Excitons in semiconductors, bound pairs of excited electrons and holes, can form the basis for new classes of quantum optoelectronic devices. A van der Waals heterostructure built from atomically thin semiconducting transition metal dichalcogenides (TMDs) enables the formation of excitons from electrons and holes in distinct layers, producing interlayer excitons with large binding energy and a long lifetime. Employing heterostructures of monolayer TMDs, we realize optical and electrical generation of long-lived neutral and charged interlayer excitons. We demonstrate the transport of neutral interlayer excitons across the whole sample that can be controlled by excitation power and gate electrodes. We also realize the drift motion of charged interlayer excitons using Ohmic-contacted devices. The electrical generation and control of excitons provides a new route for realizing quantum manipulation of bosonic composite particles with complete electrical tunability.As bosonic composite particles, long-lived excitons can be potentially utilized for the realization of coherent quantum many-body systems (1, 2) or as quantum information carriers (3,4). In conventional semiconductors, the exciton lifetime can be increased by constructing double quantum well (DQW) heterostructures, where spatially separated electrons and holes form interlayer excitons (IEs) across the quantum wells (5-10). Strongly bound IEs can also be formed in atomically thin DQW. By stacking two

When an optical dipole is in proximity to a metallic substrate, it can emit light into both far field photons and SPPs. Far-field emission can be measured directly via top-down optical microscopy, whereas SPP emission can be detected by converting SPPs into far-field light via engineered out-coupling structures (Fig. 1a). On a single-crystal silver film, our metal of choice due to its low loss 11 , SPPs are strongly polarized in the out-of-plane (z) direction in the visible frequency range (see Supplementary Information). Consequently, the emission rate into SPPs for an out-of-plane dipole can be as high as 30 times larger than that of an in-plane dipole (Figs. 1b-d, for details of the analysis see Supplementary Information). At the same time, far-field emission of an in-plane dipole is strongly suppressed (Figs. 1b and d) because the in-plane electric field is close to zero near the silver surface. We note that when a point dipole is close to a metal 12 , non-radiative recombination due to ohmic loss can be the dominant decay mechanism.Remarkably, for delocalized excitons in quantum wells and 2D materials, quenching of exciton luminescence by ohmic loss is significantly reduced, even when they are placed 10 nm above a silver surface ( see [ 13 ] and Supplementary Fig. 1 and discussion). Combined together, the net effect of a nearby silver surface is significantly enhanced (suppressed) emission of an out-ofplane (in-plane) dipole into SPPs (far field). (Fig. 1a). The spacing between the monolayer TMD and the silver surface is determined by the bottom hBN thickness, and can easily be controlled by varying hBN thickness. In our devices, the typical spacing is on the order of ten nanometers.Excitons are created using off-resonant 660-nm laser excitation, and the PL spectra are voltages. We normalize both FF and SPP-PL spectra using the intensity of a charged exciton peak X T because it is known to involve a purely in-plane transition dipole moment 16 . The ratio of SPP-PL intensity to the FF-PL intensity after the normalization provides a direct measure of the orientation of the transition dipole for each luminescent species: the unity ratio represents a purely in-plane dipole, while a value larger than one indicates that the transition dipole has some out-of-plane components. Based on our theoretical calculations presented in Fig. 1d and Supplementary Fig. 4, an optical transition with a purely out-of-plane transition dipole should have a normalized coupling ratio of 7 in our device geometry. The experimental results for X D yield a value of 16: this discrepancy between theory and experiment is likely due to small, yet non-negligible absorption of SPPs by charged excitons as they propagate through the WSe 2 , which increases the apparent coupling ratio of X D after normalization (see Supplementary Fig. 5). Indeed, when SPPs propagate through a minimal distance within WSe 2 ( Supplementary Fig. 6), the normalized coupling ratio determined by experiment is close to 7, in good agreement with the theoretical calc...

Tuning electrical conductivity of semiconducting materials through substitutional doping is crucial for fabricating functional devices. This, however, has not been fully realized in two-dimensional (2D) materials due to the difficulty of homogeneously controlling the dopant concentrations and the lack of systematic study of the net impact of substitutional dopants separate from that of the unintentional doping from the device fabrication processes. Here, we grow wafer-scale, continuous MoS2 monolayers with tunable concentrations of Nb and Re and fabricate devices using a polymer-free approach to study the direct electrical impact of substitutional dopants in MoS2 monolayers. In particular, the electrical conductivity of Nb doped MoS2 in the absence of electrostatic gating is reproducibly tuned over 7 orders of magnitude by controlling the Nb concentration. Our study further indicates that the dopant carriers do not fully ionize in the 2D limit, unlike in their three-dimensional analogues, which is explained by weaker charge screening and impurity band conduction. Moreover, we show that the dopants are stable, which enables the doped films to be processed as independent building blocks that can be used as electrodes for functional circuitry.

