphene hosts an unprecedentedly sharp van Hove singularity of 3-5-meV half-width. We demonstrate that when this van Hove singularity straddles the Fermi level, a correlated many-body gap emerges with peak-to-peak value of 9.5 meV at charge neutrality. Mean-field theoretical calculations for model with short-ranged interactions indicate that two primary candidates for the appearance of this broken symmetry state are a charge-transfer excitonic insulator and a ferrimagnet. Finally, we show that ABCA graphene hosts surface topological helical edge states at natural interfaces with ABAB graphene which can be turned on and off with gate voltage, implying that small-angle twisted double-bilayer graphene is an ideal programmable topological quantum material.
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