High Q Hybrid Mie-Plasmonic Resonances in van der Waals Nanoantennas on Gold Substrate.

Dielectric nanoresonators have been shown to circumvent the heavy optical losses associated with plasmonic devices; however, they suffer from less confined resonances. By constructing a hybrid system of both dielectric and metallic materials, one can retain low losses, while achieving stronger mode confinement. Here, we use a high refractive index multilayer transition-metal dichalcogenide WS2 exfoliated on gold to fabricate and optically characterize a hybrid nanoantenna-on-gold system. We experimentally observe a hybridization of Mie resonances, Fabry-Perot modes, and surface plasmon-polaritons launched from the nanoantennas into the substrate. We measure the experimental quality factors of hybridized Mie-plasmonic (MP) modes to be up to 33 times that of standard Mie resonances in the nanoantennas on silica. We then tune the nanoantenna geometries to observe signatures of a supercavity mode with a further increased Q factor of over 260 in experiment. We show that this quasi-bound state in the continuum results from strong coupling between a Mie resonance and Fabry-Perot-plasmonic mode in the vicinity of the higher-order anapole condition. We further simulate WS2 nanoantennas on gold with a 5 nm thick hBN spacer in between. By placing a dipole within this spacer, we calculate the overall light extraction enhancement of over 107, resulting from the strong, subwavelength confinement of the incident light, a Purcell factor of over 700, and high directivity of the emitted light of up to 50%. We thus show that multilayer TMDs can be used to realize simple-to-fabricate, hybrid dielectric-on-metal nanophotonic devices granting access to high-Q, strongly confined, MP resonances, along with a large enhancement for emitters in the TMD-gold gap.

Nonlinear Rydberg exciton-polaritons in Cu2O microcavities.

Rydberg excitons (analogues of Rydberg atoms in condensed matter systems) are highly excited bound electron-hole states with large Bohr radii. The interaction between them as well as exciton coupling to light may lead to strong optical nonlinearity, with applications in sensing and quantum information processing. Here, we achieve strong effective photon-photon interactions (Kerr-like optical nonlinearity) via the Rydberg blockade phenomenon and the hybridisation of excitons and photons forming polaritons in a Cu2O-filled microresonator. Under pulsed resonant excitation polariton resonance frequencies are renormalised due to the reduction of the photon-exciton coupling with increasing exciton density. Theoretical analysis shows that the Rydberg blockade plays a major role in the experimentally observed scaling of the polariton nonlinearity coefficient as ∝ n4.4±1.8 for principal quantum numbers up to n = 7. Such high principal quantum numbers studied in a polariton system for the first time are essential for realisation of high Rydberg optical nonlinearities, which paves the way towards quantum optical applications and fundamental studies of strongly correlated photonic (polaritonic) states in a solid state system.

Resonant Band Hybridization in Alloyed Transition Metal Dichalcogenide Heterobilayers.

Bandstructure engineering using alloying is widely utilized for achieving optimized performance in modern semiconductor devices. While alloying has been studied in monolayer transition metal dichalcogenides, its application in van der Waals heterostructures built from atomically thin layers is largely unexplored. Here, heterobilayers made from monolayers of WSe2 (or MoSe2) and MoxW1 - xSe2 alloy are fabricated and nontrivial tuning of the resultant bandstructure is observed as a function of concentration x. This evolution is monitored by measuring the energy of photoluminescence (PL) of the interlayer exciton (IX) composed of an electron and hole residing in different monolayers. In MoxW1 - xSe2/WSe2, a strong IX energy shift of ≈100 meV is observed for x varied from 1 to 0.6. However, for x < 0.6 this shift saturates and the IX PL energy asymptotically approaches that of the indirect bandgap in bilayer WSe2. This observation is theoretically interpreted as the strong variation of the conduction band K valley for x > 0.6, with IX PL arising from the K - K transition, while for x < 0.6, the bandstructure hybridization becomes prevalent leading to the dominating momentum-indirect K - Q transition. This bandstructure hybridization is accompanied with strong modification of IX PL dynamics and nonlinear exciton properties. This work provides foundation for bandstructure engineering in van der Waals heterostructures highlighting the importance of hybridization effects and opening a way to devices with accurately tailored electronic properties.

Interspecies exciton interactions lead to enhanced nonlinearity of dipolar excitons and polaritons in MoS2 homobilayers.

