The direct experimental probing of locally varying lattice parameters and anisotropic lattice deformations in atomic multilayers is extremely challenging. Here, we develop a new combined numerical/graphical method for the analysis of irregular moiré superstructures measured by scanning tunneling microscopy (STM) on a small-twist-angle ($\sim$0.6$^{\circ}$) graphene on highly oriented pyrolytic graphite (gr/HOPG). We observe distorted moiré patterns with a spatially varying period in annealed gr/HOPG. The nanoscale modulation of the moiré period observed by STM reflects a locally strained (and sheared) graphene with anisotropic variation of the lattice parameters. We use a specific algorithm based on a rigid lattice Fourier method, which is able to reconstruct the irregular and distorted moiré patterns emerging from strain-induced lattice deformations. Our model is universal and can be used to study different moiré patterns occurring in two-dimensional van der Waals heterostructures. Additionally, room temperature scanning tunneling spectroscopy measurements show electronic states at the Dirac point, localized on moiré hills, which increase significantly the apparent corrugation of the moiré pattern. The measured topography is compared to classical molecular dynamics simulations. Density functional theory (DFT) calculations confirm that an AAB stacked trilayer region itself can contribute electronic states near the Fermi-level, in agreement with the measured peak in the local density of states. Furthermore, CMD calculations reveal direction-dependent bond alternations ($\sim$0.5$\%$) around the stacking regions, induced by shear strain, which could influence electronic properties.
Stacking graphene sheets forms graphite. Two in-plane vibrational modes of graphite, E1u and E2g(2), are derived from graphene E2g mode, the shifts of which under compression are all considered as results of in-plane bond shortening. Values of Gruneisen parameter have been reported to quantify such relation. However, the reason why the shift rates of these three modes with pressure differ is unclear. In this work, we introduce a new parameter to quantify the contribution of out-of-plane strain to the in-plane vibrational frequencies, suggesting that the compression of π-electrons plays a non-…
We report that the twisted few layer graphite (tFL-graphite) is a new family of moiré heterostructures (MHSs), which has richer and highly tunable moiré flat band structures entirely distinct from all the known MHSs. A tFL-graphite is composed of two few-layer graphite (Bernal stacked multilayer graphene), which are stacked on each other with a small twisted angle. The moiré band structure of the tFL-graphite strongly depends on the layer number of its composed two van der Waals layers. Near the magic angle, a tFL-graphite always has two nearly flat bands coexisting with a few pairs of narrowe…
We study the thermal transport properties of twisted-layer graphite nanofibers. We show that in the presence of a twisted layer, the phonon thermal conductance of a graphite nanofiber varies remarkably with the twisted angle and can reach minimum values either at two critical angles $θ_1$ and $θ_2$ that conform to the rule $θ_1$ + $θ_1$ = $180^0$ or exactly at the angle $θ$ = $90^0$. A reduction of roughly 50% of the phonon thermal conductance can be achieved in some structures. We unveil that the twisting effect mainly influences the optical modes, leaving almost unaltered the acoustic ones. …
We calculate the electronic structure of AA'AA'...-stacked alternating twist N-layer (tNG) graphene for N = 3, 4, 5, 6, 8, 10, 20 layers and bulk alternating twist (AT) graphite systems where the lattice relaxations are modeled by means of molecular dynamics simulations. We show that the symmetric AA'AA'... stacking is energetically preferred among all interlayer sliding geometries for progressively added layers up to N=6. Lattice relaxations enhance electron-hole asymmetry, and reduce the magic angles with respect to calculations with fixed tunneling strengths that we quantify from few layers…
