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The unique optical properties of transition metal dichalcogenide (TMD) monolayers have attracted significant attention for both photonics applications and fundamental studies of low-dimensional systems. TMD monolayers of high optical quality, however, have been limited to micron-sized flakes produced by low-throughput and labour-intensive processes, whereas large-area films are often affected by surface defects and large inhomogeneity. Here we report a rapid and reliable method to synthesize macroscopic-scale TMD monolayers of uniform, high optical quality. Using 1-dodecanol encapsulation combined with gold-tape-assisted exfoliation, we obtain monolayers with lateral size > 1 mm, exhibiting exciton energy, linewidth, and quantum yield uniform over the whole area and close to those of high-quality micron-sized flakes. We tentatively associate the role of the two molecular encapsulating layers as isolating the TMD from the substrate and passivating the chalcogen vacancies, respectively. We demonstrate the utility of our encapsulated monolayers by scalable integration with an array of photonic crystal cavities, creating polariton arrays with enhanced light-matter coupling strength. This work provides a pathway to achieving high-quality two-dimensional materials over large areas, enabling research and technology development beyond individual micron-sized devices.

 

Exciton–polaritons have become an emerging platform for implementing non-Hermitian physics. The implementation commonly requires control of both the real and imaginary parts of the eigenmodes of the system. We present an experimental method to achieve this purpose using microcavities with sub-wavelength gratings as reflectors. The reflectivity and reflection phase of the grating can be changed by its geometric parameters, and they determine the energy and linewidth of the polariton modes. We demonstrate that this method allows a wide range of possible polariton energy and linewidth, suitable for implementing non-Hermitian polariton systems with coupled modes. 

Transition metal dichalcogenides (TMDs) are regarded as a possible material platform for quantum information science and related device applications. In TMD monolayers, the dephasing time and inhomogeneity are crucial parameters for any quantum information application. In TMD heterostructures, coupling strength and interlayer exciton lifetimes are also parameters of interest. However, many demonstrations in TMDs can only be realized at specific spots on the sample, presenting a challenge to the scalability of these applications. Here, using multi-dimensional coherent imaging spectroscopy, we shed light on the underlying physics—including dephasing, inhomogeneity, and strain—for a MoSe 2 monolayer and identify both promising and unfavorable areas for quantum information applications. We, furthermore, apply the same technique to a MoSe 2 /WSe 2 heterostructure. Despite the notable presence of strain and dielectric environment changes, coherent and incoherent coupling and interlayer exciton lifetimes are mostly robust across the sample. This uniformity is despite a significantly inhomogeneous interlayer exciton photoluminescence distribution that suggests a bad sample for device applications. This robustness strengthens the case for TMDs as a next-generation material platform in quantum information science and beyond. 

Semiconductor microcavities with a high quality‐factor are an important component for photonics research and technology, especially in the strong coupling regime. While van der Waals semiconductors have emerged as an interesting platform for photonics due to their strong exciton–photon interaction strength and engineering flexibility, incorporating them in photonic devices requires heterogeneous integration and remains a challenge. This study demonstrates a method to assemble high quality factor microcavities for van der Waals materials, using high reflectance top mirrors which, similar to van der Waals materials themselves, can be nondestructively and reliably peeled off the substrate and transferred onto the rest of the device. Microcavities are created with quality factors consistently above 2000 and up to 11000 ± 800; and the strong coupling regime is demonstrated. The method can be generalized to other types of heterogeneously integrated photonic structures and will facilitate research on cavity quantum electrodynamic and photonic systems using van der Waals materials.

 

Moiré lattices formed in twisted van der Waals bilayers provide a unique, tunable platform to realize coupled electron or exciton lattices unavailable before. While twist angle between the bilayer has been shown to be a critical parameter in engineering the moiré potential and enabling novel phenomena in electronic moiré systems, a systematic experimental study as a function of twist angle is still missing. Here we show that not only are moiré excitons robust in bilayers of even large twist angles, but also properties of the moiré excitons are dependant on, and controllable by, the moiré reciprocal lattice period via twist-angle tuning. From the twist-angle dependence, we furthermore obtain the effective mass of the interlayer excitons and the electron inter-layer tunneling strength, which are difficult to measure experimentally otherwise. These findings pave the way for understanding and engineering rich moiré-lattice induced phenomena in angle-twisted semiconductor van der Waals heterostructures.