Nonlinear interactions between excitons strongly coupled to light are key for accessing quantum many-body phenomena in polariton systems. Atomically-thin two-dimensional semiconductors provide an attractive platform for strong light-matter coupling owing to many controllable excitonic degrees of freedom. Among these, the recently emerged exciton hybridization opens access to unexplored excitonic species, with a promise of enhanced interactions. Here, we employ hybridized interlayer excitons (hIX) in bilayer MoS2 to achieve highly nonlinear excitonic and polaritonic effects. Such interlayer excitons possess an out-of-plane electric dipole as well as an unusually large oscillator strength allowing observation of dipolar polaritons (dipolaritons) in bilayers in optical microcavities. Compared to excitons and polaritons in MoS2 monolayers, both hIX and dipolaritons exhibit ≈ 8 times higher nonlinearity, which is further strongly enhanced when hIX and intralayer excitons, sharing the same valence band, are excited simultaneously. This provides access to an unusual nonlinear regime which we describe theoretically as a mixed effect of Pauli exclusion and exciton-exciton interactions enabled through charge tunnelling. The presented insight into many-body interactions provides new tools for accessing few-polariton quantum correlations.

Synthesis of mono- and few-layered n-type WSe2 from solid state inorganic precursors.

Tuning the charge transport properties of two-dimensional transition metal dichalcogenides (TMDs) is pivotal to their future device integration in post-silicon technologies. To date, co-doping of TMDs during growth still proves to be challenging, and the synthesis of doped WSe2, an otherwise ambipolar material, has been mainly limited to p-doping. Here, we demonstrate the synthesis of high-quality n-type monolayered WSe2 flakes using a solid-state precursor for Se, zinc selenide. n-Type transport has been reported with prime electron mobilities of up to 10 cm2 V-1 s-1. We also demonstrate the tuneability of doping to p-type transport with hole mobilities of 50 cm2 V-1 s-1 after annealing in air. n-Doping has been attributed to the presence of Zn adatoms on the WSe2 flakes as revealed by X-ray photoelectron spectroscopy (XPS), spatially resolved time of flight secondary ion mass spectroscopy (SIMS) and angular dark-field scanning transmission electron microscopy (AD-STEM) characterization of WSe2 flakes. Monolayer WSe2 flakes exhibit a sharp photoluminescence (PL) peak at room temperature and highly uniform emission across the entire flake area, indicating a high degree of crystallinity of the material. This work provides new insight into the synthesis of TMDs with charge carrier control, to pave the way towards post-silicon electronics.

Transition Metal Dichalcogenide Dimer Nanoantennas for Tailored Light-Matter Interactions.

Transition metal dichalcogenides have emerged as promising materials for nanophotonic resonators because of their large refractive index, low absorption within a large portion of the visible spectrum, and compatibility with a wide range of substrates. Herein, we use these properties to fabricate WS2 double-pillar nanoantennas in a variety of geometries enabled by the anisotropy in the crystal structure. Using dark-field spectroscopy, we reveal multiple Mie resonances, to which we couple WSe2 monolayer photoluminescence and achieve Purcell enhancement and an increased fluorescence by factors up to 240 for dimer gaps of 150 nm. We introduce postfabrication atomic force microscope repositioning and rotation of dimer nanoantennas, achieving gaps as small as 10 ± 5 nm, which enables a host of potential applications, including strong Purcell enhancement of single-photon emitters and optical trapping, which we study in simulations. Our findings highlight the advantages of using transition metal dichalcogenides for nanophotonics by exploring applications enabled by their properties.

Bright single photon emitters with enhanced quantum efficiency in a two-dimensional semiconductor coupled with dielectric nano-antennas.

Single photon emitters in atomically-thin semiconductors can be deterministically positioned using strain induced by underlying nano-structures. Here, we couple monolayer WSe2 to high-refractive-index gallium phosphide dielectric nano-antennas providing both optical enhancement and monolayer deformation. For single photon emitters formed on such nano-antennas, we find very low (femto-Joule) saturation pulse energies and up to 104 times brighter photoluminescence than in WSe2 placed on low-refractive-index SiO2 pillars. We show that the key to these observations is the increase on average by a factor of 5 of the quantum efficiency of the emitters coupled to the nano-antennas. This further allows us to gain new insights into their photoluminescence dynamics, revealing the roles of the dark exciton reservoir and Auger processes. We also find that the coherence time of such emitters is limited by intrinsic dephasing processes. Our work establishes dielectric nano-antennas as a platform for high-efficiency quantum light generation in monolayer semiconductors.

Emergence of Highly Linearly Polarized Interlayer Exciton Emission in MoSe2/WSe2 Heterobilayers with Transfer-Induced Layer Corrugation.

