Role of weak interlayer coupling in ultrafast exciton-exciton annihilation in two-dimensional rhenium dichalcogenides

Strong interactions between excitons are a characteristic feature of two-dimensional (2D) semiconductors, determining important excitonic properties, such as exciton lifetime, coherence, and photon-emission efficiency. Rhenium disulfide ($\mathrm{Re}{\mathrm{S}}_{2}$), a member of the 2D transition-metal dichalcogenide (TMD) family, has recently attracted great attention due to its unique excitons that exhibit excellent polarization selectivity and coherence features. However, an in-depth understanding of exciton-exciton interactions in $\mathrm{Re}{\mathrm{S}}_{2}$ is still lacking. Here we used ultrafast pump-probe spectroscopy to study exciton-exciton interactions in monolayer (1L), bilayer (2L), and triple layer $\mathrm{Re}{\mathrm{S}}_{2}$. We directly measure the rate of exciton-exciton annihilation, a representative Auger-type interaction between excitons. It decreases with increasing layer number, as observed in other 2D TMDs. However, while other TMDs exhibit a sharp weakening of exciton-exciton annihilation between 1L and 2L, such behavior was not observed in $\mathrm{Re}{\mathrm{S}}_{2}$. We attribute this distinct feature in $\mathrm{Re}{\mathrm{S}}_{2}$ to the relatively weak interlayer coupling, which prohibits a substantial change in the electronic structure when the thickness varies. This work not only highlights the unique excitonic properties of $\mathrm{Re}{\mathrm{S}}_{2}$ but also provides novel insight into the thickness dependence of exciton-exciton interactions in 2D systems.