Van der Waals heterostructures have recently emerged as a new class of materials, where quantum coupling between stacked atomically thin two-dimensional layers, including graphene, hexagonal-boron nitride and transition-metal dichalcogenides (MX2), give rise to fascinating new phenomena. MX2 heterostructures are particularly exciting for novel optoelectronic and photovoltaic applications, because two-dimensional MX2 monolayers can have an optical bandgap in the near-infrared to visible spectral range and exhibit extremely strong light-matter interactions. Theory predicts that many stacked MX2 heterostructures form type II semiconductor heterojunctions that facilitate efficient electron-hole separation for light detection and harvesting. Here, we report the first experimental observation of ultrafast charge transfer in photoexcited MoS2/WS2 heterostructures using both photoluminescence mapping and femtosecond pump-probe spectroscopy. We show that hole transfer from the MoS2 layer to the WS2 layer takes place within 50 fs after optical excitation, a remarkable rate for van der Waals coupled two-dimensional layers. Such ultrafast charge transfer in van der Waals heterostructures can enable novel two-dimensional devices for optoelectronics and light harvesting.

Moiré superlattices provide a powerful tool to engineer novel quantum phenomena in twodimensional (2D) heterostructures, where the interactions between the atomically thin layers qualitatively change the electronic band structure of the superlattice. For example, mini-Dirac points, tunable Mott insulator states, and the Hofstadter butterfly can emerge in different types of graphene/boron nitride moiré superlattices, while correlated insulating states and superconductivity have been reported in twisted bilayer graphene moiré superlattices 1-12 . In addition to their dramatic effects on the single particle states, moiré superlattices were recently predicted to host novel excited states, such as moiré exciton bands [13][14][15] . Here we report the first observation of moiré superlattice exciton states in nearly aligned WSe 2 /WS 2 heterostructures.These moiré exciton states manifest as multiple emergent peaks around the original WSe 2 A exciton resonance in the absorption spectra, and they exhibit gate dependences that are distinctly different from that of the A exciton in WSe 2 monolayers and in large-twist-angle WSe 2 /WS 2 heterostructures. The observed phenomena can be described by a theoretical model where the periodic moiré potential is much stronger than the exciton kinetic energy and creates multiple flat exciton minibands. The moiré exciton bands provide an attractive platform to explore and control novel excited state of matter, such as topological excitons and a correlated exciton Hubbard model, in transition metal dichalcogenides.

Van der Waals coupling is emerging as a powerful method to engineer physical properties of atomically thin two-dimensional materials. In coupled graphene-graphene and graphene-boron nitride layers, interesting physical phenomena ranging from Fermi velocity renormalization to Hofstadter's butterfly pattern have been demonstrated. Atomically thin transition metal dichalcogenides, another family of two-dimensional-layered semiconductors, can show distinct coupling phenomena. Here we demonstrate the evolution of interlayer coupling with twist angles in as-grown molybdenum disulfide bilayers. We find that the indirect bandgap size varies appreciably with the stacking configuration: it shows the largest redshift for AA-and AB-stacked bilayers, and a significantly smaller but constant redshift for all other twist angles. Our observations, together with ab initio calculations, reveal that this evolution of interlayer coupling originates from the repulsive steric effects that leads to different interlayer separations between the two molybdenum disulfide layers in different stacking configurations.

Abstract:Phosphorene, a single atomic layer of black phosphorus, has recently emerged as a new twodimensional (2D) material that holds promise for electronic and photonic technology. Here we experimentally demonstrate that the electronic structure of few-layer phosphorene varies significantly with the number of layers, in good agreement with theoretical predictions. The interband optical transitions cover a wide, technologically important spectrum range from visible to mid-infrared. In addition, we observe strong photoluminescence in few-layer phosphorene at energies that match well with the absorption edge, indicating they are direct bandgap semiconductors. The strongly layer-dependent electronic structure of phosphorene, in combination with its high electrical mobility, gives it distinct advantages over other twodimensional materials in electronic and opto-electronic applications.Page 3 of 17! ! Atomically thin 2D crystals have emerged as a new class of materials with unique material properties that are potentially important for electronic and photonic technologies [1][2][3][4][5][6][7][8][9][10] . Various 2D crystals have been uncovered, ranging from metallic (and superconducting) NbSe 2 and semimetallic graphene to semiconducting MoS 2 and insulating hexagonal boron nitride (hBN).The energy bandgap, a defining characteristic of an electronic material, varies correspondingly from 0 (in metals and graphene) to 5.8 eV (in hBN) in these 2D crystals. Despite the rich variety currently available, 2D materials with a bandgap in the range from 0.3 eV to 1.5 eV are notably missing 11 . Such a bandgap corresponds to a spectral range from mid-infrared to near-infrared that is important for optoelectronic technologies such as telecommunication and solar energy harvesting. It is therefore desirable to have 2D materials with a bandgap that falls in this range, and in particular, matches that of the technologically important silicon (bandgap = 1.1 eV) and III-V semiconductors like InGaAs, without compromising sample mobility 12 .Monolayer and few-layer phosphorene are predicted to bridge the much needed bandgap range from 0.3 to 2 eV (Refs. 13-17). Inside monolayer phosphorene, each phosphorus atom is covalently bonded with three adjacent phosphorus atoms to form a puckered honeycomb structure 18 . The three near sp 3 bonds together with the lone-pair orbital take up all five valence electrons of phosphorus, so monolayer phosphorene is a semiconductor with a predicted direct optical bandgap of ~ 1.5 eV at the Γ point of the Brillouin zone. The bandgap in few-layer phosphorene can be strongly modified by interlayer interactions, which leads to a bandgap that decreases with phosphorene film thickness, eventually reaching 0.3 eV in the bulk limit.Experimental observations of layer-dependent band structure in phosphorene, on the other hand, have been rather limited. Previously, photoluminescence (PL) spectroscopy has been used to probe the bandgap of monolayer and few-layer phosphorene 8,[19][20][21][22] . Such studies, howeve...

Electron valley, a degree of freedom that is analogous to spin, can lead to novel topological phases in bilayer graphene. A tunable bandgap can be induced in bilayer graphene by an external electric field, and such gapped bilayer graphene is predicted to be a topological insulating phase protected by no-valley mixing symmetry, featuring quantum valley Hall effects and chiral edge states. Observation of such chiral edge states, however, is challenging because inter-valley scattering is induced by atomic-scale defects at real bilayer graphene edges. Recent theoretical work has shown that domain walls between AB- and BA-stacked bilayer graphene can support protected chiral edge states of quantum valley Hall insulators. Here we report an experimental observation of ballistic (that is, with no scattering of electrons) conducting channels at bilayer graphene domain walls. We employ near-field infrared nanometre-scale microscopy (nanoscopy) to image in situ bilayer graphene layer-stacking domain walls on device substrates, and we fabricate dual-gated field effect transistors based on the domain walls. Unlike single-domain bilayer graphene, which shows gapped insulating behaviour under a vertical electrical field, bilayer graphene domain walls feature one-dimensional valley-polarized conducting channels with a ballistic length of about 400 nanometres at 4 kelvin. Such topologically protected one-dimensional chiral states at bilayer graphene domain walls open up opportunities for exploring unique topological phases and valley physics in graphene.