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  1. Abstract

    Localized states in two-dimensional (2D) transition metal dichalcogenides (TMDCs) have been the subject of intense study, driven by potential applications in quantum information science. Despite the rapidly growing knowledge surrounding these emitters, their microscopic nature is still not fully understood, limiting their production and application. Motivated by this challenge, and by recent theoretical and experimental evidence showing that nanowrinkles generate strain-localized room-temperature emitters, we demonstrate a method to intentionally induce wrinkles with collections of stressors, showing that long-range wrinkle direction and position are controllable with patterned array design. Nano-photoluminescence (nano-PL) imaging combined with detailed strain modeling based on measured wrinkle topography establishes a correlation between wrinkle properties, particularly shear strain, and localized exciton emission. Beyond the array-induced wrinkles, nano-PL spatial maps further reveal that the strain environment around individual stressors is heterogeneous due to the presence of fine wrinkles that are less deterministic. At cryogenic temperatures, antibunched emission is observed, confirming that the nanocone-induced strain is sufficiently large for the formation of quantum emitters. At 300 K, detailed nanoscale hyperspectral images uncover a wide range of low-energy emission peaks originating from the fine wrinkles, and show that the states can be tightly confined to regions <10 nm, even in ambient conditions. These results establish a promising potential route towards realizing room temperature quantum emission in 2D TMDC systems.

     
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  2. Abstract

    Chiral single photons are highly sought to enhance encoding capacities or enable propagation-dependent routing in nonreciprocal devices. Unfortunately, most semiconductor quantum emitters (QEs) produce only linear polarized photons unless external magnets are applied. Magnetic proximity coupling utilizing 2D ferromagnets promises to make bulky external fields obsolete. Here we directly grow Fe-doped MoS2(Fe:MoS2) via chemical vapor deposition that displays pronounced hard ferromagnetic properties even in monolayer form. This approach with monolayer ferromagnets enables full utilization of the strain from the pillar stressor to form QE in WSe2deterministically. The Fe:MoS2/WSe2heterostructures display strong hysteretic magneto-response and high-purity chiral single photons with a circular polarization degree of 92 ± 1% (74% average) without external magnetic fields. Furthermore, the chiral single photons are robust against uncontrolled twist-angle and external stray-fields. This ability to manipulate quantum states and transform linear polarized photons into high-purity chiral photons on-chip enables nonreciprocal device integration in quantum photonics.

     
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  3. Abstract

    Polar crystals can be driven into collective oscillations by optical fields tuned to precise resonance frequencies. As the amplitude of the excited phonon modes increases, novel processes scaling non-linearly with the applied fields begin to contribute to the dynamics of the atomic system. Here we show two such optical nonlinearities that are induced and enhanced by the strong phonon resonance in the van der Waals crystal hexagonal boron nitride (hBN). We predict and observe large sub-picosecond duration signals due to four-wave mixing (FWM) during resonant excitation. The resulting FWM signal allows for time-resolved observation of the crystal motion. In addition, we observe enhancements of third-harmonic generation with resonant pumping at the hBN transverse optical phonon. Phonon-induced nonlinear enhancements are also predicted to yield large increases in high-harmonic efficiencies beyond the third.

     
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  4. Collective excitations contain key information regarding the electronic order of the ground state of strongly correlated systems. Various collective modes in the spin and valley isospin channels of magic-angle graphene moiré bands have been alluded to by a series of recent experiments. However, a direct observation of collective excitations has been impossible due to the lack of a spin probe. Here we observe low-energy collective excitations in twisted bilayer graphene near the magic angle, using a resistively detected electron spin resonance technique. Two independent observations show that the generation and detection of microwave resonance relies on the strong correlations within the flat moiré energy band. First, the onset of the resonance response coincides with the spontaneous flavour polarization at moiré half-filling, but is absent in the isospin unpolarized density range. Second, we perform the same measurement on various systems that do not have flat bands and observe no indication of a resonance response in these samples. Our explanation is that the resonance response near the magic angle originates from Dirac revivals and the resulting isospin order. 
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    Free, publicly-accessible full text available August 1, 2024
  5. Abstract

    Exciton polaritons are quasiparticles of photons coupled strongly to bound electron-hole pairs, manifesting as an anti-crossing light dispersion near an exciton resonance. Highly anisotropic semiconductors with opposite-signed permittivities along different crystal axes are predicted to host exotic modes inside the anti-crossing called hyperbolic exciton polaritons (HEPs), which confine light subdiffractionally with enhanced density of states. Here, we show observational evidence of steady-state HEPs in the van der Waals magnet chromium sulfide bromide (CrSBr) using a cryogenic near-infrared near-field microscope. At low temperatures, in the magnetically-ordered state, anisotropic exciton resonances sharpen, driving the permittivity negative along one crystal axis and enabling HEP propagation. We characterize HEP momentum and losses in CrSBr, also demonstrating coupling to excitonic sidebands and enhancement by magnetic order: which boosts exciton spectral weight via wavefunction delocalization. Our findings open new pathways to nanoscale manipulation of excitons and light, including routes to magnetic, nonlocal, and quantum polaritonics.

     
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  6. Abstract The bandwidth-tuned Wigner-Mott transition is an interaction-driven phase transition from a generalized Wigner crystal to a Fermi liquid. Because the transition is generally accompanied by both magnetic and charge-order instabilities, it remains unclear if a continuous Wigner-Mott transition exists. Here, we demonstrate bandwidth-tuned metal-insulator transitions at fixed fractional fillings of a MoSe 2 /WS 2 moiré superlattice. The bandwidth is controlled by an out-of-plane electric field. The dielectric response is probed optically with the 2s exciton in a remote WSe 2 sensor layer. The exciton spectral weight is negligible for the metallic state with a large negative dielectric constant. It continuously vanishes when the transition is approached from the insulating side, corresponding to a diverging dielectric constant or a ‘dielectric catastrophe’ driven by the critical charge dynamics near the transition. Our results support the scenario of continuous Wigner-Mott transitions in two-dimensional triangular lattices and stimulate future explorations of exotic quantum phases in their vicinities. 
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