The availability of accessible fabrication methods based on deterministic transfer of atomically thin crystals has been essential for the rapid expansion of research into van der Waals heterostructures. An inherent issue of these techniques is the deformation of the polymer carrier film during the transfer, which can lead to highly nonuniform strain induced in the transferred two-dimensional material. Here, using a combination of optical spectroscopy, atomic force, and Kelvin probe force microscopy, we show that the presence of nanometer scale wrinkles formed due to transfer-induced stress relaxation can lead to strong changes in the optical properties of MoSe2/WSe2 heterostructures and the emergence of linearly polarized interlayer exciton photoluminescence. We attribute these changes to local breaking of crystal symmetry in the nanowrinkles, which act as efficient accumulation centers for interlayer excitons due to the strain-induced interlayer band gap reduction. Surface potential images of the rippled heterobilayer samples acquired using Kelvin probe force microscopy reveal variations of the local work function consistent with strain-induced band gap modulation, while the potential offset observed at the ridges of the wrinkles shows a clear correlation with the value of the tensile strain estimated from the wrinkle geometry. Our findings highlight the important role of the residual strain in defining optical properties of van der Waals heterostructures and suggest effective approaches for interlayer exciton manipulation by local strain engineering.

Publisher Correction: Interlayer excitons: Moiré or not.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

Nonlinear polaritons in a monolayer semiconductor coupled to optical bound states in the continuum.

Optical bound states in the continuum (BICs) provide a way to engineer very narrow resonances in photonic crystals. The extended interaction time in these systems is particularly promising for the enhancement of nonlinear optical processes and the development of the next generation of active optical devices. However, the achievable interaction strength is limited by the purely photonic character of optical BICs. Here, we mix the optical BIC in a photonic crystal slab with excitons in the atomically thin semiconductor MoSe2 to form nonlinear exciton-polaritons with a Rabi splitting of 27 meV, exhibiting large interaction-induced spectral blueshifts. The asymptotic BIC-like suppression of polariton radiation into the far field toward the BIC wavevector, in combination with effective reduction of the excitonic disorder through motional narrowing, results in small polariton linewidths below 3 meV. Together with a strongly wavevector-dependent Q-factor, this provides for the enhancement and control of polariton-polariton interactions and the resulting nonlinear optical effects, paving the way toward tuneable BIC-based polaritonic devices for sensing, lasing, and nonlinear optics.

Manipulating molecules with strong coupling: harvesting triplet excitons in organic exciton microcavities.

Exciton-polaritons are quasiparticles with mixed photon and exciton character that demonstrate rich quantum phenomena, novel optoelectronic devices and the potential to modify chemical properties of materials. Organic materials are of current interest as active materials for their ability to sustain exciton-polaritons even at room temperature. However, within organic optoelectronic devices, it is often the 'dark' spin-1 triplet excitons that dominate operation. These triplets have been largely ignored in treatments of polaritons, which instead only consider the role of states that directly and strongly interact with light. Here we demonstrate that these 'dark' states can also play a major role in polariton dynamics, observing polariton population transferred directly from the triplet manifold via triplet-triplet annihilation. The process leads to polariton emission that is longer-lived (>µs) even than exciton emission in bare films. This enhancement is directly linked to spin-2 triplet-pair states, which are formed in films and microcavities by singlet fission or triplet-triplet annihilation. Such high-spin multiexciton states are generally non-emissive and cannot directly couple to light, yet the formation of polaritons creates for them entirely new radiative decay pathways. This is possible due to weak mixing between singlet and triplet-pair manifolds, which - in the strong coupling regime - enables direct interaction between the bright polariton states and those that are formally non-emissive. Our observations offer the enticing possibility of using polaritons to harvest or manipulate population from states that are formally dark.

Author Correction: Resonantly hybridized excitons in moiré superlattices in van der Waals heterostructures.

An Amendment to this paper has been published and can be accessed via a link at the top of the paper.

Resonantly hybridized excitons in moiré superlattices in van der Waals heterostructures.

Atomically thin layers of two-dimensional materials can be assembled in vertical stacks that are held together by relatively weak van der Waals forces, enabling coupling between monolayer crystals with incommensurate lattices and arbitrary mutual rotation1,2. Consequently, an overarching periodicity emerges in the local atomic registry of the constituent crystal structures, which is known as a moiré superlattice3. In graphene/hexagonal boron nitride structures4, the presence of a moiré superlattice can lead to the observation of electronic minibands5-7, whereas in twisted graphene bilayers its effects are enhanced by interlayer resonant conditions, resulting in a superconductor-insulator transition at magic twist angles8. Here, using semiconducting heterostructures assembled from incommensurate molybdenum diselenide (MoSe2) and tungsten disulfide (WS2) monolayers, we demonstrate that excitonic bands can hybridize, resulting in a resonant enhancement of moiré superlattice effects. MoSe2 and WS2 were chosen for the near-degeneracy of their conduction-band edges, in order to promote the hybridization of intra- and interlayer excitons. Hybridization manifests through a pronounced exciton energy shift as a periodic function of the interlayer rotation angle, which occurs as hybridized excitons are formed by holes that reside in MoSe2 binding to a twist-dependent superposition of electron states in the adjacent monolayers. For heterostructures in which the monolayer pairs are nearly aligned, resonant mixing of the electron states leads to pronounced effects of the geometrical moiré pattern of the heterostructure on the dispersion and optical spectra of the hybridized excitons. Our findings underpin strategies for band-structure engineering in semiconductor devices based on van der Waals heterostructures9.

