Van der Waals materials offer a wide range of atomic layers with unique properties that can be easily combined to engineer novel electronic and photonic devices. A missing ingredient of the van der Waals platform is a two-dimensional crystal with naturally occurring out-of-plane luminescent dipole orientation. Here we measure the far-field photoluminescence intensity distribution of bulk InSe and two-dimensional InSe, WSe 2 and MoSe 2 . We demonstrate, with the support of ab-initio calculations, that layered InSe flakes sustain luminescent excitons with an intrinsic out-of-plane orientation, in contrast with the in-plane orientation of dipoles we find in two-dimensional WSe 2 and MoSe 2 at room-temperature. These results, combined with the high tunability of the optical response and outstanding transport properties, position layered InSe as a promising semiconductor for novel optoelectronic devices, in particular for hybrid integrated photonic chips which exploit the out-of-plane dipole orientation.
MoTe 2 belongs to the semiconducting transition-metal dichalcogenide family with certain properties differing from the other well-studied members (Mo,W)(S,Se) 2. The optical band gap is in the near-infrared region, and both monolayers and bilayers may have a direct optical band gap. We first simulate the single-particle band structure of both monolayer and bilayer MoTe 2 with density-functional-theory-GW calculations. We find a direct (indirect) electronic band gap for the monolayer (bilayer). By solving in addition the Bethe-Salpeter equation, we find similar energies for the direct exciton transitions in monolayers and bilayers. We then study the optical properties by means of photoluminescence (PL) excitation, reflectivity, time-resolved PL, and power-dependent PL spectroscopy. With differential reflectivity, we find a similar oscillator strength for the optical transition observed in PL in both monolayers and bilayers suggesting a direct transition in both cases. We identify the same energy for the B-exciton state in the monolayer and the bilayer. Following circularly polarized excitation, we do not find any exciton polarization for a large range of excitation energies. At low temperatures (T = 10 K), we measure similar PL decay times on the order of 4 ps for both monolayer and bilayer excitons with a slightly longer one for the bilayer. Finally, we observe a reduction of the exciton-exciton annihilation contribution to the nonradiative recombination in bilayers.
Gate-tunable quantum-mechanical tunnelling of particles between a quantum confined state and a nearbyFermi reservoir of delocalized states has underpinned many advances in spintronics and solid-state quantum optics. The prototypical example is a semiconductor quantum dot separated from a gated contact by a tunnel barrier. This enables Coulomb blockade, the phenomenon whereby electrons or holes can be loaded one-by-one into a quantum dot 1,2 . Depending on the tunnel-coupling strength 3,4 , this capability facilitates single spin quantum bits 1,2,5 or coherent many-body interactions between the confined spin and the Fermi reservoir 6,7 . Van der Waals (vdW) heterostructures, in which a wide range of unique atomic layers can easily be combined, offer novel prospects to engineer coherent quantum confined spins 8,9 , tunnel barriers down to the atomic limit 10 or a Fermi reservoir beyond the conventional flat density of states 11 . However, gatecontrol of vdW nanostructures 12-16 at the single particle level is needed to unlock their potential. Here we report Coulomb blockade in a vdW heterostructure consisting of a transition metal dichalcogenide quantum dot coupled to a graphene contact through an atomically thin hexagonal boron nitride (hBN) tunnel barrier. Thanks to a tunable Fermi reservoir, we can deterministically load either a single electron or a single hole into the quantum dot. We observe hybrid excitons, composed of localized quantum dot states and delocalized continuum states, arising from ultra-strong spin-conserving tunnel coupling through the atomically thin tunnel barrier. Probing the charged excitons in applied magnetic fields, we observe large gyromagnetic ratios (∼8). Our results establish a foundation for engineering next-generation devices to investigate either novel regimes of Kondo physics or isolated quantum bits in a vdW heterostructure platform. Supplementary Figure 5. Lineshape evolution of the excitons states as a function of the gate voltage.Photoluminescence spectra of quantum dots A and B for different applied gate voltage values measured at T = 3.8 K. The green and red labels indicate the charged exciton states for quantum dots A and B, respectively. Labels X 1-, X 0 , X 1+ and X H represent the negatively charged, neutral, positively charged and hybrid excitons, respectively. For comparison purposes, some spectra have been multiplied by the corresponding factors indicated at the left part of the figure.
Efficient on-chip integration of single-photon emitters imposes a major bottleneck for applications of photonic integrated circuits in quantum technologies. Resonantly excited solid-state emitters are emerging as near-optimal quantum light sources, if not for the lack of scalability of current devices. Current integration approaches rely on cost-inefficient individual emitter placement in photonic integrated circuits, rendering applications impossible. A promising scalable platform is based on two-dimensional (2D) semiconductors. However, resonant excitation and single-photon emission of waveguide-coupled 2D emitters have proven to be elusive. Here, we show a scalable approach using a silicon nitride photonic waveguide to simultaneously strain-localize single-photon emitters from a tungsten diselenide (WSe 2 ) monolayer and to couple them into a waveguide mode. We demonstrate the guiding of single photons in the photonic circuit by measuring second-order autocorrelation of g (2) (0) = 0.150 ± 0.093 and perform on-chip resonant excitation, yielding a g (2) (0) = 0.377 ± 0.081. Our results are an important step to enable coherent control of quantum states and multiplexing of highquality single photons in a scalable photonic quantum circuit.
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