We study the electronic structure of a double-twisted few layer graphite (DTFLG), which consists of three few layer graphite (FLG), i.e. ABA-stacked graphene multilayer, stacked with two twist angles. We consider two categories of DTFLG, alternately twisted case and chirally twisted one, according to the rotation direction of the two twist angles. We show that, once the middle FLG of DTFLG is not thinner than trilayer, both kinds of DTFLG can remarkably host two pairs of degenerate moiré flat bands (MFBs) at $E_f$, twice that of the magic angle twisted bilayer graphene (TBG). The doubled MFBs …
Atomic modulations of two-dimensional materials using scanning tunneling microscope (STM) tip-induced forces modifies their mechanical and electrical properties. In situ topographic and spectroscopic probing through electrical tunneling has been used for straining sheets of graphite, monolayer graphene and NbSe2. The findings also resolve a thirty-five-year-old controversy involving numerous proposed models to explain the source of anomalously high measured atomic amplitudes (of up to 24 Angstroms, expected 0.2 Angstroms) from atomic corrugation on graphite surfaces. Our findings attributes th…
Twisted bilayer graphene (TBG) exhibits a wide range of intriguing physical properties, such as superconductivity, ferromagnetism, and superlubricity. Depending on the twist angle, periodic moiré superlattices form in twisted bilayer graphene, with inhomogeneous interlayer coupling and lattice deformation. For a small twist angle (typically <2°), each moiré supercell contains a large number of atoms (>10,000), making it computationally expensive for first-principles and atomistic modeling. In this work, a finite element method based on a continuum model is used to simulate the inhomogeneous in…
We investigate the effects of uniaxial strain on the transport properties of vertical devices made of two twisted graphene layers, which partially overlap each other. We find that because of the different orientations of the two graphene lattices, their Dirac points can be displaced and separated in the $k-$space by the effects of strain. Hence, a finite conduction gap as large as a few hundred meV can be obtained in the device with a small strain of only a few percent. The dependence of this conduction gap on the strain strength, strain direction, transport direction and twist angle are clari…
We study the effect of atomic relaxation on the structure of moiré patterns in twisted graphene on graphite and double layer graphene by large scale atomistic simulations. The reconstructed structure can be described as a superlattice of `hot spots' with vortex-like behaviour of in-plane atomic displacements and increasing out-of-plane displacements with decreasing angle. These lattice distortions affect both scalar and vector potential and the resulting electronic properties. At low misorientation angles (<$\sim$1$^\circ$) the optimized structures deviate drastically from the sinusoidal modul…
By means of atomistic tight-binding calculations, we investigate the effects of uniaxial strain on the electronic bandstructure of twisted graphene bilayer. We find that the bandstructure is dramatically deformed and the degeneracy of the bands is broken by strain. As a conseqence, the number of Dirac cones can double and the van Hove singularity points are separated in energy. The dependence of these effects on the strength of strain, its applied direction and the twist angle is carefully clarified. As an important result, we demonstrate that the position of van Hove singularities can be modu…
Strain and twist angle driven electronic structure evolution in twisted bilayer graphene
Tsinghua University（清华大学）；Imdea Nanoscience（Imdea纳米科学研究所）；Beihang University（北京航空航天大学）；Princeton University（普林斯顿大学）；Donostia International Physics Center（多诺斯蒂亚国际物理中心）；Beijing Academy of Quantum Information Sciences（北京量子信息科学研究院）；Southern University of Science and Technology（南方科技大学）；Hefei National Laboratory（合肥国家实验室）
Recent experiments have measured local uniaxial strain fields in twisted bilayer graphene (TBG). Our calculations found that the finite Berry curvature generated by breaking the sublattice symmetry and the band proximity between narrow bands in these TBG induces a giant Berry dipole of order 10\,nm or larger. The large Berry dipole leads to transverse topological non-linear charge currents which dominates over the linear bulk valley current at experimentally accessible crossover in-plane electric field of $\sim 0.1 {\rm mV} / μ\rm{m}$. This anomalous Hall effect, due to Berry dipole, is strong…
