Measurement of local optomechanical properties of a direct bandgap 2D semiconductor

Strain engineering is a powerful tool for tuning physical properties of 2D materials, including monolayer transition metal dichalcogenides (TMDs)—direct bandgap semiconductors with strong excitonic response. Deformation of TMD monolayers allows inducing modulation of exciton potential and, ultimately, creating single-photon emitters at desired positions. The performance of such systems is critically dependent on the exciton energy profile and maximum possible exciton energy shift that can be achieved under local impact until the monolayer rupture. Here, we study the evolution of two-dimensional exciton energy profile induced in a MoSe2 monolayer under incremental local indentation until the rupture. We controllably stress the flake with an atomic force microscope tip and perform in situ spatiospectral mapping of the excitonic photoluminescence in the vicinity of the indentation point. In order to accurately fit the experimental data, we combine numerical simulations with a simple model of strain-induced modification of the local excitonic response and carefully account for the optical resolution of the setup. This allows us to extract deformation, strain, and exciton energy profiles obtained at each indentation depth. The maximum exciton energy shift induced by local deformation achieved at 300 nm indentation reaches the value of 36.5 meV and corresponds to 1.15% strain of the monolayer. Our approach is a powerful tool for in situ characterization of local optomechanical properties of 2D direct bandgap semiconductors with strong excitonic response

Spin-valley dynamics in alloy-based transition metal dichalcogenide heterobilayers

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 − xWxSe2/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