Localized Gradual Photomediated Brightness and Lifetime Increase of Superacid-Treated Monolayer MoS₂

Monolayer semiconducting transition-metal dichalcogenides (S-TMDs) have been extensively studied as materials for next-generation optoelectronic devices due to their direct band gap and high exciton binding energy at room temperature. Under a superacid treatment of bis(trifluoromethane)sulfonimide (TFSI), sulfur-based TMDs such as MoS₂ can emit strong photoluminescence (PL) with a photoluminescence quantum yield (PLQY) approaching unity. However, the magnitude of PL enhancement varies by more than 2 orders of magnitude in published reports. A major culprit behind the discrepancy is sulfur-based TMD's sensitivity to above-bandgap photostimulation. Here, we present a detailed study of how TFSI-treated MoS₂ reacts to photostimulation with increasing PL occurring hours after continuous or pulsed laser exposure. The PL of TFSI-treated MoS₂ is enhanced up to 74 times its initial intensity after 5 h of continuous exposure to 532 nm laser light. Photostimulation also enhances the PL of untreated MoS₂ but with a much smaller enhancement. Caution should be taken when probing MoS₂ PL spectra, as above-bandgap light can alter the resulting intensity and peak wavelength of the emission over time. The presence of air is verified to play a key role in the photostimulated enhancement effect. Additionally, the rise of PL intensity is mirrored by an increase in measured carrier lifetime of up to ∼400 ps, consistent with the suppression of nonradiative pathways. This work demonstrates why variations in PL intensity are observed across samples and provides an understanding of the changes in carrier lifetimes to better engineer next-generation optoelectronic devices.