Many-particle induced band renormalization processes in few- and mono-layer MoS₂

Abstract Band renormalization effects play a significant role for two-dimensional (2D) materials in designing a device structure and customizing their optoelectronic performance. However, the intrinsic physical mechanism about the influence of these effects cannot be revealed by general steady-state studies. Here, band renormalization effects in organic superacid treated monolayer MoS2, untreated monolayer MoS2 and few-layer MoS2 are quantitatively analyzed by using broadband femtosecond transient absorption spectroscopy. In comparison with the untreated monolayer, organic superacid treated monolayer MoS2 maintains a direct bandgap structure with two thirds of carriers populated at K valley, even when the initial exciton density is as high as 2.05 × 1014 cm−2 (under 400 nm excitations). While for untreated monolayer and few-layer MoS2, many-particle induced band renormalizations lead to a stronger imbalance for the carrier population between K and Q valleys in k space, and the former experiences a direct-to-indirect bandgap transition when the initial exciton density exceeds 5.0 × 1013 cm−2 (under 400 nm excitations). Those many-particle induced band renormalization processes further suggest a band-structure-controlling method in practical 2D devices.