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Monolayer transition metal dichalcogenides (TMDs) have the potential tounlock novel photonic and chemical technologies if their optoelectronicproperties can be understood and controlled. Yet, recent work has offeredcontradictory explanations for how TMD absorption spectra change with carrierconcentration, fluence, and time. Here, we test our hypothesis that the largebroadening and shifting of the strong band-edge features observed in opticalspectra arise from the formation of negative trions. We do this by fitting anab initio based, many-body model to our experimental electrochemical data. Ourapproach provides an excellent, global description of the potential-dependentlinear absorption data. We further leverage our model to demonstrate that trionformation explains the non-monotonic potential dependence of the transientabsorption spectra, including through photoinduced derivative lineshapes forthe trion peak. Our results motivate the continued development of theoreticalmethods to describe cutting-edge experiments in a physically transparent way.

Trion formation resolves observed peak shifts in the optical spectra of transition metal dichalcogenides