As a canonical response to the applied magnetic field, the electronic states of a metal are fundamentally reorganized into Landau levels. In Dirac metals, Landau levels can be expected without magnetic fields, provided that an inhomogeneous strain is applied to spatially modulate electron hoppings in a similar way as the Aharonov-Bohm phase. We here predict that a twisted zigzag nanoribbon of graphene exhibits strain-induced pseudo Landau levels of unexplored but analytically solvable dispersions at low energies. The presence of such dispersive pseudo Landau levels results in a negative strain…
Moiré patterns on Highly Oriented Pyrolytic Graphite surfaces due to dislocated graphene layers were studied. We observed that the apparent corrugations of the moiré patterns in scanning tunnelling microscopy images change as a function of tunnel junction bias. A simple geometric investigation of the atomic structure of the graphene layers generating moiré patterns revealed that different atomic arrangements due to different twist angles can result in similar geometric moiré periods such that, only a small fraction of the observed moiré periodicities may coincide with the real atomic periodici…
Lithium intercalation into graphite is the foundation for the lithium-ion battery, and the thermodynamics of the lithiation of graphitic electrodes have been heavily investigated. Intercalated lithium in bulk graphite undergoes structural ordering known as staging to minimize electrostatic repulsions within the crystal lattice. While this process is well-understood for bulk graphite, confinement effects become important at the nanoscale, which can significantly impact the electrochemistry of nanostructured electrodes. Therefore, graphene offers a model platform to study intercalation dynamics …
The electronic wavefunctions in moiré materials are highly sensitive to the details of the local atomic configuration enabling Bloch band geometry and topology to be controlled by stacking and strain. Here we predict that large injection currents (under circular polarized irradiation) can develop in strained twisted bilayer graphene (TBG) heterostructures with broken sublattice symmetry; such bulk photovoltaic currents flow even in the absence of a p-n junction and can be controlled by the helicity of incident light. As we argue, large injection current rates proceed from strong and highly pea…
We study the effect of twisting on bilayer graphene. The effect of lattice relaxation is included; we look at the electronic structure, piezo-electric charges and spontaneous polarisation. We show that the electronic structure without lattice relaxation shows a set of extremely flat in-gap states similar to Landau-levels, where the spacing scales with twist angle. With lattice relaxation we still have flat bands, but now the spectrum becomes independent of twist angle for sufficiently small angles. We describe in detail the nature of the bands, and study appropriate continuum models, at the sa…
The parameters of the triangular domain wall network in bilayer graphene with a simultaneously twisted and biaxially stretched bottom layer are studied using the two-chain Frenkel-Kontorova model. It is demonstrated that if the graphene layers are free to rotate, they prefer to stay co-aligned upon stretching the bottom layer and the regular triangular network of tensile domain walls is formed upon the commensurate-incommensurate phase transition. If the angle between the layers is fixed, the regular triangular network of shear domain walls is observed at zero elongation of the bottom layer. U…
We introduce a minimum tight-binding model with only three parameters extracted from graphene and untwisted bilayer graphene. This model reproduces quantitatively the electronic structure of not only these two systems and bulk graphite near the Fermi level, but also that of twisted bilayer graphene including the value of the magic angle, at which bands at $E_F$ flatten without overlap and two gaps open, one above and one below $E_F$. The Hamiltonian is sufficiently transparent and flexible to be adopted to other twisted layered systems.
