Transient Optical Modulation in Vanadium and Selenium Doped MoS₂ by Carrier–Carrier and Carrier–Phonon Interactions

Abstract Doping and alloying induce defect states in atomically thin transition metal dichalcogenides (TMDCs), leading to strong carrier–phonon interactions. The robust excitonic behavior of these layered materials can be modified by injecting a high density of charge carriers. However, comprehending the influence of carrier–phonon and carrier–carrier interactions on the optical properties of 2D materials is crucial for their optoelectronic and photonic applications. Here, transient absorption (TA) spectroscopy is employed to demonstrate the modulation of the transient optical behavior of TMDCs through doping and excitation near Mott density. The TA spectra reveal broadening attributed to carrier–carrier and carrier–phonon interactions, with the broadening being particularly pronounced in vanadium (V) doped TMDCs due to the hybridization of defect and exciton transitions. Analysis of TA kinetics suggests the involvement of various carrier species in the carrier dynamics of TMDCs, with the influence of mid‐gap carriers dominating at higher excitation densities. Nonetheless, the presence of strong carrier–phonon coupling in V‐doped TMDCs is demonstrated by temperature‐dependent Raman and photoluminescence spectroscopy. The results reveal that the enhanced coupling between acoustic phonons and carriers can lead to multiphonon emission. The findings of this study hold promise for controlling the optical response of TMDCs in ultrafast optoelectronic applications.