Encapsulating graphene in hexagonal Boron Nitride has several advantages: the highest mobilities reported to date are achieved in this way, and precise nanostructuring of graphene becomes feasible through the protective hBN layers. Nevertheless, subtle effects may arise due to the differing lattice constants of graphene and hBN, and due to the twist angle between the graphene and hBN lattices. Here, we use a recently developed model which allows us to perform band structure and magnetotransport calculations of such structures, and show that with a proper account of the moiré physics an excellent agreement with experiments can be achieved, even for complicated structures such as disordered graphene, or antidot lattices on a monolayer hBN with a relative twist angle. Calculations of this kind are essential to a quantitative modeling of twistronic devices.
Ferroelectric hysteresis in singly aligned graphene-hBN moiré superlattices
CIC nanoGUNE（纳米科技联合研究中心）；University of the Basque Country (UPV/EHU)（巴斯克大学）；National Institute for Materials Science（物质材料研究机构）；Centro de Física de Materiales (CFM-MPC) Centro Mixto CSIC-UPV/EHU（物质物理中心（CFM-MPC）CSIC-巴斯克大学联合中心）
The specific rotational alignment of two-dimensional lattices results in a moiré superlattice with a larger period than the original lattices and allows one to engineer the electronic band structure of such materials. So far, transport signatures of such superlattices have been reported for graphene/hBN and graphene/graphene systems. Here we report moiré superlattices in fully hBN encapsulated graphene with both the top and the bottom hBN aligned to the graphene. In the graphene, two different moiré superlattices form with the top and the bottom hBN, respectively. The overlay of the two superl…
We report experimental and computational studies of thermal transport properties in hexagonal boron nitride (hBN) encapsulated molybdenum disulfide (MoS2) structure using refined optothermal Raman techniques, and reveal very high interfacial thermal conductance between hBN and MoS2. By studying the Raman shift of hBN and MoS2 in suspended and substrate-supported thin films under varying laser power and temperature, we calibrate lateral (in-plane) thermal conductivity of hBN and MoS2 and the vertical interfacial thermal conductance in the hBN/MoS2/hBN heterostructure as well as the interfaces b…
We identify features in the angle-resolved photoemission spectra (ARPES) arising from the periodic pattern characteristic for graphene heterostructure with hexagonal boron nitride (hBN). For this, we model ARPES spectra and intensity maps for five microscopic models used previously to describe moire superlattice in graphene/hBN systems. We show that detailed analysis of these features can be used to pin down the microscopic mechanism of the interaction between graphene and hBN. We also analyze how the presence of a moire-periodic strain in graphene or scattering of photoemitted electrons off h…
In this paper a systematic examination of graphene/hexagonal boron nitride (g/hBN) bilayers is presented, through a recently developed two-dimensional phase field crystal model that incorporates out-of-plane deformations. The system parameters are determined by closely matching the stacking energies and heights of graphene/hBN bilayers to those obtained from existing quantum-mechanical density functional theory calculations. Out-of-plane deformations are shown to reduce the energies of inversion domain boundaries in hBN, and the coupling between graphene and hBN layers leads to a bilayer defec…
Fast carrier cooling is important for high power graphene based devices. Strongly Coupled Optical Phonons (SCOPs) play a major role in the relaxation of photoexcited carriers in graphene. Heterostructures of graphene and hexagonal boron nitride (hBN) have shown exceptional mobility and high saturation current, which makes them ideal for applications, but the effect of the hBN substrate on carrier cooling mechanisms is not understood. We track the cooling of hot photo-excited carriers in graphene-hBN heterostructures using ultrafast pump-probe spectroscopy. We find that the carriers cool down f…
Artificial semiconductor heterostructures played a pivotal role in modern electronic and photonic technologies, providing a highly effective mean for the manipulation and control of carriers, from the visible to the Terahertz (THz) frequency range. Despite the exceptional versatility, they commonly require challenging epitaxial growth procedures due to the need of clean and abrupt interfaces, which proved to be a major obstacle for the realization of room-temperature (RT), high-efficiency devices, like source, detectors or modulators, especially in the far-infrared. Two-dimensional (2D) layere…
