Energy-resolved Photoconductivity Mapping in a Monolayer-bilayer WSe2 Lateral Heterostructure

Vertical and lateral heterostructures of van der Waals materials provide tremendous flexibility for band structure engineering. Since electronic bands are sensitively affected by defects, strain, and interlayer coupling, the edge and heterojunction of these two-dimensional (2D) systems may exhibit novel physical properties, which can be fully revealed only by spatially resolved probes. Here, we report the spatial mapping of photoconductivity in a monolayer-bilayer WSe2 lateral heterostructure under multiple excitation lasers. As the photon energy increases, the light-induced conductivity detected by microwave impedance microscopy first appears along the hetero-interface and bilayer edge, then along the monolayer edge, inside the bilayer area, and finally in the interior of the monolayer region. The sequential emergence of mobile carriers in different sections of the sample is consistent with the theoretical calculation of local energy gaps. Quantitative analysis of the microscopy and transport data also reveals the linear dependence of photoconductivity on the laser intensity and the influence of interlayer coupling on carrier recombination. Combining theoretical modeling, atomic scale imaging, mesoscale impedance microscopy, and device-level characterization, our work suggests an exciting perspective to control the intrinsic band-gap variation in 2D heterostructures down to the few-nanometer regime.Comment: 18 pages, 5 figures; Nano Lett., Just Accepted Manuscrip

Tailoring excitonic states of van der Waals bilayers through stacking configuration, band alignment and valley-spin

Excitons in monolayer semiconductors have large optical transition dipole for strong coupling with light field. Interlayer excitons in heterobilayers, with layer separation of electron and hole components, feature large electric dipole that enables strong coupling with electric field and exciton-exciton interaction, at the cost that the optical dipole is substantially quenched (by several orders of magnitude). In this letter, we demonstrate the ability to create a new class of excitons in transition metal dichalcogenide (TMD) hetero- and homo-bilayers that combines the advantages of monolayer- and interlayer-excitons, i.e. featuring both large optical dipole and large electric dipole. These excitons consist of an electron that is well confined in an individual layer, and a hole that is well extended in both layers, realized here through the carrier-species specific layer-hybridization controlled through the interplay of rotational, translational, band offset, and valley-spin degrees of freedom. We observe different species of such layer-hybridized valley excitons in different heterobilayer and homobilayer systems, which can be utilized for realizing strongly interacting excitonic/polaritonic gases, as well as optical quantum coherent controls of bidirectional interlayer carrier transfer either with upper conversion or down conversion in energy

Point Defects and Localized Excitons in 2D WSe2

Identifying the point defects in 2D materials is important for many applications. Recent studies have proposed that W vacancies are the predominant point defect in 2D WSe2, in contrast to theoretical studies, which predict that chalcogen vacancies are the most likely intrinsic point defects in transition metal dichalcogenide semiconductors. We show using first principles calculations, scanning tunneling microscopy (STM) and scanning transmission electron microscopy experiments, that W vacancies are not present in our CVD-grown 2D WSe2. We predict that O-passivated Se vacancies (O_Se) and O interstitials (Oins) are present in 2D WSe2, because of facile O2 dissociation at Se vacancies, or due to the presence of WO3 precursors in CVD growth. These defects give STM images in good agreement with experiment. The optical properties of point defects in 2D WSe2 are important because single photon emission (SPE) from 2D WSe2 has been observed experimentally. While strain gradients funnel the exciton in real space, point defects are necessary for the localization of the exciton at length scales that enable photons to be emitted one at a time. Using state-of-the-art GW-Bethe-Salpeter-equation calculations, we predict that only Oins defects give localized excitons within the energy range of SPE in previous experiments, making them a likely source of previously observed SPE. No other point defects (O_Se, Se vacancies, W vacancies and Se_W antisites) give localized excitons in the same energy range. Our predictions suggest ways to realize SPE in related 2D materials and point experimentalists toward other energy ranges for SPE in 2D WSe2

G band Raman double resonance in twisted bilayer graphene: an evidence of band splitting and folding

The stacking faults (deviates from Bernal) will break the translational symmetry of multilayer graphenes and modify their electronic and optical behaviors to the extent depending on the interlayer coupling strength. This paper addresses the stacking-induced band splitting and folding effect on the electronic band structure of twisted bilayer graphene. Based on the first-principles density functional theory study, we predict that the band folding effect of graphene layers may enable the G band Raman double resonance in the visible excitation range. Such prediction is confirmed experimentally with our Raman observation that the resonant energies of the resonant G mode are strongly dependent on the stacking geometry of graphene layers.Comment: 16 pages, 4 figures, Accepted by Phys. Rev.

Atomically Thin Resonant Tunnel Diodes built from Synthetic van der Waals Heterostructures

Vertical integration of two-dimensional van der Waals materials is predicted to lead to novel electronic and optical properties not found in the constituent layers. Here, we present the direct synthesis of two unique, atomically thin, multi-junction heterostructures by combining graphene with the monolayer transition-metal dichalocogenides: MoS2, MoSe2, and WSe2.The realization of MoS2-WSe2-Graphene and WSe2-MoSe2-Graphene heterostructures leads toresonant tunneling in an atomically thin stack with spectrally narrow room temperature negative differential resistance characteristics