Moiré superlattices in twisted van der Waals materials constitute a promising platform for engineering electronic and optical properties. However, a major obstacle to fully understanding these systems and harnessing their potential is the limited ability to correlate the local moiré structure with optical properties. By using a recently developed scanning electron microscopy technique to image twisted WSe2/WSe2 bilayers, we directly correlate increasing moiré periodicity with the emergence of two distinct exciton species. These can be tuned individually through electrostatic gating, and feature different valley coherence properties. Our observations can be understood as resulting from an array of two intralayer exciton species residing in alternating locations in the superlattice, and illuminate the influence of the moiré potential on lateral exciton motion. They open up new avenues for controlling exciton arrays in twisted TMDs, with applications in quantum optoelectronics and explorations of novel many body systems. Engineered moiré superlattices arising from lattice mismatch or relative twist angle between layers can induce periodic potentials for charge carriers and excitons. While

Structural engineering of van der Waals heterostructures via stacking and twisting has recently been used to create moiré superlattices 1,2 , enabling the realization of new optical and electronic properties in solid-state systems. In particular, moiré lattices in twisted bilayers of transition metal dichalcogenides (TMDs) have been shown to lead to exciton trapping 3-8 , host Mott insulating and superconducting states 9 , and act as unique Hubbard systems 10-13 whose correlated electronic states can be detected and manipulated optically. Structurally, these twisted heterostructures also feature atomic reconstruction and domain formation 14-20. Unfortunately, due to the nanoscale sizes (~10 nm) of typical moiré domains, the effects of atomic reconstruction on the electronic and excitonic properties of these heterostructures could not be investigated systematically and have often been ignored. Here, we use near-0 o twist angle MoSe2/MoSe2 bilayers with large rhombohedral AB/BA domains 21 to directly probe excitonic properties of individual domains with far-field optics. We show that this system features broken mirror/inversion symmetry, with the AB and BA domains supporting interlayer excitons with out-of-plane (z) electric dipole moments in opposite directions. The dipole orientation of ground-state -K interlayer excitons (XI,1) can be flipped with electric fields, while higher-energy K-K interlayer excitons (XI,2) undergo fieldasymmetric hybridization with intralayer K-K excitons (X0). Our study reveals the profound impacts of crystal symmetry on TMD excitons and points to new avenues for realizing topologically nontrivial systems 22,23 , exotic metasurfaces 24,25 , collective excitonic phases 26-28 , and quantum emitter arrays 29,30 via domain-pattern engineering. To date, most studies of twisted TMD bilayers have assumed a rigid rotation of layers without atomic-scale rearrangement 3-8. However, recent theoretical 14-16 and experimental 17-20 studies have

We study the impact of electrode band structure on transport through single--molecule junctions by measuring the conductance of pyridine--based molecules using Ag and Au electrodes. Our experiments are carried out using the scanning tunneling microscope based break--junction technique and are supported by density functional theory based calculations. We find from both experiments and calculations that the coupling of the dominant transport orbital to the metal is stronger for Au--based junctions when compared with Ag--based junctions. We attribute this difference to relativistic effects, which results in an enhanced density of d--states at the Fermi energy for Au compared with Ag. We further show that the alignment of the conducting orbital relative to the Fermi level does not follow the work function difference between two metals and is different for conjugated and saturated systems. We thus demonstrate that the details of the molecular level alignment and electronic coupling in metal--organic interfaces do not follow simple rules, but are rather the consequence of subtle local interactions.

The twist degree of freedom provides a powerful new tool for engineering the electrical and optical properties of van der Waals heterostructures. Here, we show that the twist angle can be used to control the spin-valley properties of transition metal dichalcogenide bilayers by changing the momentum alignment of the valleys in the two layers. Specifically, we observe that the interlayer excitons in twisted WSe 2 =WSe 2 bilayers exhibit a high (>60%) degree of circular polarization (DOCP) and long valley lifetimes (>40 ns) at zero electric and magnetic fields. The valley lifetime can be tuned by more than 3 orders of magnitude via electrostatic doping, enabling switching of the DOCP from ∼80% in the n-doped regime to <5% in the p-doped regime. These results open up new avenues for tunable chiral light-matter interactions, enabling novel device schemes that exploit the valley degree of freedom.

We demonstrate a new approach for dynamically manipulating the optical response of an atomically thin semiconductor, a monolayer of MoSe2, by suspending it over a metallic mirror. First, we show that suspended van der Waals heterostructures incorporating a MoSe2 monolayer host spatially homogeneous, lifetime-broadened excitons. Then, we interface this nearly ideal excitonic system with a metallic mirror and demonstrate control over the exciton-photon coupling. Specifically, by electromechanically changing the distance between the heterostructure and the mirror, thereby changing the local photonic density of states in a controllable and reversible fashion, we show that both the absorption and emission properties of the excitons can be dynamically modulated. This electromechanical control over exciton dynamics in a mechanically flexible, atomically thin semiconductor opens up new avenues in cavity quantum optomechanics, nonlinear quantum optics, and topological photonics.