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Quantum confinement in atomically-thin TMDCs enables the realization of deterministic single-photon emitters. The position and polarization control of single photons have been achieved via local strain engineering using nanostructures. However, most existing TMDC-based emitters are operated by optical pumping, while the emission sites in electrically pumped emitters are uncontrolled. Here, we demonstrate electrically driven single-photon emitters located at the positions where strains are induced by atomic-force-microscope indentation on a van der Waals heterostructure consisting of graphene, hexagonal-boron nitride, and tungsten diselenide. The optical, electrical, and mechanical properties induced by the local strain gradient were systematically analyzed. In particular, single-photon emission was observed at the indentation sites at 4 K. The emission exhibits photon anti-bunching behavior with a g(2)(0) value of ~0.3, intensity saturation and a linearly cross-polarized doublet. This robust spatial control of electrically driven single-photon emitters will pave the way for the practical implementation of integrated quantum light sources.
Moire patterns with a superlattice potential can be formed by vertically stacking two layered materials with a relative twist or lattice constant mismatch. The moire superlattice can generate flat bands that result in new correlated insulating, super conducting, and topological states. Strong electron correlations, tunable by the fractional filling, have been observed in both graphene and transition metal dichalcogenide (TMD) based systems. In addition, in TMD based systems, the moire potential landscape can trap interlayer excitons (IX) at specific atomic registries. Here we report that spatially isolated trapped IX in a molybdenum diselenide/tungsten diselenide heterobilayer device provide a sensitive optical probe of carrier filling in their immediate environment. By mapping the spatial positions of individual trapped IX, we are able to spectrally track the emitters as the moire lattice is filled with excess carriers. Upon initial doping of the heterobilayer, neutral trapped IX form charged IX (IX trions) uniformly with a binding energy of ~7 meV. Upon further doping, the empty superlattice sites sequentially fill, creating a Coulomb staircase: stepwise changes in the IX trion emission energy due to Coulomb interactions with carriers at nearest neighbour moire sites. This non-invasive, highly local technique can complement transport and non-local optical sensing techniques to characterise Coulomb interaction energies, visualise charge correlated states, or probe local disorder in a moire superlattice.
Transition metal dichalcogenide heterobilayers offer attractive opportunities to realize lattices of interacting bosons with several degrees of freedom. Such heterobilayers can feature moire patterns that modulate their electronic band structure, lea ding to spatial confinement of single interlayer excitons (IXs) that act as quantum emitters with $C_3$ symmetry. However, the narrow emission linewidths of the quantum emitters contrast with a broad ensemble IX emission observed in nominally identical heterobilayers, opening a debate regarding the origin of IX emission. Here we report the continuous evolution from a few trapped IXs to an ensemble of IXs with both triplet and singlet spin configurations in a gate-tunable $2H$-MoSe$_2$/WSe$_2$ heterobilayer. We observe signatures of dipolar interactions in the IX ensemble regime which, when combined with magneto-optical spectroscopy, reveal that the narrow quantum-dot-like and broad ensemble emission originate from IXs trapped in moire potentials with the same atomic registry. Finally, electron doping leads to the formation of three different species of localised negative trions with contrasting spin-valley configurations, among which we observe both intervalley and intravalley IX trions with spin-triplet optical transitions. Our results identify the origin of IX emission in MoSe$_2$/WSe$_2$ heterobilayers and highlight the important role of exciton-exciton interactions and Fermi-level control in these highly tunable quantum materials.
Photon antibunching, a hallmark of quantum light, has been observed in the correlations of light from isolated atomic and atomic-like solid-state systems. Two-dimensional semiconductor heterostructures offer a unique method to create a quantum light source: a small lattice mismatch or relative twist in a heterobilayer can create moire trapping potentials for excitons which are predicted to create arrays of quantum emitters. While signatures of moire trapped excitons have been observed, their quantum nature has yet to be confirmed. Here we report photon antibunching from single moire trapped interlayer excitons in a heterobilayer. Via polarization resolved magneto-optical spectroscopy, we demonstrate the discrete anharmonic spectra arise from bound band-edge electron-hole pairs trapped in moire potentials. Finally, using an out-of-plane electric field, we exploit the large permanent dipole of interlayer excitons to achieve large DC Stark tuning, up to 40 meV, of the quantum emitters. Our results confirm the quantum nature of moire confined excitons and open opportunities to investigate their inhomogeneity and interactions between the emitters or tune single emitters into resonance with cavity modes or other emitters.
Van der Waals heterostructures offer attractive opportunities to design quantum materials. For instance, transition metal dichalcogenides (TMDs) possess three quantum degrees of freedom: spin, valley index, and layer index. Further, twisted TMD heter obilayers can form moire patterns that modulate the electronic band structure according to atomic registry, leading to spatial confinement of interlayer exciton (IXs). Here we report the observation of spin-layer locking of IXs trapped in moire potentials formed in a heterostructure of bilayer 2H-MoSe$_2$ and monolayer WSe$_2$. The phenomenon of locked electron spin and layer index leads to two quantum-confined IX species with distinct spin-layer-valley configurations. Furthermore, we observe that the atomic registries of the moire trapping sites in the three layers are intrinsically locked together due to the 2H-type stacking characteristic of bilayer TMDs. These results identify the layer index as a useful degree of freedom to engineer tunable few-level quantum systems in two-dimensional heterostructures.
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