Recombination dynamics and manybody effect of excitons in large-area monolayer MoS₂ capped with (111) NiO epitaxial layer

Abstract

CVD grown monolayer MoS2 films on c-sapphire substrates are vacuum annealed and capped with (111) NiO epitaxial films using pulsed laser deposition (PLD) technique. Time, energy, and polarization resolved optical techniques are used to understand the effect of capping on the excitonic properties of the monolayer MoS2. It has been observed that trion contribution in the photoluminescence (PL) spectra increases after the capping, suggesting an enhancement of electron concentration in the conduction band. This has been attributed to the capping driven reduction of physisorbed air molecules from the sulphur vacancy (VS) sites. Note that the air molecules act as passivating agents for the VS-donors. Low temperature polarization resolved PL spectroscopy and ultrafast pump and probe transient absorption spectroscopy (TAS) show an increase of the biexcitonic population in the system after the encapsulation. The TAS study further reveals longer lifetime for both A and B excitons in capped samples implying a reduction of non-radiative recombination rate of the excitons after the capping. It has also been observed that in the capped samples, K/K′ valleys are populated with trions under sufficiently high pump powers. This has been attributed to the lower non-radiative recombination rates of the high energy photoexcited carriers and the faster transfer of either electrons or holes from the high energy pockets to the K/K′ valleys. The study further reveals different many-body effects in excitons and trions.