Strong-coupling of WSe2 in ultra-compact plasmonic nanocavities at room temperature.

Strong coupling of monolayer metal dichalcogenide semiconductors with light offers encouraging prospects for realistic exciton devices at room temperature. However, the nature of this coupling depends extremely sensitively on the optical confinement and the orientation of electronic dipoles and fields. Here, we show how plasmon strong coupling can be achieved in compact, robust, and easily assembled gold nano-gap resonators at room temperature. We prove that strong-coupling is impossible with monolayers due to the large exciton coherence size, but resolve clear anti-crossings for greater than 7 layer devices with Rabi splittings exceeding 135 meV. We show that such structures improve on prospects for nonlinear exciton functionalities by at least 104, while retaining quantum efficiencies above 50%, and demonstrate evidence for superlinear light emission.

On-Chip Waveguide Coupling of a Layered Semiconductor Single-Photon Source.

Fully integrated quantum technology based on photons is in the focus of current research, because of its immense potential concerning performance and scalability. Ideally, the single-photon sources, the processing units, and the photon detectors are all combined on a single chip. Impressive progress has been made for on-chip quantum circuits and on-chip single-photon detection. In contrast, nonclassical light is commonly coupled onto the photonic chip from the outside, because presently only few integrated single-photon sources exist. Here, we present waveguide-coupled single-photon emitters in the layered semiconductor gallium selenide as promising on-chip sources. GaSe crystals with a thickness below 100 nm are placed on Si3N4 rib or slot waveguides, resulting in a modified mode structure efficient for light coupling. Using optical excitation from within the Si3N4 waveguide, we find nonclassicality of generated photons routed on the photonic chip. Thus, our work provides an easy-to-implement and robust light source for integrated quantum technology.

Imaging of Interlayer Coupling in van der Waals Heterostructures Using a Bright-Field Optical Microscope.

Vertically stacked atomic layers from different layered crystals can be held together by van der Waals forces, which can be used for building novel heterostructures, offering a platform for developing a new generation of atomically thin, transparent, and flexible devices. The performance of these devices is critically dependent on the layer thickness and the interlayer electronic coupling, influencing the hybridization of the electronic states as well as charge and energy transfer between the layers. The electronic coupling is affected by the relative orientation of the layers as well as by the cleanliness of their interfaces. Here, we demonstrate an efficient method for monitoring interlayer coupling in heterostructures made from transition metal dichalcogenides using photoluminescence imaging in a bright-field optical microscope. The color and brightness in such images are used here to identify mono- and few-layer crystals and to track changes in the interlayer coupling and the emergence of interlayer excitons after thermal annealing in heterobilayers composed of mechanically exfoliated flakes and as a function of the twist angle in atomic layers grown by chemical vapor deposition. Material and crystal thickness sensitivity of the presented imaging technique makes it a powerful tool for characterization of van der Waals heterostructures assembled by a wide variety of methods, using combinations of materials obtained through mechanical or chemical exfoliation and crystal growth.

All-optical formation of coherent dark states of silicon-vacancy spins in diamond.

Spin impurities in diamond can be versatile tools for a wide range of solid-state-based quantum technologies, but finding spin impurities that offer sufficient quality in both photonic and spin properties remains a challenge for this pursuit. The silicon-vacancy center has recently attracted much interest because of its spin-accessible optical transitions and the quality of its optical spectrum. Complementing these properties, spin coherence is essential for the suitability of this center as a spin-photon quantum interface. Here, we report all-optical generation of coherent superpositions of spin states in the ground state of a negatively charged silicon-vacancy center using coherent population trapping. Our measurements reveal a characteristic spin coherence time, T2*, exceeding 45 nanoseconds at 4 K. We further investigate the role of phonon-mediated coupling between orbital states as a source of irreversible decoherence. Our results indicate the feasibility of all-optical coherent control of silicon-vacancy spins using ultrafast laser pulses.