We report the observation of proximity effect in measurements performed on highly oriented pyrolitic graphite (HOPG) samples when electrical current is injected through the superconducting electrodes placed on the sample surface few millimeters apart from each other. Such anomalously large effect is surprising, as proximity-induced superconducting features in normal conductors hardly surpass few micrometers. The obtained results can be consistently understood, however, considering pre-existing superconducting correlations in graphite, supported by recent observations of the intrinsic global su…
The low-energy bands of twisted bilayer graphene form Dirac cones with approximate electron-hole symmetry at small rotation angles. These crossings are protected by the emergent symmetries of moiré patterns, conferring a topological character to the bands. Strain accumulated between layers (heterostrain) shifts the Dirac points both in energy and momentum. The overlap of conduction and valence bands favors an excitonic instability of the Fermi surface close to the neutrality point. The spontaneous condensation of electron-hole pairs breaks time reversal symmetry and the separate conservation o…
Thermal conductivity of homogeneous twisted stacks of graphite is found to strongly depend on the misfit angle. The underlying mechanism relies on the angle dependence of phonon-phonon couplings across the twisted interface. Excellent agreement between the calculated thermal conductivity of narrow graphitic stacks and corresponding experimental results indicates the validity of the predictions. This is attributed to the accuracy of interlayer interactions descriptions obtained by the dedicated registry-dependent interlayer potential used. Similar results for h-BN stacks indicate overall higher…
Twist and strain identification in moiré heterostructures
Wuhan University（武汉大学）；Key Laboratory of Artificial Micro- and Nano-structures of Ministry of Education（教育部人工微结构和介观物理重点实验室）；School of Physics and Technology, Wuhan University（武汉大学物理科学与技术学院）；IMDEA Nanoscience（IMDEA纳米科学研究所）；Weizmann Institute of Science（魏茨曼科学研究所）；Department of Condensed Matter Physics, Weizmann Institute of Science（魏茨曼科学研究所凝聚态物理系）；University of Washington（华盛顿大学）；Department of Physics, University of Washington（华盛顿大学物理系）；Hainan University（海南大学）；Center for Theoretical Physics, Hainan University（海南大学理论物理中心）；School of Physics and Optoelectronic Engineering, Hainan University（海南大学物理与电子工程学院）；Donostia International Physics Center（圣塞巴斯蒂安国际物理中心）
We present a theoretical study of the effects of heterostrain and lattice relaxation on the optical conductivity of twisted bilayer graphene near the magic angle, based on the band structures obtained from a continuum model. We find that heterostrain, lattice relaxation and their combination give rise to very distinctive spectroscopic features in the optical conductivity, which can be used to probe and distinguish these effects. From the spectrum at various Fermi energies, important features in the strain- and relaxation-modified band structure such as the bandgap, bandwidth and van Hove singu…
Van der Waals heteroepitaxy allows deterministic control over lattice mismatch or azimuthal orientation between atomic layers to produce long wavelength superlattices. The resulting electronic phases depend critically on the superlattice periodicity as well as localized structural deformations that introduce disorder and strain. Here, we introduce Bragg interferometry, based on four-dimensional scanning transmission electron microscopy, to capture atomic displacement fields in twisted bilayer graphene with twist angles < 2°. Nanoscale spatial fluctuations in twist angle and uniaxial heterostra…
IMDEA Nanoscience（IMDEA纳米科学研究所）；Key Laboratory of Artificial Micro- and Nano-structures of Ministry of Education and School of Physics and Technology, Wuhan University（武汉大学物理科学与技术学院人工微纳结构教育部重点实验室）；School of Artificial Intelligence, Wuhan University（武汉大学人工智能学院）；Wuhan Institute of Quantum Technology（武汉量子技术研究院）；Donostia International Physics Center（圣塞巴斯蒂安国际物理中心）
In two-dimensional (2D) twisted bilayers, the van der Waals (vdW) interlayer interaction introduces atomic-scale reconstruction at interface by locally rotating lattice to form strain-field vortex networks in their moiré superlattice. However, direct imaging the tiny local lattice rotation of the strain-field vortex requires extremely high spatial resolution and is an outstanding challenge in experiment. Here, a topmost small-period graphene moiré pattern is introduced to magnify sub-Angstrom distortions of the lattice and tiny local lattice rotation in underlying twisted bilayer graphene (TBG…
The bands of graphite are extremely sensitive to topological defects which modify the electronic structure. In this paper we found non-dispersive flat bands no farther than 10 meV of the Fermi energy in slightly twisted bilayer graphene as a signature of a transition from a parabolic dispersion of bilayer graphene to the characteristic linear dispersion of graphene. This transition occurs for relative rotation angles of layers around $1.5^o$ and is related to a process of layer decoupling. We have performed ab-initio calculations to develop a tight binding model with an interaction Hamiltonian…
