Defect-mediated exciton localization and relaxation in CVD-grown monolayer MoS2

Abstract Defects in CVD-grown monolayer MoS₂ are unavoidable and provide a powerful approach to create single-photon emitters and quantum information systems through localizing excitons. However, insight into A⁻ trion and B/C exciton localization in monolayer MoS₂ remains elusive. Here, we investigate defect-mediated A⁻ trion and B/C exciton localization and relaxation in CVD-grown monolayer MoS₂ samples via transient absorption spectra. The localization rate of A⁻ trions exhibits five times faster than B excitons, which is attributed to the distinctions in Bohr radius, diffusion rate and multi-phonon emission. Furthermore, we obtain unambiguous experimental evidence for free C exciton localization and the direct excitation of localized C excitons. Varying gap energy at the band-nesting region revealed by first-principles calculations explains anomalous dependence of localized C exciton energy on delay time. We also find that the rapid dissociation of localized C excitons features a short characteristic time of ~0.14 ps, while the measured relaxation time is much longer. Our results provide a comprehensive picture of the defect-mediated excitonic relaxation and localization dynamics in monolayer MoS₂.