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Exciton-polariton dynamics in 2D materials have garnered substantial attention across diverse scientific domains for fundamental research with potential applications in optoelectronics. However, practical implementation has been hindered by the challenge of maintaining stable and long-range polariton propagation. Here, we present an innovative material platform featuring extensive monolayer WS 2 /Al 2 O 3 superlattices (a square with a length of >0.5 cm) coupled to a waveguide mode designed to host exciton-polaritons with operation at room temperature. Time-resolved transient absorption spectra show picosecond nonlinear energy transfer phenomena between upper and lower polariton states, clarifying the dynamic behavior within this quantum realm. In addition, we observed population inversion behavior between the two polariton states that facilitate potential avenues for creating polariton-based ultrafast modulators and switches. This research not only advances our fundamental understanding of polariton dynamics but also promotes the development of innovative technologies that harness these fascinating quantum phenomena.

Polaritons in layered materials (LMs) are a promising platform to manipulate and control light at the nanometer scale. Thus, the observation of polaritons in wafer-scale LMs is critically important for the development of industrially relevant nanophotonics and optoelectronics applications. In this work, phonon polaritons (PhPs) in wafer-scale multilayer hexagonal boron nitride (hBN) grown by chemical vapor deposition are reported. By infrared nanoimaging, the PhPs are visualized, and PhP lifetimes of ≈0.6 ps are measured, comparable to that of micromechanically exfoliated multilayer hBN. Further, PhP nanoresonators are demonstrated. Their quality factors of ≈50 are about 0.7 times that of state-of-the-art devices based on exfoliated hBN. These results can enable PhP-based surface-enhanced infrared spectroscopy (e.g., for gas sensing) and infrared photodetector applications., (© 2023 Wiley-VCH GmbH.)

Atomically thin transition metal dichalcogenides (TMDs), a subclass of two-dimensional (2D) layered materials, have numerous fascinating properties that make them a promising platform for photonic and optoelectronic devices. In particular, excited state transport by TMDs is important in energy harvesting and photonic switching; however, long-range transport in TMDs is challenging due to the lack of availability of large area films. Whereas most previous studies have focused on small, exfoliated monolayer flakes, in this work we demonstrate metal-organic chemical vapor deposition grown centimeter-scale monolayers of WS 2 that support polariton propagation lengths of up to 60 μm. The polaritons form through the strong coupling of excitons with Bloch surface waves (BSWs) supported by all-dielectric photonic structures. We observe that the propagation length increases with the number of dielectric pairs due to the increased quality factor of the supporting distributed Bragg reflector. Furthermore, a longer propagation length is observed as the guided or BSW content of the polariton is increased. Our results provide a practical approach for the systematic engineering of long-range energy transport mediated by exciton-polaritons in TMD layers. Along with the accessibility of large area TMDs, our work enables applications for practical TMD-based polaritonic devices that operate at room temperature.

Van der Waals heterostructures (vdWHSs) enable the fabrication of complex electronic devices based on two-dimensional (2D) materials. Ideally, these vdWHSs should be fabricated in a scalable and repeatable way and only in the specific areas of the substrate to lower the number of technological operations inducing defects and impurities. Here, we present a method of selective fabrication of vdWHSs via chemical vapor deposition by electron-beam (EB) irradiation. We distinguish two growth modes: positive (2D materials nucleate on the irradiated regions) on graphene and tungsten disulfide (WS 2 ) substrates, and negative (2D materials do not nucleate on the irradiated regions) on the graphene substrate. The growth mode is controlled by limiting the air exposure of the irradiated substrate and the time between irradiation and growth. We conducted Raman mapping, Kelvin-probe force microscopy, X-ray photoelectron spectroscopy, and density-functional theory modeling studies to investigate the selective growth mechanism. We conclude that the selective growth is explained by the competition of three effects: EB-induced defects, adsorption of carbon species, and electrostatic interaction. The method here is a critical step toward the industry-scale fabrication of 2D-materials-based devices.

Two-dimensional (2D) crystals have renewed opportunities in design and assembly of artificial lattices without the constraints of epitaxy. However, the lack of thickness control in exfoliated van der Waals (vdW) layers prevents realization of repeat units with high fidelity. Recent availability of uniform, wafer-scale samples permits engineering of both electronic and optical dispersions in stacks of disparate 2D layers with multiple repeating units. Here we present optical dispersion engineering in a superlattice structure comprising alternating layers of 2D excitonic chalcogenides and dielectric insulators. By carefully designing the unit cell parameters, we demonstrate greater than 90% narrow band absorption in less than 4 nm of active layer excitonic absorber medium at room temperature, concurrently with enhanced photoluminescence in square-centimetre samples. These superlattices show evidence of strong light-matter coupling and exciton-polariton formation with geometry-tuneable coupling constants. Our results demonstrate proof of concept structures with engineered optical properties and pave the way for a broad class of scalable, designer optical metamaterials from atomically thin layers., (© 2021. The Author(s), under exclusive licence to Springer Nature Limited.)