Here we study the evolution of local electronic properties of a twisted graphene bilayer induced by a strain and a high curvature. The strain and curvature strongly affect the local band structures of the twisted graphene bilayer; the energy difference of the two low-energy van Hove singularities decreases with increasing the lattice deformations and the states condensed into well-defined pseudo-Landau levels, which mimic the quantization of massive Dirac fermions in a magnetic field of about 100 T, along a graphene wrinkle. The joint effect of strain and out-of-plane distortion in the graphen…
The spatial texture of internal degree of freedom of electrons has profound effects on the properties of materials. Such texture in real space can manifest as an emergent magnetic field (or Berry curvature), which is expected to induce interesting valley/spin-related transport phenomena. Moiré pattern, which emerges as a spatial variation at the interface of 2D atomic crystals, provides a natural platform for investigating such real space Berry curvature effects. Here we study moiré structures formed in homobilayer transition metal dichalcogenides (TMDs) due to twisting, various uniform strain…
We show how the pairing symmetry of superconducting states in twisted bilayer graphene can be experimentally identified by theoretically studying effects of externally applied in-plane magnetic field and strain. In the low field regime, superconducting critical temperature $T_c$ is suppressed by in-plane magnetic field $\boldsymbol{B}_{\parallel}$ in singlet channels, but is enhanced by weak $\boldsymbol{B}_{\parallel}$ in triplet channels, providing an important distinction. The in-plane angular dependence of the critical $\boldsymbol{B}_{\parallel, c}$ has a six-fold rotational symmetry, whi…
We demonstrate that stacking layered materials allows a novel type of strain engineering where each layer is strained independently, which we call heterostrain. We combine detailed structural and spectroscopic measurements with tight-binding calculations to show that small uniaxial heterostrain suppresses Dirac cones and leads to the emergence of flat bands in twisted graphene layers (TGLs). Moreover, we demonstrate that heterostrain reconstructs much more severely the energy spectrum of TGLs than homostrain for which both layers are strained identically ; a result which should apply to virtua…
Proximity effects are one of the pillars of exotic phenomena and technological applications of two dimensional materials. However, the interactions nature depends strongly on the materials involved, their crystalline symmetries, and interfacial properties. Here we used large-scale first-principle calculations to demonstrate that strain and twist-angle are efficient knobs to tailor the spin-orbit coupling in graphene transition metal dichalcogenide heterobilayers. We found that by choosing a twist-angle of 30 degrees, the spin relaxation times increase by two orders of magnitude, opening a path…
Moiré-superlattices are ubiquitous in 2D heterostructures, strongly influencing their electronic properties. They give rise to new Dirac cones and are also at the origin of the superconductivity observed in magic-angle bilayer graphene. The modulation amplitude (corrugation) is an important yet largely unexplored parameter in defining the properties of 2D superlattices. The generally accepted view is that the corrugation monotonically decreases with increasing twist angle, while its effects on the electronic structure diminish as the layers become progressively decoupled. Here we found by latt…
Moiré superlattices in graphene supported on various substrates have opened a new avenue to engineer graphene's electronic properties. Yet, the exact crystallographic structure on which their band structure depends remains highly debated. In this scanning tunneling microscopy and density functional theory study, we have analysed graphene samples grown on multilayer graphene prepared onto SiC and on the close-packed surfaces of Re and Ir with ultra-high precision. We resolve small-angle twists and shears in graphene, and identify large unit cells comprising more than 1,000 carbon atoms and exhi…
Correlated insulators are frequently observed in magic angle twisted bilayer graphene at even fillings of electrons or holes per moiré unit-cell. Whereas theory predicts these insulators to be intervalley coherent excitonic phases, the measured gaps are routinely much smaller than theoretical estimates. We explore the effects of random strain variations on the intervalley coherent phase, which have a pair-breaking effect analogous to magnetic disorder in superconductors. We find that the spectral gap may be strongly suppressed by strain disorder, or vanish altogether, even as intervalley coher…
