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Focused ion beam (FIB) is an effective tool for precise nanoscale fabrication. It has recently been employed to tailor defect engineering in functional nanomaterials such as two-dimensional transition metal dichalcogenides (TMDCs), providing desirable properties in TMDC-based optoelectronic devices. However, the damage caused by the FIB irradiation and milling process to these delicate, atomically thin materials, especially in extended areas beyond the FIB target, has not yet been fully characterised. Understanding the correlation between lateral ion beam effects and optical properties of 2D TMDCs is crucial in designing and fabricating high-performance optoelectronic devices. In this work, we investigate lateral damage in large-area monolayer WS2 caused by the gallium focused ion beam milling process. Three distinct zones away from the milling location are identified and characterised via steady-state photoluminescence (PL) and Raman spectroscopy. The emission in these three zones have different wavelengths and decay lifetimes. An unexpected bright ring-shaped emission around the milled location has also been revealed by time-resolved PL spectroscopy with high spatial resolution. Our findings open up new avenues for tailoring the optical properties of TMDCs by charge and defect engineering via focused ion beam lithography. Furthermore, our study provides evidence that while some localised damage is inevitable, distant destruction can be eliminated by reducing the ion beam current. It paves the way for the use of FIB to create nanostructures in 2D TMDCs, as well as the design and realisation of optoelectrical devices on a wafer scale.

Two-dimensional semiconducting transition metal dichalcogenides embedded in optical microcavities in the strong exciton-photon coupling regime may lead to promising applications in spin and valley addressable polaritonic logic gates and circuits. One significant obstacle for their realization is the inherent lack of scalability associated with the mechanical exfoliation commonly used for fabrication of two-dimensional materials and their heterostructures. Chemical vapor deposition offers an alternative scalable fabrication method for both monolayer semiconductors and other two-dimensional materials, such as hexagonal boron nitride. Observation of the strong light-matter coupling in chemical vapor grown transition metal dichalcogenides has been demonstrated so far in a handful of experiments with monolayer molybdenum disulfide and tungsten disulfide. Here we instead demonstrate the strong exciton-photon coupling in microcavities composed of large area transition metal dichalcogenide/hexagonal boron nitride heterostructures made from chemical vapor deposition grown molybdenum diselenide and tungsten diselenide encapsulated on one or both sides in continuous few-layer boron nitride films also grown by chemical vapor deposition. These transition metal dichalcogenide/hexagonal boron nitride heterostructures show high optical quality comparable with mechanically exfoliated samples, allowing operation in the strong coupling regime in a wide range of temperatures down to 4 Kelvin in tunable and monolithic microcavities, and demonstrating the possibility to successfully develop large area transition metal dichalcogenide based polariton devices.

Semiconducting ferromagnet-nonmagnet interfaces in van der Waals heterostructures present a unique opportunity to investigate magnetic proximity interactions dependent upon a multitude of phenomena including valley and layer pseudospins, moiré periodicity, or exceptionally strong Coulomb binding. Here, we report a charge-state dependency of the magnetic proximity effects between MoSe2 and CrBr3 in photoluminescence, whereby the valley polarization of the MoSe2 trion state conforms closely to the local CrBr3 magnetization, while the neutral exciton state remains insensitive to the ferromagnet. We attribute this to spin-dependent interlayer charge transfer occurring on timescales between the exciton and trion radiative lifetimes. Going further, we uncover by both the magneto-optical Kerr effect and photoluminescence a domain-like spatial topography of contrasting valley polarization, which we infer to be labyrinthine or otherwise highly intricate, with features smaller than 400 nm corresponding to our optical resolution. Our findings offer a unique insight into the interplay between short-lived valley excitons and spin-dependent interlayer tunneling, while also highlighting MoSe2 as a promising candidate to optically interface with exotic spin textures in van der Waals structures., One advantage of van der Waals materials is the ability to combine different materials in layers to form new heterostructures. Here, the authors investigate heterostructures of CrBr3 and MoSe2, and find that the ferromagnetism of CrBr3 enhances the valley dependent optical response of the MoSe2.

Van der Waals heterobilayers based on 2D transition metal dichalcogenides have been recently shown to support robust and long-lived valley polarization for potential valleytronic applications. However, the roles of the chemical composition and geometric alignment of the constituent layers in the underlying dynamics remain largely unexplored. Here we study spin–valley relaxation dynamics in heterobilayers with different structures and optical properties engineered via the use of alloyed monolayer semiconductors. Through a combination of time-resolved Kerr rotation spectroscopic measurements and theoretical modeling for Mo1 − x W x Se2/WSe2 samples with different chemical compositions and stacking angles, we uncover the contributions of the interlayer exciton recombination and charge carrier spin depolarization to the overall valley dynamics. We show that the corresponding decay rates can be tuned in a wide range in transitions from a misaligned to an aligned structure, and from a hetero- to a homo-bilayer. Our results provide insights into the microscopic spin–valley polarization mechanisms in van der Waals heterostructures for the development of future 2D valleytronic devices.