Unusually large exciton binding energy in multilayered 2H-MoTe2

Abstract

Although large exciton binding energies of typically 0.6-1.0 eV are observed for monolayer transition metal dichalcogenides (TMDs) owing to strong Coulomb interaction, multilayered TMDs yield relatively low exciton binding energies owing to increased dielectric screening. Recently, the ideal carrier-multiplication threshold energy of twice the bandgap has been realized in multilayered semiconducting 2H-MoTe₂ with a conversion efficiency of 99%, which suggests strong Coulomb interaction. However, the origin of strong Coulomb interaction in multilayered 2H-MoTe₂, including the exciton binding energy, has not been elucidated to date. In this study, unusually large exciton binding energy is observed through optical spectroscopy conducted on CVD-grown 2H-MoTe₂. To extract exciton binding energy, the optical conductivity is fitted using the Lorentz model to describe the exciton peaks and the Tauc-Lorentz model to describe the indirect and direct bandgaps. The exciton binding energy of 4 nm thick multilayered 2H-MoTe₂ is approximately 300 meV, which is unusually large by one order of magnitude when compared with other multilayered TMD semiconductors such as 2H-MoS₂ or 2H-MoSe₂. This finding is interpreted in terms of small exciton radius based on the 2D Rydberg model. The exciton radius of multilayered 2H-MoTe₂ resembles that of monolayer 2H-MoTe₂, whereas those of multilayered 2H-MoS₂ and 2H-MoSe₂ are large when compared with monolayer 2H-MoS₂ and 2H-MoSe₂. From the large exciton binding energy in multilayered 2H-MoTe₂, it is expected to realize the future applications such as room-temperature and high-temperature polariton lasing.