Monolayer transition metal dichalcogenides (TMDs) exhibit a remarkably strong Coulomb interaction that manifests in tightly bound excitons. Due to the complex electronic band structure exhibiting several spin-split valleys in the conduction and valence band, dark excitonic states can be formed. They are inaccessibly by light due to the required spin-flip and/or momentum transfer. The relative position of these dark states with respect to the optically accessible bright excitons has a crucial impact on the emission efficiency of these materials and thus on their technological potential. Based on the solution of the Wannier equation, we present the excitonic landscape of the most studied TMD materials including the spectral position of momentum-and spin-forbidden excitonic states. We show that the knowledge of the electronic dispersion does not allow to conclude about the nature of the material's band gap, since excitonic effects can give rise to significant changes. Furthermore, we reveal that an exponentially reduced photoluminescence yield does not necessarily reflect a transition from a direct to a non-direct gap material, but can be ascribed in most cases to a change of the relative spectral distance between bright and dark excitonic states.

Monolayer transition metal dichalcogenides (TMDs) are known to be highly sensitive to externally applied tensile or compressive strain. In particular, strain can be exploited as a tool to control the optical response of TMDs. However, the role of excitonic effects under strain has not been fully understood yet. Utilizing the strain-induced modification of electron and phonon dispersion obtained by first principle calculations, we present in this work microscopic insights into the strain-dependent optical response of various TMD materials. In particular, we explain recent experiments on the change of excitonic linewidths in strained TMDs and predict their behavior for tensile and compressive strain at low temperatures.

The rapidly increasing use of sensors throughout different research disciplines and the demand for more efficient devices with less power consumption depends critically on the emergence of new sensor materials and novel sensor concepts. Atomically thin transition metal dichalcogenides have a huge potential for sensor development within a wide range of applications. Their optimal surface-to-volume ratio combined with strong light–matter interaction results in a high sensitivity to changes in their surroundings. Here, we present a highly efficient sensing mechanism to detect molecules based on dark excitons in these materials. We show that the presence of molecules with a dipole moment transforms dark states into bright excitons, resulting in an additional pronounced peak in easy accessible optical spectra. This effect exhibits a huge potential for sensor applications, since it offers an unambiguous optical fingerprint for the detection of molecules—in contrast to common sensing schemes relying on small peak shifts and intensity changes.

Strain presents a straightforward tool to tune electronic properties of atomically thin nanomaterials that are highly sensitive to lattice deformations. While the influence of strain on the electronic band structure has been intensively studied, there are only a few works on its impact on optical properties of monolayer transition-metal dichalcogenides (TMDs). Combining microscopic theory based on Wannier and Bloch equations with nearest-neighbor tight-binding approximation, we present an analytical view on how uni-and biaxial strain influences the optical fingerprint of TMDs, including their excitonic binding energy, oscillator strength, optical selection rules, and the radiative broadening of excitonic resonances. We show that the impact of strain can be reduced to changes in the lattice structure (geometric effect) and in the orbital functions (overlap effect). In particular, we demonstrate that the valley-selective optical selection rule is softened in the case of uniaxial strain due to the introduced asymmetry in the lattice structure. Furthermore, we reveal a considerable increase of the radiative dephasing due to strain-induced changes in the optical matrix element and the excitonic wave functions.