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The optical and electronic properties of multilayer transition metal dichalcogenides differ significantly from their monolayer counterparts due to interlayer interactions. The separation of individual layers can be tuned in a controlled way by applying pressure. Here, we use a diamond anvil cell to compress bilayers of 2H-MoS$_2$ in the gigapascal range. By measuring optical transmission spectra, we find that increasing pressure leads to a decrease in the energy splitting between the A and interlayer exciton. Comparing our experimental findings with ab initio calculations, we conclude that the observed changes are not due to the commonly assumed hydrostatic compression. This effect is attributed to the MoS$_2$ bilayer adhering to the diamond, which reduces in-plane compression. Moreover, we demonstrate that the distinct real-space distributions and resulting contributions from the valence band account for the different pressure dependencies of the inter- and intralayer excitons in compressed MoS$_2$ bilayers., 8 pages, 5 figures

Mechanical strain is a powerful tool to tune the optical and optoelectronic properties of atomically thin semiconductors. Inhomogeneous strain plays an important role in exciton funneling and the activation of single-photon emitters in 2D materials. Here, we create an inhomogeneous strain profile in a 2D semiconductor on a micrometer scale by a nanoimprint process. We present a nanoimprint setup, where a mold is used to apply pressure in a controlled way to a WS2 monolayer on a heated polymer layer. After printing, the strain created in the 2D semiconductor is verified by hyperspectral optical imaging. The developed nanoimprint technique is scalable and could be transferred to commercial nanoimprint machines., Comment: 8 pages, 6 figures

Understanding the ultrafast coupling and relaxation mechanisms between valleys in transition metal dichalcogenide semiconductors is of crucial interest for future valleytronic devices. Recent ultrafast pump-probe experiments showed an unintuitive significant bleaching at the excitonic $B$ transition after optical excitation of the energetically lower excitonic $A$ transition. Here, we present a possible microscopic explanation for this surprising effect. It is based on the joint action of exchange coupling and phonon-mediated thermalization into dark exciton states and does not involve a population of the B exciton. Our work demonstrates how intra- and intervalley coupling on a femtosecond timescale governs the optical valley response of 2D semiconductors.

Excitons dominate the optical properties of monolayer transition metal dichalcogenides (TMDs). Besides optically accessible bright exciton states, TMDs exhibit also a multitude of optically forbidden dark excitons. Here, we show that efficient exciton-phonon scattering couples bright and dark states and gives rise to an asymmetric excitonic line shape. The observed asymmetry can be traced back to phonon-induced sidebands that are accompanied by a polaron redshift. We present a joint theory-experiment study investigating the microscopic origin of these sidebands in different TMD materials taking into account intra- and intervalley scattering channels opened by optical and acoustic phonons. The gained insights contribute to a better understanding of the optical fingerprint of these technologically promising nanomaterials.