Imaging dynamic exciton interactions and coupling in transition metal dichalcogenides.

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 MoSe2 monolayer and identify both promising and unfavorable areas for quantum information applications. We, furthermore, apply the same technique to a MoSe2/WSe2 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.

Nanoscale Trapping of Interlayer Excitons in a 2D Semiconductor Heterostructure.

For quantum technologies based on single excitons and spins, the deterministic placement and control of a single exciton is a longstanding goal. MoSe2-WSe2 heterostructures host spatially indirect interlayer excitons (IXs) that exhibit highly tunable energies and unique spin-valley physics, making them promising candidates for quantum information processing. Previous IX trapping approaches involving moiré superlattices and nanopillars do not meet the quantum technology requirements of deterministic placement and energy tunability. Here, we use a nanopatterned graphene gate to create a sharply varying electric field in close proximity to a MoSe2-WSe2 heterostructure. The dipole interaction between the IX and the electric field creates an ∼20 nm trap. The trapped IXs show the predicted electric-field-dependent energy, saturation at low excitation power, and increased lifetime, all signatures of strong spatial confinement. The demonstrated architecture is a crucial step toward the deterministic trapping of single IXs, which has broad applications to scalable quantum technologies.

Macroscopic transition metal dichalcogenides monolayers with uniformly high optical quality.

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.

2D semiconductor nonlinear plasmonic modulators.

A plasmonic modulator is a device that controls the amplitude or phase of propagating plasmons. In a pure plasmonic modulator, the presence or absence of a plasmonic pump wave controls the amplitude of a plasmonic probe wave through a channel. This control has to be mediated by an interaction between disparate plasmonic waves, typically requiring the integration of a nonlinear material. In this work, we demonstrate a 2D semiconductor nonlinear plasmonic modulator based on a WSe2 monolayer integrated on top of a lithographically defined metallic waveguide. We utilize the strong interaction between the surface plasmon polaritons (SPPs) and excitons in the WSe2 to give a 73 % change in transmission through the device. We demonstrate control of the propagating SPPs using both optical and SPP pumps, realizing a 2D semiconductor nonlinear plasmonic modulator, with an ultrafast response time of 290 fs.