Controlling interlayer excitons in van der Waals heterostructures holds promise for exploring Bose-Einstein condensates and developing novel optoelectronic applications, such as excitonic integrated circuits. Despite intensive studies, several key fundamental properties of interlayer excitons, such as their binding energies and interactions with charges, remain not well understood. Here we report the formation of momentum-direct interlayer excitons in a high-quality MoSe2/hBN/MoSe2 heterostructure under an electric field, characterized by bright photoluminescence (PL) emission with high quantum yield and a narrow linewidth of less than 4 meV. These interlayer excitons show electrically tunable emission energy spanning ~180 meV through the Stark effect, and exhibit a sizable binding energy of ~81 meV in the intrinsic regime, along with trion binding energies of a few millielectronvolts. Remarkably, we demonstrate the long-range transport of interlayer excitons with a characteristic diffusion length exceeding ten micrometers, which can be attributed, in part, to their dipolar repulsive interactions. Spatially and polarization-resolved spectroscopic studies reveal rich exciton physics in the system, such as valley polarization, local trapping, and the possible existence of dark interlayer excitons. The formation and transport of tightly bound interlayer excitons with narrow linewidth, coupled with the ability to electrically manipulate their properties, open exciting new avenues for exploring quantum many-body physics, including excitonic condensate and superfluidity, and for developing novel optoelectronic devices, such as exciton and photon routers.
We study the superlattice minibands produced by the interplay between moiré pattern induced by hexagonal BN substrate on graphene layer and the interlayer coupling in bilayer graphene with Bernal stacking (BLG). We compare moiré miniband features in BLG, where they are affected by the interlayer asymmetry of BLG-hBN heterostructure and trigonal warping characteristic for electrons in Bernal-stacked bilayers with those found in monolayer graphene.
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…
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…
We perform extensive first-principles calculations for heterostructures composed of monolayer graphene and hexagonal boron nitride (hBN). Employing a symmetry-derived minimal tight-binding model, we extract orbital and spin-orbit coupling (SOC) parameters for graphene on hBN, as well as for hBN encapsulated graphene. Our calculations show that the parameters depend on the specific stacking configuration of graphene on hBN. We also perform an interlayer distance study for the different graphene/hBN stacks to find the corresponding lowest energy distances. For very large interlayer distances, on…
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…
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 …
Van der Waals heterostructures constitute a platform for investigating intriguing many-body quantum phenomena. In particular, transition-metal dichalcogenide (TMD) hetero-bilayers host long-lived interlayer excitons which exhibit permanent out-of-plane dipole moments. Here, we develop a microscopic theory for interlayer exciton-exciton interactions including both the dipolar nature of interlayer excitons as well as their fermionic substructure, which gives rise to an attractive fermionic exchange. We find that these interactions contribute to a drift force resulting in highly non-linear excito…
Interlayer coupling between twisted graphenes through atomically-precise barriers
The University of Hong Kong（香港大学）；State Key Laboratory of Optical Quantum Materials, The University of Hong Kong（香港大学光学量子材料国家重点实验室）；National Graphene Institute, University of Manchester（曼彻斯特大学国家石墨烯研究所）；Department of Physics and Astronomy, University of Manchester（曼彻斯特大学物理与天文学系）；Research Center for Electronic and Optical Materials, National Institute for Materials Science（物质材料研究机构电子与光学材料研究中心）；Research Center for Materials Nanoarchitectonics, National Institute for Materials Science（物质材料研究机构材料纳米结构研究中心）
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…
Electric-field-driven magnetic switching and tightly bound interlayer excitons in bilayer CrSBr
Wuhan National High Magnetic Field Center and School of Physics, Huazhong University of Science and Technology（华中科技大学物理学院）；School of Physics and Technology, Wuhan University（武汉大学物理科学与技术学院）；National Institute for Material Science（日本国立材料研究所）
We demonstrate gate-tunable resonant tunneling and negative differential resistance in the interlayer current-voltage characteristics of rotationally aligned double bilayer graphene heterostructures separated by hexagonal boron-nitride (hBN) dielectric. An analysis of the heterostructure band alignment using individual layer densities, along with experimentally determined layer chemical potentials indicates that the resonance occurs when the energy bands of the two bilayer graphene are aligned. We discuss the tunneling resistance dependence on the interlayer hBN thickness, as well as the reson…
The use of high quality hexagonal boron nitride (hBN) as a dielectric material has made possible the realization of graphene devices with very high mobility. In addition hBN can be made as thin as few atomic layers and, as recently demonstrated experimentally, can be used to isolate electrically two graphene layers only few nanometers apart. The combined use of graphene and hBN has therefore opened the possibility to create novel electronic structures. In this work we study the "hybrid" heterostructure formed by one sheet of single layer graphene (SLG) and one sheet of bilayer graphene (BLG) s…
