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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.

 

Transient absorption spectroscopy is a powerful tool to monitor the out-of-equilibrium optical response of photoexcited semiconductors. When this method is applied to two-dimensional semiconductors deposited on different substrates, the excited state optical properties are inferred from the pump-induced changes in the transmission/reflection of the probe,i.e., ΔT/Tor ΔR/R. Transient optical spectra are often interpreted as the manifestation of the intrinsic optical response of the monolayer, including effects such as the reduction of the exciton oscillator strength, electron-phonon coupling or many-body interactions like bandgap renormalization, trion or biexciton formation. Here we scrutinize the assumption that one can determine the non-equilibrium optical response of the TMD without accounting for the substrate used in the experiment. We systematically investigate the effect of the substrate on the broadband transient optical response of monolayer MoS₂(1L-MoS₂) by measuring ΔT/Tand ΔR/Rwith different excitation photon energies. Employing the boundary conditions given by the Fresnel equations, we analyze the transient transmission/reflection spectra across the main excitonic resonances of 1L-MoS₂. We show that pure interference effects induced by the different substrates explain the substantial differences (i.e., intensity, peak energy and exciton linewidth) observed in the transient spectra of the same monolayer. We thus demonstrate that the substrate strongly affects the magnitude of the exciton energy shift and the change of the oscillator strength in the transient optical spectra. By highlighting the key role played by the substrate, our results set the stage for a unified interpretation of the transient response of optoelectronic devices based on a broad class of TMDs.

 

Two-dimensional materials from layered van der Waals (vdW) crystals hold great promise for electronic, optoelectronic, and quantum devices, but technological implementation will be hampered by the lack of high-throughput techniques for exfoliating single-crystal monolayers with sufficient size and high quality. Here, we report a facile method to disassemble vdW single crystals layer by layer into monolayers with near-unity yield and with dimensions limited only by bulk crystal sizes. The macroscopic monolayers are comparable in quality to microscopic monolayers from conventional Scotch tape exfoliation. The monolayers can be assembled into macroscopic artificial structures, including transition metal dichalcogenide multilayers with broken inversion symmetry and substantially enhanced nonlinear optical response. This approach takes us one step closer to mass production of macroscopic monolayers and bulk-like artificial materials with controllable properties.