Excitonic properties of semiconducting monolayer and bilayer MoTe2

MoTe2 belongs to the semiconducting transition-metal dichalcogenide family with certain properties differing from the other well-studied members (Mo, W)(S, Se)(2). The optical band gap is in the near-infrared region, and both monolayers and bilayers may have a direct optical band gap. We first simulate the single-particle band structure of both monolayer and bilayer MoTe2 with density-functional-theory-GW calculations. We find a direct (indirect) electronic band gap for the monolayer (bilayer). By solving in addition the Be the-Salpeter equation, we find similar energies for the direct exciton transitions in monolayers and bilayers. We then study the optical properties by means of photoluminescence (PL) excitation, reflectivity, time-resolved PL, and power-dependent PL spectroscopy. With differential reflectivity, we find a similar oscillator strength for the optical transition observed in PL in both monolayers and bilayers suggesting a direct transition in both cases. We identify the same energy for the B-exciton state in the monolayer and the bilayer. Following circularly polarized excitation, we do not find any exciton polarization for a large range of excitation energies. At low temperatures (T = 10 K), we measure similar PL decay times on the order of 4 ps for both monolayer and bilayer excitons with a slightly longer one for the bilayer. Finally, we observe a reduction of the exciton-exciton annihilation contribution to the nonradiative recombination in bilayers.