Moiré superlattices in van der Waals heterostructures have emerged as a powerful tool for engineering novel quantum phenomena. Here we report the observation of a correlated interlayer exciton insulator in a double-layer heterostructure composed of a WSe2 monolayer and a WS2/WSe2 moiré bilayer that are separated by an ultrathin hexagonal boron nitride (hBN). The moiré WS2/WSe2 bilayer features a Mott insulator state at hole density p/p0 = 1, where p0 corresponds to one hole per moiré lattice site. When electrons are added to the Mott insulator in the WS2/WSe2 moiré bilayer and an equal number …
The intriguing physics of carrier-carrier interactions, which likewise affect the operation of light emitting devices, stimulate the research on semiconductor structures at high densities of excited carriers, a limit reachable at large pumping rates or in systems with long-lived electron-hole pairs. By electrically injecting carriers into WSe$_2$/MoS$_2$ type-II heterostructures which are indirect in real and k-space, we establish a large population of typical optically silent interlayer excitons. Here, we reveal their emission spectra and show that the emission energy is tunable by an applied…
Vertically stacked van der Waals heterostructures are a lucrative platform for exploring the rich electronic and optoelectronic phenomena in two-dimensional materials. Their performance will be strongly affected by impurities and defects at the interfaces. Here we present the first systematic study of interfaces in van der Waals heterostructure using cross sectional scanning transmission electron microscope (STEM) imaging. By measuring interlayer separations and comparing these to density functional theory (DFT) calculations we find that pristine interfaces exist between hBN and MoS2 or WS2 fo…
The predicted formation of moire superlattices leading to confined excitonic states in heterostructures formed by stacking two lattice mismatched transition metal dichalcogenide (TMD) monolayers was recently experimentally confirmed. Such periodic potential in TMD heterostructure functions as a diffusion barrier that affects the energy transport and dynamics of interlayer excitons (electron and hole spatially concentrated in different monolayers). Understanding the transport of excitons under such condition is essential to establish the material system as a next generation device platform. In …
We investigated experimentally the valley Zeeman splitting of excitonic peaks in the photoluminescence (PL) spectra of high-quality hBN/WS2/MoSe2/hBN heterostructures at near-zero twist angles under perpendicular magnetic fields up to 20 T. We identify two neutral exciton peaks in the PL spectra: the lower energy one exhibits a reduced g-factor relative to that of the higher energy peak, and much lower than the recently reported values for interlayer excitons in other van der Waals (vdW) heterostructures. We provide evidence that such a discernible g-factor stems from the spatial confinement o…
Squeezing bubbles and impurities out of interlayer spaces by applying force through a few-layer graphene capping layer leads to van der Waals heterostructures with ultra-flat structure free from random electrostatic potential arising from charged impurities. Without the graphene capping layer, a squeezing process with an AFM tip induces applied-force-dependent charges of n ~ 2 x 10^12 cm^-2 uN^-1, resulting in strong intensity of trions in photoluminescence spectra of MoSe2 at low temperature. We found that a hBN/MoSe2/hBN prepared with the "modified nano-squeezing method" shows a strong excit…
Monolayers of transition metal dichalcogenides (TMDCs) feature exceptional optical properties that are dominated by excitons, tightly bound electron-hole pairs. Forming van der Waals heterostructures by deterministically stacking individual monolayers allows to tune various properties via choice of materials and relative orientation of the layers. In these structures, a new type of exciton emerges, where electron and hole are spatially separated. These interlayer excitons allow exploration of many-body quantum phenomena and are ideally suited for valleytronic applications. Mostly, a basic mode…
Ultralow-Tensile Strain Enables Exciton Funneling and Energy Transfer to Boost MoSe2 Photoluminescence Quantum Yield
Faculty of Physics, University of Warsaw（华沙大学物理学院）；SPEC, CEA, CNRS, Université Paris-Saclay（法国原子能和替代能源委员会、国家科学研究中心、巴黎萨克雷大学SPEC实验室）；Université Paris-Saclay, ONERA, CNRS, Laboratoire d’étude des microstructures (LEM)（巴黎萨克雷大学、ONERA、国家科学研究中心微结构研究实验室）；School of Basic Sciences, Indian Institute of Technology Bhubaneswar（布巴内斯瓦尔印度理工学院基础科学学院）；Research Center for Materials Nanoarchitectonics, National Institute for Materials Science（物质材料研究机构材料纳米架构研究中心）；Research Center for Electronic and Optical Materials, National Institute for Materials Science（物质材料研究机构电子与光学材料研究中心）
Moire-Engineered Excitonic Landscape and Phonon-Mediated Recombination in Twisted WSe2 Bilayers
Indian Institute of Technology Mandi（印度技术学院曼迪分校）；CSIR-National Physical Laboratory（印度科学工业研究理事会国家物理实验室）；Academy of Scientific and Innovative Research (AcSIR)（科学与创新研究学院）；Indian Institute of Science（印度科学学院）；National Institute of Material Science（国家物质科学研究所）
Atomically-thin layers of two-dimensional materials can be assembled in vertical stacks held together by relatively weak van der Waals forces, allowing for coupling between monolayer crystals with incommensurate lattices and arbitrary mutual rotation. A profound consequence of using these degrees of freedom is the emergence of an overarching periodicity in the local atomic registry of the constituent crystal structures, known as a moiré superlattice. Its presence in graphene/hexagonal boron nitride (hBN) structures led to the observation of electronic minibands, whereas its effect enhanced by …