When using hexagonal boron-nitride (hBN) as a substrate for graphene, the resulting moiré pattern creates secondary Dirac points. By encapsulating a multilayer graphene within aligned hBN sheets the controlled moiré stacking may offer even richer benefits. Using advanced tight-binding simulations on atomistically-relaxed heterostructures, here we show that the gap at the secondary Dirac point can be opened in selected moiré-stacking configurations, and is independent of any additional vertical gating of the heterostructure. On the other hand, gating can broadly tune the gap at the principal Di…
We calculate the electronic structure in quasiperiodic double-moiré systems of graphene sandwiched by hexagonal boron nitride, and identify the topological invariants of energy gaps. We find that the electronic spectrum contains a number of minigaps, and they exhibit a recursive fractal structure similar to the Hofstadter butterfly when plotted against the twist angle. Each of the energy gaps can be characterized by a set of integers, which are associated with an area in the momentum space. The corresponding area is geometrically interpreted as a quasi Brillouin zone, which is a polygon enclos…
Among two-dimensional atomic crystals, hexagonal boron nitride (hBN) is one of the most remarkable materials to fabricate heterostructures revealing unusual properties. We perform first-principles calculations to determine whether intercalated metal atoms and vacancies can mediate interfacial coupling and influence the structural and electronic properties of the graphene/hBN heterostructure. Metal impurity atoms (Li, K, Cr, Mn, Co, and Cu) as extrinsic defects between the graphene and hBN sheets produce $n$-doped graphene. We also consider intrinsic vacancy defects and find that a boron monova…
Graphene on hBN (G/hBN) has a long period moiré superstructure owing to the lattice mismatch between two materials. Long periodic potential caused by the moiré superstructure induces modulation of electronic properties of the system. In this paper, we numerically calculate optical conductivity of G/hBN under circularly polarized light irradiation. The lack of spatial inversion symmetry in G/hBN induces the valley polarization. In further, the valley polarization becomes most pronounced in the infrared and terahertz regions if the twist angle between two materials is close to zero for non-dopin…
We use confocal Raman microscopy and modified vector analysis methods to investigate the nanoscale origin of strain and carrier concentration in exfoliated graphene-hexagonal boron nitride (hBN) heterostructures on silicon dioxide (SiO2). Two types of heterostructures are studied: graphene on SiO2 partially coved by hBN, and graphene fully encapsulated between two hBN flakes. We extend the vector analysis methods to produce spatial maps of the strain and doping variation across the heterostructures. This allows us to visualise and directly quantify the much-speculated effect of the environment…
Hexagonal boron nitride (hBN) is a van der Waals semiconductor with a wide bandgap of ~ 5.96 eV. Despite the indirect bandgap characteristics of hBN, charge carriers excited by high energy electrons or photons efficiently emit luminescence at deep-ultraviolet (DUV) frequencies via strong electron-phonon interaction, suggesting potential DUV light emitting device applications. However, electroluminescence from hBN has not been demonstrated at DUV frequencies so far. In this study, we report DUV electroluminescence and photocurrent generation in graphene/hBN/graphene heterostructures at room tem…
We study room temperature spin transport in graphene devices encapsulated between a layer-by-layer-stacked two-layer-thick chemical vapour deposition (CVD) grown hexagonal boron nitride (hBN) tunnel barrier, and a few-layer-thick exfoliated-hBN substrate. We find mobilities and spin-relaxation times comparable to that of SiO$_2$ substrate based graphene devices, and obtain a similar order of magnitude of spin relaxation rates for both the Elliott-Yafet and D'Yakonov-Perel' mechanisms. The behaviour of ferromagnet/two-layer-CVD-hBN/graphene/hBN contacts ranges from transparent to tunneling due …
ABC-stacked trilayer graphene/hBN moiré superlattice (TLG/hBN) has emerged as a playground for correlated electron physics. We report spectroscopy measurements of dual-gated TLG/hBN using Fourier transformed infrared photocurrent spectroscopy. We observed a strong optical transition between moiré mini-bands that narrows continuously as a bandgap is opened by gating, indicating a reduction of the single particle bandwidth. At half-filling of the valence flat band, a broad absorption peak emerges at ~18 meV, indicating direct optical excitation across an emerging Mott gap. Similar photocurrent s…
While Fabry-Pérot resonances and Moiré superlattices are intensively studied in graphene on hexagonal boron nitride (hBN), the two effects have not been discussed in their coexistence. Here we investigate the FP oscillations in a ballistic pnp-junctions in the presence and absence of a Moiré superlattice. First, we address the effect of the smoothness of the confining potential on the visibility of the FP resonances and carefully map the evolution of the FP cavity size as a function of densities in and outside the cavity in the absence of a superlattice, when the cavity is bound by regular pn-…
In van der Waals heterostructures, the relative alignment of bands between layers, and the resulting band hybridisation, are key factors in determining a range of electronic properties. This work examines these effects for heterostructures of transition metal dichalcogenides (TMDs) and hexagonal boron nitride (hBN), an ubiquitous combination given the role of hBN as an encapsulating material. By comparing results of density functional calculations with experimental angle-resolved photoemission spectroscopy (ARPES) results, we explore the hybridisation between the valence states of the TMD and …
Monolayer graphene aligned with hexagonal boron nitride (hBN) develops a gap at the charge neutrality point (CNP). This gap has previously been extensively studied by electrical transport through thermal activation measurements. Here, we report the determination of the gap size at the CNP of graphene/hBN superlattice through photocurrent spectroscopy study. We demonstrate two distinct measurement approaches to extract the gap size. A maximum of ~ 14 meV gap is observed for devices with a twist angle of less than 1 degree. This value is significantly smaller than that obtained from thermal acti…
Moiré superlattices of van der Waals heterostructures provide a powerful new way to engineer the electronic structures of two-dimensional (2D) materials. Many novel quantum phenomena have emerged in different moiré heterostructures, such as correlated insulators, superconductors, and Chern insulators in graphene systems and moiré excitons in transition metal dichalcogenide (TMDC) systems. Twisted phosphorene offers another attractive system to explore moiré physics because phosphorene features an anisotropic rectangular lattice, different from the isotropic hexagonal lattice in graphene and TM…
Second-order nonlinear optical response allows to detect different properties of the system associated with the inversion symmetry breaking. Here, we use a second harmonic generation effect to investigate the alignment of a graphene/hexagonal Boron Nitride heterostructure. To achieve that, we activate a commensurate-incommensurate phase transition by a thermal annealing of the sample. We find that this structural change in the system can be directly observed through a strong modification of a nonlinear optical signal. This result reveals the potential of a second harmonic generation technique …
We investigate the effect of sliding motion of layers in Moiré heterostructures on the electronic state. We show that the sliding Moiré heterostructure can generate nontrivial topology characterized by the first and second Chern number in the high dimensional manifold spanned by the physical dimensions and synthetic dimensions associated with the sliding displacement. The nontrivial topology implies a topological charge pumping caused by the sliding motion. We demonstrate the nontrivial topology and charge pumping explicitly in a one dimensional bi-chain model and the small-angle twisted bilay…
Recent works have revealed that van der Waals (vdW) epitaxial growth of 2D materials on crystalline substrates, such as hexagonal boron nitride (hBN), leads to formation of self-aligned grains, which results in defect-free stitching between the grains. However, how the weak vdW interaction causes strong limitation on orientation of grains is still not understood yet. In this work, we have focused on investigation of mechanism of self-alignment of MoS2 grains in vdW epitaxial growth on hBN. Through calculation based on density functional theory and the Lennard-Jones potential, we found that int…
We propose a theory of optical absorption in monolayer graphene-hexagonal boron nitride (hBN) heterostructures. In highly oriented heterostructures, the hBN underlay produces a long-range moiré superlattice potential for the graphene electrons which modifies the selection rules for absorption of incoming photons in the infrared to visible frequency range. The details of the absorption spectrum modification depend on the relative strength of the various symmetry-allowed couplings between the graphene electrons and the hBN, and the resulting nature of the reconstructed band structure.
We reexamine the electronic structure of graphene on SiC substrate by angle-resolved photoemission spectroscopy. We directly observed multiply cloning of Dirac cone, in addition to ones previously attributed to reconstruction. The locations, relative distances and anisotropy of Dirac cone replicas fully agree with the moiré pattern of graphene-SiC heterostructure. Our results provide a straightforward example of moiré potential modulation in engineering electronic structure with Dirac fermions.
We theoretically investigate the electronic structures of moiré superlattices arising in monolayer / bilayer graphene stacked on hexagonal boron nitride (hBN) in presence and absence of magnetic field. We develop an effective continuum model from a microscopic tight-binding lattice Hamiltonian, and calculate the electronic structures of graphene-hBN systems with different rotation angles. Using the effective model, we explain the characteristic band properties such as the gap opening at the corners of the superlattice Brillouin zone (mini-Dirac point). We also investigate the energy spectrum a…
The properties of van der Waals (vdW) heterostructures are drastically altered by a tunable moiré superlattice arising from periodic variations of atomic alignment between the layers. Exciton diffusion represents an important channel of energy transport in semiconducting transition metal dichalcogenides (TMDs). While early studies performed on TMD heterobilayers have suggested that carriers and excitons exhibit long diffusion lengths, a rich variety of scenarios can exist. In a moiré crystal with a large supercell size and deep potential, interlayer excitons may be completely localized. As the…
Interlayer excitons (IXs) possess a much longer lifetime than intralayer excitons due to the spatial separation of the electrons and holes; hence, they have been pursued to create exciton condensates for decades. The recent emergence of two-dimensional (2D) materials, such as transition metal dichalcogenides (TMDs), and of their van der Waals heterostructures (HSs), in which two different 2D materials are layered together, has created new opportunities to study IXs. Here we present the observation of IX gases within two stacked structures consisting of hBN/WSe$_2$/hBN/p: WSe$_2$/hBN. The IX en…
We investigate interlayer tunneling in heterostructures consisting of two tungsten diselenide (WSe2) monolayers with controlled rotational alignment, and separated by hexagonal boron nitride. In samples where the two WSe2 monolayers are rotationally aligned we observe resonant tunneling, manifested by a large conductance and negative differential resistance in the vicinity of zero interlayer bias, which stem from energy- and momentum-conserving tunneling. Because the spin-orbit coupling leads to coupled spin-valley degrees of freedom, the twist between the two WSe2 monolayers allows us to prob…
The current research in graphene spintronics strives for achieving a long spin lifetime, and efficient spin injection and detection in graphene. In this article, we review how hexagonal boron nitride (hBN) has evolved as a crucial substrate, as an encapsulation layer, and as a tunnel barrier for manipulation and control of spin lifetimes and spin injection/detection polarizations in graphene spin valve devices. First, we give an overview of the challenges due to conventional SiO$_2$ substrate for spin transport in graphene followed by the progress made in hBN based graphene heterostructures. T…
Monolayer transition metal dichalcogenides(2D) and zero dimensional quantum dots(QD) are known to have unique optical properties in their individual limit such as high binding energy of excitons. The combination of these two systems is of particular interest in understanding various aspects of energy transfer, charge transfer, dynamics of excitons, etc. In this manuscript, we report the anomalous photoluminescence(PL) emission in one such heterostructure MoS2-CdSe QD. We observe multiple exciton emission peaks of the heterostructure on hBN substrate which are absent on SiO2. Our observation op…
Electric field tunable magnetoexcitons in Xenes-hBN-TMDC, Xenes-hBN-BP, and Xenes-hBN-TMTC heterostructures
New York City College of Technology, The City University of New York（纽约市立学院，纽约市立大学）；The Graduate School and University Center, The City University of New York（研究生院与大学中心，纽约市立大学）；Institut für Physik, Universität Augsburg（奥格斯堡大学物理研究所）
Ultrafast charge transfer processes provide a facile way to create interlayer excitons in directly contacted transition metal dichalcogenide (TMD) layers. More sophisticated heterostructures composed of TMD/hBN/TMD enable new ways to control interlayer exciton properties and achieve novel exciton phenomena, such as exciton insulators and condensates, where longer lifetimes are desired. In this work, we experimentally study the charge transfer dynamics in a heterostructure composed of a 1 nm thick hBN spacer between MoSe$_{2}$ and WSe$_{2}$ monolayers. We observe the hole transfer from MoSe$_{2…
The quantum anomalous Hall (QAH) effect is sometimes observed in twisted bilayer graphene (tBG) when it is nearly aligned with an encapsulating hexagonal boron nitride (hBN) layer. We propose that the appearance or absence of the QAH effect in individual devices could be related to commensurability between the graphene/graphene and graphene/hBN moiré patterns. We identify a series of points in the $(θ_{\rm GG},θ_{\rm GBN})$ twist-angle space at which the two moiré patterns are commensurate, allowing moiré band theory to be applied, and show that the band Chern numbers are in this case sensitiv…
